Onses 2015

www.MaterialsViews.
com
Printing
Mechanisms, Capabilities, and Applications of

High-Resolution Electrohydrodynamic Jet Printing
M. Serdar Onses,* Erick Sutanto, Placid M. Ferreira, Andrew G. Alleyne,
and John A. Rogers*
From the Contents
1. Introduction ........................................ 4238

This review gives an overview of techniques used for high-
2. Jet Formation and Important Factors..... 4240 resolution jet printing that rely on electrohydrodynamically
induced flows. Such methods enable the direct, additive
3. Modifications to the Electrohydrodynamic
patterning of materials with a resolution that can extend
Jet Printer ............................................ 4244
below 100 nm to provide unique opportunities not only
4. Other Printing Techniques that Exploit in scientific studies but also in a range of applications
Electrohydrodynamics and Related that includes printed electronics, tissue engineering,
Phenomena ......................................... 4247 and photonic and plasmonic devices. Following a brief
5. Materials and Resolution ..................... 4249 historical perspective, this review presents descriptions
of the underlying processes involved in the formation
6. Applications of E-jet Printing ................ 4251 of liquid cones and jets to establish critical factors in
7. Concluding Remarks ............................ 4262
the printing process. Different printing systems that
share similar principles are then described, along with
key advances that have been made in the last decade.
Capabilities in terms of printable materials and levels of
resolution are reviewed, with a strong emphasis on areas of
potential application.
small 2015, 11, No. 34, 4237–4266 © 2015 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim www.small-journal.com 4237
reviews
www.MaterialsViews.com
1. Introduction described above for additive methods and also benefits from
the tool infrastructure and knowledge developed in graphic
Techniques for fabricating structures on surfaces at micro- arts applications. Inkjet printing relies on the generation of
meter and nanometer length scales are critically important droplets at or near a nozzle aperture, followed by noncontact
to many existing and emerging technologies. The electronics deposition on a substrate with high spatial control. The drop-
industry has been the strongest driver for the development lets emerge from the nozzle due to the action of pressure
of lithographic methods as routes to dense integrated cir- pulses generated, most commonly, by thermal or piezoelectric
cuits that combine different materials and structures pat- means. Simultaneous control of the ejection and location of
terned at high resolution and with precise registration on the print head or substrate allows localized delivery of mate-
semiconductor wafers.[1] Here, size reductions translate into rials in layouts defined by the user. A wide variety of mate-
improved performance and increased integration density, rials can be patterned by inkjet printing, with demonstrated
thereby providing immense incentives to improve the fabri- applications in thin-film transistors, optical elements, organic
cation processes. Today, optical lithographic techniques can light-emitting diodes, photonic crystals, and DNA micro-
fabricate features with sizes and pitches well below 100 nm. arrays.[7–11] In some of these cases, inkjet printing technology
This miniaturization trend will likely continue to play a key is used in commercial manufacturing.
role in sustaining advances in the semiconductor industry.[2] A critical challenge for inkjet printing is in the practically
At the same time, developments in other areas of applica- achievable levels of resolution. The smallest volumes of liq-
tion and fields of research suggest important opportunities uids that can be readily ejected from thermal/piezoelectric
for alternative approaches that offer complementary capa- print heads are in the picoliter range, thereby establishing
bilities.[3] Key goals here involve expanding of the diver- minimum sizes of patterned features as ≈10 micrometers.[12]
sity of materials and substrates that can be used as well as Although future research might lead to improvements, the
the extending of manufacturing into the third, out-of-plane, resolution defined by the droplet size is typically further
dimension. For example, the chemical and thermal sensitivi- degraded by the spreading of droplets as they impact at
ties of organic and biological materials often prevent their high speeds onto the surfaces of target substrates. Besides
manipulation with fabrication approaches adapted from the resolution, these same issues also impose limitations on the
semiconductor industry. Additionally, flexible and stretchable thicknesses and spatial uniformities of the printed materials.
substrates have emerged as important platforms for devices Although these operational features are acceptable for many
that integrate with the human body. In these areas as well, uses, they preclude expanded adoption for applications that
conventional techniques have limited utility.[4] As a practical require fine resolution. Some improvements are possible by
concern, high capital costs of advanced lithographic equip- modifying the wetting properties of the substrates to mini-
ment further hinder its use in scientific research or in innova- mize spreading, by using inkjet printing in combination with
tive engineering. lithographically defined chemical and/or topographical pat-
Additive fabrication[5,6] approaches that rely on the local- terns, by self-aligning consecutive droplets to generate small
ized delivery of materials of interest directly to substrates gaps, and by engineering the inks to enhance flow from the
offer a solution to these challenges. This type of single-step nozzle and to minimize spreading on the substrate.[12–14] For
patterning process represents a dramatic simplification com- example, Sirringhaus and co-workers demonstrated the fab-
pared to widely used subtractive methods, which involve rication of printed transistors with channel lengths of 5 µm
repetitive deposition, patterning, and removal of materials. and several hundreds of nanometers by using lithographically
Additive operation also expands the selection of materials defined surface-energy patterns[15] and a de-wetting assisted
and substrates, simply because subtractive processes often
introduce contamination, chemical impurities, and other
Prof. M. S. Onses
forms of degradation, particularly for chemically, mechani- Department of Materials Science and Engineering
cally, or thermally fragile materials. Constraints associated Nanotechnology Research Center (ERNAM)
with the planarity of the substrate, typically imposed by the Erciyes University
limited depth of field in traditional lithographic techniques, Kayseri 38039, Turkey
are greatly relaxed in printing approaches, thereby allowing E-mail: onses@erciyes.edu.tr
the direct formation of flexible, stretchable, or curved devices. Dr. E. Sutanto
A further inherent advantage of additive methods is in 3D The Dow Chemical Company
Collegeville, PA 19426, USA
fabrication: the out-of-plane dimensions of the patterned
Prof. P. M. Ferreira, Prof. A. G. Alleyne
materials can be readily controlled and varied, to create
Department of Mechanical Science and Engineering
options in 3D patterning of materials and in applications University of Illinois at Urbana-Champaign
where thickness control is critical. The efficiency of mate- Urbana, IL 61801, USA
rials utilization also has advantages, ranging from minimized Prof. J. A. Rogers
waste streams to reduced costs of manufacturing. Departments of Materials Science and Engineering
Inkjet printing technology represents a highly established Beckman Institute and Frederick Seitz Materials Research Laboratory
and successful additive fabrication approach, originally devel- University of Illinois at Urbana-Champaign
oped for use in graphic arts. Inkjet printing has since been Urbana, IL 61801, USA
E-mail: jrogers@illinois.edu
adapted for applications in electronics, optics, bioengineering,
and other areas.[7–9] The process possesses all the strengths DOI: 10.1002/smll.201500593
4238 www.small-journal.com © 2015 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim small 2015, 11, No. 34, 4237–4266
self-alignment process,[16] respectively. These methods are

useful and, in some circumstances, they can generate sub- M. Serdar Onses received his BS in Chemical
micrometer features or gaps, but they do not allow the pat- Engineering and MS in Materials Science
terning of nanoscale features in arbitrary geometries solely and Engineering from the Istanbul Technical
defined by printing and they are not generally applicable to a University in 2006. From the University of
wide selection of materials and substrates. Wisconsin-Madison, he received a PhD in

Chemical Engineering in 2012. He is current-
Electrohydrodynamic jet (e-jet or EHD jet) printing
ly an assistant professor in the Department
offers a solution to the limited resolution of the conventional of Materials Science and Engineering and a
inkjet printer systems by exploiting different means to gen- co-director of the Nanotechnology Research
erate the droplets.[17] In thermal and piezeoelectric printers, Center at the Erciyes University. His interests
it becomes impractical to eject liquids from small nozzles due include conventional and unconventional
to the extremely high levels of pressure required to overcome nanofabrication approaches and self-assem-
bling materials.
the capillary forces. While pushing fluids from a fine capil-
lary is difficult, it is relatively easy to pull the liquids from Andrew G. Alleyne obtained a BS degree
the nozzle tip through the use of applied electric fields.[18] As in Aerospace Engineering from Princeton
shown in Figure 1, e-jet printing imposes a voltage between University in 1989 and an MS and PhD in
the nozzle and an opposing conducting support to initiate the Mechanical Engineering from the University
flow of inks from a nozzle via electrohydrodynamics. Typi- of California at Berkeley in 1992 and 1994.
He currently holds the Ralph M. and Cath-
cally, a back-pressure supply (e.g., syringe pump) delivers the
erine V. Fisher Professorship in Engineering
ink to the tips of the nozzles, whose inner diameters can be
at the University of Illinois at Urbana-
as small as ≈100 nm. In laboratory experiments, these nozzles Champaign. His research includes theoretical
are typically fabricated by pulling glass pipettes and coating and experimental automation and robotics
them with a thin layer of metal (e.g., Au), sometimes with fur- related to manufacturing systems, with a
ther chemical modifications to prevent wetting of the ink on focus on additive fabrication techniques for
the shaft of the pipette. The electric field leads to the accu- biomedical and electronic applications.
mulation of mobile ions in the ink to regions near the sur-

face of the pendant meniscus. Coulombic repulsion between John A. Rogers obtained BA and BS
these ions deforms the meniscus into a conical shape known degrees in chemistry and in physics from the
University of Texas, Austin, in 1989. From
as a Taylor cone.[19] At sufficiently high electric fields, drop-
MIT, he received MS degrees in physics and
lets eject from the cone as the electrostatic stresses overcome
in chemistry in 1992 and a PhD in physi-
the surface tension. Although mobile charges are required, cal chemistry in 1995. From 1995 to 1997,
experiments demonstrate that printing is possible even Rogers was a Junior Fellow in the Harvard
with liquids that have low electrical conductivities (10−13 to University Society of Fellows. He was with
10−3 Sm−1).[20] Here the ionic mobility of the ink also plays a Bell Laboratories from 1997 to 2002. He
critical role. The simultaneous coordination of the position of is currently Swanlund Chair Professor at
University of Illinois at Urbana/Champaign.
the substrate and the ejection of droplets enables patterned
His interests are unconventional materials
deposition of the ink materials. Three aspects of e-jet printing and patterning techniques for electronics
allow high resolution operation: i) the inner diameters of the and photonics.
nozzles are smaller than those used in inkjet printing; ii) elec-
trohydrodynamics generates droplets that can be significantly
smaller than this diameter; iii) focusing due to the distribu-
tion of electric field lines minimizes lateral variations in the and hence the delivery of biological molecules to desired
droplet placement. regions on a substrate. One of the earliest versions of e-jet
Although only recently extended for use in micro-/nanoprinting[24] demonstrated the formation of arrays of dots of
patterning, this concept for electric field-based printing has rhodamine B with diameters smaller than 5 µm. This resolu-
a long history. The electrostatic siphon recorder (1867), a tion followed from the use of pulsed voltages at magnitudes
tool to print telegraph messages on paper, relied on the smaller than those required to initiate electrospray. Aksay
flow of inks from a delivery tube held at a high potential and co-workers performed the first systematic studies[26,27] on
relative to a grounded substrate. Similarly, Taylor described the generation and placement of droplets using setups similar
processes for the ejection of droplets under electrohydrody- to the ones described above, with a demonstrated resolution
namic forces almost 50 years ago.[19] The formation of drop- of ≈10 micrometers, comparable to some of the best results
lets from a capillary remains an active area of research due achievable with thermal and piezoelectric inkjet techniques.
to the importance of this phenomenon in fields as diverse as Several reports[28–31] describe electrohydrodynamic printing
electrospray deposition and the dynamics of water droplets for graphic arts, scaffold fabrication, and conductive material
in thunderstorms.[21,22] Early reports[23–25] on the use of this patterning with minimum feature sizes greater than 10 µm.
phenomenon for the controlled deposition of materials drew Stark et al.[32] demonstrated that an array of dots with dia-
inspiration from electrospray techniques for the genera- meters as small as 1.37 µm could be obtained using voltage-
tion of charged droplets. In one example,[23] electrospraying modulated printing with 4 µm inner diameter nozzles. Rogers
through different types of masks localized the electric field and co-workers presented extensive demonstrations[17,33] of
reviews
specific sets of conditions are essential.

