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Group and phase birefringence

dispersion of pure and doped lithium


niobate crystals obtained by analysis
of interference pattern observed
behind a plane polariscope

Norbert Tarjányi
Daniel Káčik

Norbert Tarjányi, Daniel Káčik, “Group and phase birefringence dispersion of pure and doped lithium
niobate crystals obtained by analysis of interference pattern observed behind a plane polariscope,”
Opt. Eng. 58(3), 034101 (2019), doi: 10.1117/1.OE.58.3.034101.

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Optical Engineering 58(3), 034101 (March 2019)

Group and phase birefringence dispersion of pure and


doped lithium niobate crystals obtained by analysis of
interference pattern observed behind a plane polariscope
Norbert Tarjányi* and Daniel Káčik
University of Žilina, Department of Physics, Faculty of Electrical Engineering and Information Technology, Žilina, Slovakia

Abstract. A sample of lithium niobate crystal with known thickness is set on a vertical rotary stage, placed in
between two crossed plane polarizers and illuminated by a collimated beam of white light. The sample is rotated
to an appropriate position, and interference fringes observed behind an analyzer are recorded by a fiber-optic
spectrometer. The recorded channeled spectrum is then analyzed, and from measured positions of interference
minima (dark fringes) and known crystal’s thickness, the group birefringence of the crystal sample is obtained
as a function of wavelength. The fringe order versus position of the fringe within the spectrum is fitted by
appropriate dispersion function, and as the result phase birefringence as a function of wavelength is found.
The measurement is performed for a sample declared as undoped, a sample doped with 0.025 wt. % of Fe,
and a sample doped with 0.025 wt. % of Fe and 0.075 wt. % of Mn in the wavelength ranges (470 to 780) nm
and (900 to 1700) nm. A good agreement between group birefringence dispersion obtained from positions of
interference minima and known sample’s thickness and that calculated from phase birefringence dispersion
given by Sellmeier dispersion model (used for undoped sample) and Cauchy model (used for doped samples)
is found. © 2019 Society of Photo-Optical Instrumentation Engineers (SPIE) [DOI: 10.1117/1.OE.58.3.034101]
Keywords: phase birefringence; group birefringence; lithium niobate; polariscope; interference fringes; channeled spectrum.
Paper 181761 received Dec. 9, 2018; accepted for publication Feb. 15, 2019; published online Mar. 5, 2019.

1 Introduction properties,21–24 they do not cover the huge amount of really


Lithium niobate (LiNbO3 or LN) belongs to one of techno- existing cases. It is understandable as these include various
logically the most important crystalline materials intended combinations of dopants mixed with various mutual concen-
mainly for holographic data storage1,2 and constructing trations. So, according to the definition of birefringence,
integrated optics and photonics devices, such as optical for determining the birefringence of an anisotropic sample,
waveguides,3 modulators,4,5 lightwave circuits in combina- one has to measure directly the dispersion of the refractive
tion with silicon,6 sensors,7 photovoltaic optoelectronic indices, both no and ne first, and after that use them for
tweezers,8 and substrates for manipulation and patterning of calculating the birefringence.25 In general, performing the
nanoobjects,9 to illustrate the wide scope of its use. However, measurement of refractive index dispersion is not, indeed,
due to its natural uniaxial birefringence, a crystal plate with an easy task. Fortunately, there is another way of determining
appropriate thickness can be utilized also as a passive optical the birefringence of an optically anisotropic sample that does
retarder or even an active one due to existence of rather not require knowledge of dispersion of refractive indices.
The method is appropriate to use in case we need to know
strong electro-optic effect observed in LiNbO3 crystals. The
just the birefringence itself. It is based on observation of bire-
birefringence, for example, can be used for determination of
fringence by means of a set of polarizers and analyzing the
the Li/Nb ratio in LiNbO3 ,10 and, recently, Twu and Chu11
intensity of light behind the analyzer.26,27
showed usefulness of measuring the so-called photorefrac-
tive birefringence for analyzing the photorefractive effect in 2 Experiment
photorefractive crystals.
As doping influences the refractive index,12–15 the bire- 2.1 Principles of the Method
fringence of a crystal will depend on the type and the amount
The method of investigation is based on a well-known fact
of the used doping element. Naturally, in order to determine
that a monochromatic linearly polarized light wave entering
the birefringence, it is necessary to know the dispersion of a uniaxially birefringent medium in a proper way exists in-
ordinary and extraordinary refractive indices. In case of side the medium in two mutually orthogonal linear polariza-
LN, such dependences were derived for undoped congruent tion states that propagate within the medium with different
crystal16–18 and magnesium-doped crystal18–20 but are not velocities and are characterized by refractive indices no and
available for crystals doped by many other elements or by ne . The resulting polarization state of light wave at the end of
combinations of multiple elements and in different ratios. the birefringent medium is determined by a phase retardation
Though measured data of dispersion of ordinary (no ) and δ between these two polarizations, i.e.,
extraordinary (ne ) refractive indices do exist for LN crystals
doped by some elements significantly influencing the crystal 2π 2π
δ¼ · d · ðne − no Þ ¼ · d · Δn; (1)
λ λ
EQ-TARGET;temp:intralink-;e001;326;118

