IOSR Journal of Applied Physics (IOSR-JAP)

ISSN: 2278-4861. Volume 2, Issue 2 (Sep-Oct. 2012), PP 15-23

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Femtosecond Electronic Thermal Oscillation in Electron

Temperature Dynamics in Thin Gold Film
F. M. Jasim 1 ,M. I. Azawe
Dept. of Physics, Mosul University, Mosul, Iraq

ABSTRACT : High intense femtosecond laser pulse is irradiated on thin gold film. Electron temperature was
evaluated using the two-temperature and the dual- phase lag models. Numerical results showed a thermal
oscillation in electron temperature dynamics. To assess thermal oscillation, analytical solution of the
characteristic equation for heat conduction was obtained by the Laplace transformation method and implied
with the Van Neumann condition. More than one temperature locations in the surface of thin gold film were
observed.
Another feature was also observed from the numerical solutions was the shallow concentration of
temperature distribution of the film. Instabilities and non-homogeneous temperature distribution on front
surface of the gold target were also studied in terms of plume expansion. Plume expansion (in vacuum) in terms
of Knudsen layer thickness will be presented for different laser fluence and pulse duration. These results suggest
that the laser parameters can influence the plume characteristics. Plume expansion in two dimensions of the
surface exposed to the laser will be presented in order to show that the plume expansion was abroad and can be
interpreted in terms of laser fluence.
Keywords - femtosecond laser pulse, gas dynamics, laser plume expansion, thin film gold foil, two-temperature
model.

I. Introduction
Laser pulse of very short duration irradiation to a very small geometrical dimension of gold foil, can
produce an extreme temperature gradients in the object. Such an ultrafast heating of the thin gold film can be
well described by the so-called two- temperature model, initial conditions and boundary-valued partial
differential equations [1]. Theory of heat transmission based on Fourier’s law predicts infinite propagation speed
heat disturbances. This law relates heat flux and the temperature gradient. According to this law, heat flux
adjusts immediately to the imposed temperature gradient, i.e., there is no relaxation time for the heat flux [2].
So, one has to consider the lag between the heat flux and the temperature gradient. This lagging behavior in the
transient process is caused by the finite time required for the microscopic interactions to take place [3]. In 1995,
Tzou [4] proposed the dual-phase lag (DPL) model to explain the non-Fourier heat conduction phenomenon
found in many mediums. In this model, i.e., the dual lags, the heat flux time lag and the temperature gradient
time lag, supersedes the Fourier law for micro-scale heat transport mechanisms. Micro-scale heat transport is
governed by electron-lattice interaction in metallic films. The parabolic two-step model [5] can express energy
transport equations for the flow of heat from the hot electrons to the lattice. The model takes into account the
laser energy absorption by the conduction band electrons, energy transfer from hot electrons to the atomic
vibrations due to the electron-phonon coupling, and the electronic heat diffusion from the irradiated surface to
the bulk of the target [6]. Quintanilla and Racke studied the theory of the heat conduction model with three-
phase-lag [7].
Nonequilibrium thermal distribution had been subjected to intensive research efforts due to the above
applications and to establish a theoretical explanation of thermal transport of both subsystems (electrons and
phonons). Many research works have demonstrated that Fourier’s Law of heat conduction is not suited for
modeling ultrafast heat transport processes, in which the energy excitation times are shorter than or comparable
to the relaxation times of heat carriers [8]. For this reason, the two temperature models (TTM) have been
employed for describing ultrashort laser-metal interactions [9], and the TTM was revised by Qiu and Tien [10]
based on Boltzmann transport equation. They showed that in the short time-step heating regime, the microscopic
energy transfer among photon, electrons, and phonons enlarges the size of the heat affected region and lowers
the lattice temperature rise significantly.
In this article, the two-temperature model (TTM) will be considered for conduction heat transfer, where
the ballistic nature of electrons and phonons is maintained in the governing equations. When the thickness of the
target is less than the electron mean free path, ballistic electron transport would lead to electron-phonon

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 Femtosecond Electronic Thermal Oscillation in Electron Temperature Dynamics in Thin Gold Film
coupling. The general TTM can be simplified to produce the so-called hyperbolic TTM, parabolic TTM, and
even the dual-phase lag model. Interesting features of the electron energy exchange will be presented and
interpreted as transient or instabilities or even oscillating thermalization to the surroundings.

