We report on polymer liquid crystals with periodically oriented mesogenic side chains and demonstrate that the resulting two-dimensional polarization gratings multiplex-diffract the laser beam and convert the polarization state at the same time. Two-dimensional diffraction patterns with various kinds of polarization states can be successfully generated by designing a combination of one-dimensional polarization gratings. This study is a considerable advance towards the realization of highly functionalized passive optical devices that can control both the beam propagation direction and the polarization state.
©2003 Optical Society of America
The increasing need to manipulate optical signals, following in the wake of the introduction of fiber optics into communications, computations and the development of parallel optical information processing systems, has stimulated interest in highly functionalized optical devices. Polymers are widely exploited because of their advantages properties, including mechanical strength, stability, flexibility, low cost, and ease of processing. Furthermore, the promise of combining these properties with large optical anisotropy has prompted a great interest in polymer liquid crystals [1–4]. The usefulness of our recently proposed photo-cross-linkable polymer liquid crystals has been demonstrated by preparing thermally stable anisotropic optical films by the use of linearly polarized ultraviolet light and subsequent annealing [5–7]. The orientation direction of the mesogenic side chains in the polymer liquid crystal is parallel to the polarization direction of the linearly polarized ultraviolet light, and three-dimensional orientation is feasible by oblique irradiation with ultraviolet light.
Polarization holographic grating was first reported in the early 1980s . Theoretical and experimental research followed in the 1980s with the achievement of real-time recording and erasing in azo-dye-doped polymer films [9–10]. Since the 1990s, numerous studies have reported that irradiating polymers containing azobenzene molecules with linearly polarized light results in the reorientation of the azobenzene groups perpendicularly to the polarized light based on the axis-selective photoisomerization and creates polarization-dependent optical recordings [12–21]. These studies show the feasibility of recording an interference pattern formed by the interaction of two optical waves with orthogonal polarizations, both linear and circular, bearing information about the polarization of the object wave. Here, we report on polymer liquid crystals with periodically oriented mesogenic side chains and demonstrate that the resulting two-dimensional polarization gratings multiplex-diffract the laser beam and convert the polarization state at the same time. Because of their stable photochemically cross-linked structures, the pure polarization grating devices show high-temperature durability for a practical use.
2. Theoretical background of polarization conversion
The interference pattern of two coherent waves of equal amplitude and orthogonal polarizations (orthogonal linear; OL, and orthogonal circular; OC) has a constant intensity, but it has a polarization state that is periodically modulated. The interference pattern of two coherent waves, E 1 and E 2, of equal amplitude E and orthogonal polarizations has a constant intensity, but it has a polarization state that is periodically modulated as described in Table 1. In the case of orthogonal linear (OL) exposure, E 1 is vertically linearly polarized, while E 2 is horizontally linearly polarized, and the resulting two waves are linearly polarized waves with mutually perpendicular polarization directions. The resulting light field is described for the OL exposure case by [8, 13, 14, 22]
where the phase difference between two writing waves δ is a function of the position x and of the grating spacing Λ, and can be expressed as
In the case of orthogonal circular (OC) exposure, E 1 and E 2 are left- and right-hand side circularly polarized waves. The resulting light field is described for the OC exposure case by [8, 13, 14, 22]
Table 1 summarizes the polarization states of the two writing beams and the resulting electric field distribution of the two beams coupling for each irradiation mode.
We assume that only linear birefringence is induced in the polarization-sensitive material. In the case of OL exposure, the intensity of the interfering field is constant and only changes in the resultant polarizations among linear, elliptical, and circular states are effective as shown in Table 1. The characteristic ellipsoid does not change the direction of its principal axes but only its ratio. The Jones matrix describing the transmission of the recorded holograms has the form [8–10, 13, 14, 22]
where ere Δφ=πΔnd/λ, Δn is the photoinduced birefringence, d is the film thickness, and λ is the wavelength of the reading beam. The Jones matrix describing the holographic recording in the case of OC exposure is [8–10, 13, 14, 22]
for phase recording. In order to determine the polarization properties of the reconstructing light wave from the polarization holograms described by Eqs. (4) and (5), we consider the light field S diffracted from them, given by
where R is the reading beam. The polarization of S depends on the polarization of R. Table 2 summarizes the polarization properties of the reconstructing light on varying the polarization state of the reading beam.
3. Experimental results and discussion
In order to realize the optical device with the functions summarized in Table 2, polarization-sensitive materials, in which linear birefringence is induced by irradiating the polarized light, are necessary. As one of the candidates, numerous kinds of azobenzene-containing polymers have received a considerable amount of attention over the last decade [1–4, 8–21]. The polarization holographic recording originates in the photoinduced reorientation of the azo-dye molecules. These unique features of azobenzene-containing polymers are preferable to reversible holographic media because the recorded information can be erased by either optical or thermal processes in most cases. However, setting aside the applications far into the future, this phenomenon is disadvantageous for many sophisticated optical systems in which such reversibility, that is, instability cannot be accepted.
