AMERICAN JOURNAL OF SCIENTIFIC AND INDUSTRIAL RESEARCH

© 2015,Science Huβ, http://www.scihub.org/AJSIR

ISSN: 2153-649X, doi:10.5251/ajsir.2015.6.4.69.73
Experimental studies on the nonlinear optical properties of linb03 crystal
Md. Masud Parvez1
1
Department of Computer Science and Engineering, Southeast University, Dhaka, Bangladesh.

ABSTRACT

The nonlinear refractive index, and the absorption co-efficient β, of an undoped z-cut
photorefractive LiNbO3 crystal has been investigated here by the Z-scan technique using a
continuous wave (cw) laser beam from a multiline argon-ion laser at two different wavelengths.
Here both the sign and magnitude of the measured and β are considerably different from each
other. In the present work, the Z-scan measurement shows that LiNbO3 has both negative and
positive nonlinear refractive index and its magnitudes are and
at the wavelengths of 514 nm and 488 nm respectively. A fit of the absorption co-
efficient data gives the value of to be and at the 514 nm
and 488 nm.

Key words: Absorption co-efficient; Z-scan technique; Nonlinear refractive index, z-cut
photorefractive LiNbO3 crystal.
quality measurement [8] two color time-resolved
INTRODUCTION thermal lensing [9], nondegenerate two photon
absorption, and nondegenerate nonlinear refractive
Refractive index changes induced by light are index [10]. It has also been used for the investigation
commonly described by the relationship of Gaussian beam propagation [11]. In the Z-Scan
( ) technique, a sample is scanned along the optical axis
where, is the linear refractive index, is the in the focal region of a single Gaussian beam.
nonlinear refractive index coefficient and I is the The transmission through the sample, with and
intensity of the light beam. When a Gaussian beam without an aperture in the far field is then recorded.
impinges on a nonlinear medium, the light intensity at The transmission with an aperture (closed aperture)
the centre of a beam is larger than that of the edge; characterizes the sign and magnitude of the
as a result, the refractive index of the medium is nonlinear index, while the transmission without an
maximum along its optical axis, and decreases aperture (open aperture) characterizes the nonlinear
radially as a function of distance from the center of absorption. This is a simple and sensitive technique
the beam, which is responsible for the refractive for measuring the change in phase induced on a
index being spatially inhomogeneous. This light- laser beam upon propagation through a nonlinear
induced refractive index change can have a material. It gives both the sign and magnitude of this
considerable effect on laser beam propagation in a phase change, , which is simply related to the
nonlinear medium, which leads to the well known self nonlinear refractive index, .
action effect phenomena, such as self-focusing, self
de-focusing, self-phase modulation, self-bending, In 1990 S. Bahae et al. [12] presented a sensitive
beam fanning, and multiple ring patterns [1-6]. A lot measurement of the optical nonlinearity using a
of materials have been found to exhibit laser-induced single beam. Employing the Z-scan technique, a
refractive index changes, such as liquid crystals, solid sensitivity of better than ⁄ wavefront distortion
crystals, fullerenes etc. The reliable Z-scan was achieved in measurements of BaF2 using a
technique, first introduced by S. Bahae et al. [7], is a picoseconds frequency-doubled Nd:YAG laser pulse.
simple sensitive, single beam method to determine They demonstrated this method for ZnSe at 532 nm
both the nonlinear refractive index and the where two-photon absorption was present and
nonlinear absorption co-efficient of a given material. was negative. In 1995 Fryad et al. [13] presented
This method has sensitivity comparable to beam waist change in a photorefractive LiNbO3
interferometric methods. This technique has been crystal during the Z-scan measurement. Their
extended to other measurements such as laser beam experimental results showed that the minimum beam

