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Characterization of the transient thermal-lens effect using top-hat beam Z-scan

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2009 J. Phys. B: At. Mol. Opt. Phys. 42 225404

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IOP PUBLISHING JOURNAL OF PHYSICS B: ATOMIC, MOLECULAR AND OPTICAL PHYSICS
J. Phys. B: At. Mol. Opt. Phys. 42 (2009) 225404 (5pp) doi:10.1088/0953-4075/42/22/225404

Characterization of the transient

thermal-lens effect using top-hat beam
Z-scan
Junyi Yang1 , Yuxiao Wang2 , Xueru Zhang2 , Changwei Li2 , Xiao Jin2 ,
Min Shui2 and Yinglin Song1
1
School of Physical Science and Technology, Soochow University, Suzhou 215006, People’s Republic
of China
2
Department of Physics, Harbin Institute of Technology, Harbin 15001, People’s Republic of China
E-mail: ylsong@hit.edu.cn

Received 20 May 2009, in final form 22 September 2009

Published 30 October 2009
Online at stacks.iop.org/JPhysB/42/225404

Abstract
The transient thermal-lens effect in a solution is investigated by using the top-hat beam Z-scan
technique. The numerical results show that the sensitivity of the top-hat beam Z-scan
measurements is about 3.5 times greater than the Gaussian beams for the transient
thermal-lens effect when the phase shift is small, which is greater than that for the Kerr effect
and the steady-state thermal-lens effect. The reasons are also discussed in detail.

1. Introduction
The thermal-lens effect (TLE) caused by the absorption
of light in materials has been intensively investigated both
experimentally and theoretically for various time scales of
the input laser pulses [1–9]. Previous studies on the TLE
almost focused on the problem of the TLE produced inside
the material on microsecond or longer time scales. The
TLE has been shown to be efficient even with nanosecond
pulses [10] but still within the steady-state regime. Few
papers reported the experimental and theoretical study of a
thermally induced refractive change in the transient regime
[5–8], and these papers investigated the TLE only by using the
Gaussian beam Z-scan technique [11]. The Gaussian beam
Z-scan technique has been widely applied in characterizing
the optical nonlinearity of materials because of some salient
features such as simplicity and high sensitivity. However,
it has the vital frailty of low reliability because the trace of
Z-scan depends critically on the spatial profile of the beam
used. In particular, the desired spatial profile of beams (perfect
Gaussian) is not readily acquired. The top-hat beam Z-scan
has higher sensitivity than the Gaussian-beam Z scan by a
factor of 2.5 times. The other more remarkable feature is that
one can readily obtain the top-hat beam by picking up a small
portion of the expanded beam with an arbitrary spatial profile
[12, 13]. So far, to our knowledge, the transient thermal lens
has not been investigated by using the top-hat beam Z-scan
technique.
In this paper, we investigate the transient TLE by using
the top-hat Z-scan technique. The theoretical results show
that the transient TLE has different characterization of the
sensitivity. The numerical results indicate that the sensitivity
of the top-hat beam is about 3.5 times greater than that of the
Gaussian beam when the nonlinear phase shift of the transient
TLE is smaller than 0.2. The nonlinear refraction of the
(TCBD)2 OPV3 /CH2 Cl2 solution is investigated by using the
top-hat Z-scan technique. The experimental results show that
the nonlinear refraction of the solution is dominantly induced
by the transient TLE.
2. Theoretical model and discussion
Figure 1 shows the top-hat beam Z-scan arrangement, which
is similar to that in [12]. The laser beam was expanded
and subsequently illuminated a circular aperture A1 with a
diameter d to generate a top-hat beam, and then was focused
by a lens L with a focal length of f . The transmitted
pulse energy in the presence and absence of the far field
aperture A2 was probed by a detector D, as a function of
the sample position z, obtaining the closed-aperture and open-
aperture Z-scan, respectively. The aperture A2 with a fixed
linear transmittance in the far field is used for the closed-
aperture Z-scan.