*Address all correspondence to Norbert Tarjányi, E-mail: tarjanyi@fyzika


.uniza.sk 0091-3286/2019/$25.00 © 2019 SPIE

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Tarjányi and Káčik: Group and phase birefringence dispersion of pure and doped lithium. . .

where λ is the wavelength of light in vacuum, d is the geo-


metrical thickness of the medium, and Δn denotes the phase
birefringence.
If the wave at the output of the medium is linearly polar-
ized again, by rotating a plane polarizer (usually called ana-
lyzer) placed between the end of the birefringent medium
and a detector one will experience changing intensity of light
depending on the analyzer’s angle of rotation.
In case a polychromatic polarized light source is used
for illuminating the birefringent medium, the situation is
basically the same. The only difference is that with an angle
of rotation of the analyzer the intensity of light will change
for each color in a different way. This effect is due to depend-
ence of the phase retardation δ on the wavelength, as the no
and ne are functions of wavelength, too. Thus, for the prop-
erly oriented birefringent sample and rotating the analyzer, Fig. 1 Experimental setup for investigating the birefringence in LN
one will observe modulated spectrum of light, i.e., interfer- crystals. The double-sided black arrows denote the orientation of the
ence pattern or interference fringes.27 In general, the intensity plane of polarization. “z” is the optical axis of the crystal.
observed behind the analyzer depends on the angles of rota-
tion of the analyzer, the sample, and the polarizer used for
polarizing light incident on the sample. For example, if we of two plane polarizers and a white light source. The inves-
set the polarizer and the analyzer to be fixed in a mutually tigated samples were small plates of lithium niobate declared
crossed positions, i.e., their planes of polarizations are per- as pure, doped with 0.025 wt. % of Fe; and with 0.025 wt. %
pendicular to each other, the intensity of light leaving the of Fe and 0.075 wt. % of Mn with thicknesses ð1.072 
analyzer will depend on the retardation δðλÞ and the angle γ 0.001Þ mm, ð1.055  0.002Þ mm, and ð0.995  0.002Þ mm,
that makes a chosen axis (fast or slow) of the birefringent respectively. The undoped sample was provided by Crytur,
sample with the analyzer’s plane of polarization27 Ltd. (Czech Republic); the provider of the doped samples
was Photox, Ltd. (Great Britain). A crystal sample under
I ∝ ½sinð2γÞ2 · fsin½δðλÞ∕2g2 :
EQ-TARGET;temp:intralink-;e002;63;455 (2) investigation was set on a rotary stage enabling rotation
by 360 deg and placed in between two crossed plane polar-
The dispersion of group birefringence of the sample with izers. Two sets of polarizers were used: one designed for VIS
known thickness can be evaluated from positions of the (400 to 800) nm and one designed for NIR (900 to 1700) nm
successive minima (or maxima) of the interference fringes. spectral region. As the light source, a halogen lamp-based
Applying the condition for observing the minimum of inter- source SLS201/M (from Thorlabs) was used. Light behind
ference from Eqs. (1) and (2), we get for the group bire- the analyzer was focused by a lens with a focal length f ¼
fringence25,27 25 mm onto an optical fiber end and collected by optical-
fiber spectrometers (OFS) HR2000þ (from Ocean Optics) in
λ1 λ2 VIS and NIRQuest 512 (from Ocean Optics) in NIR spectral
Δng ¼ ; (3)
ðλ1 − λ2 Þ · d regions. Both spectrometers were equipped with optical fiber
EQ-TARGET;temp:intralink-;e003;63;358

