Thin Solid Films: Sciencedirect
Thin Solid Films: Sciencedirect
Thin Solid Films: Sciencedirect
Department of Materials Science and Engineering, Northwestern University, Evanston, IL 60208, USA
ABSTRACT
While positive correlation between fracture toughness and H/E and H3/E2 has been reported for some ceramic coatings, we outline an argument that such correlation
cannot be true in general, especially for nanolayer and nanocomposite coatings that present multiple interfaces to impede crack growth. Literature data are presented
to support this argument.
Hard coatings, mostly derived from ceramic materials, are widely higher toughness where there is no plastic deformation.
used for wear protection applications. High hardness, while desirable The proxy H3/E2 very likely originated from the sphere-on-flat
under conditions of abrasive wear, is not the only important physical Hertzian contact analysis [9]. Given the contact between a sphere of
property for these applications. Given the brittle nature of most ceramic radius R, elastic modulus E and an infinitely rigid flat surface with a
materials, fracture toughness is another important property to consider. normal load N, the maximum Hertzian contact stress Pmax is given by:
Many papers have been written about measuring fracture toughness of 1 1
coatings [1–7]. In general, accurate determination of fracture toughness 1 6NE 2 3 NE 2 3
Pmax = 0.578
of coatings without substrate effects requires rather involved mea- R2 R2
surements and/or sample preparation. Therefore, it is desirable to find No significant plastic deformation occurs when Pmax < σy, which
an easier method to determine or rank fracture toughness of coatings. can be assumed to scale with the coating hardness H, i.e.,
Over the past 15 years or so, two ratios, viz., H/E and H3/E2 (H being
1
the hardness and E the elastic modulus) have been proposed as proxies NE 2 3
0.578 < = H
for fracture toughness of coatings. In some publications, E* = E/ R2
y
⁎
Corresponding author.
E-mail address: ywchung@northwestern.edu (Y.-W. Chung).
https://doi.org/10.1016/j.tsf.2019.04.040
Received 4 April 2019; Received in revised form 22 April 2019; Accepted 24 April 2019
Available online 25 April 2019
0040-6090/ © 2019 Elsevier B.V. All rights reserved.
X. Chen, et al. Thin Solid Films 688 (2019) 137265
Fig. 2. Correlation between fracture toughness and H/E and H3/E2 for a series
of aluminosilicate glasses with varied network modifier ions (data from Ref.
Fig. 1. Correlation between fracture toughness and H/E and H3/E2 in Ti-Ni-N
[27]).
and Al-Cu-O coatings (data from Ref. [13] and [16]).
correlation only at light impact forces, but not at higher forces. A clear
growth of coatings are all important factors contributing to cracking
effect of plasticity was shown in Shi et al.'s work [29] on multilayer W/
resistance [17].
VC coatings, in which they demonstrated either an inverse or zero
More recent work by Hahn et al. [18] on TiN/CrN superlattice
correlation between toughness and H/E and H3/E2 (toughness being
coatings shows a slightly positive correlation between H/E and fracture
measured by a modified Vickers method), as shown in Fig. 3. In their
toughness, the latter being measured by a microcantilever bending
experiments, the W thickness fraction within the four multilayer coat-
method. The significance of H/E in wear control has been discussed by
ings ranges between 60 and 90%. Daniel et al. [30] synthesized a series
Leyland and Matthews [19] and Lackner et al. [20].
of monolithic TiN coatings with a chevron-like microstructure and
It is attractive to use H/E and H3/E2 as proxies for fracture tough-
found no correlation between fracture toughness and H/E and H3/E2,
ness of coatings because H and E can be readily measured by na-
with toughness measured by the microcantilever bending method. In
noindentation. In spite of initial reports on such positive correlations,
the investigation on WC-Co coatings, Lima et al [31] found an inverse or
we explore in this commentary if such correlation is applicable in
no correlation between toughness and H/E, with coating toughness
general. Since H/E represents elastic strain to failure and H3/E2 re-
measured by the Vickers method. These two datasets are shown in
presents the resistance to plastic deformation, neither ratios address the
Fig. 4.
contribution of plasticity to fracture toughness. Moreover, the quantity
More examples of either inverse or no correlation can be found in
H3/E2 was derived from surfaces in contact while the property of
diverse material systems reported in the literature, e.g., Fe/VC multi-
fracture toughness has no intrinsic dependence on contact. For fracture
layer coatings [32], TiB2-TiC-Al2O3 composite coatings [33], CrN/AlN
events dominated by ceramic materials, plastic deformation is negli-
multilayers [34], and CrN/Cr and TiN/SiOx multilayers [35].
gible. Therefore, in coating systems where elasticity dominates fracture
In summary, H/E and H3/E2 may have been good proxies for frac-
toughness, H/E and H3/E2 could be good approximations to rank the
ture toughness of coatings if coating fracture involves no plasticity and
fracture toughness of coatings. However, in cases where plastic de-
leads to instant failure. However, the latter conditions may not be sa-
formation plays a role and cracks do not propagate to instant failure,
tisfied in most nanolayer and nanocomposite coatings, in which pro-
the positive correlation discussed in the preceding paragraphs might
pagating cracks are arrested frequently at interfaces. As such, use of H/
not hold.
E or H3/E2 as a measure of coating toughness is not generally applic-
There have been discussions about the use of micro/nanostructure
able.
control to improve fracture toughness, e.g., nanolayers, nanocompo-
sites, or matrix-precipitate lattice mismatch [21–25]. Such micro/na-
nostructure could toughen the coating through crack deflection at in-
terfaces, interface delamination, ductile interlayer ligament bridging,
and crack tip blunting because of nanoscale plasticity [26]. For ex-
ample, Wang et al. [21] synthesized Cu/Zr metallic glass nanolaminates
and achieved tensile ductility > 10% (Zr metallic glass has almost zero
ductility). Such toughening mechanisms may not have a proportional
effect on H/E and H3/E2. Under these conditions, H/E and H3/E2 will
not be good proxies for toughness – this statement applies to coatings as
well as bulk materials.
To illustrate, let us examine the correlation between fracture
toughness (as measured by the Vickers method) and H/E and H3/E2 for
a series of (bulk) aluminosilicate glasses with varied network modifier
ions [27]. As shown in Fig. 2, fracture toughness does not correlate with
either H/E or H3/E2. From publications that report H, E, and some
measures of toughness on coatings, we have found many examples of
either no correlation or inverse correlation. For example, Beake [28]
synthesized TiFeN and TiFeMoN films and assessed their fracture
Fig. 3. Correlation between fracture toughness and H/E and H3/E2 for VC, W,
toughness from repeated nano-impact tests. He found positive
and four W/VC multilayer coatings (shaded) from Ref. [29].
2
X. Chen, et al. Thin Solid Films 688 (2019) 137265
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