The second part of this section highlights
work in this area.
2.1. Experimental Studies on the Jet

Formation Process
The electrohydrodynamic effects that

cause liquids to eject from a nozzle tip,
as qualitatively described in the Intro-
Figure 1. High-resolution, electrohydrodynamic jet printing. a) Schematic illustration of a
duction Section, lead to different modes
printing system. Applying a voltage between a metal-coated nozzle (with inner diameters of jetting depending on parameters such
ranging from hundreds of nanometers to tens of micrometers) and a grounded substrate as the strength of the electric field (E)
leads to the flow of inks due to electrohydrodynamic forces. A computer-controlled stage and the flow rate (Q). The general phase
determines the location and geometry of the patterns. A syringe pump or pneumatic pressure diagram shown in Figure 2a qualitatively
controller provides the pressure necessary to fill the nozzle with fluid inks. b) A magnified shows these modes and their depend-
view of the nozzle–substrate configuration. The distance between the substrate and the
ence on these parameters. At low Q and
nozzle tip is typically in the range of tens of micrometers. Schematic illustration of the
printing of a line through the movement of the stage to the right. The inset shows a scanning E, droplets are jetted from the end of
electron microscope image of a nozzle. Adapted with permission.[17] Copyright 2007, Nature the nozzle by the help of gravitational
Publishing Group. forces in a mode called “dripping.”[35] A
slight increase in Q and/or E results in
a range of different materials and complex pattern geome- a pulsating liquid jet where streams of distinct droplets are
tries and layouts, with resolutions extending down to 100 nm, ejected by repeated Taylor cone formation and relaxation.
thereby establishing e-jet printing as a high-resolution pat- “Pulsating” jets can either be achieved at Q values that are
terning approach with capabilities in nanofabrication. smaller than the minimum flow rate (Qm) needed for the
This review covers recent progress in the development of steady cone-jet mode or at voltages smaller than a critical
advanced techniques for and applications of e-jet printing. In value of E when Q > Qm.[36] A further increase in the electric
Section 2 the droplet generation process is described, with field leads to a continuous stream of liquid from the nozzle,
separate subsections on experimental and modeling studies. often referred to as the “cone-jet mode,” because of the con-
Section 3 summarizes various modifications to the basic e-jet tinuous presence of the Taylor cone. The voltage at which the
printer design including multinozzle setups and desktop sys- transition occurs from pulsating to cone-jet mode is called
tems. Recently developed nanoprinting approaches that rely the Taylor, or critical, voltage, which depends on the prop-
on similar phenomena are covered in Section 4, with indi- erties of the ink and the applied back pressure.[37] At much
vidual subsections devoted to each approach. Section 5 pre- higher E, complex jetting behavior occurs, including tilted
sents a short summary of printed materials with an emphasis jets and multiple jets. Ultimately, very high E results in an
on advances in resolution. Section 6 provides an extensive atomization or spray mode. High-resolution and controllable
review of e-jet printing in applications ranging from elec- deposition of inks favor either the pulsating jet or cone-jet
tronics to biotechnology. The final section presents a perspec- mode.
tive on the field and its future. These jetting modes can be observed at the end of the
nozzle during printing with the use of high-speed cameras.
Park et al.[17] studied the processes of Taylor cone forma-
2. Jet Formation and Important Factors tion and droplet ejection in an e-jet printer using a blend
of polymeric aqueous inks. They observed the pulsating jet
Understanding the physics of jet formation and determining mode at moderate ratios of E/H such as 3.5 V µm−1 (H is the
the key parameters that affect the process are critical to high- separation distance between the nozzle and substrate). In
resolution, uniform, and reproducible printing. Even though this mode, printing occurred via cycles (3–10 ms) of expan-
the mechanisms are conceptually simple, the actual process sion and contraction of the meniscus at the end of the nozzle.
is quite complex and is strongly dependent on the properties In each cycle, accumulation of the ink and formation of the
of the ink such as the viscosity, surface tension, electrical con- Taylor cone was followed by droplet ejection. This ejection
ductivity, and evaporation rate.[34] Additionally, the process is relaxes the electrostatic stress on the meniscus, which sub-
further affected by environmental- (e.g., humidity) and setup- sequently contracts to its original shape. Here, the flow rate
specific factors that are often neglected. These attributes provided by the pump, the properties of the ink, and the size
often lead to demands for careful control and optimization of the nozzle all play important roles in setting the frequency
for each ink material. We begin by summarizing experimental of droplet ejection. A stable jet was achieved when E/H was
studies of the dynamics of jet formation. These investigations increased to 9 V µm−1. These studies suggest that the use of
typically use simple inks, such as pure solvents, to yield essen- sharp nozzles and low E and H values are critical in achieving
tial information on the printing process. Modeling methods high-resolution printing due to reductions in lateral devia-
that can simulate and predict the nature of jet formation for tions provided by the narrow electric-field distributions.[17]
approach based on dimensionless analysis and parametric

maps of the jetting process. The findings identified 10 key
variables related to properties of the ink, geometry of the
system, and processing conditions. These variables were
reduced to 6 dimensionless numbers using the Buckingham
π theorem. Mixtures of pure organic solvents (ethanol and
terpineol) were printed through steel capillary tubes with
inner diameters of 180 µm. A high-speed camera captured
images of jetting for different dimensionless numbers, as
shown in Figure 2b. These images were used to construct jet-
ting maps for different mixtures of solvents as a function of
the dimensionless voltage (β) and the dimensionless flow rate
(α), as shown in Figure 2c. This approach enabled a quantita-
tive description of the different jetting modes in terms of the
dimensionless numbers, thereby providing useful information
for choosing the process conditions. Such jetting maps for dif-
ferent setups, fine nozzles, and a range of inks that contains
particles, polymers, and other materials will play a key role in
the continued development of e-jet printing techniques.
The pulsating jet mode has received significant interest
due to its favorable properties for printing, such as the ability
to deposit micro- and nanometer-sized individual droplets.
Also, the conditions for this mode lie far away, in parametric
space, from unwanted multi-jet and spraying modes. Here, the
pulsation can either be attained using the natural frequency
of the jetting or using an externally controlled, pulsed electric
field. The first reports[39] in this area focused on the frequency
of pulsation that naturally occurs depending on the flow rate
and electric field. Vertes and co-workers explored this fre-
quency with an emphasis on electrospray applications and
proposed scaling laws for the pulsation frequency using the
capillary wave frequency spectrum of a charged droplet.[40–42]
This intrinsic pulsation was later investigated for use in high-
resolution printing. Chen et al.[27] developed scaling laws for
flow rate, jet diameter, and intrinsic pulsation frequency and
experimentally validated these laws using water as the ink
with a 50 µm inner diameter nozzle. Choi et al.[43] studied the
effect of electric field on frequency (f) using a nozzle with an
inner diameter of 30 µm and 0.1 mM KBr aqueous solution
as the ink. They found that f (1–10 kHz) scales with E/d1/2
(where d is the inner diameter of the nozzle) with ≈1.5 power
dependence on a logarithmic scale. Another conclusion
of this study was that low back pressure in the ink supply
system resulted in higher frequencies and smaller droplets in
comparison to the high-pressure case.
A convenient way to define the frequency of jetting and
size of the droplets in e-jet printing involves the use of a
pulsed electric field. The natural frequency of jetting allows
Figure 2. Formation of electrohydrodynamically induced jets under an
applied electric field. a) Different modes of jetting, depending on the
limited control over e-jet printing. Here, the size of the drop-
strength of the electric field and flow rate. Reproduced with permission.[35] lets and the frequency of jetting are both coupled to the
Copyright 2007, Cambridge University Press. b) Jetting behavior of applied voltage such that they cannot be varied indepen-
mixtures of ethanol and terpineol depending on the dimensionless dently.[44] As a solution to this limitation, researchers[44–48]
parameters (α: dimensionless flow rate, β: dimensionless voltage). modulated the voltage with time to reach printing frequen-
c) Diagram showing the dependence of jetting modes on dimensionless cies and droplets sizes beyond those associated with natural
flow parameters. Reproduced with permission.[38] Copyright 2013,
jetting. Figure 3 presents an example of this approach, where
American Chemical Society.
pulses of high voltage are superimposed over a lower base-
Systematic and quantitative approaches to determining line constant voltage. Here, the duration of the pulse and the
the modes of jetting for a given ink and printer setup are time between the consecutive pulses can be varied, as well as
important for optimization. Lee et al.[38] presented such an the baseline and the pulse voltages. The key to success in this
reviews
The direction of flow of the electric charges plays a key

role in the jetting behavior. Most past studies used a direct
current (dc) voltage such that charges flow in one direction.
A significant disadvantage of dc-based e-jet systems is that a
build-up of residual charges on the printed droplets can alter
the dynamics of printing, particularly on insulating substrates.
Byun and co-workers[52] investigated e-jet printer systems
that use alternating current (ac) modes, where the polarity
switches periodically to yield zero total voltages in a time-
averaged sense. Here, ejection of the droplets may happen
at both the positive and negative peaks when the applied
frequency of the electric field is lower than a critical value
(100 Hz). In other words, the frequency of the droplet gen-
eration is two times larger than the applied frequency. It is
possible to apply a combination of ac and dc voltages by
superimposing one upon another. The application of a high-
frequency electric field in this case may lead to the ejection
of one droplet in every two cycles. Besides the frequency of
jetting, the polarity of the electric field affects the behavior
of the ejected droplet and may lead to deviations in droplet
positioning on a substrate.[53] In the case of a dc voltage,
these deviations are typically in the form of deflections from
the substrate that may lead to shifts in the positions of the
droplets or satellite droplets. Such behavior is pronounced on
insulating substrates, even to the extent that, in certain cir-
cumstances, the fields can cause the droplets to return to the
nozzle in the case of an ac voltage. Observations of this type
of effect[52,53] used nozzles with inner diameters ≥200 µm and
nozzle to substrate separations ≥1.5 mm. Related effects are
possible with much smaller nozzles and working distances.
In addition to the polarization of the electric field, different
electrode structures such as plane, hole, and pin types can
provide options for additional control.[54,55] While the pres-
ence and accumulation of charges in the droplets may pre-
Figure 3. Drop-on-demand electrohydrodynamic jet printing. sent challenges, the same phenomena can be used to fabricate
a) Illustrative temporal voltage profile for the pulsed jet. Td denotes the patterns of negative and positive charges, as will be described
time between successive pulses while Tp denotes the pulse width. Vh in Section 6.6.
and Vl are the high and low voltages, respectively. b) Dependence of
The electrical and chemical properties of the substrate
the diameter of the droplet on the pulse width. c) Optical microscope
image showing droplets with different diameters. Reproduced with
are important to consider. Unlike conventional ink-jet
permission.[44] Copyright 2010, IOP Publishing. methods, the electrical conductivity of the substrate is highly
relevant in e-jet printing. In particular, the cumulative build-
up of charge can be significant on insulating substrates, where
mode is the correct choice of the baseline voltage. The value it can distort the electric field and alter the trajectories of
should be sufficiently low such that there is no printing but the droplets. These effects result in variations in the size and
sufficiently high that the cone is prepared for the pulsation. position of the droplets.[53,56] While this phenomenon may
This approach enables high-speed printing of droplets, with provide a means[57] to control the positions of droplets on
frequencies that can reach 10–50 kHz. Stachewicz and co- surfaces, this phenomenon is typically unwanted in a printing
workers[47] demonstrated that the hydrodynamic phenomena process. Methods for dissipating these charges, or eliminating
inside the capillary puts an upper limit on the voltage pulse them entirely, range from the use of conductive substrates or
frequency. In particular, droplet ejection cannot occur effec- substrate supports, ac fields for printing, or means to exter-
tively beyond a certain frequency that depends on the inner nally introduce counterions. Some applications, such as the
diameter of the nozzle. Xu et al. studied low frequency pul- fabrication of electrical devices, often require printing on
sation (<100 Hz) and found that the printing frequency is insulating substrates, where modulation of the electric field
approximately equal to the applied pulse frequency divided and advanced electrode setups can be helpful, as will be
by an integer that depends on the printing parameters.[49] discussed in detail in the next section. As for other printing
Additional levels of control over printing can be obtained processes,[58,59] the wetting properties of the substrate play
through the use of advanced voltage pulse shapes such as an important role in the final sizes and morphologies of the
sinusoids[50] or pulses that involve more than two voltage resultant features. Substrates and inks that lead to high con-
values.[51] tact angles are preferred for patterns that consist of individual
spots.[60] Printed films and continuous lines typically require

