Photonics Based on Wavelength Integration and Manipulation

IPAP Books 2 (2005) pp. 187–192

Spatial Light Modulators and Surface Relief Gratings Using an Electrooptic Polymer

Kenji HARADA *,1, Masahide ITOH2 and Toyohiko YATAGAI2

1
Department of Computer Science, Kitami Institute of Technology, 165 Koen-cyo, Kitami 090-8507, Japan
2
Institute of Applied Physics, University of Tsukuba, 1-1 Tennodai, Tsukuba 305-8573, Japan

An electrically addressed spatial light modulator is designed using nonlinear azobenzene polymer. A modulation efficiency of
4.7% has been realized with 5.1 V rms applied voltage at a wavelength of 633 nm. Very fast modulation at over 10 MHz was
demonstrated. Surface relief gratings are a lso fabricated by irradiation of laser interference patterns on a zobenzene polymer film.
Functionalized surface relief holograms are investigated.

KEYWORD: spatial light modulator, surface relief, hologram, electrooptic polymer, azobenzene polymer, corona poling, corona
charging

1. Introduction 0 0 r13
Nonlinear organic materials are very attractive because of 0 0 r13
their large optical nonlinearity and short response times. 0 0 r33
Polymer films are one of the most promising organic ,
materials. Liquid crystal spatial light modulators (SLMs) 0 r13 0
generally used in optical computing have a very slow r13 0 0
modulation speed and a low contrast ratio. Development of 0 0 0
sophisticated SLMs with very fast modulation speed is
where r33=3r13.
essential. A candidate for SLM material is an amorphous
For an electric field in the direction of the surface
nonlinear polymer. These are very attractive for
normal(z-direction), the equation for the refractive index
electrooptical applications. Their fabrication is easy
ellipsoid is
compared with growing single crystals of organic and
 1   
inorganic materials. The dielectric constants of polymeric
materials are approximately 3, which is 1/10 of LiNbO3. A

 n2
+ r13 E z ( 
)
 X 2 + Y 2 +  1 + r33 E z  Z 2 = 0 ,
 n2 
(1)
 0   e 
low dielectric constant makes it possible to operate polymer
where X, Y, and Z refer to the laboratory axes parallel to the
devices at a very high frequency.1)
principal dielectric axes of the film, and n 0 and n e are the
Recently, direct fabrication of relief structures in a zo-
ordinary and extraordinary refractive indices respectively.
polymers have been reported.2-5) A surface relief structure
On application of an electric field in the direction of the
is recorded through photoisomerization and the movements
surface normal, the change in refractive index experienced
of polymer chains.6,7) The surface relief structure is
by an ordinary ray is thus,
fabricated by irradiation of interference laser fringes onto
1 3
azobenzene functionalized polymers such as side-chain- ∆ n0 = − n 0 r13 E z (2)
type and main-chain-type azo-polymers. The relief structure 2
is stable at room temperature, and can be erased by heating and for an extraordinary ray,
at over the glass transition temperature. 1 3
∆ ne = − ne r33E z . (3)
In this report, an electrically addressed spatial light 2
modulator is designed using nonlinear azobenzene Changes in the indices of refraction experienced by the
polymer.[P4] We have simulated and demonstrated the ordinary ray can be related to the modulation voltage V by
electrically induced changes in light intensity using the expressions, using (2) as
polymeric thin film in a Fabry-Perot structure. Surface relief 1 3 V
nonlinear optical devices are also fabricated by irradiation ∆ n0 = − n 0 r13 (4)
2 l
of laser interference patterns on azobenzene polymer
where l is the separation between the two indium tin oxide
film.[P7-16,P18,P20] Electrically controlled hologram and second-
(ITO) electrodes. This induced ∆ n 0 changes the device
harmonic generating hologram are investigated.
transfer characteristics by the phase change in the
polymeric layer. The use of a resonator structure is
2. Polymeric Spatial Light Modulators
proposed to minimize the driving voltages. Figure 1 shows
2.1 Simulation the device structure. A polymer film was sandwiched
We simulated the light modulation of the polymeric between dielectric mirrors. Quarter-wave stacks of dielectric
Fabry-Perot etalons. A film poled in the direction of the material are arranged in such way t hat alternating layers
surface normal has its electrooptic tensor expressed as have a low index of reflection n 1=1.46 (SiO2) and a high
index of reflection n 2=2.35 (TiO2). The thicknesses of the
*e-mail address: haraken@cs.kitami-it.ac.jp layers are λ /4n 1, and λ /4n 2, where λ is the free-space
wavelength (633 nm). The t ransmission spectrum can be