0953-4075/09/225404+05$30.00 1 © 2009 IOP Publishing Ltd Printed in the UK

J. Phys. B: At. Mol. Opt. Phys. 42 (2009) 225404
Figure 1. Schematic of the top-hat beam Z-scan experiment: A1 ,
A2 , apertures; L, lens with a focal length f ; D, detector.
On the plane z, the transverse field distribution of a
focused top-hat beam can be described according to the Fresnel
diffraction theory of propagation of electromagnetic waves, as
follows:
 
t 2 2J1 (π r/ω0 ) exp(iπ r 2 /λz)
E(r, z, t) ∝ exp − 2 ⊗ ∂t
2τ π r/ω0 λz
(1)
where r is the transverse polar coordinate, λ is the wavelength
of the laser beam used, J1 () is the first-order Bessel function
of the first kind and ⊗ is the operator of convolution. Here we
also follow the same rule as in [12] to define the waist of the
focused top-hat beam and the Rayleigh range, i.e. ω0 = λf/D.
 T (r, z, t) =
ω(z) = ω0 [1 + (z/z0 )2 ]1/2 is the beam radius. z0 = π ω02 λ is
the diffraction length of the beam. τ is the laser pulse width.
Considering a thin medium and using the slowly varying
envelope approximation, we can divide the beam propagation
equation into a pair of equations, one for the phase and another
for the irradiance, as follows:
dI
= −αI
dz
dφ
= kn
dz
where φ represents the nonlinear phase shift and z is the
propagation length in the sample; I is the intensity in the
sample and I (r, z, t) = |E(r, z, t)|2 at z = 0; α and n
denote the absorptive coefficient and change of refractive
index, respectively.
In most previous studies of the TLE in the transient
regime, numerical simulations are obtained by solving photo-
acoustic and electromagnetic wave equations simultaneously
(a)
Figure 2. Z-scan traces for the top-hat and Gaussian beams. (a) Kerr effect. (b) Transient TLE.
J Yang et al
[6, 7]. However, this process demands complicated
computation and takes much computing time. In fact, it is
yet available to compute the pulsed laser beam propagation
through nonlinear optical materials when we consider the TLE
by using equations (2) and (3) if the sample thickness is smaller
than z0 , that is, a ‘thin’ sample. We only need to acquire the
real-time thermally induced nonlinear refraction change nth
in the nanosecond pulse duration by solving the photo-acoustic
equation. For the TLE in the transient regime, the change in
the refractive index can be obtained by solving the photo-
acoustic equation [6, 7]. The temperature change T in the
sample occurs after the material absorbs the laser energy. The
diffusion equation of conduction of heat is [6, 7]
∂T (r, z, t)
ρ0 Cp − κ∇T (r, z, t) = αI. (4)
Here κ is the thermal conductivity of the sample, Cp denotes
the isobaric specific heat and ρ0 is the density of the solution.
In equation (4), we can neglect the diffusion term, which does
not occur in the transient regime. As a result, T at time t can
be obtained as
 t
1
αI dt. (5)
ρ0 Cp −∞
When the leading edge of a pulse (t = −∞) encounters
the sample, T (r, z, −∞) = 0. The thermal index change
induced by the propagation of a nanosecond laser pulse
through the sample can be described by the following photo-
acoustic wave equation [6, 7]:
∂ 2 nth (r, z, t)
(2) − vs2 ∇ 2 (nth (r, z, t))
∂t 2
(3) = (dn/dT )vs2 ∇ 2 (T (r, z, t)) (6)
where dn/dT represents the thermo-optic coefficient and vs
is the velocity of sound in the sample. For the interaction
of a pulse with the sample, we substitute T derived from
equation (5) into equation (6) to solve for nth with the initial
condition of nth = 0 and ∂(n ∂t
th )
= 0 at t = −∞.
Figure 2 shows the numerical Z-scan traces by using the
top-hat beam and Gaussian beam with the same on-axis phase
shift at the focus (φ0 ) for the Kerr effect and transient TLE,
respectively. The same as for the results in [12], for the Kerr
(b)
2
J. Phys. B: At. Mol. Opt. Phys. 42 (2009) 225404
Figure 3. The variations of the sensitivity ratio of the top-hat beam
Z-scan compared to the Gaussian beam Z-scan as a function of φ0
for the Kerr effect, steady-state TLE and transient TLE.
effect shown in figure 2(a), the transmittance difference Tpv
between extrema of the normalized transmittance peak and
valley, Tpv = Tp − Tv , obtained with the top-hat beam is
about 2.5 times greater than that with the Gaussian beam.
However, for the transient TLE, as shown in figure 2(b), the
sensitivity of top-hat beam Z-scan is about 3.5 times greater
than that of Gaussian beams for the small φ0 , which is greater
than that in the case of the Kerr effect.
The variations in the sensitivity ratio of the top-
hat beam Z-scan to the Gaussian beam Z-scan rs =
top−hat   spot of 29.4 μm in radius on the focal plane. The buildup
Gaussian
Tpv Tpv as a function of φ0 for the Kerr effect
and transient TLE are illustrated in figure 3. As a comparison,
the steady-state TLE is also investigated, represented with a