relatively low contact angles. Deng and Gomez[61] studied the
role of charge on the wetting behavior of droplets generated
by electrospraying. On a conductive substrate, the droplets
first spread outward to a maximum diameter and then recoil
due to the surface tension. These motions are accompanied
and/or followed by evaporation of solvent to lead to the final
equilibrium shape and size. Charged droplets spread to a
larger degree and have lower contact angles in comparison
to neutral droplets. The electrical charges force the liquid to
move outward in a manner that opposes surface tension.
An essential aspect of high-resolution and uniform
printing relates to the properties of the nozzle. The inner
diameter of the nozzle directly affects the size of drop-
lets and is therefore a key factor in the resolution. The size
of the nozzle also affects the scaling laws that govern e-jet
printing.[62] Nozzles with small inner diameters can be readily
formed by pulling glass pipettes, where commercial processes
allow dimensions down to 100 nm. These pulled pipettes
can be coated with a thin metal layer or a metal wire can be
dipped into the ink solution as an electrode for applying the Figure 4. Theoretical studies of the process of electrohydrodynamically
electric field. An ideal nozzle surface is one that is nonwet- induced jet formation. a) Time evolution of a droplet under an applied
electric field. The electric field first distorts the initially spherical drop
ting toward the ink materials. Since the metallic coating is
to a spheroidal shape and then leads to formation of two Taylor cones
inherently hydrophilic, the surface of the nozzle is often func- at the ends. Later, tip streaming occurs resulting in a small droplet that
tionalized with a hydrophobic self-assembled monolayer, par- disintegrates from the jet. The last image shows a magnified view of
ticularly for aqueous inks.[17] In the absence of such a layer, a the one of the ends after tip streaming. Reproduced with permission.[22]
large meniscus that extends toward the outer surface of the Copyright 2013, National Academy of Sciences. b) Distribution of
nozzle can form.[63] Stachewicz et al.[64,65] found that, besides electric field intensity for a hydrophobic (left) and a hydrophilic nozzle.
the size of the meniscus and droplets, electrohydrodynamic Adapted with permission.[63] Copyright 2010, The Japan Society of
Applied Physics.
behavior during printing can be affected by the presence of
the hydrophobic coating. Special nozzle setups such as those
that involve the insertion of a nonconductive fiber inside the under the action of electrohydrodynamic forces has been
nozzle may be used to improve the stabilization of jets by studied since the early 20th century, several issues remain
reducing the backflow in the meniscus due to the tangential topics of theoretical study.[70,71] Basaran and co-workers
electrical stress.[66,67] developed modeling approaches for EHD tip-streaming
Techniques for visualizing the jetting behavior during from a film[72] and a droplet[22] to capture the mechanisms of
printing can be valuable both to research on the funda- drop formation and the associated scaling laws. In a recent
mental mechanisms and to process control. High-speed study,[22] they demonstrated the existence of three different
cameras and specialized optics are often used to achieve the regimes for the size and charge of droplets depending on the
required spatial and temporal resolution, although the finest conductivity of the fluid. The authors could simulate the time
nozzle tips and the smallest droplet sizes cannot be resolved evolution of a droplet under a strong electric field, as shown
by optical methods. A simple alternative to high-speed vid- in Figure 4a. The deformation of the drop, formation of the
eography exploits strobe illumination using light emitting Taylor cone, and disintegration of the small droplets are all
diodes (LEDs). Kwon et al.[68] developed an analysis algo- captured. An important aspect of such modeling studies is
rithm for images obtained with such a light source, to allow their ability to reveal details that are difficult or impossible
automatic extraction of the meniscus profile and generation to measure using experimental approaches. Higuera et al.[73]
of a 3D graphical representation. The data enabled the study used numerical calculations to reveal the distribution of the
of the effects of pulse shape on the jetting behavior. Jetting electrical stress on the meniscus that forms at the tip of the
behavior can also be analyzed by tomography to reconstruct nozzle and different modes of pulsation as a function of
3D profiles of the droplets using multidirectional projection time. A numerical study performed by Kim et al.[63] explored
data.[69] the impact of wetting behavior of the nozzle. Calculations
showed that uniform droplet ejection from hydrophobic noz-
zles relates to the intense fields at the tip of the meniscus
2.2. Modeling Studies (Figure 4b). Numerical simulation techniques developed for
electrospraying can be used with slight modifications for e-jet
An enhanced fundamental understanding and computa- printing. Wei et al.,[74] for example, used a Lagrangian model
tional models that can simulate the jet formation process will to simulate electrospraying of nanoparticles on a surface and
be needed for the practical use of e-jet printers in routine studied the effect of the spatial distribution and density of
nanomanufacturing. Although the behavior of liquid droplets surface charges.
reviews
Post-printing processes such as evaporation of the sol-

vent or thermal annealing may have a significant impact on
the function and durability of the printed structures. In some
cases, the formation of cracks results from stresses generated
in the printed structures during thermal curing/cooling due
to the different thermal expansion and mechanical proper-
ties of the ink and substrate. Zohdi[75] developed a thermo-
mechanical model to analyze such systems and to determine
conditions that lead to compressive stresses, as a means to
avoid fracture-inducing tensile stresses. Numerical simula-
tion approaches developed for inkjet printers to measure the
velocities and volume profiles of droplets can be applied to
e-jet printers.[76]
Control approaches for the automatic operation of e-jet
printers must be developed in large-scale manufacturing
processes. Most work has been performed in laboratory
environments where the processes are manually controlled
by an operator in an open-loop manner. A particular issue
is in the simultaneous characterization of structures as they
are printed, to provide necessary feedback for determina-
tion of parameters such as the voltage and printing speed.
Two aspects of the process complicate the characterization
of the printed structures. The first relates to the small length
scales associated with e-jet printing: standard optical micros-
copy techniques become inadequate as the size of printed
features extends down to 100 nm and below. A second is
the short time scales associated with droplet ejection. These
challenges motivate the need for control approaches that use
alternative information. One option involves measurement of
the current in the nozzle or substrate, immediately after the
ejection or deposition of the droplet. Barton et al.[77,78] devel-
oped control systems based on the sensing of current meas-
ured from the nozzle to maintain constant jetting frequency.
Mishra and co-workers[79] performed an extensive study on
the correlation between the current measured on the sub- Figure 5. Multi-nozzle printing systems. a) Schematic illustration of a
strate and the diameter and height of the printed droplets. printing head containing multiple nozzles. b) A fluorescence image of
an array of two different fluorescent molecules printed with the multi-
The authors developed a model based on simultaneous high-
nozzle setup. The image shows the capability to automatically align
speed camera imaging and substrate-side current measure- printed features within 2 µm accuracy. Reproduced with permission.[83]
ments for three different types of inks. This model allowed Copyright 2012, IOP Publishing.
the prediction of the diameters and heights of the printed
droplets, with average absolute errors of ≈5% and ≈10%, A vision-based control scheme detects the position of the
respectively. An environmental correction factor can capture nozzle with respect to the substrate, for accurate positioning
the effects of the humidity and temperature of the surround- of different nozzles with excellent overlay registration. Suc-
ings. Iterative learning control approaches[80,81] can further cessful printing of silver interconnects and multiple fluores-
improve the repeatability in resolution and registration. cent species with registration accuracy better than 2 µm can
Recently, Park et al. proposed two expressions to predict the be achieved easily (Figure 5b). Such capabilities are valuable
size of e-jet printed dots and lines based on the contact angle in several different application contexts, including printed
of the ink.[82] electronics and biotechnology, which are reviewed in Sec-
tion 6. This design can be extended to enable simultaneous
printing of the same material using a tilted nozzle array.[84]
3. Modiﬁcations to the Electrohydrodynamic In any such scheme, electrostatic interference between the
Jet Printer individual nozzles must be considered, as established from
previous studies of electrohydrodynamic ejection of drop-
Printing materials from multiple nozzles allows not only the lets from arrays of large scale nozzles.[85–88] The small sizes
rapid patterning of structures that incorporate more than of nozzles associated with high resolution e-jet printing
one component, but also a means for significantly increasing demand a re-consideration of the electrostatics. Experi-
the total throughput of the process by parallelizing the dep- ments indicated that simultaneous printing from 3 different
osition. Sutanto et al.[83,84] designed and developed print- nozzles with inner diameters of 2 µm can be performed with
head systems with such capabilities, as shown in Figure 5a. negligible cross-talk effects when the nozzles are separated
by more than 80 µm.[84] On the other hand, defects such as of the diameter of the hole, thickness and intrinsic proper-
misplaced and missing droplets appear increasingly as this ties of the plate, and distances between the nozzle, plate, and
spacing decreases. This limitation in the density of nozzles substrate are critical to high-resolution printing. This design
per unit area can be overcome by using electrode setups allows uniform printing onto substrates that are insulating
that deliver different electric fields to each individual nozzle. and/or have significant topography. Another route to uni-
Truly high-throughput e-jet printing will require the devel- form printing on insulating substrates involves modulation of
opment of approaches to fabricate print heads that contain the polarity of the electric field. Dong and co-workers[97,98]
large arrays of nozzles comparable in scale to those used in studied ac-pulse modulated e-jet printing and demonstrated
conventional ink-jet printers or developed for other direct- the patterning of continuous structures on insulating sub-
write systems.[89] Initial efforts with large-scale nozzles show strates such as polyethylene terephthalate (Figure 6b). Here,
promise. Conventional microfabrication methods can be used the frequency of the pulse, voltage magnitude, and dura-
to form multi-nozzle arrays for e-jet printing, as explored by tion can be used to control printing. Edirisinghe and co-
several different research groups.[90,91] In another approach, workers[99] investigated the effect of the print head design on
Choi and co-workers[92,93] used a molding technique to gen- e-jet printing using silk fibroin as the ink. The authors showed
erate a fixture made of polydimethylsiloxane for multiple the ability to print lines with widths that approach 1 µm using
glass capillaries with inner diameters of 30 µm. An interesting a design, referred to as the pinhole reservoir print head, that
alternative scheme involves the use of the multi-jet mode incorporates a nozzle with an inner diameter of 800 µm and a
associated with multiple openings from the same nozzle as second opening between the nozzle and the substrate with a
used for electrospraying.[94] diameter of 300 µm. The authors suggest that high-resolution
Improved control over the electric-field distribution printing from large nozzles is possible by placing the nozzle
between the nozzle and substrate is necessary for printing on 5 mm above the meniscus.
highly insulating or rough substrates. One class of approach Improvements in printing capabilities can be achieved
to manipulate the electric field uses an additional electrode from careful design of the nozzle itself, which serves not only
with a hole between the nozzle and substrate. Lee et al.[95] as a controlled opening for the flow of inks but also as one
found that, with a ring-type gate electrode, the electric-field of the electrodes that generates the electric field. Nguyen
vectors can be directed toward the substrate, thereby sup- et al.[100] showed that it is possible to print using a single
pressing the formation of satellite droplets that tend to occur electrode below the substrate without a separate nozzle elec-
when printing on insulating substrates. Recently, Barton and trode. This configuration, which works only with ac voltage,
co-workers[96] used a plate with a hole between the nozzle simplifies the process by eliminating the need to establish
and substrate to direct the electric field. Plates with top and an electrical connection to the nozzle and reduces the sus-
bottom conductive layers separated by a dielectric layer ceptibility to electrical breakdown. Byun and co-workers[101]
(Figure 6a) offered the most efficient means for shaping the explored the use of a circular hole, referred to as a “flat”
electric field toward the substrate by eliminating the hori- nozzle, as an alternative to the more commonly used long
zontal components. The authors found that proper choices protruding capillary type nozzles. Although the goal was to
Figure 6. Printing on insulating substrates. a) Schematic description of a printing system with a double layer field shaping print head (FSP) to
enable uniform patterning on insulating substrates. b) Optical microscope image showing uniform droplets with a diameter of 7 µm printed on an
insulating substrate using FSP. Reproduced with permission.[96] Copyright 2014, American Institute of Physics Publishing. c) Schematic illustration
of an ac-pulse modulated jet printing system that enables uniform printing on insulating substrates. Charge accumulation on the insulating
substrate is prevented by neutralization through consecutive positively and negatively charged droplets. d) Optical microscope image of letters
printed on a glass slide showing the uniformity of the generated droplets. Reproduced with permission.[97] Copyright 2014, IOP Publishing.
reviews
Figure 7. Design and pictures of printer systems. a) Layout and b) pictures of a small scale electrohydrodynamic jet printer system designed to fit
on a typical laboratory desktop. Reproduced with permission.[107] Copyright 2010, Elsevier. c) Schematic illustration and d) picture of a roll-to-roll
electro-hydrodynamic jet printer system. Reproduced with permission.[108] Copyright 2014 Erick Sutanto.
simplify the fabrication process, jets generated by flat noz- Most current and previous e-jet systems operate in a
zles are often not stable or reproducible. Improvements are batch mode on a single substrate. This approach is well
possible by rendering the surface of the nozzle superhydro- matched to use with substrates such as silicon wafers or glass
phobic using an argon and oxygen plasma-assisted process on plates. Recent advances in flexible electronics have moti-
a polyfluorotetraethylene film. In another effort,[102] nozzles vated the exploration of printing on flexible substrates. Roll-
with inner diameters of 20 µm, and heights of 150 µm were to-roll[108–110] e-jet fabrication systems have been developed
fabricated using photolithography assisted by a glass reflow that are suitable for continuous manufacturing systems on
process. The high aspect ratios of the nozzles enabled the flexible substrates (Figure 7c,d).
printing of structures smaller than those possible with con- The integration of e-jet printing with other micro-/
ventional nozzles of the same size. Other studies include the nanomanufacturing processes may provide hybrid technolo-
use of tilted[103] nozzles and conductive inner coatings[104] on gies that enable new avenues of research and capabilities in
the capillary to access smaller length scales with an improved applications. One possibility includes the combination of pie-
focusing of the electric field. The use of co-axial nozzles[105,106] zoelectric inkjet and e-jet printing technology.[111–113] Here,
may provide additional levels of control over the structure the meniscus at the end of the nozzle is formed by a piezo-
and geometry of printed features. electric actuator and the droplet is ejected with the action
The e-jet approach is amenable to printer designs that of the electric field. Advantages of this system lie mainly in
are compact, user friendly, and low cost. Most current high- the ability to generate small droplet sizes at a high frequency
resolution printers are research-oriented and involve custom- using voltages that are lower than those associated with
built parts, leading to issues in the reproducibility of results typical e-jet systems. The frequency of droplet formation is
as well as limited access to the broader research community. determined by the piezoelectric actuation, while the droplet
Efforts at the University of Illinois at Urbana-Champaign size is determined by electrohydrodynamic phenomena.
led to the development of a desktop[107] e-jet printer system Electric field-induced deposition of materials can be inte-
built mostly using commercial off-the-shelf technology grated with an atomic force microscope (AFM) cantilever for
(Figure 7a,b). The hardware and user interface, including generating extremely small droplets. With a structure called
essential components such as the positioning, visualization, the nanofountain AFM probe, Espinoza and co-workers[114]
and electronics systems, can be purchased for a total cost of showed that sub-micrometer features of proteins can be
less than $50 000. Completely assembled systems are now delivered from AFM probes by the application of an elec-
available commercially from other groups (e.g., http://pso- trical potential between the probe reservoir and substrate. An
lution.kr, http://www.sijtechnology.com, accessed: January integrated microfluidic system allows the continuous delivery
2015). of materials to the probes. The transport of proteins from
the probe tip to the substrate via electric field was suggested that, for voltages of ≈100–300 V, increasing the voltage results
to involve electrophoretic or electro-osmotic flow. In an in a decrease in the sizes of the features and an increase
approach called atomic-force-controlled capillary electropho- in the ejection frequency. High-resolution features can be
retic nanoprinting,[115] protein arrays that consist of bovine defined at a spacing down to ≈100 nm, as further discussed in
serum albumin were printed. The approach relied on the posi- Section 5. In related work,[120] the authors demonstrated that
tioning capabilities of an AFM and electrophoretic effects such high aspect-ratio structures can be bent due to dielec-
to transport proteins inside a nanopipette. Both electrodes trophoretic forces associated with the application of an elec-
required for application of the necessary electric field were tric field following printing or with the interaction between
placed on the nanopipette itself, which has an opening with a the two structures.
diameter of 100–500 nm. Yamada and co-workers[116,117] used Dielectrophoretic forces rely on inhomogeneous electric
an AFM cantilever modified with focused ion-beam lithog- fields to enable the printing of neutral materials. Schirmer
raphy to generate an opening with a diameter of ≈200 nm. et al.[121,125,126] investigated this mechanism for printing a col-
The deposition of the liquid was accomplished by applying a loidal suspension of gold nanoparticles (3–7 nm) in a non-
voltage bias between the ionic liquid and a conductive sub- polar solvent (n-tetradecane). An electric field gradient that
strate. Droplets with diameters as small as 65 nm could be forms near the end of the nozzle pushes the particles and the
printed with this approach. In another experiment, An et surrounding solvent, as shown in Figure 8b. The absence of
al.[118] used a pulled borosilicate nozzle with an inner diam- Taylor cone formation during the ejection process suggests a
eter of 30 nm as the tip of a quartz tuning-fork AFM. They dielectrophoretic mechanism. Arrays of dots that consist of
could deposit materials with widths smaller than 100 nm at gold nanoparticles with diameters of ≈175 nm are possible
a voltage bias as low as 12 V. It was suggested that the water with this approach. Interestingly, ring-like deposits, attrib-
meniscus formed between the nozzle and the surface of the uted to single particles and secondary clusters present in
substrate leads to a several-orders-of-magnitude decrease in the stream, form around these dots. Further details on the
the voltage required to print materials. physics of the process and the effect of various parameters
on the uniformity of the printed structures are reported.[126]
4. Other Printing Techniques that Exploit