187
188 Photonics Based on Wavelength Integration and Manipulation IPAP Books 2

calculated theoretically by solving the boundary condition

of each layer. The device shows a sharp spectrum in a 1.0

Transmittance
specific wavelength determined by the polymer film
0.8
thickness and refractive index. Figure 2 shows the
calculated transmission spectrum when each dielectric 0.6
mirror is composed of 10 layers and the optical thickness of
the polymer is λ /2, where λ is the free-space wavelength 0.4
(633 nm). In this simulation, there is no optical loss of the
sample. We can control the intensity of monochromatic 0.2
light by changing the refractive index of the polymer by 0.0
applying an electric field. Figure 3 shows the applied 500 550 600 650 700 750 800
voltage dependence of transmission spectrum at around Wavelength (nm)
633 nm when each dielectric mirror is composed of 10 layers
and the electrooptic coefficient is 20 pm/V. Transmission Fig. 2 Calculated transmission spectrum when each
peak shifts by applying an electric field. The contrast ratio dielectric mirror is composed of 10 layers.
of 10 layered sample in this case is estimated as
0 V/µm
approximately 40:1 when the applied voltage is 50 V/µm. 10 V/µm
1.0 25 V/µm
50 V/µm
2.2 Experiment 0.8

Transmittance
A polymeric spatial light modulator with 5 ×5 pixels is
designed. Side-chain polymer poly-orange tom-1 0.6
isophoronedisocyanate is used as a polymeric material in
0.4
this study. Figure 4 shows the chemical structure of poly-
orange tom-1 isophoronedisocyanate. The polymer has 0.2
large second or third nonlinearity.[P5,P 19] Absorption
spectrum of the material is shown in Fig. 5. Cutoff 0.0
632.0 632.5 633.0 633.5
wavelength of the material is approximately 600 nm and it is
Wavelength (nm)
transparent at 633 nm. The glass transition temperature Tg is
136° C. The refractive index is 1.7 at a wavelength of 633 nm. Fig. 3 Applied voltage dependence of transmission
The electrooptic coefficient r33 is measured by a reflection spectrum when each dielectric mirror is composed of 10
technique.8) The measured electrooptic coefficient r33 is 23 layers and electrooptic coefficient is 20 pm/V.
pm/V at the wavelength of 633 nm. The half-wave voltage NH
of the device using this material is estimated to be H3C
approximately 20 kV. The use of a resonator structure is O N O NH
proposed to minimize the driving voltages. The polymer O O H3C CH3
dissolved in cyclohexanone is spin-coated on the glass
plate with a multilayered dielectric mirror and an ITO n
electrode. Then another multilayered dielectric mirrors and
N
ITO electrode are coated on the polymer film. Photo- N
assisted poling was performed to align the chromophore
orientation with an applied voltage of 100 V across the
polymer film for 20 min by irradiating an Ar+ laser.
CN
(n 2=2.35) ITO glass plate
(n 1=1.46) Polymeric material Fig. 4 Chemical structure of poly-orange tom-1.
a
a 0.8
a
Absorbance

a 0.6

a 0.4

a
0.2
a

λ /4n 1 λ /2n 3 λ /4n 2 0.0

400 500 600 700 800
W a v e l e n g t h ( n m )