69
 Am. J. Sci. Ind. Res., 2015, 6(4): 69-73

waist had been broadened and they measured the reference beam representing the incident light and
sign of the nonlinear refractive index as negative and the transmitted beam was focused by a convex lens,
the magnitude was found to be . In with a focal length of 252 mm, to achieve the focal
1996 H. Li et al. [14] investigated both the sign and waist radius of . The sample was mounted on
the magnitude of of LiNbO3 with a picoseconds a linear translator and was moved with a high degree
pulsed laser at 532 nm. They observed the sign of of precision. The c-axis of the sample was set parallel
the as positive and the magnitude to be to the gradient direction of the Gaussian beam, i.e.,
. In 2007 Y. Chen et al. [15] the z-axis. This beam was made to pass through the
investigated optical nonlinearities of periodically LiNb03 sample (thickness of 1 mm). The open
poled LiNbO3 crystal by the same technique with a aperture Z-scan measurement was then performed
cw beam at 532 nm. They observed the sign on the crystal
nonlinear refractive index as negative and the
magnitude to be . The nonlinear Beam
refractive index of LiNbO3 determined using the Z- Laser Splitter Lens Sample
scan technique, with a picoseconds pulsed laser at
532 nm, is different in both sign and magnitude from
the obtained result using a cw laser beam at 514 nm
with a low laser power. The positive sign of nonlinear
absorption obtained with the 488nm has been related
Z ← Z=0 → +Z
to the generation of the small bound polarons Detector 1
absorbing in 488 nm laser light. Application of green
light of wavelength 514nm results in the light-induced (a)
transparency, i.e., the Z-scan traces show negative
sign of nonlinear absorption. Intensity dependence of
Z-scan traces allows for conclusion that the photo-
4+ 4+ Aperture
induced dissociation of small NbLi :NbNb bipolarons Beam
Laser Sample Aperture
and sequent generation of small polarons gives the Splitter
dominating contribution to the nonlinear optical

Detector
absorption in reduced crystals with a large bipolarons

2
concentration. There is much room for investigation
of the sign and magnitude of and β of LiNbO3 at
different wavelengths. Furthermore, LiNbO3 is an
important nonlinear optical material with a variety of -Z ← Z=0 +Z
Detector 1
applications. Nonlinear optical properties of LiNbO3
have been subjected to numerous investigations. (b)
Therefore, in order to clear the ambiguity of the sign Fig 1: (a) Experimental setup for open aperture Z-scan
measurements. (b) Experimental setup for open closed Z-scan
and magnitude of of LiNbO3, an experimental
measurements.
investigation was undertaken to find the nonlinear
refractive index and nonlinear absorption co-efficient
The ratio of the power of two beams was determined
of LiNbO3 by the Z-scan technique using a cw laser
as a function of the crystal position. The second
beam at 514 nm and 488nm respectively.
detector was used as a reference to control the
possible temporal variations of the laser power. In
Experimental details: The geometry of the
every position of z, the measurement was made after
experiment is shown in Fig.1. The experiment was
the build-up of the beam distortion. By plotting the
performed using an air cooled multiline Ar-ion laser of
ratio of the signal of two detectors as a function of z,
14.4 mW output power, operating at the wavelength
The Z-scan trace was obtained as shown in Fig. 2.
of 457-514 nm. A 5276 lines/cm diffraction grating
For the closed aperture Z-scan measurement, an
was used to separate the wavelengths. Among the
aperture was inserted in front of one of the detectors
various diffracted light waves, the wavelength of 514
to select the central part of the beam. The size of the
nm (green light) was chosen for the measurement
aperture (1 mm in diameter) was much smaller than
because of its maximum wavelength of our laser light
the beam size in the plane of the aperture, and the
range. This beam was separated into two parts by a
lens-aperture distance was much larger than the
beam splitter. The reflected part was taken as the
scanning range. In every position of z, the

70
 Am. J. Sci. Ind. Res., 2015, 6(4): 69-73

measurement was made, after the build up of the

beam distortion. This experiment was repeated for 1.3
the wavelength of 488nm. The Z-scan method cannot

Normalized Transmittance T(z)

be used to obtain a quantative result for the light- 1.2
induced change in refraction because this is only
possible through the fitting process. If the beam 1.1

preserves its circular cross section, the material

parameter, and β can be determined from the 1.0

fitting of the Z-scan traces.