In the present article, we used a photo-cross-linkable polymethylmethacrylate liquid crystal with 4-(4-methoxycinnamoyloxy)biphenyl side groups in order to fabricate thermally stable polarization gratings. According to our previous studies, the polymer used here exhibits thermally stable reorientation of mesogenic side groups by the use of linearly polarized ultraviolet light and subsequent annealing [5–7]. The chemical structure and details about the synthesis and polymer characterization can be found elsewhere [5–7], and preliminary data for simple one-dimensional phase gratings have also been presented [23–25]. Photo-cross-linkable polymer liquid crystal films were prepared from a methylene chloride solution by spin-coating onto a quartz substrate, which resulted in 300-nm-thick films. The films were irradiated with two different types of polarization holographic exposures using 325 nm light beams from a He-Cd laser. A linearly polarized beam from a continuous-wave He-Cd laser was divided into two beams with equal intensity by a beam splitter. The two writing beams with equal intensities crossing at the θ=9.8° angle impinge upon the sample films. The corresponding spatial periodicity of the holographic gratings was 1.9 µm. The polarization states of the two coherent writing beams were controlled by half- and/or quarter-wave plates and set to be orthogonal linear or orthogonal circular. The diffraction was invisible after irradiating with interference light, while the sample was annealed at the liquid crystal temperature of 150°C. The grating was thereupon thermally organized and the diffraction spot appeared. The resulting grating devices were characterized by probing them with a linearly or circularly polarized He-Ne laser (633 nm) beam. The polarization state of the diffracted beam was characterized by Glan-Thompson polarizing prisms, and the diffraction efficiencies were characterized by plots varying the polarization directions (polar plots). Additionally, in order to decide the rotation direction of the circular polarization, we used a combination of a quarter-wave plate and Glan-Thompson polarizing prisms.
Figure 1 shows the typical examples of fundamental functions of our optical devices. For the polarization grating formed by OL exposure [Fig. 1(a)], the ± first-order diffraction beams were linearly p-polarized when the reading beam was linearly s-polarized. The zero-order polarization state was linearly p-polarized, that is, the same as that of the reading beam. For the polarization grating formed by OC exposure [Figs. 1(b) and 1(c)], when the reading beam was linearly s-polarized [Fig. 1(b)], the polarization of the+first-order diffraction beam was left-hand circularly polarized and that of the - first-order diffraction beam was right-hand circularly polarized. When the reading beam was right-hand circularly polarized, the+first-order diffraction beam was left-hand circularly polarized and the - first-order diffraction beam was invisible [Fig. 1(c)]. These experimentally observed properties were consistent with the theoretical expectations, as summarized in Table 2.
Additionally, two-dimensional crossed polarization gratings were also fabricated using the same photo-cross-linkable polymer liquid crystal by overwriting the polarization gratings at the same place. These two-dimensional polarization gratings can generate two-dimensional diffraction patterns with various kinds of polarization states, as demonstrated in Figs. 2 and 3. Figure 2 shows the diffraction patterns from the crossed gratings formed by overwriting the same polarization gratings, while Fig. 3 displays the diffraction patterns from the crossed gratings formed by alternately overwriting the two kinds of polarization gratings. Thus, in response to the demands from various types of optical systems, two-dimensional diffraction patterns with various kinds of polarization states can be generated by designing a combination of one-dimensional polarization gratings. The thermal durability of the developed device is very important for a practical uses. Our polarization-grating device exhibited thermal stability up to 150°C. These results are a considerable advance towards the realization of highly functionalized passive optical devices and will have a significant impact on the future of optoelectronics.
The pure polarization crossed gratings were fabricated by the thermally stable reorientation of mesogenic side groups in the photocrosslinkable polymer liquid crystal by the use of two orthogonal polarized beams and subsequent annealing. The stable crossed gratings can control the two-dimensional propagation direction and convert the polarization state of the light at the same time. The high temperature durability of the crossed polarization gratings, not observed in other kinds of materials, suggest that the choice of the photocrosslinkable polymer liquid crystal is significant for a practical device and this study is a considerable advance towards the realization of highly functionalized passive optical devices.
This work was partially supported by a Grant-in-Aid for Science Research from the Ministry of Education, Science, and Culture of Japan.