Electrohydrodynamics and Related 4.2. Pyro-electrohydrodynamic Printing
Phenomena An intriguing concept in electrohydrodynamic printing

involves delivering materials to surfaces at micrometer
The promise of using electric fields as a driver for physical and nanometer length scales by use of pyroelectric effects,
mass flows in the additive patterning of materials has stim- without nozzles or electrodes. The concept, developed by
ulated the development of a range of different techniques Ferraro and co-workers,[122,127,128] uses electric fields induced
that share similar principles and/or mechanisms with e-jet by local heating of a pyroelectric substrate such as lithium
printing. In this section we present a short overview of these niobate. Here, thermal stimulation using an infrared beam or
techniques. soldering iron, schematically depicted in Figure 8c, generates
an electric field through the well-known pyroelectric effect.
Beyond a threshold electric potential, this field pulls ink
4.1. High-Resolution E-jet Printing Based on Autofocusing and from a reservoir that rests on a second opposing substrate to
Dielectrophoresis form a conical jet similar to the Taylor cone. Controlling the
translation of an additional substrate inserted between the
Impressive feature sizes and aspect ratios in printed struc- lithium niobate and the opposing substrate with the liquid
tures can be obtained by autofocusing droplets printed with reservoir allows additive patterning of the ink materials. The
the action of electric fields.[119] The approach developed by use of drop reservoirs with small volumes allows the delivery
Poulikakos and co-workers exploits the dripping mode, in of droplets with volumes of a few attoliters, corresponding
which an applied voltage between a nozzle and a substrate to printed features as small as 300 nm. Numerical calcula-
leads to the periodic ejection of the droplets, as shown in tions[129] show that electric fields similar in strength to those
Figure 8a. Here, gold nanoparticles with sub-10 nm diameters of conventional e-jet printers can be obtained with the pyro-
dispersed in n-tetradecane served as the ink. The solvent electrohydrodynamic printing approach.
evaporates during the ejection period, thereby leading to The use of pyroelectric effects provides new capabili-
the deposition of only nanoparticles. The novelty is that the ties that are useful in different application contexts. In one
printed structure itself functions as an electrode, to attract example, the rapid curing of polymeric inks during the printing
newly formed droplets in a manner that allows the generation process, has allowed the fabrication of 3D structures.[123] In
of high aspect-ratio nanostructures. The authors obtained this particular, polydimethylsiloxane (PDMS) ink subjected to
printing regime with a working distance of 3–4 µm and noz- electric fields formed using the approach described above ena-
zles with outer diameters of 0.55 µm and 1.3 µm. An inter- bles capture of liquid instabilities in the form of solid struc-
esting aspect is that printed structures as small as 80 nm are tures by thermal crosslinking over a duration on the order of
possible with nozzles that have micrometer length scales. seconds. The aspect ratio of the fabricated structures can be
Experimental observations and numerical calculations show as high as 186, enabled by the high viscosity of the PDMS and
reviews
Figure 8. Other printing approaches that use electrohydrodynamic or related mechanisms. a) Schematic illustration of the electrostatic
nanodroplet autofocussing (ENA) printing process. The droplets are ejected with a DC voltage at a period τe. The continuous repetition of this
event leads to accumulation of nanoparticles. The tip of the printed structure behaves like a sharp electrode forcing the incoming droplets towards
it. The inset shows an scanning electron microscope (SEM) image of a nanopillar grown with the ENA approach. Reproduced with permission.[119]
Copyright 2012, Nature Publishing Group. b) Schematic illustration of a dielectrophoretically driven process for printing uncharged polarizable
particles. A DC voltage between a substrate and the tip of a fine nozzle containing a nanoparticle suspension generates a strong dielectrophoretic
force on the nanoparticles. This force leads to movement and dispensing of the particles from the nozzle. The inset shows an SEM image of the
printed Au dots. Reproduced with permission.[121] c) Schematic illustration of a pyro-electrohydrodynamic printer system. A local thermal stimulus
induces the pyroelectric effect in a lithium niobate (LN) substrate. This stimulus results in electrohydrodynamic effects in a thin layer of ink on the
opposing glass substrate and leads to dispensing of droplets onto the target substrate. The inset shows an optical microscope image of printed
droplets with sub-micrometer dimensions. Reproduced with permission.[122] Copyright 2010, Nature Publishing Group. d) Rapid crosslinking of
the polymeric structures generated by pyro-electrohydrodynamic effects enables patterning of 3D structures. Shown here is a fluorescence image
of such a 3D structure. Reproduced with permission.[123] Copyright 2011, National Academy of Sciences. e) Patterning organic nanowires based on
electrohydrodynamic effects. A schematic illustration of the set-up is shown on the left. Organic nanowires are generated by operation in a near-
field electrospinning mode and aligned with the controlled movement of the stage. An optical microscope and SEM image of the printed nanowires
are shown, respectively. Reproduced with permission.[124] Copyright 2013, Nature Publishing Group.
rapid cross-linking (Figure 8d). Demonstrations of the use of obtained with electrospinning can be fabricated and patterned
these structures include optical tweezers and microresonators; with an adaption of this approach. Advantages of fiber fab-
the latter employed quantum dots embedded in the PDMS. In rication in this manner include access to high-viscosity inks
another example,[130] the fabrication of microlens arrays was without clogging problems and the ability to scale up the pro-
shown by pyro-electrohydrodynamic printing from reservoirs cess by using multiple ink reservoirs.
of poly(methyl methacrylate) dissolved in organic solvents. A The use of electric fields to generate droplets by drawing
recent demonstration[131] indicated that fibers similar to those liquids in a nozzle-free configuration can be induced in
different ways. Angelis et al.[132] used (near infrared) NIR decompose to form the desired product.[141] A wide range of
light sources to generate local heating in pyroelectric mate- materials including conjugated polymers,[142] semiconductor
rials with gold nanorods as plasmonic absorbers. By compar- layers,[143] and block-copolymers[144] have been deposited
ison to far-IR sources, this development improves the ease on substrates in the form of continuous thin films with this
of alignment, reduces the size, and increases the convenience approach. We note that the term electrospraying is also used
and robustness of operation, all associated with the wide in several different publications[45,65,145,146] to describe general
availability of NIR sources. electrohydrodynamic processes (i.e., e-jet printing) which are
based on the flow of materials through fine capillaries under
electric fields.
4.3. Near-Field Electrospinning Several other approaches that rely on electric fields have
been developed for the additive patterning of substrates.
Electrospinning, a convenient process for fabricating fibers A widely adopted method for printing hard materials such
with diameters that range from several tens of nanometers up as metals and ceramics is to prepare nanoparticles of these
to micrometers, relies on electrohydrodynamic phenomena materials and suspend them in a solvent, so that they can
similar to those in e-jet printing. Highly viscous polymer flow out of a nozzle. Saleh et al.[147] developed a scheme to
solutions subjected to applied pressure forces flow through a directly pattern materials from bulk sources using electrical
needle, while a voltage bias between the needle and collector discharge. Here a high voltage applied across a gap between
substrate leads to the formation of a Taylor cone and jetting. two gold electrodes leads to electrical discharge and release
Under appropriate conditions, this jet thins and extends to a of heat sufficient to melt and vaporize the electrode mate-
fiber due to bending instabilities. Electrospinning has been rial. A metal tube between the electrodes and grounded
explored in a wide range of materials for different applica- substrates focuses the electric field and controls the position
tions including reinforced composites, scaffolds for tissue of deposited nanoparticles. The minimum size of features
engineering, textiles, and sensors.[133] Conventional electro- demonstrated with this approach was ≈50 µm. In another
spinning is not suitable for applications such as the fabrica- approach, Hong et al.[148] used an electric field to induce
tion of devices where control over the position and individual a liquid bridge between the substrate and nozzle set in an
alignment of the fibers is necessary. Recent work[124,134–136] inverted position. The movement of the substrate resulted in
from different research groups showed that this limitation the break-up of the liquid bridge and deposition of droplets
can be overcome by operating in a near-field mode and using on the substrate. Electrically insulating substrates could be
the fast motion of the substrate. Here, decreasing the dis- patterned in this approach. In an method developed by Wang
tance between the needle and collector below ≈1 cm reduces et al.,[149] local electric fields were generated with optical
the whipping motion. Movement of the stage at a high speed illumination to deliver droplets from a dielectric film in a
imparts a mechanical force that leads to the alignment of the nozzle-free configuration. Here, the optical illumination of
fibers (Figure 8e). Further details on this topic can be found a photosensitive layer induced local electrical stress, which
in a recent review article.[137] Lee and co-workers[124,138,139] led to the ejection of droplets from the film to an opposing
presented advanced demonstrations of this approach to fab- substrate.
ricate electronic devices based on printed organic nanowires.
Organic field-effect transistors could be fabricated with con-
trol over the position and alignment of individual fibers whose 5. Materials and Resolution
diameters were as small as ≈100 nm. Ahn and co-workers[135]
studied patterning of polystyrene and polydiacetylene (PDA)- The most recent decade of work has yielded demonstrations
embedded PS nanofibers. The diameter of the fibers varied of e-jet printing for a diverse range of materials, with a sig-
between ≈60 nm and ≈200 nm depending on the printing con- nificant emphasis on inorganic nanoparticles and organic
ditions such as the concentration of the ink, working distance polymers. Several criteria govern the selection of inks for
and voltage. electrohydrodynamically induced flows. First, the material
should be in a flowable form. Solutions, suspensions, or liquid
precursors that can be cured with light or temperature are
4.4. Other Electrohydrodynamic Processes good examples of candidate inks. A common approach is to
dissolve/suspend the target material in a solvent to prepare
One of the most widely studied electrohydrodynamic pro- a solution that can flow out of a nozzle. The use of additives
cesses is electrospraying, i.e., the generation of charged drop- can adjust the surface tension, viscosity and electrical conduc-
lets whose size can vary from the micro- to nanoscale with a tivity. A second criterion is that the sizes of particles in the
narrow size distribution. Such ionized droplets are commonly ink should be much smaller than the inner diameters of the
used in mass spectroscopy, particularly for the detection and nozzles. This issue is particularly important for high-resolu-
analysis of large molecules such as proteins.[140] Electro- tion operation based on nozzles with openings that can be as
spraying shares similar physics with e-jet printing; however, small as 100 nm. Nozzle-free configurations and methods that
the spraying effect is typically accomplished at much higher use autofocusing effects as described previously relax some
electric fields. A common usage of electrospraying is in the of these constraints in particle size. While such considerations
deposition of homogeneous thin films by directly spraying set the prerequisites for printing, further engineering of the
either the material of interest or a precursor which can later ink formulations is almost always necessary to find the right
reviews
combination of surface tension, viscosity, and conductivity. approaches to generate features with critical dimensions
Details of materials can be found in the following section. below 100 nm. As mentioned previously, Poulikakos and co-
Resolution is one of the most important advantages of workers[119] showed that strong electric-field focusing effects
e-jet printing. Here we highlight some examples of the sizes enable high resolution and high aspect ratios. The authors
of features that can be attained (Figure 9) to convey an idea could print fully separated linear structures down to a pitch
of the capabilities. Early work from Park et al. showed that of 100 nm and pillars with a diameter of 50 nm and an aspect
DNA oligonucleotides can be printed as spots with diameters ratio of 17 with this approach (Figure 9b). Work by Onses
as small as 100 nm using a nozzle with an inner diameter of et al.[150] demonstrated an approach to generate chemical pat-
500 nm (Figure 9a). Subsequent studies employed special terns that consist of polymer brushes with feature sizes well
below 100 nm. This study implemented e-jet printing in a near-
field electrospinning mode to form fibrous polymer structures
rather than isolated droplets. The patterned polymer brushes
had feature sizes much smaller than the inner diameter of the
nozzle. For example, line-widths as small as 50 nm were pos-
sible as shown in Figure 9c using a nozzle with an inner dia-
meter of 1 µm. The resulting pattern was sufficiently small to
influence the self-assembly of block copolymer domains with
widths of ≈40 nm. Finally, Figure 9d presents an example of an
array of spots with diameters that are less than 50 nm via elec-
tric field assisted printing from a hollow AFM tip.[117]
Different strategies can be employed to pattern features
with diverse geometries using e-jet printing. Dots constitute
the most basic structure, and can consist of either isolated
droplets or multiple coalesced droplets. The location of the
droplets can be controlled with the movement of the stage
in synchronization with the applied voltage, either in a mode
of continuous pulses or in individually actuated droplets fol-
lowed by each movement. The latter provides exact control
over the positions of droplets, but can be relatively slow. Line
patterns can form as a result of the coalescence of the indi-
vidual droplets through a suitable combination of proper
stage speeds and wetting of the substrate by the ink. Finally,
continuous films can be obtained by raster scanning lines in
a defined area. Here, over-lapping lines result in continuous
films below certain spacings between adjacent lines. The
thickness of the printed film typically scales linearly with the
Figure 9. Nanoscale resolution in printing. a) DNA oligonucleotide dots