dashed line in figure 3. As shown in figure 3, with the increase
of the phase shift φ0 from 0 to π , the sensitivity ratios rs
for three cases are all decreased. The sensitivity ratios rs of
the Kerr effect and the steady-state effect are reduced slowly,
but decrease quickly for the transient TLE. Furthermore, the
sensitivity ratio for the transient TLE is greater than that for the
Kerr effect and steady-state TLE when the phase shift is small.
In order to explain the results obtained in figure 3, the intensity
spatial distributions of the two beams at the focus and the
position corresponding to the normalized peak transmittance
Tp are investigated. As shown in figure 4(a), the on-axis peak
intensities for the top-hat beam and Gaussian beam are the
same at the focal plane. However, as can be seen in figure 4(b),
at the position corresponding to the peak transmittance Tp , the
radial intensity distributions are obviously different. The on-
axis peak intensity of the top-hat beam is greater than that of
the Gaussian beam, which is the main reason for the enhanced
sensitivity of the top-hat beam Z-scan in the case of the Kerr
effect. For the transient TLE with a top-hat beam, except
for the greater on-axis peak intensity, the intensity spatial
distribution is also different. According to equations (5) and
(6), the transient thermal index change is also dependent on
the second derivative of the intensity spatial distribution. The
second derivative of the spatial intensity distribution for the
top-hat beam is greater than that of the Gaussian beam; hence,
the sensitivity ratio for the transient TLE is greater than that
3
J Yang et al
for the Kerr effect. When the phase shift becomes large, the
sensitivity ratio for the transient TLE becomes smaller than
that for the Kerr effect, which results dominantly from the
different changes in the normalized peak transmittance Tp and
the normalized valley transmittance Tv for these two cases with
the top-hat beam, as shown in figure 5. The normalized peak
transmittance Tp for the transient TLE is almost unchanged
when the phase shift becomes large. However, Tp for the Kerr
effect increases with greater phase shift.
3. Experiment
Intramolecular charge-transfer compounds are widely
used as nonlinear optical materials [14]. In this paper,
the optical nonlinearities of an intramolecular charge-
transfer compound, 3, 3 -(4, 4 -(1E, 1 E)-2, 2 -(2, 5-
bis(dodecyloxy)-1, 4-phenylene)bis(ethene-2, 1-diyl)bis(4, 1-
phenylene))bis(2-(4-(dimethylamino)phenyl)buta-1, 3-diene-
1, 1, 4, 4-tetracarbonitrile) ((TCBD)2 OPV3 ), are investigated
by using the top-hat Z-scan technique. (TCBD)2 OPV3 is
synthesized according to the procedure of [15] and dissolved
in CH2 Cl2 . The concentration of the solution is prepared
to be 9.4 × 10−5 mol L−1 . The linear transmittance is
measured to be 36%. A frequency-doubled Continuum
Surelite Q-switched Nd:YAG pulse laser with a wavelength
of 532 nm and a pulse-width of 4 ns is used as the laser
resource. The diameter of the circular aperture A1 is 7.6 mm
and the focal length of L is 420 mm, which produces an Airy
time of thermally induced optical nonlinearities is determined
by the time required for a sound wave to propagate across
a beam size, τac = ω0 /vs . In our experiment, the velocity
of sound in CH2 Cl2 is vs = 1090 m s−1 , and the buildup
time of the thermal nonlinearity τac can be obtained as about
27 ns. The TLE may occur even though the laser pulse width
of 4 ns is smaller than τac , which belongs to the problem
of the thermally induced optical nonlinearities in liquids in
the transient regime [6]. The solution is placed in quartz
cells of 2 mm thickness. The quartz cells with the sample
were placed on a translation stage controlled by a computer
that moved the sample along the z-axis with respect to the
focal point of the lens. The transmittance of the sample is
measured with and without an aperture in the far field. The
diameter of aperture A2 is 4 mm. The laser pulses adjusted by
an attenuator are separated into two beams by using a splitter.
The two beams were simultaneously measured by using two
energy detectors (Rjp-765 energy probe) linked to energy
meter (Rj-7620 ENERGY RATIOMETER, Laserprobe). A
personal computer is used to collect the data coming from the
energy meter through the GPIB interface. The measurement
system is calibrated with CS2 .
Figure 6 shows the top-hat Z-scan traces for the
(TCBD)2 OPV3 /CH2 Cl2 solution with a pulse energy of
8.3 μJ at 532 nm. Figure 6(a) shows the result of the nonlinear
absorption, and it indicates that the nonlinear absorption of
the (TCBD)2 OPV3 /CH2 Cl2 solution is saturation absorption
under our experimental conditions. The absorption coefficient
α can be expressed by α = a0 + βI . α0 is the linear
J. Phys. B: At. Mol. Opt. Phys. 42 (2009) 225404 J Yang et al