Fig. 1 Resonator structure for polymeric materials. Fig. 5 Absorption spectrum of poly-orange tom-1.
Photonics Based on Wavelength Integration and Manipulation IPAP Books 2 189

There are simple matrices with 25 pixels and the size of

one pixel is 1 mm×1 mm. Each mirror is composed of 12
layers. The reflectivity of the dielectric mirror is

Modulation efficiency (a.u.)

approximately 95% at the wavelength of 633 nm.
Using a spectrometer (Nihon Bunko Co.,Ltd., Jusco-530),
we measured the transmittance characteristics of the device
when the incident light was normal to the sample (Fig. 6).
The spectrum of the device has sharp peaks at 590 nm and
680 nm. A He-Ne laser (633 nm) is used in this experiment.
There is no transmission peak at 633 nm. Maximum
modulation efficiency is expected by choosing the
transmission peak at the experimental wavelength. By
changing the input angle, we can adjust the transmission
0 5 10
peak at a proper wavelength. Figure 7 shows the angle
Time (ms)
dependence of transmission intensity at the wavelength of
633 nm. A maximum transmittance of 20% is obtained at the Fig. 8 Light modulation of laser beam. Current voltage of 1
incident angle of 47°. kHz with 5.1 V rms is applied.
Figure 8 shows the results of the light modulation at the
input angle of 47°. A m odulation efficiency of 4.7 % is
obtained at 1 kHz with 5.1 V rms applied voltage. A
maximum modulation efficiency of 18.8% is obtained at an
applied voltage of 34 V rms. Figure 9 shows the frequency
dependence of light modulation. Operation at 10 MHz is
demonstrated with each pixel.
50

40
Transmittance (%)

30
Fig. 9 Frequency dependence of light modulation.
20
3. Surface Relief Optical Device
10 3.1 Recording of surface relief grating
The surface relief grating is fabricated by the irradiation
0 of two-beam interference fringes. The experimental setup is
400 500 600 700 800 shown in Fig. 10. A polarized Ar+ laser beam at a
Wavelength (nm) wavelength of 488 nm is used as the light source. The laser
beam is collimated to 6 mm in diameter, half of the laser
Fig. 6 Transmittance characteristics of device. beam is reflected by a mirror and the two beams interfere on
the sample. The angle between the sample and the mirror is
90° and the period of the grating can be adjusted by
0.20 varying the angle θ between the beam propagation axis and
mirror plane.
Figure 11 shows the polarization dependence of
Transmittance

0.15
diffraction efficiency. The period of the surface relief
grating is selected as 1 µm. There is a strong polarization
0.10 dependence of recording of the writing laser beam. A high
diffraction efficiency is obtained using a p- or circularly
0.05 polarized writing beam. The relief structure is not recorded
using an s-polarized writing beam. A high diffraction
efficiency can be obtained in a short time by high-power
0.00 recording. Figure 12 indicates an atomic force microscopy
0 10 20 30 40 50 60
Input angle (degree) image of a surface relief structure recorded using a p -
polarized beam. The laser beam power was 220 mW/cm2 for
Fig. 7 Angle dependence of transmission intensity at 10 min. A minimum relief structure of 275 nm period was
wavelength of 633 nm. recorded. The surface relief depth was 16 nm.
190 Photonics Based on Wavelength Integration and Manipulation IPAP Books 2

+
Ar laser Collimator Mirror
488nm

θ
λ /2 phase plate
Sample

Fig. 10 Optical setup for surface relief grating fabrication

by the surface deformation method.

25 Fig. 12 Atomic force microscopy image of surface relief

s polarization
20 p polarization structure.
Efficiency (%)

circular polarization
15
10
5
0
0 5 10 1 5 2 0 25 30
Time (min)

(a)
Fig. 11 Polarization dependence of diffraction efficiency.