with average diameters of ≈100 nm. An AFM image (left) and a height
profile of the printed dots. Reproduced with permission.[33] Copyright
2008, American Chemical Society. b) Printed gold nanostructures with
varying pitch (250, 200, 150, 100 and 75 nm) are shown in the top
SEM image. The height profiles of the printed nanostructures are shown
at the bottom right. A magnified view of gold nanopillars printed with
the autofocusing approach is given at the bottom left. Reproduced
with permission.[119] Copyright 2012, Nature Publishing Group. c) High-
resolution chemical patterns consisting of polymer brushes with feature
sizes below 100 nm. The top left is an AFM image of printed polymer
brushes before grafting and washing. The resulting chemical patterns
lead to perpendicular assembly of block-copolymer films as shown
in the SEM image (bottom left). Line widths as small as ≈50 nm are
possible, as shown in the SEM image (right). This line width results in
the alignment of the polymer domains. Reproduced with permission.[150]
Copyright 2014, American Chemical Society. d) Electric field-assisted
deposition of inks from a hollow tip using dynamic mode AFM. Shown
are an AFM image (top) and a height profile (bottom) of the printed
structures. The diameters of the printed spots are less than 50 nm.
Reproduced with permission.[117] Copyright 2012, American Institute of
Physics Publishing.
inverse of this spacing. Previous research showed that highly printed silver dots and explored the effects of surface energy
uniform printed films with a roughness smaller than 2 nm is and temperature of the substrate.[166] Using a commercially
possible using e-jet printing.[151] available silver nanoparticle ink in butyl-carbitol and a nozzle
with an inner diameter of 6 µm, the authors generated silver
dots with diameters between 7 µm and 20 µm. As shown
6. Applications of E-jet Printing in Figure 10a, the process allows for generation of uniform
arrays of Ag dots with diameters less than 10 µm. The use
6.1. Printed Electronics of low surface energy (hydrophobic) and high-temperature
substrates coupled with repeated printing on the same spot
One of the most prominent areas of application for e-jet increases the height of structures and suppresses any coffee-
printing is in the fabrication of electronic devices. Printed ring effects and other sources of nonuniformities. Rahman
electronics is an emerging field that is expected to reach a et al.[167] showed that overlapping such droplets can define
market value of several hundred billion dollars.[152–155] Sev- continuous linear structures that are suitable as interconnects
eral different considerations motivate the development of in electronic devices. The diameters of the droplets could be
this industry: i) There is strong interest in unusual forms of varied from 3.8 µm to ≈100 µm using a nozzle with an inner
electronics devices that can be worn or integrated with the diameter of 10 µm, by controlling printing conditions such
human body; these require fabrication approaches that are as the pulse time, applied pressure, and voltage. The authors
compatible with flexible/stretchable substrates and curved found that uniform lines result when the spacings between
or structured surfaces; ii) some active materials (i.e., organic the individual droplets are less than ≈70% of their diameters.
semiconductors, biomaterials for sensing) are chemically, The widths of the lines depends linearly on the diameters
mechanically, or thermally incompatible with traditional of the droplets (Figure 10b). Arrays of uniform lines with
approaches from the existing semiconductor industry, such as widths of 6.5 µm were successfully printed on insulating glass
photolithography; iii) there is a need for low-cost and envi- substrates. In a recent study by Son et al.,[168] the effects of
ronmentally friendly fabrication of electronic devices where repeated printing and sintering of printed silver lines were
the material usage is minimal. Ink-jet printing technology explored, as well as the influence of printing parameters such
represents a leading fabrication approach for this area, and as the working distance, stage speed, and applied voltage
is already used by several companies. As with conventional range. Here, repeated printing over the same line resulted
electronics, reductions in critical device feature sizes decrease in an increase in the thickness of the line without signifi-
operating voltages, increase switching speeds and increase cant change in the width. Nevertheless, the uniformity of the
levels of integration. E-jet printing has a strong potential to thickness across the width of the line decreased (Figure 10c).
extend these trends by enabling structures in printed elec- With the use of laser sintering, the authors patterned metal
tronics at sub-micrometer and nanometer length scales. lines with widths of 3 µm and heights of 230 nm, and an elec-
trical resistivity less than 20 µΩcm. Hybrid electrodes can be
6.1.1. Printing Conductive Materials fabricated by printing silver nanoparticles on graphene for
achieving low sheet resistance and high optical transmittance
One challenge in printed electronics is to define device necessary for transparent heaters.[171] Reports on the fabri-
components such as interconnects, electrodes, and contact cation of silver electrodes on curved glass[172] and flexible
pads with sufficient resolution and electrical conductivity. polyethylene terephthalate[173] substrates show the promise
Conducting inks must offer properties (e.g., viscosity, sur- of e-jet printing for fabrication of unusual electronic devices.
face tension) that allow flow through the tips of fine noz- Recent efforts have focused on copper and aluminium
zles. These requirements focus research on inks that exploit nanoparticles, as a low-cost alternative to silver. Choi and co-
metal nanoparticles, carbon nanotubes, and other conductive workers[174,175] explored e-jet printing of copper nanoparticles
nanomaterials. Extensive reviews on such inks for printed- with average diameters of 40 nm. Nozzles with inner dia-
electronics applications can be found elsewhere.[153,156,157] meters of 60 µm yielded copper lines with widths of 12 µm and
Silver nanoparticles are the most widely studied material resistivities of 2.42 × 10−7 Ωm (Figure 10d). Synthetic routes
for patterning conductive tracks by e-jet printing.[158–168] A exist[176] to prevent the formation of copper oxide through
common approach is to use silver nanoparticles suspended in the use of passivation layers. In another effort, Yoon and co-
an organic solvent as the ink. A subsequent thermal process workers[177,178] explored e-jet printing of aluminum particles
sinters the particles into continuous metal structures. This with diameters in the micrometer length scale. The authors
heating step removes ligands that cover the nanoparticles, to demonstrated the printability of these inks but with a relatively
allow their coalescence into a dense structure. The process coarse resolution due to the large particle sizes. Alternatively,
involves interactions between the ligands and the metal sur- microstructures may be fabricated through the combined use
faces as well as the adsorption and transfer of heat through of e-jet printing with conventional etching processes.[179]
and between the particles.[169,170] To achieve necessary thick-
nesses, it is often necessary to print repetitively in the same 6.1.2. Transistors
targeted area. As in the case of other materials, the proper-
ties of the ink as well and the relevant printing conditions As the most fundamental element of electronic circuits, the
are important in achieving uniform structures. Byun and co- fabrication of transistors using e-jet printing has received
workers performed a detailed study of the uniformity of e-jet significant attention. In one effort, Paik and co-workers[180]
reviews
Figure 10. Silver nanoparticles for printed electronics. a) An array of Ag dots generated by electrohydrodynamic jet printing a suspension of Ag
nanoparticles. Shown is an AFM image of dots with a pitch of ≈40 µm. Reproduced with permission.[166] Copyright 2013, IOP Publishing. b) The
width of the line as a function of the diameter of the droplets. Droplets consisting of Ag nanoparticles can form lines necessary for electrical
interconnects. Reproduced with permission.[167] Copyright 2013, Springer. c) The plot shows the relation between the thickness of the printed
Ag lines and the number of passes over the same. Reproduced with permission.[168] Copyright 2014, Elsevier. d) Current-Voltage (I–V) curve of
printed conductive tracks. The width of the line is 12 µm. The lines were generated by printing a suspension of Cu nanoparticles. Reproduced with
permission.[174] Copyright 2012, IOP Publishing.
fabricated thin-film transistors by patterning amorphous reported.[182,183] Organic transistors with channel lengths of
oxide semiconductors using e-jet printing. Indium zinc several micrometers can be achieved by directly printing
oxide served as the semiconductor and was printed from a metallic nanoparticle on top of the organic layers.[184]
precursor solution that contained indium nitrate hydrate,
zinc acetate dehydrate, 2-methoxyethanol and mono-etha- 6.1.3. Memristors
nolamine. The authors demonstrated line widths as small as
1.5 µm using a nozzle with an inner diameter of 2 µm, ena- Another electronic circuit element of interest is the mem-
bling transistor fabrication at a 10 µm length scale. Figure 11a ristor, a two-terminal device in which the resistance can be
presents a schematic depiction and characterization results reversibly switched with appropriate voltages. Choi and co-
from thin-film transistors fabricated with this approach. workers[185,186] demonstrated a flexible memristor device
While serpentines were patterned using e-jet printing, source fabricated by e-jet printing. The cross-bar structure shown
and drain electrodes were defined by photolithography in Figure 11c consists of an active layer of zirconium dioxide
and a lift-off process. The devices displayed mobilities of sandwiched between bottom and top silver electrodes. This
3.7 cm2V−1s−1 and on/off current ratios better than 105. In structure was printed on a flexible polyimide substrate using
another example,[181] e-jet printed patterns of indium gallium a dispersion of silver and zirconium dioxide particles as the
zinc oxide precursor solutions with formamide as a cosolvent ink in a cone-jet and spraying mode, respectively. The devices
were used in thin-film transistors. The incorporation of for- retain sufficient on/off ratios after 100 cycles of switching and
mamide resulted in an increase in the field-effect mobility. 500 cycles of mechanical bending. Memristors can also be
In another demonstration, Jeong et al.[176] fabricated gra- printed with copper and titanium dioxide as the bottom elec-
phene-based thin-film transistors using e-jet printing. Here, trode and active layer, respectively.[187]
source and drain electrodes were defined by printed copper
nanoparticles; graphene served as the channel as shown in 6.1.4. Display Devices
Figure 11b. The transistors showed ambipolar behavior with
hole mobilities of 1260 cm2V−1s−1. The fabrication of zinc–tin E-jet printing may also find use in the fabrication of dis-
oxide transistors with channel widths of 60 µm have also been plays. In one effort, Byun et al.[188] showed that e-jet
a substitute for the current materials and