(a) (b)

Figure 4. Radial intensity distribution: (a) on the focal plane and (b) at the Tp position.

(a) (b)

Figure 5. The variations of Tp and Tv of the top-hat Z-scan trace as a function of φ0 for (a) the transient TLE and (b) the Kerr effect.

(a) (b)

Figure 6. The experimental top-hat Z-scan traces for the (TCBD)2 OPV3 /CH2 Cl2 solution. (a) The result of nonlinear absorption. (b) The
result of nonlinear refraction. The solid line is the theoretical fit to the experimental result.

absorption coefficient and β denotes the effective nonlinear
absorption coefficient. As can be seen in figure 6(b), the
nonlinear refraction of this sample is negative. The error
in the experimental data in figure 6(a) is about ±5%. The
theoretical curve superposed on the data in figure 6(a) is
obtained by using the parameter β = −2 × 10−10 W m−2 .
Here, dn/dt = 5.4 × 10−4 K−1 , ρ0 = 1.33 × 103 kg m−3
and Cp = 1.6 × 103 J m−3 K−1 are taken from [4]. It is
confirmed that the theoretical fitting is in good agreement
with the experimental result. Figure 7(a) shows the results
of the top-hat Z-scan for the (TCBD)2 OPV3 /CH2 Cl2 solution
with different pulse energy at the same beam radius of
ω0 = 29.4 μm. The results indicate that the TLE is enhanced
by the increase of the energy. Figure 7(b) illustrates the
dependence of the nonlinearity on the beam size. Top-
hat Z-scan experiments were performed in three geometric
configurations: the radius of the aperture A1 is 4.7 mm,
3.8 mm and 3.2 mm, respectively, and then the beam is
focused by the same focal-length lenses (420 mm), which
produce beam waist radii of 23.8, 29.4 and 34.9 μm,
respectively. The total incident energy is adjusted in each
case to be equal to 8.3 μJ. The curves displayed present
Tpv that depends on the beam waist radii used. The
smaller the beam size, the more efficient the nonlinearity.
According to the results, a conclusion can be drawn that
the dominant contribution to the nonlinear refraction of the

4
J. Phys. B: At. Mol. Opt. Phys. 42 (2009) 225404
(a)
Figure 7. (a) The top-hat Z-scan traces for the (TCBD)2 OPV3 /CH2 Cl2 solution with different pulse energy at the same beam radius of
ω0 = 29.4 μm. (b) The top-hat Z-scan traces for the (TCBD)2 OPV3 /CH2 Cl2 solution with different beam radius at the same input energy
(8.3 μJ).The solid line is the theoretical fit to the experimental result.
(TCBD)2 OPV3 /CH2 Cl2 solution is the transient TLE under
our experimental conditions.
4. Conclusion
In summary, we have applied the top-hat Z-scan technique
to investigate the characterization of the transient TLE in a
solution. The numerical results indicate that the measurement
sensitivity of the top-hat beam Z-scan is greater than for the
Gaussian beam by a factor of 3.5 when the nonlinear phase
shift is small, which is due to the on-axis peak intensity,
and the second derivatives of the spatial distribution for the
top-hat beam are greater than for the Gaussian beam. The
optical nonlinearities of the (TCBD)2 OPV3 /CH2 Cl2 solution
are measured by using the top-hat Z-scan. We find that
the nonlinear refraction is mainly induced by the transient
TLE. The top-hat beam Z-scan technique is a good method to
investigate the transient TLE.
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