of 50 μm diameter and numerical aperture NA equal to


where λ1 and λ2 are the wavelengths corresponding to suc- 0.22 (Fig. 1).
cessive minima of the order m and m þ 1, respectively.
Knowing the dispersion dependences for ordinary and extra- 3 Results and Discussion
ordinary refractive indices, one can calculate the dispersion Prior to investigation, all samples were put into an oven and
of the phase birefringence Δn from which one gets the group kept heated at 110°C for 4 h to ensure any possible photo-
birefringence according to [e.g., Ref. 28] refractive inhomogeneities induced due to previous acci-
dental illumination were erased. After placing the sample
∂Δn on the rotary stage, it was rotated to a proper position.
Δng ¼ Δn − λ · : (4)
∂λ For all investigated samples, the value of the angle γ between
EQ-TARGET;temp:intralink-;e004;63;247

polarizing plane of the analyzer and the optical axis (“z”-


If dispersion dependences for the material are not known, axis) of the crystal was set to π∕4 in order to excite ordinary
one can follow the approach used by Hlubina29 and obtain and extraordinary waves inside the crystal equally, thus get
the phase birefringence by finding the appropriate dispersion the best observable interference pattern behind the analyzer.
function that fits to the measured dependence of the fringe However, any other values from interval ð0; π∕2Þ could be
order versus position of the fringe within the spectrum. chosen, just the magnitude of the signal would change. The
The dispersion function found in this way can then be used end of the optical fiber collecting light did not change its
to calculate the group birefringence dispersion according position during the whole measurement for VIS (NIR) spec-
to Eq. (4). tral region, only samples and polarizers were replaced. The
magnitude of the signal measured by spectrometers could
also be controlled by integrating time, which was set to 5 ms
2.2 Experimental Set-Up when measuring samples with HR2000þ in VIS spectral
The birefringence of LN crystal samples was investigated region and 100 ms for measurements with NIRQuest 512 in
by an optical setup called plane polariscope. It consisted NIR spectral region.

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Tarjányi and Káčik: Group and phase birefringence dispersion of pure and doped lithium. . .

3.1 Group and Phase Birefringence of Undoped a2o;e þ b1o;e · fðtÞ


EQ-TARGET;temp:intralink-;e005;326;752

LN Crystal n2o;e ðλ; tÞ ¼ a1o;e þ


λ − ½a3o;e þ b2o;e · fðtÞ2
2

In Figs. 2(a) and 2(b), there are shown channeled spectra þ b3o;e · fðtÞ þ a4o;e · λ2 ; (5)
measured for undoped LN crystal in VIS and NIR spectral
regions, respectively. From the measured dependences, we where fðtÞ ¼ ðt − t0 Þ · ðt þ t0 þ 546°CÞ, t0 ¼ 24.5°C, t ¼
determined wavelengths λm and λmþ1 (m denotes the fringe 25°C, λ is the wavelength in nanometers and coefficients
order) corresponding to neighboring minima and computed appearing in Eq. (5) are as follows:24 a1o ¼ 4.9048, a2o ¼
group birefringence according to Eq. (3). However, the value 1.1775 · 105 nm2 , a3o ¼ 2.1802 · 102 nm, a4o ¼ −2.7153 ·
of Δng obtained from wavelengths λm and λmþ1 is an average 10−8 nm−2 , b1o ¼ 2.2314 · 10−2 nm2 °C−1 , b2o ¼ −2.9671 ·
value corresponding to the wavelength interval (λm , λmþ1 ) 10−5 nm °C−1 , b3o ¼ 2.1429 · 10−8 °C−1 , a1e ¼ 4.5820,
so when plotted, these values of the group birefringence a2e ¼ 0.9921 · 105 nm2 , a3e ¼ 2.1090 · 102 nm, a4e ¼
were assigned to wavelengths corresponding to central wave- −2.1940 · 10−8 nm−2 , b1e ¼ 5.2716 · 10−2 nm2 °C−1 , b2e ¼
lengths of the particular intervals (λm , λmþ1 ). −4.9143 · 10−5 nm°C−1 , and b3e ¼ 2.2971 · 10−8 °C−1 .
As can be seen in Fig. 2, the visibility of the interference The values of Δn were then used for calculating the group
pattern is lower for shorter wavelengths. This is due to a lim- birefringence dispersion according to Eq. (4) and the result
ited resolving power of the spectrometers the measuring is shown in Fig. 3.
steps of which were 0.4 and 2.3 nm for VIS and NIR spectral
regions, respectively. 3.2 Group and Phase Birefringence of LN:Fe and
Moreover, in case of VIS spectral region, the effect could LN:Fe:Mn
also be combined with increased absorption of short wave-
lengths in LN crystal. These facts are reflected in the calcu- The same measuring procedure was repeated also for the LN:
lation of the group birefringence and as the result Δng shows Fe and LN:Fe:Mn samples. The recorded channeled spectra
increased variance in the spectral region with lower visibility. for the investigated samples are shown in Fig. 4. The dis-
persion of the group birefringence was obtained in the same
To reduce this variance, the computed values of the group
way as in case of the undoped LN, i.e., we determined the
birefringence were smoothed by the piecewise use of a sym-
wavelengths of neighboring minima and computed group
metric nearest-neighbor linear least-squares fitting on each
birefringence according to Eq. (3).
element in originally measured data set, in which the number
As Eq. (5) with coefficients listed in Sec. 3.1 cannot be
of nearest neighbors was adaptively chosen. correctly used for calculating the phase birefringence for
Since dispersion relations for ordinary and extraordinary doped samples, we used an approach applied by Hlubina.29
refractive indices of undoped congruent LN are known, one We fitted the fringe order versus position of the fringe within
can calculate the phase birefringence dispersion Δn and then, the spectrum by appropriate dispersion function and found
using Eq. (4) also the dispersion of the group birefringence phase birefringence as a function of wavelength.
Δng . The Δn was calculated using Sellmeier equations for From Eq. (5) and according to comparison between the
ne and no given in the generic form24 characters of the dependences shown in Figs. 2 and 4, one