processes. Other elements of displays
such as color filters can also be fabricated
with e-jet printing. In an effort towards
this goal, Ahn and co-workers investi-
gated carbon black as an ink for e-jet
printing.[190] Another possible use of e-jet
printing could be in repair of the defects
that are present in flat panel displays.[191]
6.2. Sensors
E-jet printing may find additional appli-

cation in sensing platforms. E-jet printing
can not only be used to fabricate whole
sensors, but also for site-specific delivery
of analytes to enable capabilities that
are not present in conventional systems.
Figure 12 presents several such demon-
strations. Song et al.[192] prepared arrays
of dots and lines that consist of porphyrin,
of interest for sensing applications due
to its high selectivity and quick response
to different gases. The authors showed
that the fluorescence from patterned por-
phyrin arrays decreases to low levels in
the presence of nitric acid vapor, there by
presenting a route to acid sensing. Choi
et al.[110] fabricated a temperature sensor
on a flexible poly(ethyleneterephthalate)
substrate by e-jet printing silver nano-
Figure 11. Fabrication of electronic devices with electrohydrodynamic jet printing. particles. The sensor shown in Figure 12a
a) Schematic illustration of the fabrication of thin film transistors (TFTs) with printed indium consists of a series of connected silver
zinc oxide (IZO) semiconductors and an SEM image of the device. Scale bar: 400 µm. The IZO
lines and operates based on the measure-
channels were defined by printing and the source and drain electrodes were patterned by
photolithography. Representative output characteristics of the device are shown on the right.
ment of resistivity changes that depend
Reproduced with permission.[180] Copyright 2012, American Institute of Physics Publishing. linearly on the temperature. Pikul et
[193] e-jet printed polymer droplets on
b) Schematic illustration of graphene TFTs with printed Cu electrodes. The graphene layer al.
serves as the channel and the printed Cu as the source/drain electrodes. The plot on the right a microcantilever sensor, which offers
shows source/drain current (ID) versus back-gate bias (VG). Reproduced with permission.[176] high sensitivity detection of various ana-
Copyright 2013, The Royal Society of Chemistry. c) Schematic illustration of the fabrication lytes through changes in the mechanical
of a memristor by electrohydrodynamic jet printing. ZrO2 layer and the Ag electrodes were
resonance of the cantilever (Figure 12b).
defined by printing. Effect of multiple voltage sweeps on the resistance of the fabricated
device is given on the right. Reproduced with permission. [185]
Copyright 2013, Elsevier. An advantage of this approach is in the
ability to deposit multiple analytes at a
high resolution. An important additional
printing technology can define alignment layers in liquid aspect of this study was the use of a heated nozzle to melt
crystal displays as a replacement for the conventional spin- polymer inks that exist as solids at room temperature. A sim-
coating process. Here, polyimide was printed in a multi- ilar approach was used to determine the viscoelastic proper-
jet mode at a thickness of 50 nm, followed by thermal ties of microstructured hydrogels, of interest for biomedical
annealing and mechanical rubbing. The results indicate that applications. As depicted in the 3D reconstructed image of
the alignment properties of liquid crystals on such films are Figure 12c,[194] e-jet printing provided high-resolution place-
as good as those on films cast in the usual way. The potential ment of polymer droplets on resonant sensors based on a
of e-jet printing for the patterned deposition of polyimide microelectromechanical system (MEMS). E-jet printing has
may provide additional capabilities. Park et al.[189] explored additional promise in the fabrication of high-temperature
the use of e-jet printing to pattern spacers to define the gap MEMS sensors made of ceramics, where polymer solutions
distance between the transistor and color filter substrates. serve as inks that are precursors to ceramics.[146] In another
The authors fabricated the spacer by printing a negative example, biomolecules printed onto the surface of a silicon
tone photolithography resist (SU-8). The transmittance and photonic crystal provides enhanced fluorescence and sensi-
thermal stability of the printed spacer showed promise as tive detection from biomarkers (Figure 12d).[195] An area of
reviews
Figure 12. Fabrication of sensors and integration of analytes using electrohydrodynamic jet printing. a) Image of a flexible temperature sensor
formed by electrohydrodynamic jet printing of Ag nanoparticle inks. A picture and the layout of the sensor are shown on the left. The temperature is
detected by the change in the resistivity of the printed electrodes. The resistivity changes linearly with temperature (on the right). Reproduced with
permission.[110] Copyright 2014, The Japan Society of Applied Physics. b) Controlled deposition of polymers onto microcantilever gravimetric sensors
for detection of multiple materials. Shown is an optical microscope image of three droplets of polyethylene printed from the melt. Reproduced with
permission.[193] Copyright 2011, IEEE. c) Analysis of the mechanical properties of hydrogel microstructures using microelectromechanical systems
(MEMS) resonant sensors. The hydrogel microstructures were deposited on the sensor by electrohydrodynamic jet printing. Shown is the volume
reconstruction of the hydrogel on the sensor. Reproduced with permission.[194] Copyright 2013, Springer. d) Sensitive detection of biomolecules
printed on a silicon photonic crystal using a resonance coupling laser scanning platform. Fluorescence images of the same region with two
different resonance angles. The face and vase parts were printed with an oligonucleotide and a protein, respectively. The difference in the density
of adsorbed molecules leads to different resonance angles. Reproduced with permission.[195] Copyright 2013, The Royal Society of Chemistry.
interest for e-jet printing is in the fabrication of radio-fre- lithographic methods, particularly in the case of arrays of
quency identification systems.[196] multiple species on a single substrate.[198,199] Several publica-
tions demonstrate the use of e-jet printing in the fabrication of
DNA and protein microarrays. A second area of interest within
6.3. Biotechnology the field of biotechnology is in controlling cell–substrate inter-
actions for tissue engineering, drug assays, and basic studies
Related to examples described above, e-jet printing has been of cell behavior. Here, patterning of materials that serve as
explored in biotechnology, where high-resolution patterning of attachment sites or as environments to support cell growth is
biomolecules and other soft materials is often needed. Due to often a goal. The possibility of patterning such materials at the
the sensitive nature of such materials, single-step direct addi- nanoscale with control over their geometry and sizes in three
tive printing approaches are advantageous over conventional dimensions may be a critical enabler for future applications.
6.3.1. Arrays of DNA Oligonucleotides and Proteins processes motivate the development of platforms where the
sizes and geometries of printed patterns of proteins can be
Methods that allow the patterning of DNA with high spatial precisely controlled. Poellmann et al.[202] showed that e-jet
resolution have applications that range from genomics to printing can be used to pattern fibronectin, an extracellular
nanoelectronics. Central to this interest is highly sequence matrix protein, at a micrometer length scale on polyacryla-
specific Watson–Crick base pairing between single-stranded mide substrates. An important aspect of this study was the
DNA molecules. The most established use of such base use of soft substrates with controllable mechanical proper-
pairing in this context is in DNA microarrays,[200] which ties. Because the elasticity of the substrate plays a critical role
consist of patterned spots of oligonucleotides each with a in the interaction between the cell, the ability to pattern on
unique sequence that serves as a probe site that can recog- such substrates represents an important capability. In another
nize an analyte with a complementary sequence. This analyte study by Shigeta et al.,[197] patterned arrays of diverse
could include a fluorescent molecule or a nanoparticle as classes of proteins such as streptavidin, IgG, fibrinogen, and
a signal of the recognition event. Reducing the dimensions γ-globulin were prepared via e-jet printing. The use of auto-
of each spot in such an array increases the number of rec- mated multinozzle print heads enabled the placement of
ognition sites per area. Another motivation for patterning these proteins into complex geometries on single substrates,
DNA oligonucleotides is in the use of self-assembled DNA as shown in Figure 13b. The experiments further revealed
nanostructures as templates for the assembly of other nano- that the e-jet printing process does not cause any degrada-
materials.[201] The need for patterning multiple sequences of tion of the proteins. These processes can also be performed
oligonucleotides with minimal amounts of contamination on structured surfaces such as plasmonic[197] and photonic[195]
and high spatial resolution makes e-jet printing an attractive crystals, thereby expanding the options in analysis of protein
option for these purposes. Rogers and co-workers[33] showed arrays. Similar approaches can also deliver drug molecules to
that DNA can be e-jet printed into different geometries specific wells for microfluidic drug-delivery systems.[203]
with minimum feature sizes that approach ≈100 nm. Besides
single-stranded oligonucleotides, the authors demonstrated 6.3.2. Directing Cell–Substrate Interactions
printing of double-stranded DNA without any denaturation
effects. Aptamer-based biosensing and programmed material The natural environment of a cell is complex, with topo-
assembly were two key capabilities enabled by e-jet printing graphical, chemical, and mechanical variations at length
of oligonucleotides. Results related to the latter capability scales that range from micrometers to nanometers. Artificial
appear in Figure 13a where the location of gold nanoparticles substrates that can mimic certain features of natural systems
can be controlled through the use of particles functionalized are of interest for the study of cell–substrate interactions and
with oligonucleotides having sequences that are complemen- for applications in biomedical devices and scaffolds. E-jet
tary to the printed oligonucleotides. printing provides relevant capabilities in these contexts. In
Protein microarrays serve as platforms for studies of the one study, Wagoner-Johnson and co-workers[204] developed
interactions and functionalities of proteins. The complex a fabrication method to pattern multiple hydrogels.[205] As
structure of proteins and their high sensitivity to parameters shown in Figure 14a,b, the process starts with e-jet printing of
such as temperature and pH create additional challenges polyacrylamide hydrogel precursors which include monomers
in the formation of protein microarrays in comparison to and crosslinkers. Following the polymerization of the printed
their DNA counterparts. This same complexity, however, hydrogel by exposure to UV light, a second prepolymer solu-
along with the critical roles of proteins in nearly all cellular tion was backfilled on the patterned substrate. The hydrogel
Figure 13. DNA and protein arrays. a) Printing multiple sequences of single stranded DNA molecules. Shown in the left is a fluorescence micrograph
of printed letters A and B using two different sequences of single-stranded oligonucleotides. Both oligonucleotides bear the same fluorophore
at the end of the strands. Selective hybridization of Au nanoparticles coated with complementary sequences leads to the SEM images (middle
and right). Reproduced with permission.[33] Copyright 2008, American Chemical Society. b) Fluorescence microscope images of a printed pattern
of a peacock consisting of three different fluorescently labeled proteins. The first three fluorescence images show the parts of the pattern using
channels specific to the individual fluorophores. The fourth image is generated by merging the individual images. The last fluorescence image is
taken from a dot array of four different proteins. Reproduced with permission.[197] Copyright 2012, American Chemical Society.
reviews
Figure 14. Controlling the spatial position of cells by electrohydrodynamic jet printing. a,b) Hydrogel patterning by printing to prepare substrates
for cell culture. a) Schematic illustration of the process to define patterns of a hydrogel in a background of another hydrogel. An ink containing
hydrogel prepolymers is printed on a functionalized silicon substrate and polymerized by UV light. The spaces between the printed hydrogels are
backfilled with a second hydrogel material. The hydrogel is peeled from the silicon substrate and transferred to a glass substrate bringing the film
upside down. b) The adhesion of cells profilerated over the fabricated hydrogel arrays described in (a). Shown is the cell behavior on small (24 µm,
left) and large (70 µm, right) hydrogel spots. Reproduced with permission.[204] Copyright 2014, IOP Publishing. c,d) Patterning proteins on hydrogel
substrates to control cell adhesion. c) Immunofluorescently labeled fibronectin protein patterns printed by electrohydrodynamic jet printing.
d) Fluorescence images of MC3T3-E1 cells stained with rhodaminephalloidin (red) and DAPI (blue) on the fibronectin patterns. Reproduced with
permission.[206] Copyright 2013, Springer. e) Aerodynamic assisted electrospraying of cells. Shown is a fluorescence microscope image of the jetted
HEK 293T cells. Reproduced with permission.[208] Copyright 2008, IOP Publishing. f) Printing bacterial cells with electrohydrodynamically induced
flows. An optical microscope image of the printed spots using a bacterial suspension. The inset shows the low magnification image of the patterns.
Reproduced with permission.[209] Copyright 2010, American Chemical Society. g) An electrohydrodynamic process to print suspensions containing
3T3 mouse fibroblast cells. Fluorescence microscopy images of the printed cells after 1 day (left) and 7 days (right) of culture. The green and red
colors show live and dead cells, respectively. Reproduced with permission.[210] Copyright 2014, Mary Ann Liebert, Inc.
film was placed upside down following a

