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Optical Materials Express

Optical Materials Express

  • Editor: David Hagan
  • Vol. 4, Iss. 5 — May. 1, 2014
  • pp: 960–968
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Secondary electro-optic effect in liquid crystalline cholesteric blue phases

Hiroyuki Yoshida, Shuhei Yabu, Hiroki Tone, Yuto Kawata, Hirotsugu Kikuchi, and Masanori Ozaki  »View Author Affiliations


Optical Materials Express, Vol. 4, Issue 5, pp. 960-968 (2014)
http://dx.doi.org/10.1364/OME.4.000960


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Abstract

The electro-optic Kerr effect in cubic blue phase liquid crystals comprises two components with different characteristic response times: one attributed to the primary (purely electro-optic) effect and another attributed to the secondary, or indirect (photoelastic) effect. Through simultaneous measurement of the polarized reflection spectrum and transmitted phase, we show that the contribution of the secondary electro-optic effect can be as large as 20% of the total change in refractive index, and that it is suppressed in the polymer-stabilized blue phase. Our results show the importance of stabilizing the lattice structure to realize blue-phase devices with fast response.

© 2014 Optical Society of America

1. Introduction

Liquid crystalline cholesteric blue phases (BPs) typically appear between the cholesteric phase and the isotropic liquid in a chiral liquid crystal (LC) [1

1. D. C. Wright and N. D. Mermin, “Crystalline liquids: the blue phases,” Rev. Mod. Phys. 61, 385–432 (1989). [CrossRef]

4

4. H. Kikuchi, “Liquid crystalline blue phases,” Struct. Bond. 128, 99–117 (2008). [CrossRef]

]. The cubic orientational order exhibited by BPs I and II makes them interesting both as subjects of soft matter physics [5

5. G. P. Alexander and D. Marenduzzo, “Cubic blue phases in electric fields,” Europhys. Lett. 81, 66004 (2008). [CrossRef]

8

8. A. Tiribocchi, G. Gonnella, D. Marenduzzo, E. Orlandini, and F. Salvadore, “Bistable defect structures in blue phase devices,” Phys. Rev. Lett. 107, 237803 (2011). [CrossRef] [PubMed]

] and as candidate materials for next-generation electro-optic applications [9

9. W. Cao, A. Munoz, P. Palffy-Muhoray, and B. Taheri, “Lasing in a three-dimensional photonic crystal of the liquid crystal blue phase II,” Nature Mater. 1, 111–113 (2002). [CrossRef]

12

12. S. Yabu, Y. Tanaka, K. Tagashira, H. Yoshida, A. Fujii, H. Kikuchi, and M. Ozaki, “Polarization-independent refractive index tuning using gold nanoparticle-stabilized blue phase liquid crystals,” Opt. Lett. 36, 3578–3580 (2011). [CrossRef] [PubMed]

]. It is known that when a field is applied, both the refractive index and Bragg reflection wavelength change approximately with a quadratic dependence on the electric field, and using either of these properties, applications such as tunable lenses, reflectors and flat panel displays have been proposed.

The two effects observed in BPs in response to electric fields, namely, refractive index modulation and shift of Bragg reflection wavelength, are a result of the same phenomenon, i.e., molecular reorientation, manifest at different temporal and spatial scales. Figure 1 illustrates the structure of BP I and the two effects observed. The change in refractive index is mainly due to the local reorientation of shortly correlated nematic domains existing in the BP lattice, and because of the small helical pitch, the effect occurs at submillisecond response times, which is faster than the reorientation dynamics in nematics by about an order of magnitude [13

13. G. Heppke, “Electric field induced variation of the refractive index in cholesteric blue phases,” Mol. Cryst. Liq. Cryst. Lett. 2, 59–65 (1985).