0.9

1.00 0.8

0.7
Normalized Transmittance T(z)

0.95 -15 -10 -5 0 5 10 15

z in mm
Fig.4 Measured closed Z-scan trace of a l mm thick LiNb03
0.90
sample using a multiline Argon-ion laser at
indicating the negative nonlinearity. The solid curve is a
theoretical fit with and
0.85

0.80
1.3

0.75 1.2
Normalized Transmittance T(z)

-20 -15 -10 -5 0 5 10 15 20

z in mm
1.1
Fig. 2 Measured open aperture Z-scan trace of a l mm thick
LiNb03 sample using a multiline Argon-ion laser at
.The solid line shows the theoretical fit 1.0

1.7 0.9

1.6
0.8
Normalized Transmittance T(z)

1.5
0.7
1.4 -20 -15 -10 -5 0 5 10 15 20

z in mm
1.3 Fig. 5 Measured closed aperture Z-scan trace of a l mm thick
LiNb03 sample using a multiline Argon-ion laser at
1.2 indicating the positive nonlinearity. The solid curve is
a theoretical fit with and .
1.1
RESULT AND DISCUSSION
1.0
-20 -15 -10 -5 0 5 10 15 20
For the open apurture Z-scan measrument the
z in mm normalized transmittance can be written as [13],
( )
Fig. 3 Measured open aperture Z-scan trace of a l mm thick ( ) ( ) ( )
LiNb03 sample using a multiline Argon-ion laser at √
. The solid line shows the theoretical fit. With
( ) ( )
( )

71
 Am. J. Sci. Ind. Res., 2015, 6(4): 69-73

Z = pixel irradiance
where, is the nonlinear absorption co-efficient of s = Gaussian surface irradiance
the sample, n = number of pixels
is the intensity of the laser beam at the By fitting, the obtained nonlinear absorption co-
focus ( ), efficient was and
is the effective length of the at the 514 nm and 488 nm
sample, respectively.
is the confocal parameter, where Fig.4 shows transmittance changes as a function of
is the Gaussian beam waist radius position of the sample used to measure normalized
at the focus, peak-valley transmittance difference, . The
is the linear absorption coefficient and 𝜆 is normalized transmittance for the closed aperture Z-
scan is given by [13] ,
the wavelength of the laser .
Fig. 2 and Fig. 3 show the measured open aperture
Z-scan trace of a l mm thick LiNb03 sample using a
multiline Argon-ion laser at and 488 nm
respectively. The solid lines in these two figures are
Here, and is the on-axis phase change
the theoretical curve while the symbol is the
experimental data. caused by the nonlinear refractive index of the
sample. The solid line in Fig. 4 and Fig. 5 are
The desired beam irradiance profile is a Gaussian obtained from fitting the above equation using
beam with its irradiance at any point in the X/Y plane and respectively. The value of
corresponding to Equation 4. There are a number of on-axis phase change can also be calculated from
ways to perform a fit of the real beam to the the peak-valley transmission difference using the
Gaussian equation. One of these is to minimize the following equation [7]:
deviation, which is defined in Equation 5. This fit can
either be along an X/Y axis, a major/minor axis, or
can be performed over the entire laser beam. Being where, is the aperture linear
performed over the entire beam is useful in that it transmittance with denoting the aperture radius
means that any energy off axis contributes to and denoting the beam radius at the aperture in
determining how well the beam fits a perfect the linear regime. The non linear refractive index,
Gaussian. In addition to these equations, the actual is given by [13]
data of beam profile irradiance can be exported to a
spreadsheet and a user can perform the calculations
according to his own method.