second photoinduced cross-linking expo-
sure through a glass slide. This method
allowed the fabrication of micrometer-
sized patterns of hydrogels that consist of
two different materials. The use of such a
platform is demonstrated in Figure 14b,
where MC3T3-E1 pre-osteoblast cells
are cultured on the patterned hydrogels.
The proliferation behavior of the cells
depended strongly on the dimensions and
geometries of the patterns. In a related
report from Poellmann and Wagoner-
Johnson,[206] polyacrylamide hydrogels
were functionalized with N-hydroxysuc-
cinimide to provide covalent attachment
of printed proteins as sites for adhesion
and spreading of the cells (Figure 14c,d).
An alternative approach[207] used printed,
microsized fibers of a biocompatible
polymer, polycaprolactone, to study Figure 15. Fabrication of 3D scaffolds by electrohydrodynamic jet printing. a–d) 3D
polycaprolactone (PCL) scaffolds for enhanced cartilage regeneration. a,b) SEM images
attachment and migration of fibroblast
of printed PCL scaffolds. c) SEM image of the morphology of the fibers after coating with
cells. The cells showed cycles of attach- polydopamine for the functionalization of the scaffolds. d) Collagen is grafted to increase the
ment and detachment to the microfibers, bioactivity of the scaffold. The presence of collagen is validated by the red color observed in
as revealed by time-lapse microscopy. fluorescence microscopy. Reproduced with permission.[214] Copyright 2013, The Royal Society
The direct printing of live cells rep- of Chemistry. e) High resolution 3D scaffold fabrication by electrohydrodynamic jet printing
[215] Copyright 2014,
resents an interesting research direction at elevated temperatures from melted PCL. Reproduced with permission.
that may be enabling for a range of uses in Elsevier. f) Patterns of nanometer hydroxyapatite by an electrohydrodynamic atomization
process to guide the cell adhesion on substrates. Shown is a fluorescence microscope image of
biotechnology. Initial efforts in this direc- osteoblast cells on the patterns of hydroxyapatite. Reproduced with permission.[219] Copyright
tion indicate promise for e-jet printing 2011, Elsevier. g–i) Fabrication of porous PCL scaffolds for bone tissue regeneration using a
techniques. Early work from Jayasinghe grounded bath solution. g,h) SEM images of the highly porous printed scaffold structures.
and co-workers[211,212] demonstrated that i) Cell viability is much higher in the case of printed scaffold (EHD-PCL, green) in comparison
living cells can survive the high electric to the control scaffold (rapid prototyped PCL, RP-PCL, red). Reproduced with permission.[220]
fields and pressure effects associated with Copyright 2011, American Chemical Society.
the jetting process. The printed cells sur-
vived without any damage and showed normal rate of cell tissues and organs. These structures must, of course, be bio-
division. The results were similar for different cell lines such compatible but they must also offer proper mechanical prop-
as human peripheral blood monocytes, mouse CAD cells, and erties and 3D architectures suitable for the penetration and
undifferentiated neuronal cells. The diameters of the depos- proliferation of cells.[213] Figure 15 presents several examples
ited spots ranged from 200 µm to 1000 µm and contained of the use of e-jet printing to fabricate such scaffolds. Wang
different numbers of cells. This approach could be combined and co-workers[214] fabricated 3D structures from polycapro-
with an aerodynamic assisted jetting process to generate lactone for enhanced cartilage regeneration. Here, polymer
stable cone-jets for additional levels of control as shown in is printed from a single fiber that emerges from the nozzle,
Figure 14e.[208] In another study, Kim et al.[209] printed bacte- where it deposits on the substrate with controlled alignment.
rial cells on a bare silicon wafer with a resolution of ≈10 µm. Sequential printing of 20 layers of fibers having diameters
As shown in Figure 14f, individual Staphylococcus epider- of 20 µm yielded the 3D scaffold structure shown in Figure
midis cells appear as dark spots in optical microscopy. The 15a,b. Further functionalization of the fibers with polydopa-
residue of other components of the ink, following evapora- mine and collagen (Figure 15c,d) increases the attachment,
tion of the solvent, remains and surrounds the cells. This spreading and viability of the cells by increasing the hydro-
approach allows printing of cells with single-cell resolution, philicity of the polycaprolactone. In a recent study by Dong
though some spots may have more than one cell or even no and co-workers,[215] e-jet printing was used in combination
cells. In another study, Gasperini et al.[210] printed a mixture with an extrusion deposition technique to prepare scaf-
of cells and alignate and investigated the viability of the cells folds that have features ranging between the millimeter and
via confocal microscopy, as shown in Figure 14g. The alignate micrometer length scales. Thick filaments formed by extru-
cross-links on the substrate and therefore facilitates attach- sion provided mechanical support to thin filaments created
ment of cells. using an e-jet printer with a heated nozzle. Figure 15e pre-
Tissue engineering represents an expanding area of sents high resolution patterns of polycaprolactone printed
development for the treatment of many types of patients. from the melt using e-jet printing. The widths of the filaments
Typically, scaffolds are designed to support growth of cells, were as small as 5 µm. Edirisinghe and co-workers reported
reviews
several studies[30,216–219]
on the use of e-jet printing tech- printing process [119]
based on the autofocusing of droplets, as
niques for scaffold fabrication. The authors investigated dif- described earlier. The authors demonstrated lines and spots
ferent polymers, including polycaprolactone, polyurethane, with critical dimensions of 120 nm and 180 nm (Figure 16a),
polyhedraloligomericsilsesquioxane–poly(carbonate-urea) respectively, with this process. This resolution can be further
urethane, and polyhedral oligomeric silsesquioxane–poly- scaled down to ≈30 nm spots that are sparsely located along
caprolactone–poly(carbonate-urea)urethane as the scaffold a line using dilute inks and high stage speeds. The autofo-
materials. Additional work[218,219] also demonstrated printing cusing effects provided a convenient way to deposit QDs
of nanosized hydroxyapatite crystals, which are essential with high precision on structured surfaces. For example, QDs
components of bone. In earlier efforts,[218] these same authors could be printed on the apexes of gold wedges which are of
explored the effect of printing conditions such as working interest for plasmonics. The authors also demonstrated the
distance and applied voltage on the jet formation and showed use of printed QDs in a plasmonic circuit by integrating gold
that hydroxyapatite can be printed in spraying or cone-jet nanostructures fabricated with lithography (Figure 16a). In
modes. Line widths as small as 50 µm have been achieved other work by Kim et al.,[224] high-resolution patterns of QDs
using a nozzle with an inner diameter of 260 µm. Using a were prepared by e-jet printing with application demonstra-
template assisted e-jet printing process,[219] hydroxyapatite tions in light emitting diodes (LEDs). QDs could be printed
nanoparticles were patterned with feature sizes about 10 µm in stacked and interdigitated geometries (Figure 16b) with
which results in guided attachment of human osteoblast cells a resolution of a few hundred nanometers. The maximum
as shown in Figure 15f. Kim and co-workers[220] developed a luminance and external quantum efficiency of the LEDs
modified e-jet printing process to fabricate highly porous and were better than those of similar devices fabricated by spin-
multilayer polycaprolactone scaffolds. In this modified setup, casting and/or vacuum deposition techniques. Interestingly,
the solid target substrate was replaced with a bath of 5% QDs formed highly closed packed structures in the both of
poly(ethylene oxide) solution. The scaffolds were recovered the studies, probably due to inter-particle interactions in the
from the solution by dissolving the PEO in water followed small volumes of ink. Such work highlights the promise of
by a drying step. The authors found that this modification high-resolution printing of QDs in an additive and material-
prevented crumbling of the deposited materials and allowed efficient way.
generation of highly porous structures in a multi-layered Another area of interest for e-jet printing is in fabrica-
configuration as shown in Figure 15g–i. The viability of oste- tion of metamaterials, as engineered structures with prop-
oblast-like cells was much higher on the e-jet printed scaf- erties that are different from those seen in natural systems.
folds in comparison to ones fabricated by conventional rapid The properties are determined by the unit structure whose
prototyping techniques. dimensions must be controlled to match the wavelength
of interest.[226] Byun and co-workers[225] showed that e-jet
printing can be used to fabricate terahertz metamaterials
6.4. Photonic and Plasmonic Devices with unit cell dimensions of several micrometers. The authors
defined the necessary cells on a polyimide substrate using
A promising research direction for which e-jet printing may an ink based on silver nanoparticles. Encapsulation of the
enable new capabilities is in the fabrication of optical devices, silver electrodes by a second polyimide layer was followed
from waveguides to light-emitting diodes (LEDs). Recent by separation of the entire layer from the silicon substrate,
work from Alleyne and co-workers[221] presented several resulting in a free-standing, flexible terahertz metamaterial
such examples, including a microlens array, an optical wave- (Figure 16c,d). The fabricated metamaterial showed a reso-
guide multiplexer, and a multi-refractive index diffraction nant frequency of 0.5 THz and a refractive index of 18.4, in
grating. The authors fabricated such devices using a UV cur- good agreement with simulations.
able ink widely used in optical systems. The ability to pattern
multiple materials with high resolution is a critical advan-
tage of e-jet printing in such applications. In another study 6.5. Self-assembly of Nanomaterials
by Cunningham and co-workers,[222] e-jet printing was used
to define channels with submicrometer heights on a photonic The use of self-assembling materials as inks for e-jet printing
crystal surface, to confine the liquid volume and provide sig- may provide unique capabilities not only for engineering
nificant enhancement of the fluorescence. These channels applications, but also for fundamental studies of self-assembly
can be easily defined due to the additive and high resolution under geometric confinement. Recently, Onses et al.[151] pro-
nature of e-jet printing. posed a hybrid approach in nanofabrication that exploits high
Quantum dots (QDs), which are nanoscale crystals of resolution e-jet printing together with self-assembly of block-
semiconducting materials, represent a material of interest for copolymers (BCPs). In thin films, BCPs can form ultra-small
applications in photonics and plasmonics. The size dependent (e.g., 5 nm) and dense (e.g., 10 nm) features. These capabilities
optical and electrical properties of QDs make them appealing have potential relevance to the semiconductor industry, as a
as active or passive materials in devices. Recently, two groups means to extend the current capabilities of optical lithography
independently demonstrated the power of e-jet printing systems.[227] These materials can serve as “smart” inks that
techniques for high-resolution patterning of QDs. In a study form self-assembled nanostructures within the geometries
by Kress et al.,[223] nanoscale patterns of QDs were gener- defined by e-jet printing. A unique capability of this approach
ated on flat and structured substrates using a modified e-jet for BCP thin-film studies is in the generation of multiple
Figure 16. Optical devices by electrohydrodynamic jet printing. a) High-resolution e-jet printing of QDs on flat and structured substrates. Shown
on the left is a SEM image of a printed spot of CdSe/CdS core/shell QDs. Shown on the right is the use of such printed QD arrays in a plasmonic
circuit. 3D profile of scattered light in a circular gold bump fabricated by focused ion beam lithography. A printed QD spot at the center of this circle
generates plasmonic waves that are then scattered in the gold structures. Reproduced with permission.[223] Copyright 2014, American Chemical
Society. b) E-jet printed QD arrays for LEDs. On the left is a fluorescence microscope image of an array of green and red QDs. Schematic illustration
and photograph of the fabricated LEDs is given on the right. Reproduced with permission.[224] Copyright 2015, American Chemical Society.
c,d) Flexible terahertz metamaterials by electrohydrodynamic jet printing. c) A photograph and an optical microscope image of the fabricated
metamaterial on a flexible substrate by printing Ag nanoparticles. d) Transmission and refractive index of the tetrahertz metamaterials. Reproduced
with permission.[225] Copyright 2013, American Institute of Physics Publishing.
reviews
Figure 17. Printed block-copolymer (BCP) films. a) SEM images of a butterfly pattern printed with poly(styrene-block-methyl methacrylate) (PS-b-
PMMA) films with two different molecular weights. The images on the left and right are magnified views of the regions printed with 37–37 kg mol−1
and 25–26 kg mol−1, respectively. The nanostructures form after phase-separation by thermal annealing following the printing. b) SEM image of
BCP films printed onto lithographically defined trenches for directed self-assembly. The trenches were printed with 37–37 kg mol−1 (left) and
25–26 kg mol−1 (right) PS-b-PMMA. c) Continuous tuning of the periodicity of the nanoscale domains by mixing BCPs on the substrate. The plot
shows the periodicity of the domains with respect to the thickness fraction of one of the components. d,e) Individual printed dots and lines for
investigation of BCP self-assembly under confinement. d) SEM images of individual printed dots with different molecular weights. e) A printed
line of PS-b-PMMA on a preferential wetting substrate. A SEM (left) and 3D simulation image of the printed BCP line. a–d, Reproduced with
permission.[151] Copyright 2013, Nature Publishing Group. e) Reproduced with permission.[150] Copyright 2014, American Chemical Society.
nanostructures with independently defined size, periodicity, brushes are macromolecules that are end grafted to a surface.
and morphology over a single substrate. An example is pre- E-jet printing of such end-functional polymers[150] provides a
sented in Figure 17a, where a complex image was printed using way to control the chemical functionality of surfaces. A unique
BCP inks. Here continuous BCP films can be patterned by advantage of polymer brushes in this context is that the thick-
printing lines or dots in a raster-scanning mode to define com- ness of the brushes is determined by the molecular weight of
plex images. Phase separation of the BCP induced by thermal the polymer. Therefore, patterns of polymer brushes can be
annealing leads to self-assembled nanostructures within prepared with extreme uniformity in thickness, regardless of
the printed geometries. The use of inks that consist of BCPs any nonuniformities in the printing step. The dimensions and
with different molecular weights allows precise control of geometries of polymer brushes can be defined in the plane by
the size and periodicity of the self-assembled nanostructures. printing, with a resolution that extends below 100 nm. These
This approach can be integrated with common techniques approaches may be useful in patterning wetting layers[228] and
for the directed self-assembly of BCPs to register individual functional polymers[229,230] for different applications.
domains with respect to the lithographically prepared tem- An additional research direction within this theme is in
plates, as shown in Figure 17b. The size and periodicity of the the control of particle assembly within printed patterns. This
nanostructures can be continuously tuned by mixing multiple type of process can be driven by capillary forces that act on
BCP inks that are printed on top of each other (Figure 17c). the particles during the evaporation of the printed drop-
Finally, high-resolution printing of BCPs allows access to geo- lets, as spontaneous organization of the materials defined
metrically confined structures at length scales close to the solely by the printing. An early example of this approach
size and periodicity of the domains formed by self-assembly was presented by Korkut et al.[231] using polystyrene micro-
(Figure 17d,e). Various confinement effects can be readily spheres with an average diameter of 5.7 µm. The particles
observed on such structures and can provide a vehicle for were printed from solutions that contain high-molecular-
experimental and simulation[150] studies of the fundamental weight poly(ethylene oxide), ethanol, and water using nozzles
effects of geometric confinement on BCP self-assembly. with inner diameters as small as 340 µm. The particles self-
Integration of another type of molecular assembly process assemble into arrays of clusters within the printed features,
with e-jet printing can be used to define chemical patterns on a as shown in Figure 18a, as a result of capillary interactions
substrate with high spatial resolution and uniformity. Polymer between the particles and substrate during evaporation of the
20 µm suspended in a water/ethanol solution that contains