II. Theory
Energy transport after a very short laser pulse (in femtoseconds) absorption will be given. The equation
for electron temperature can be written as [11-16]:

T e
C e (T e ).  .(K e (T e ).T e )  G [T e T l ]  s (r , t ) (1)
t
and the equation for the lattice temperature is:
T l
C l (T l ).  G [T e T l ] (2)
t
where C, T, and G are the specific heat capacity, temperature, and electron-phonon coupling, respectively.
The subscripts e and l stand for the electron and lattice, respectively. s is the heat deposition rate due to laser
source radiation absorption. K e is the effective electron thermal conductivity which accounts for electron-
electron and electron-phonon scatterings, and is defined as [17,18]:
T 
K e (T e )  K 0 .  e  (3)
Tl 
The value of K 0 used in the calculations is 315 W m-1 K-1 [19].
The electronic specific heat capacity is taken to be proportional to the electron temperature as [20,21]:
C e (Te )   .Te (4)
where  is the coefficient for electronic heat capacity. The value of  for gold used in the calculations is 71 J
m-3 K-2 [22]. A value of 2.5x106 Jm-3K-1 for C l will be used in the computations here.
The electron-phonon coupling G has been under active investigations in the field of superconductivity for
several decades and now has attracted renewed interest in femtosecond laser applications [22]. A constant value
for the electron-phonon coupling is used as for low electronic temperatures, rather than temperature dependence.
The value of (2.2x1016 Wm-3K-1 ),which was obtained from reflectivity experiments by Ref. [23], will be
considered in our calculations for the electron-phonon coupling G. The ratio of ( C e /G) is called the time
constant for the electron-phonon interaction, and for Au it is 0.75 ps [5].
The laser source s (x , z , t ) can affect both the electron and lattice temperatures and hence the laser heat
source has to be characterized properly, i.e., a flat-top laser beam (uniform intensity over the entire laser spot) is
considered [24]. The following assumption has to be made that the excited electrons are immediately and fully
thermalized when the laser pulse is applied [25]. The laser source (power density in W/m 3) can be written as
[26]:

B (1  R )J 0   z  t  2t p 
2

 2x     B  
s (x , z , t )  1   cos    .exp  (5)
 t p   L     t 
  p  
where J 0 is the laser fluence (J m-2), R is the gold surface reflectivity (R=0.93 [25]), t p is the laser pulse
duration ( t p =100 fs [25]) at FWHM, ,  (=15.3 nm [25]) is the optical penetration depth of photons in gold
(where the intensity amplitude is decreased by a factor e), L is the spatial period with   L 2  x  L 2
and z is the depth coordinate of gold film. .  is the coefficient of the periodic amplitude  0    1 , and
B  4ln(2) , is the normalization factor that describes the temporal Gaussian pulse function [26]. In other
words, the laser source is assumed a cosine function along the surface (along x-axis) and attenuates
exponentially into the gold skin depth (along z-axis). Lasing is assumed to start at t=0 and ends at t  4t p , and
the laser energy outside this period of time is neglected since it is too small to significantly to affect the electron
temperature [25]. The initial values and boundary conditions of the TTM are as follows. The initial conditions
for both electrons and phonons are:

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 Femtosecond Electronic Thermal Oscillation in Electron Temperature Dynamics in Thin Gold Film
Te (z , 2t p )  T l (z , 2t p )  To (6)
While the boundary conditions, assuming that the gold film front and back surfaces were thermally insulated:
T e T T T
(0, t )  e (L , t )  l (0, t )  l (L , t )  0 (7)
x x x x
The characteristic equation of thermal transport taking into account the dual phase lag under the influence of
laser heat pulse can be written as [27]:
 q  2T 1 T  2T  3T 1 s 
  2  T   s q  (8)
 t 2
 t x x t k 
2
t 
where  q is the relaxation time of heat flux, T is the relaxation time of the temperature gradient, k is
the electron thermal conductivity.
The laser heat source, s , is expressed as [27]:
s (x ,t )  I (t )(1  R ) exp(x ) (9)

where the laser source is assumed to be effective in the surface of the gold film, since we are interested in the
electron temperature distribution rather than skin deep of the film.  is the absorption coefficient of gold. The
laser heat source s (Wm-3) is assumed to be Gaussian and had been separated in variables in time and
dimension.
Equation (9) can be written in a dimensionless form as:
s  x , t   I (t ) 1  R   exp   X  (10)
where  is the dimensionless absorption coefficient, given by:
  2wt k  (11)

w (  ) is the speed of thermal heat wave propagation (sound wave) and  is the thermal diffusivity
q
 k 
of gold   ( C p )  .
 
Equation (8) can be written as:
 2T T  2T  3T 1  s 
q        s q  (12)
t t x x t c p t 
T

2 2 2

The following variables were adopted and defined as:

x t s q T T o
 ,  ,  , 
2 2 q c p (T m T o ) T m T o
Equation (12) is expressed in terms of the above dimensionless variables as:
 2   2 T  3 
2  2 2  4 (13)
 2
  2 q  
2

The function will be given in the following equation when the laser source had been taken in to account:
q
 (  , )  I (2 q ) 1  R   exp    (14)
c p T m T o 
To modify the laser heat source term I (2 q ) in terms of arbitrary reference laser intensity I r as:
I  2 q   I r ( ) (15)
with  () is the dimensionless rate of energy absorbed in the medium. Hence, the function  will be in the form
of:
q
 (  , )   ()I r 1  R   exp    (16)
c p T m T o 

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 Femtosecond Electronic Thermal Oscillation in Electron Temperature Dynamics in Thin Gold Film
In other words, the function , can be written as:
 (  , )   o( ) exp    (17)
With  o is given by:
I r 1  R   q
o  (18)
c p T m T o 
The characteristic equation, given by Eq. (13), will be using the above substitutions as:

 2   2 T  3 
 2  2  2 o (  2 ) exp     (19)
 2
  2 q  
2

Now, the initial dimensionless conditions will be:
   , 0  0 (20)

  , 0   2  2 0  0  exp    (21)

The dimensionless boundary conditions for our present problem are:

 0,   0 (22)


 L ,   0 (23)

The Laplace transformation of the characteristic equation (Eq.(19)), will be [22]:

_
d 2  l (  ,u ) _ _
 u u  2   l   , u   2 u  2   u  exp    (24)
d 2
0

This equation had been obtained using the above dimensionless initial conditions given by Eq.(13) and Eq.
(14). Knowing that the Laplace transforms are:
_
 l   ,u   L    ,  (25)

_
 u   L  ( ) (26)

The satisfying boundary conditions are given by:

_
d l
 0,u   0 (27)
d
_
d l
 L ,u   0 (28)
d
We had assumed that the target is isolated.
The analytical solution (Van Neumann condition) of the characteristic equation (Eq.(24)), taking in to
account the above boundary conditions is of the form:
_
 l   ,u   c 2 sin     c 3 exp    (29)
with is given by:
   u u  2 
2
(30)
where is the Laplace variable.
Substituting Eq. (29) in to Eq.(24) we get:

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 Femtosecond Electronic Thermal Oscillation in Electron Temperature Dynamics in Thin Gold Film
c 2 sin   x  
c 2 2 sin   x   c 3  2 exp   x    2    2 0  s  2  exp   x 
 c 3 exp    x 
(31)
Resulting from the above equation is the following equation for the constant :
_
2 0  u  2 
c3  (32)
u u  2    2
In order to calculate the constant , we had solved the analytical solution for the boundary condition as:
d
   l   0  c 2 cos  l   c3    exp   l  (33)
d
We get:
_
2 0  u  2  exp    l 
c2  (34)
u u  2    u u  2
1
2 2 cos  l 
Finally we get the following equation that is to be solved numerically

_ 2 0 u  2  exp(  l ) 2 0 (u  2)
   ,u   sin( )  exp(  ) (35)
1
u (u  2)   2
(u (u  2)   )[u (u  2)] cos(l )
2 2

The equation of laser plume gas dynamics represents the surface temperature distribution for the plume of
gold film irradiated by Gaussian femtosecond laser pulse [28] :

1
F   2 t
p (t  t ' )d 2 (t ' )dt ' z 2 r2
T (r , t , z )  max  
   0 t ' 12 (4t '  d 2 (t ' )) exp[ 4t '  4t '  d 2 (t ' ) ] (36)

with Fmax is the laser peak flux density . The symbols given in the above equation is for thermal properties of

gold.  is the thermal conductivity,    c is the thermal diffusivity,  is density, c is heat capacity .

p (t ) is the normalized pulse magnitude (0  p (t )  1) .

III. Results And Discussion

The above equations will be solved numerically with the aid of Matlab for different conditions. We had
used typical parameters of the noble metal (gold) as given in Table I.

Table I: Typical parameters of gold used in the simulation

Property K L
Definition Thermal Absorption Thermal Film Ambient Thermal
diffusivity coefficient conductivity thickness temperature wave speed
Numerical 1.2 1x109 m-1 315 W/( mK) 20 nm 300 K 1.9085 m/s
value

Fig.1 show the 3D plot after adjusting the grid size from convergence test and time step was set to 0.25 ps to
reach numerical analysis consistency. The electron temperature was plotted as a function of time and distance
(penetration from the front surface of the gold film). We can notice that the electron temperature reached its
maximum value in less than one femtosecond and the complete electron thermalization was 4 nm in depth of the
gold film. This will be studied more in depth and thoroughly when considering the dual phase lag.

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 Femtosecond Electronic Thermal Oscillation in Electron Temperature Dynamics in Thin Gold Film

Fig.1 Electron temperature simulation as a function of time and gold skin depth computed for gold film of
20 nm thickness when irradiated by 13.7 Jm-2 laser fluence and 100 fs pulse duration.

Fig. 2 Numerical simulation of the electron temperature dynamics of gold nanostructure induced by the
influence of the variation of laser pulse duration. The simulation was carried out first with 300 fs
and then 200 fs, laser pulse duration.

To study the influence of pulse duration of the laser on the electron temperature taking into account
relaxation times  q and  t in the simulation, Fig. 2 shows the results of this simulation. Two values of laser
pulse duration were taken as (200fs) and (300fs).
The influence of relaxation time on the electron temperature dynamics, Fig. 3, shows this effect. The values
of,  q (relaxation time of heat flux), and T (the relaxation time of temperature gradient) were taken as shown

in the figure. When the simulation was carried out with  q  T  , we found an interesting feature for the
electron dynamics, that is, the electron temperature started to decrease with oscillating behavior. The oscillations
get larger as electron kinetics with time proceeds to lattice exchange. This behavior of electron dynamics, to our
knowledge, had not been published. The explanation of this behavior can be interpreted as,  q means a finite
time is required to raise the temperature of electrons, while T indicates the delay that exists in electron-phonon
exchange. This delay is shown as oscillations.

Fig. 3 The time evolution of electron temperature for two cases, showing oscillations when  q  T . Laser
-2
irradiation of front surface of the nanostructure gold film was with fluence 13.7 Jm and pulse duration of 96 fs.