3.2 Recording of rewritable hologram

Surface relief structures were fabricated by irradiation of
interference fringes. This structure can be erased by
heating above Tg. Figure 13 shows a n example of surface
relief image before and after heating. The relief structure
was erased by heating. We fabricated the rewritable Fresnel
hologram on polymer films. Polarized Ar+ laser (488 nm) at a (b)
power of 69 mW/cm2 is used. Japanese chess pieces are Fig. 13 Surface structures (a) before and (b) after heating.
used as specimens. Recording time was 15 min and erasing
time was 30 s at Tg. Figure 14 shows the reconstructed
image of the hologram using the He-Ne laser. They are
successfully reconstructed and erased.

3.3 Electrically controlled hologram

3.3.1 Control by corona charging
Diffraction efficiency and relief depth of a surface relief
structure is markedly increased by corona charging at
temperatures near or above Tg.[P1-3] This increase depends 1cm
on the corona charging conditions, specifically, corona
charging temperature, applied voltage and corona charging
time. Figure 15 shows the corona charging setup. The
electric charge was deposited on the surface relief grating
using this setup. A sharp needle electrode was positioned
above the ground electrodes. An azobenzene polymer film
was placed on the ground electrode. Surface relief structure
can be made using this setup with the irradiation of Ar+
laser. In the corona charging process, voltage was applied
at a temperature near Tg and the polymer film was heated to
the corona charging temperature with applied voltage,
because the surface relief structure is thermally erased
above Tg without applied voltage. Fig. 14 Reconstructed image of rewritable hologram.
Photonics Based on Wavelength Integration and Manipulation IPAP Books 2 191

Electric charge is deposited on the surface relief structure

in a corona-depositing poling setup at the glass transition
temperature. First-order diffraction efficiency is monitored

Surface relief depth (nm)

using a He-Ne laser. Figure 16 shows the measurement of
the surface relief depth control of the hologram. The
recording condition of the surface relief structure was 220
mW/cm2 for 30 s. A voltage of 6.5 kV was applied to the
sample at the glass transition temperature at t = 50 s. The
surface relief depth of the recorded hologram was increased
by corona charging. At t = 250 s, the applied voltage of
corona charging was turned off and the surface relief depth
of the recorded hologram was decreased. The diffraction Time (s)
efficiency of the hologram was dependent on the applied
voltage of the corona charging.[P3] Figure 17 shows the Fig. 16 Surface relief depth control of the hologram.
reconstructed images of an electrically controlled hologram.
By changing the charging conditions, the diffraction
efficiency of the image can be controlled.

3.3.2 Control by electrooptic effect

Surface relief deformation by corona charging is very
large, but the response time is rather slow. A higher
modulation speed can be expected using the electrooptic
effect. A surface relief electrooptic holographic grating is
also fabricated. After poling the surface relief grating with
an ITO-coated glass plate, an Al electrode was evaporated
on the grating. The poled sample exhibits the electrooptic
effect and the refractive index can be electrically modulated.
The measured electrooptic coefficient r33 is 23 pm/V. The
modulation efficiency of the electrooptic grating at a
wavelength of 633 nm is measured. The voltage was applied Fig. 17 Reconstructed image of electrically controlled
between the two electrodes. The modulation of the first- hologram.
order diffraction intensity is measured by a lock-in amplifier.
The modulation efficiency of the first-order diffraction beam 2
power vs applied voltage is shown in Fig. 18. The
Modulation (%)

modulation efficiency is proportional to an applied voltage. 1.5

The modulation efficiency at 1 kHz with 30 Vp -p is 1.7%.
Light modulation at 2 MHz is demonstrated. 1

0.5

0
He-Ne laser 0 10 20 30
Ar+ laser Applied voltage (Vp-p)
needle

Fig. 18 Modulation efficiency of electrooptic grating.