References and links
2. G. Iftime, F. L. Labarthet, A. Nathansohn, and P. Rochon, “Control of chirality of an azobenzene liquid crystalline polymer with circularly polarized light,” J. Am. Chem. Soc. 122, 12646–12650 (2000). [CrossRef]
3. S. Yoneyama, T. Yamamoto, O. Tsutsumi, A. Kanazawa, T. Shiono, and T. Ikeda, “High-performance material for holographic gratings by means of a photoresponsive polymer liquid crystal containing a tolane moiety with high birefringence,” Macromolecules 35, 8751–8758 (2002). [CrossRef]
4. V. Shibaev, A. Bobrovsky, and N. Boiko, “Light-responsive chiral photochromic liquid crystalline polymer systems,” J. Photochemistry and Photobiology A: Chemistry 155, 3–19 (2003). [CrossRef]
5. N. Kawatsuki, K. Matsuyoshi, and T. Yamamoto, “Alignment of photo-cross-linkable copolymer liquid crystals induced by linearly polarized ultraviolet irradiation and thermal treatment,” Macromolecules 33, 1698–1702 (2000). [CrossRef]
6. N. Kawatsuki, M. Hayashi, and T. Yamamoto, “Alignment of photo-cross-linkable copolymer liquid crystals induced by linearly polarized ultraviolet light irradiation and annealing: effect of heating rate,” Macromol. Chem. Phys. 202, 3087 (2001). [CrossRef]
7. N. Kawatsuki, K. Goto, T. Kawakami, and T. Yamamoto, “Reversion of alignment direction in the thermally enhanced photoorientation of photo-cross-linkable polymer liquid crystals,” Macromolecules 35, 706–713 (2002). [CrossRef]
8. T. D. Ebralidze, “Model of an anisotropic diffraction grating,” Opt. Spektrosk. 53, 944–946 (1982).
9. L. Nikolova and T. Todorov, “Diffraction efficiency and selectivity of polarization holographic recording,” Optica Acta 31, 579–588 (1984). [CrossRef]
10. L. Nikolova, K. Stoyanova, and T. Todorov, “Polarization wavefront conjugation by means of transient holograms in rigid dye solutions,” Opt. Commun. 64, 75–80 (1987). [CrossRef]
11. C. Solano, R. A. Lessard, and P. C. Roberge, “Methylene blue-sensitized gelatin as a photosensitive medium for conventional and polarization holography,” Appl. Opt. 26, 1989–1997 (1987). [CrossRef] [PubMed]
12. P. Rochon, J. Gosselin, A. Nathansohn, and S. Xie, “Optically induced and erased birefringence and dichroism in azoaromatic polymers,” Appl. Phys. Lett. 60, 4–5 (1992). [CrossRef]
15. H. Akiyama, K. Kudo, and K. Ichimura, “Novel polymethacrylate with latrerally attached azobenzene groups displaying photoinduced optical anisotropy,” Macromol. Rapid. Commun. 16, 35–41 (1995). [CrossRef]
16. L. Nikolova, M. Todorov, M. Ivanov, F. Andruzzi, S. Hvisted, and P. S. Ramanujam, “Polarization holographic gratings in side-chain azobenzene polyesters with linear and circular photoanisotropy,” Appl. Opt. 35, 3835–3840 (1996). [CrossRef] [PubMed]
17. I. Naydenova, T. Nikolova, T. Todorov, F. Andruzzi, S. Hvilsted, and P. S. Ramanujam, “Polarimetric investigation of materials with both linear and circular anisotropy,” J. Mod. Opt. 44, 1643–1650 (1997). [CrossRef]
18. F. L. Labarthet, T. Buffeteau, and C. Sourisseau, “Analysis of the diffraction efficiencies, birefringence, and surface relief gratings on azobenzene-containing polymer films,” J. Phys. Chem. B 102, 2654–2662 (1998). [CrossRef]
19. T. Yamamoto, M. Hasegawa, A. Kanazawa, T. Shiono, and T. Ikeda, “Phase-type gratings formed by photochemical phase transition of polymer azobenzene liquid crystals,” J. Phys. Chem. B 103, 9873–9878 (1999). [CrossRef]
20. M. Kidowaki, T. Fujiwara, S. Morino, K. Ichimura, and J. Stumpe, “Thermal amplification of photo-induced optical anisotropy of p-cyanoazobenzene polymer films monitored by temperature scanning ellipsometry,” Appl. Phys. Lett. 76, 1377–1379 (2000). [CrossRef]
21. G. Cipparrone, A. Mazzulla, and L. M. Blinov, “Permanent polarization gratings in photosensitive Langmuir-Blodgett films for polarimetric applications,” J. Opt. Soc. Am. B 19, 1157–1161 (2002). [CrossRef]
22. A. Gerrard and J. M. Burch, Introduction to Matrix Method in Optics. 179–262 (Dover Publications, Inc. New York, 1994).
23. H. Ono, A. Emoto, N. Kawatsuki, and T. Hasegawa, “Self-organized phase gratings in photoreactive polymer liquid crystals,” Appl. Phys. Lett. 82, 1359–1361 (2003). [CrossRef]
24. N. Kawatsuki, T. Hasegawa, H. Ono, and T. Tamoto, “Formation of polarization gratings and surface relief gratings in photocrosslinkable polymer liquid crystals by polarization holography,” Adv. Mater. 15, 991–994 (2003). [CrossRef]
25. H. Ono, A. Emoto, F. Takahashi, N. Kawatsuki, and T. Hasegawa, “Highly stable polarization gratings in photo-cross-linkable polymer liquid crystals,” J. Appl. Phys. 94, 1298–1303 (2003). [CrossRef]