high-molecular-weight poly(ethylene oxide) served as the
ink. The incorporation of poly(ethylene oxide) increased
the viscosity and reduced the surface tension of the ink and
aided jet formation. The concentration of silver nanowires
and the flow rate were critical parameters for the width and
uniformity of the e-jet printed lines. Silver nanowires aligned
within the printed lines as a result of the flow and electrical
field as shown in Figure 18b. Stark and Wang[145,233] explored
e-jet printing of spherical gold nanoparticles with diameters
of 10 nm and found that particles form clusters within the
printed spots as shown in Figure 18c. These clusters likely
form due to capillary interactions between the particles
during the evaporation of water. Such colloidal assemblies
can be useful in photonic crystals with multiple wavelength
bands as recently demonstrated with ink-jet printing.[234]
6.6. Charge Printing
E-jet printing can be used to pattern charges on surfaces, as a

complementary capability to all of the previously mentioned
studies, each of which involves formation of solid material
structures. Park et al.[235] showed that negative and/or posi-
tive charges can be printed using a wide variety of ink com-
positions and that these charges can be retained for several
days in low-humidity environments (Figure 19). Positive and
negative charges could be printed by applying a positive and
Figure 18. Assembly of particles by electrohydrodynamic jet printing.
a) SEM images of linear arrays of microspheres self-assembled within negative voltage at the nozzle with respect to a grounded
the printed features. The inset shows the details of the clusters that substrate, respectively. Charges could be printed with a range
can be achieved with the approach. The assembly is driven by capillary of different inks that contain polymers, metallic nanoparticles
forces during the evaporation of the liquid in the ink. Reproduced with and oligonucleotides. The authors demonstrated the use of
permission.[231] Copyright 2008, American Chemical Society. b) Aligned such charges to tune the properties of silicon nanomembrane
Ag nanowires: an optical microscope (left) and SEM image (right) of transistors, as shown in Figure 19b, where the printed charges
the linear arrays of Ag nanowires. Reproduced with permission.[232]
resulted in a change of the threshold voltages through elec-
c) Clusters of Au nanoparticles: SEM images of an array of printed dots
(left) and a magnified view of the individual dots. Reproduced with trostatic doping effects (Figure 19c). Additional possibilities
permission.[233] Copyright 2010, Springer. include the use of the printed charge to guide the deposition
of charged particles or other material building blocks.
liquid. These clusters included different numbers of particles
with some level of deformation to fill the interstitial voids.
Recently, Byun and co-workers[232] demonstrated that silver 6.7. 3D Printing
nanowires can be aligned within the printed lines in an ori-
entation that is parallel to the long axis of the lines. Silver The use of additive manufacturing processes to fabricate 3D
nanowires with average diameters of 40 nm and lengths of objects represents a valuable means for the rapid prototyping
Figure 19. High-resolution charge printing. a) Printed dots of positive (top row) and negative (bottom) charges. Shown is a Kelvin force microscopy
image of the charges. Each column corresponds to a different time between the printing and measurement of the charge. The patterns were printed
using aqueous NaCl solution and the substrates were stored in a low humidity environment. b,c) Fabrication of devices using the charge printing.
b) Schematic illustration of charge printing on the center of a transistor channel for electrostatic doping. c) Drain current (Id) as a function of gate
voltage (Vg). The threshold voltage shifts with the amount of printed charge. Reproduced with permission.[235] Copyright 2010, American Chemical
Society.
reviews
paper[246]and organics.[247]
Biotechnology represents another
area where e-jet printing has strong potential. Additive pat-
terning of biomaterials with high resolution in three dimen-
sions may enable controlled cellular environments that are
central to tissue engineering[248] and biology.[249–251] Direct
and high-resolution printing of individual cells and compo-
nents of an extracellular matrix may play a key role in fur-
ther developments in this area.[252] A relatively unexplored
but growing area of opportunity is in the fabrication of
photonic and plasmonic devices, where patterning of nano-
materials at high resolution is important. The integration of
Figure 20. Electrohydrodynamic 3D printing using a phase change e-jet printing with other approaches such as conventional
material (wax) as the ink. The printing system was modified with a lithography, inkjet printing, and self-assembling materials to
heater to melt the wax. SEM images of various 3D structures with develop hybrid approaches may bring unique capabilities
sub 10 µm resolution: a,b) a pillar array and a magnified view of an that are not present in the individual techniques. Standard-
individual pillar with an aspect ratio ≈8, c,d) tubular structures with thin ized printing systems, including control algorithms, will accel-
walls. Reproduced with permission.[238] Copyright 2014, Elsevier. erate the development of these applications and proliferation
of the technology to the broader research community.
and production of specialized or customized objects for All such applications of e-jet printing demand a detailed
industrial and household applications. Currently employed understanding of the underlying aspects of the process,
techniques such as stereolithography have resolutions on including ink formulation, jet formation, and droplet–sub-
the order of 50 micrometers. Extrusion-based, direct-write strate interactions. Systematic studies that establish rela-
3D printing approaches developed by Lewis and co-workers tionships between the fabricated patterns, the properties of
can extend this resolution below 10 micrometers.[236,237] E-jet ink and substrate, and the printing conditions will be highly
printing has the potential to improve this resolution, but most valuable in this context. When combined with modeling
printed structures in the literature have low aspect ratios, approaches, such work will improve an understanding of the
with limited three dimensionality. Recent work by Dong and physical processes, including additional effects that may play
co-workers[238,239] showed that 3D objects can be fabricated prominent roles in nozzles with extreme nanoscale dimen-
by e-jet printing with critical dimensions smaller than 10 µm sions, and guide the development of advanced capabilities,
and aspect ratios as large as ≈8, as shown in Figure 20. An including continued improvements in resolution, potentially
appealing aspect of this work is that the authors used wax, a well into the sub-100 nm regime, and high-density nozzle
material that is already used in conventional additive manu- arrays for high-throughput printing.
facturing systems. This material rapidly solidified following
e-jet printing from a nozzle that was heated to 110 °C. Fur-
ther extension of this resolution down to the nanometer
length scale may provide a unique opportunity to fabricate
surfaces with an extreme level of control over the structure Acknowledgements
and composition, and may be enabling in preparation of, for
example, scaffolds that perfectly mimic natural systems. MSO acknowledges support from Erciyes University Scientiﬁc
Research Fund (FBG-2014–5376).
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Mechanisms, Capabilities, and Applications of

From the Contents

1. Introduction ........................................ 4238

self-alignment process,[16] respectively. These methods are

wide selection of materials and substrates. Wisconsin-Madison, he received a PhD in

mulation of mobile ions in the ink to regions near the sur-

specific sets of conditions are essential.

2.1. Experimental Studies on the Jet

The electrohydrodynamic effects that

approach based on dimensionless analysis and parametric

The direction of flow of the electric charges plays a key

spots.[60] Printed films and continuous lines typically require

Post-printing processes such as evaporation of the sol-

4. Other Printing Techniques that Exploit

Phenomena An intriguing concept in electrohydrodynamic printing

Figure 9. Nanoscale resolution in printing. a) DNA oligonucleotide dots

a substitute for the current materials and

E-jet printing may find additional appli-

film was placed upside down following a

20 µm suspended in a water/ethanol solution that contains

6.6. Charge Printing

E-jet printing can be used to pattern charges on surfaces, as a

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