V
3.4 Second-harmonic generating (SHG) hologram
à à à à Fourier transform hologram is recorded using an Ar+ laser
azobenzene at the wavelength of 514 nm for 15 min. Character “A” was
used as an input image. The sample was corona-poled for
glassplate 10 min to align the chromophore orientation. The hologram
electrode has second-order nonlinearity and generates a wave at the
double frequency. It forms the reconstructed image without
heater
any delay. Figure 19 show the reconstructed hologram. A
Nd:YAG laser at the wavelength of 1064 nm is used to
reconstruct the hologram. A double-frequency hologram
Fig. 15 Corona charging setup. (532 nm) is successfully reconstructed. Th e c onversion
efficiency of the SHG hologram was 0.00002%.
192 Photonics Based on Wavelength Integration and Manipulation
Fig. 19 Reconstructed image of SHG hologram.
4. Conclusions
Surface relief optical devices were fabricated by
irradiation of laser interference patterns on an azobenzene
polymer film. The diffraction efficiency of the hologram
could be electrically controlled. A second-harmonic
generating hologram was also investigated. We have
already reported the application for a waveguide laser
amplifier.[P6,P17,P21] This fabrication technique can be applied
to holographic devices.
References
1) C. C. Teng: Appl. Phys. Lett. 60 (1992) 1538.
2) D. Y. Kim, L. Li, X. L. Jiang, V. Shivshankar, J. Kumar and S. K.
Tripathy: Macromolecules 28 (1995) 8835.
3) C. J. Barrett, A. L. Natansohn and P. L. Rochon: J. Phys. Chem.
100 (1996) 8836.
4) N. C. R. Holme, L. Nikolva, P. S. Ramanujam and S. Hvilsted:
Appl. Phys. Lett. 70 (1997) 1518.
5) M. Itoh, K. Harada, H. Matsuda, S. Ohnishi, A. Parfenov, N.
Tamaoki and T. Yatagai: J. Phys. D: Appl. Phys. 31 (1998)
463.
6) C. J. Barrett, P. L. Rochon and A. L. Natanshon: J. Chem. Phys.
109 (1998) 1505.
7) D. Y. Kim, S. K. Tripathy, L. Li and J. Kumar: Appl. Phys.
Lett. 66 (1995) 1166.
8) C. C. Teng and H. T. Man: Appl. Phys. Lett. 56 (1990) 1734.
Publications
Journal papers
[P1] K. Munakata, K. Harada, H. Anji, M. Itoh and T. Yatagai:
“Diffraction efficiency increase by corona discharge in
photoinduced surface-relief gratings on an azo polymer film,”
Optics Letters, Vol.26, No.1, pp.4-6 (Jan. 2001).
[P2] K. Munakata, K. Harada, H. Anji, M. Itoh and T. Yatagai: “A
new holographic recordin g material and its diffraction
efficiency increase effect: the use of photoinduced surface
deformation in azo-polymer film ,” Optics Communications,
Vol.191, Issues 1-2, pp.15-19 (May, 2001).
[P3] K. Harada, H. Inoue, M.A. El-Morsy, M. Itoh, S. Umegaki and
T . Yatagai: “ Holographic recording and control of diffraction
efficiency using photoinduced surface deformation on azo-
polymer films, ” Japanese Journal of Applied Physics, Vol.41,
No.3B, pp.1851-1854 (March, 2002).
[P4] K. Harada, K. Munakata, M. Itoh, S. Umegaki and T. Yatagai:
“ Spatial light manipulation devices using nonlinear polymeric
materials,” Optical and Quantum Electronics, Vol.34, Issue 12,
pp.1183-1189 (Dec. 2002).
[P5] C.C. Hsu, J.H. Lin, T.H. Huang and K. Harada: “ Temperature
dependent photoinduced third harmonic generation variation
in azo-doped polymer thin films, ” Applied Physics Letter,
Vol.82, Issue 15, pp. 2440-2442 (April, 2003).
IPAP Books 2