(a)

(b)

Fig. 2 The channeled spectra for LN crystal obtained in (a) VIS and (b) NIR spectral regions.

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Tarjányi and Káčik: Group and phase birefringence dispersion of pure and doped lithium. . .

Fig. 3 Group birefringence dispersion for undoped LN crystal obtained from recorded channeled
spectra (and smoothed) and calculated from phase birefringence according to Eq. (4).

(a) (c)

(b) (d)

Fig. 4 The channeled spectra measured in VIS and NIR spectral regions for (a, b) LN:Fe and
(c, d) LN:Fe:Mn crystals, respectively.

can deduce that used samples of LN, both doped and un- d 104 · d 109 · d
doped, behave like a material with normal dispersion. Aþ 3
Bþ C ¼ m þ k; (8)
λ λ λ5
EQ-TARGET;temp:intralink-;e008;326;319

Therefore, the three-term Cauchy equations might be suit-


able for describing no and ne 30 k being the number of observed distinguishable interference
minima. Fitting Eq. (8) to the dependence of the fringe order
104 · Bo;e 109 · Co;e versus position of the fringe within the spectrum gives the
no;e ðλÞ ¼ Ao;e þ þ ; (6) values of the parameters A, B, C, and m. Figure 5 shows the
λ2 λ4
EQ-TARGET;temp:intralink-;e006;63;275

dependences of the fringe order on the wavelength obtained


where λ is the wavelength in nanometers and Ao;e , Bo;e , Co;e from the channeled spectra for LN:Fe and LN:Fe:Mn (in VIS
are the parameters of the equation characterizing the birefrin- and NIR spectral regions) that are shown in Fig. 4.
gent medium. For simplicity, the form of Eq. (6) considers The parameters A, B, and C obtained by fitting were used
the used LN crystals are a well-transparent media. From for calculating the phase birefringence according to Eq. (7).
Eq. (6), we get for the phase birefringence dispersion From the phase birefringence, the dispersion of the group
birefringence was calculated using Eq. (4) and comparison
between measured and calculated dependences for samples
104 · B 109 · C LN:Fe and LN:Fe:Mn is shown in Figs. 6(a) and 6(b).
ΔnðλÞ ¼ A þ þ ; (7)
λ2 λ4
EQ-TARGET;temp:intralink-;e007;63;177

We can estimate the accuracy of determination of the


phase birefringence dispersion if the wavelength λ of the
where A ¼ ðAo − Ae Þ, B ¼ ðBo − Be Þ, and C ¼ ðCo − Ce Þ. minimum is known with an error δλ and the thickness d
According to Eq. (2), the interference minimum is observed of the sample is known with an error δd.29 For the error
when δ∕2 ¼ mπ. Applying Eqs. (1) and (7) into this condi- δλ given by the measuring step of the spectrometers that
tion, we can write for k interference minima observed in the equals 0.4 nm for VIS spectrometer and 2.3 nm for NIR
channeled spectrum spectrometer and the error δd ¼ 1 μm for undoped sample

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Tarjányi and Káčik: Group and phase birefringence dispersion of pure and doped lithium. . .