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 Femtosecond Electronic Thermal Oscillation in Electron Temperature Dynamics in Thin Gold Film
The temperature distribution on the front surface of nanostructure gold film when irradiated by a
femtosecond laser pulse will be studied numerically with the help of (DPL) model. The simulation was
performed using FDTD (finite-difference time-domain) algorithm to solve the characteristic equation of heat
conduction. The time increment for simulation and grid size were adjusted until the stability and convergence
criteria were obtained satisfactory, giving time step few femtoseconds and spatial increment of 3nm. Many mesh
grid size were tested in simulation, until the above condition was reached.

Fig. 4 shows the numerical simulation of temperature distribution of the front surface of the gold film
irradiated by (96 fs) laser pulse duration and fluence of (13.7 Jm-2 ) by solving the characteristic equation of
DPL model.

Fig. 4 Temperature distribution of the front surface of gold film when exposed to laser Gaussian pulse of
duration of (96 fs) and power density of so=5.88x1020Wm-3.

_
The calculations of the dimensionless surface temperature    as a function of dimensionless
 
displacement    , for various values of the dimensionless absorption coefficient , while keeping the other
variables  and o as constants is shown in Fig. 5. It is obvious from the figure that for small values of  the
temperature distribution extends more than for greater value of  . This behavior needs no explanation as can
be predicted from the simple law of absorption for certain material.

Fig.5 Dimensionless surface temperature as a function of dimensionless displacement for different values of
dimensionless absorption coefficient (0.5, 1, 1.5, 3) and keeping dimensionless rate of energy
absorbed in the medium constant   and dimensionless internal heat source also constant  o  .

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 Femtosecond Electronic Thermal Oscillation in Electron Temperature Dynamics in Thin Gold Film

Fig. 6 Illustrates the expansion of plume (in terms of temperature distribution of vapour
plume) for two different values of laser fluence of 13.4 & 23.4 J/m 2 as a function of
kundsen layer thickness.

The expansion of the plume was taken into account the effects of laser fluence in order to show how this
can influence the expansion in terms of Knudsen layer thickness which had been evaporated by thermal effect of
laser pulse, Fig. 6 . Laser ablation has to conceder this result in its application.
Laser spot radius was found to be effective on the plume expansion as shown in Fig. 7. Two values
were used in the numerical simulation. As can be seen from the graph, higher value of laser spot gives higher
temperature distribution and expansion.

Fig. 7 Representce the influence of laser spot diameter on the temperature distribution of the plume in
terms of Knudsen layer thickness.

IV. Conclusions
Numerical simulation for the heated gold film had been carried out using TTM and DPL to obtain the
electron temperature. TTM numerical results showed that electron temperature had slow time decrease in
comparison to DPL. Simulations of the characteristic equation (DPL) by FDTD algorithm to study the electron
temperature (Te) taking into account the relaxation times reveals that T e can be affected by laser fluence as well
as laser pulse duration. A thermal oscillation in T e dynamics was found when  q  T . A temperature
distribution on the front surface of the gold film was studied showing part of the surface was extremely at high
temperature besides zones of lower temperatures.
The problem of the characteristic equation of thermal transport, taking into account the DPL for thin
gold film and irradiated by femtosecond laser pulse, was solved analytically by the Laplace transform method
for the case of IVBP.
Dimensionless surface temperature with respect to the dimensionless displacement for various values
of the dependent parameters which are; the dimensionless internal heat source, the dimensionless rate of energy
absorbed in the medium, and the dimensionless absorption coefficient were studied.
Laser plume expansion from thin gold film was investigated in this article in terms of Knudsen layer
for Adiabatic, non-isothermal case of gas dynamics. The results showed that the plume expansion was

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 Femtosecond Electronic Thermal Oscillation in Electron Temperature Dynamics in Thin Gold Film
completely dependent on the laser pulse parameters, the pulse duration, fluence, and beam waist. This
dependence had been shown implicitly in the plots given. The analytical equations were solved numerically for
special case as spatially constant temperature of the laser plume.

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