[P6] T . Hirose, T . Omatsu, R. Kato, K. Hoshino, K. Harada, T .
Watanabe and M. Fujii: “Azo-benzene polymer thin -film laser
amplifier with grating couplers based on light-induced relief
hologram,” Optics Communications, Vol. 228, Issues 4-6
pp.279-283 (Dec. 2003).
[P7] M. Itoh, K. Harada, S. Kamemaru and T. Yatagai:
“Holographic recording on azo-benzene functionalized
polymer film,” Japanese Journal of Applied Physics, Vol.43,
No.7B, pp.4968-4971 (July, 2004).
International conferences
[P8] K. Harada, K. Munakata, M. Itoh, S. Umegaki and T . Yatagai:
“ Photoinduced surface deformation on azo-polymer films and
its holographic application,” CLEO/Pacific Rim 2001, Chiba,
ThH1-2 (July, 19, 2001).
[P9] K. Harada, M. Itoh, S. Umegaki and T. Yatagai: “ Direct
fabrication method of surface relief structures on azo-polymer
films and it’s application,” 2nd Chitose International Forum
(CIF'2) on Photonics, Chitose, S5 -5 (Sep. 8, 2001).
[P10] K. Harada, H. Inoue, K. Munakata, M. Itoh, S. Umegaki and
T . Yatagai: “ Holographic recordings of surface relief structures
on azo-polymer films and its device applications, ” OSA
Annual Meeting 2001, Long Beach, OTuA4 (Oct. 16, 2001).
[P11] K. Harada, M. Itoh, H. Inoue, S. Umegaki and T . Yatagai:
“ Holographic recording using photoinduced surface
deformation on azo-polymer films, ” ISOM'01, Taipei, Th-J-
12 (Oct. 18, 2001).
[P12] K. Harada and T . Yatagai: “Holographic recording on azo-
polymer film,” SPIE, San Jose, SPIE proceedings Vol.4659
(Jan. 21, 2002).
[P13] K. Harada, H. Inoue, M. Itoh and T . Yatagai: “ Recording of
rewritable surface relief hologram on azo-polymer films, ” The
16th Sen’i Gakkai International Symposium, Tokyo, 2AS05
(May, 23, 2002).
[P14] T . Yatagai and K. Harada: “Surface relief DOE with azo-
polymer film,” IEEE/LEOS Annual Meeting, Glasgow, ML4
(Nov. 11, 2002).
[P15] K. Harada, T . Maeda, S. Kamemaru, M. Itoh and T . Yatagai:
“ Active surface relief hologram using azo benzene containing
polymer film ,” Optics in Engineering’03, Ivalo, A4 (Aug. 7,
2003).
[P16] M. Itoh, T. Yatagai, K. Harada and S. Kamemaru: “ Functional
surface relief hologram using azobenzene contain ing polymer
film,” ISOM’03, Nara, We-F-61 (Nov. 5, 2003).
[P17] T . Hirose, T . Omatsu, R. Kato, K. Hoshino, T . Watanabe and
K. Harada: “ Azo-benzene polymer thin -film laser amplifier
with grating couplers based on light-induced relief hologram,”
CLEO/Pacific Rim 2003, Taipei, TH4H-(7)-6 (Dec. 18,
2003).
[P18] K. Harada, T . Maeda, S. Kamemaru, T . Asami, M. Itoh and T .
Yatagai: “Holographic recording using azo-polymer film and
its replication,” CLEO/Pacific Rim 2003, Taipei, TH4H-(7)-6
(Dec. 18, 2003).
[P19] C.C. Hsu, J.H. Lin, T.H. Huang and K. Harada, “ Temperature
effect on photoinduced third harmonic generation variation in
azo polymer thin films, ” CLEO/Pacific Rim 2003, Taipei,
TH1F-(5)-3 (Dec. 18, 2003).
[P20] K. Harada, T. Maeda, M. Itoh, T. Yatagai and S. Kamemaru:
“ Application of surface relief hologram using azobenzene
containing polymer film,” ICO’04, Chiba, 13D2-49 (July, 13,
2004).
[P21] T. Hirose, T. Omatsu, T. Matsuo, K. Harada and K. Hoshino:
“Distributed feedback dye-doped polymer laser using light
induced surface relief hologram in azo-polymer film ,” ICO’04,
Chiba, 14D2-38 (July, 14, 2004).