(a) (c)

(b) (d)

Fig. 5 Dependence of the fringe order on wavelength obtained from channeled spectra measured in VIS
and NIR spectral regions for (a, b) LN:Fe and (c, d) LN:Fe:Mn crystals, respectively. Crosses and squares
denote measured data; the fitting curve is represented by the solid line.

(a)

(b)

Fig. 6 Dispersion of group birefringence for (a) LN:Fe and (b) LN:Fe:Mn crystals computed from
recorded channeled spectra according to Eq. (3) and calculated from phase birefringence according
to Eq. (4).

and δd ¼ 2 μm for doped samples, the relative error of the The obtained dependences of the group and phase bire-
measurement of the phase birefringence dispersion is less fringences on wavelength for all investigated samples are
than 2.2 · 10−3 for all measurements performed in VIS spec- shown in Figs. 7(a) and 7(b), respectively. It is apparent that
tral region and less than 3.2 · 10−3 for measurements in NIR all curves are well distinguishable from each other. This
spectral region. means the doping affects the dispersion of refractive indices

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Tarjányi and Káčik: Group and phase birefringence dispersion of pure and doped lithium. . .

(a)

(b)

Fig. 7 (a) Computed data representing group birefringence dispersion and (b) phase birefringence
dispersion of LiNbO3 samples with different dopants.

and thus the birefringence of the LN crystal significantly. region. One can achieve higher accuracy using the spectrom-
The result is consistent with findings of Bodnar and eter with the smaller measuring step and/or using a thicker
Yarunichev who explored the effect of impurities introduced sample. The obtained results confirm that the method is suit-
into LN crystal on refractive indices dispersion.31 According able for determining the dispersion of the group birefringence
to their findings, the extraordinary refractive index of without knowing the dispersion dependences of the refrac-
LiNbO3 increases due to Fe doping and decreases due to tive indices and can be used for simple and nondestructive
Mn doping. estimation of the crystal composition.
From Fig. 7, it can be clearly seen that the birefringence
of LN:Fe sample is higher than that of the pure LN crystal. Acknowledgments
The birefringence of the LN:Fe:Mn sample is higher than This work was supported by Slovak National Grant Agency
birefringence of the pure LN but lower than that of doped No. 1/0069/19, Slovak Research and Development Agency
by iron. In this sample, the effect of Fe and Mn impurities under the projects Nos. APVV-15-0441 and APVV-SK-
acts against each other resulting in birefringence dispersion FR-2017-0017 as well as by project ITMS: 26210120021,
curve being in intermediate position comparing to LN:Fe and cofunded from EU sources and European Regional Develop-
LN cases. ment Fund. We declare that we have no financial interests in
the manuscript and no competing conflicts of interest with
4 Conclusions any persons or organizations.
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19. A. L. Aleksandrovskii et al., “Dispersion of the refractive indices of Physics, University of Žilina, Slovakia. He received his MS and PhD
LiNbO3 ∶Mg and LiNbO3 ∶Y crystals,” Sov. J. Quantum Electron. degrees from the University of Žilina in telecommunication engineer-
21(2), 225–227 (1991). ing in 1999, and in physics of condensed matter and acoustics in
20. K. Maaider et al., “New approach to study the influence of the defect 2004, respectively. His current research interests include photoelas-
structure on the refractive indices of Mg-doped lithium niobate,”
Moroccan J. Condensed Matter 12(2), 155–158 (2010). ticity of polymers and birefringence. He is a member of the European
21. K. Chah et al., “Influence of chromium doping on the electro-optic Physical Society.
properties of lithium niobate,” Opt. Commun. 136(3–4), 231–234
(1997). Daniel Káčik: Biography is not available.

Optical Engineering 034101-7 March 2019 • Vol. 58(3)

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