(4) where is the on-focus intensity inside the

sample with P the laser power and
Minimization of the deviation can be performed by the linear absorption coefficient. The peak-valley
varying the parameters of Equation 4 using the sequence of Fig. 4 indicates a self-defocusing effect,
spreadsheet solve feature. A is an offset term which i.e., LiNb03 has a negative refractive nonlinearity but
is set to zero, i.e. disregarded in beam analyzers, the peak-valley sequence of Fig. 5 indicates a self-
because as stated above, the background is carefully focusing effect, i.e., LiNb03 has a positive
set to zero. The definition of the Deviation is: nonlinearity. Using the value of operating laser
power, the on-axis intensity inside the
sample, and
are measured respectively and
at this value of , the measured value of the
refractive index of LiNbO3 crystal is
where: and at the
= standard deviation wavelengths of 514 nm and 488 nm respectively. The
first result is in good agreement with the experimental

72

results reported by Fryad. Z. Henry et al. [13]. It is
found that the sign of nonlinear refractive index of
LiNbO3 induced by a cw laser beam at wavelength of
514 nm is negative and the magnitude is
and whereas the sign of is
positive and the magnitude is 0 at
the wavelength of 488 nm. This observed
discrepancy seems to be significant.
CONCLUSION
We have presented an investigation of the nonlinear
refractive index of pure z-cut LiNb03 crystal by the Z-
scan technique using a cw laser beam from an air-
cooled multiline Ar-ion laser at two different
wavelengths of 514 nm and 488 nm. By fitting, the
nonlinear absorption co-efficient of LiNbO3 is found to
be and at the
514 nm and 488 nm respectively, using the
normalized peak-valley transmittance difference, the
nonlinear refractive indices and
are measured. The first result is
same in sign to the result observed previously using
a cw laser beam at the wavelength of 514 nm.
However the second result exhibits a positive sign at
the wavelength of 488 nm which is in agreement with
the result observed by a picoseconds pulsed laser at
the wavelength of 532 nm. Further investigations are
in progress in this issue to be done at different
wavelengths to verify these results. The origins of our
observed nonlinearities are believed to be attributed
to the photorefractive effect in the LiNbO3 crystal.
73
Am. J. Sci. Ind. Res., 2015, 6(4): 69-73
REFERENCES
[1] P. N. Prasad and D. J. Williams, Introduction to
nonlinear Optical Effects in Molecules and Polymers,
(Wiely, New York, 1991).
[2] Y. R. Shen, The Principles of Nonlinear Optics (Wiley,
New York, 1984; Nauka, Moscow, 1989).
[3] S. Brugioni and R. Meucci, Opt. Comm. 206, 445
(2002).
[4] F. Z. Henari, S. MacNamara, O. Stevenson, et al., Adv.
Mater. 5, 930 (1993).
[5] J. C. Khoo, M. V. Wood, and B. D. Guenther, MRS
Proc. 474, 229 (1997).
[6] H. Abdeldayem, W. K. Witherow, A. Shields, et al.,
Opt. Lett. 19, 2068 (1994).
[7] M. Sheik-Bahae, A.A. Said, and E.W. Van Stryland,
Opt. Lett. 14, 955 (1989)
[8] A.Agnesi, G. C. Reali, and A. Tomaselli, Opt. Lett. 17,
1764, (1990).
[9] J. Castillo, V. P. kozich, and A. Marcano, Opt. Lett. 19,
171, (1990).
[10] M. Sheik Bahae, J. ang, R. De Savo, J. Hagan, and
E. Van Stryland, Opt. Lett. 7, 258, (1992).
[11] P. P Banergee, R. M. Misra, and m. maghraouri, J.
Opt. Soc. Am. B 8, 1072, (1991).
[12] M. Sheik-Bahae, A.A. Said, T.H. Wei, D.J. Hagan, and
E.W. Van Stryland, IEEE Journal of Quantum
Electronics, QE-26, 760 (1990).
[13] Fryad. Z. Henri, Karl Cazzani, Fathi El Akkari, and
Werner J. Blau, Appl. Phys. 78(2), (1995).
[14] Heping Li, Feng Zhau, Xuejun, Wei ji, App. Phys. B
64, 659 (1997).
[15] Yunlin Chen, S. W. Liu, Dongdong Wang, Tianlin
Chen, and Min Xiao, Appl. Opt., 46, 7693 (2007).