16

16. S. Yabu, H. Yoshida, G. Lim, K. Kaneko, Y. Okumura, N. Uehara, H. Kikuchi, and M. Ozaki, “Dual frequency operation of a blue phase liquid crystal,” Opt. Mater. Express 1, 1577–1584 (2011). [CrossRef]

]. On the other hand, the shift of the Bragg reflection wavelength is a result of the electrostriction of the lattice, which occurs so as to relax the increase in the elastic energy gained by the local reorientation of the LC molecules. Because the effect involves as many as 107 LC molecules, it has a characteristic time much longer than that of the Kerr effect, ca. several milliseconds to even seconds or more. [17

17. H. Gleeson, R. Simon, and H. J. Coles, “Electric field effects and two frequency colour switching in the cholesteric and blue phases of Nematic/Cholesteric mixtures,” Mol. Cryst. Liq. Cryst. 129, 37–52 (1985). [CrossRef]

, 18

18. H.-S. Kitzerow, P. P. Crooker, S. L. Kwok, J. Xu, and G. Heppke, “Dynamics of blue-phase selective reflections in an electric field,” Phys. Rev. A 42, 3442–3448 (1990). [CrossRef] [PubMed]

]

Fig. 1 (a) Structure of body-centered BP I, which is characterized by a doubly twisted cylindrical structure, (b) local reorientation of shortly correlated nematic domains, giving rise to the electro-optic Kerr effect, and (c) electrostriction of the lattice.

In crystal optics, the electro-optic effect (in which an electric field causes a change in the refractive index) is known to comprise two components. In addition to the purely electro-optic component which is referred to as the primary effect, there exists a secondary or a photoelastic effect, in which the refractive index changes as a result of the change in crystal symmetry [19

19. J. F. Nye, Physical Properties of Crystals: Their Representation by Tensors and Matrices (Oxford University Press, Oxford, 1984), 1.

]. While the crystal structure of BPs is much larger than typical crystals composed of atoms, they are not an exception and have been shown theoretically to contain both of these effects [20

20. V. E. Dmitrienko, “Electro-optic effects in blue phases,” Liq. Cryst. 5, 847–851 (1989). [CrossRef]

]. Experimentally, however, many studies to date have not distinguished the two electro-optic effects. Many studies which measure the dynamic response of the Kerr effect have focused on the primary response, which occurs with sub-ms response times, and while some studies have commented on the presence of a slow response in the refractive index [14

14. P. R. Gerber, “Electro-optical effects of a small-pitch blue-phase system,” Mol. Cryst. Liq. Cryst. 116, 197–206 (1985). [CrossRef]

, 21

21. F. Porsch, H. Stegemeyer, and K. Hiltrop, “Electric field-induced birefringence in liquid-crystalline blue phases,” Z. Naturforsch. 39a, 475–480 (1984).

, 22

22. K.-M. Chen, S. Gauza, H. Xianyu, and S.-T. Wu, “Hysteresis effects in blue-phase liquid crystals,” J. Disp. Technol. 6, 318–322 (2010). [CrossRef]

], quantitative measurements had not been performed. Moreover, in many cases the two effects have been measured independently: the Kerr effect has often been investigated by applying a horizontal electric field and measuring the induced birefringence [14

14. P. R. Gerber, “Electro-optical effects of a small-pitch blue-phase system,” Mol. Cryst. Liq. Cryst. 116, 197–206 (1985). [CrossRef]

16

16. S. Yabu, H. Yoshida, G. Lim, K. Kaneko, Y. Okumura, N. Uehara, H. Kikuchi, and M. Ozaki, “Dual frequency operation of a blue phase liquid crystal,” Opt. Mater. Express 1, 1577–1584 (2011). [CrossRef]

, 21

21. F. Porsch, H. Stegemeyer, and K. Hiltrop, “Electric field-induced birefringence in liquid-crystalline blue phases,” Z. Naturforsch. 39a, 475–480 (1984).

23

23. U. Singh and P. H. Keyes, “Measurement of the kerr effect in cholesteric blue phases,” Liq. Cryst. 8, 851–860 (1990). [CrossRef]

], while electrostriction has been investigated by applying a vertical field and measuring the shift in the Bragg reflection wavelength [17

17. H. Gleeson, R. Simon, and H. J. Coles, “Electric field effects and two frequency colour switching in the cholesteric and blue phases of Nematic/Cholesteric mixtures,” Mol. Cryst. Liq. Cryst. 129, 37–52 (1985). [CrossRef]

, 18

18. H.-S. Kitzerow, P. P. Crooker, S. L. Kwok, J. Xu, and G. Heppke, “Dynamics of blue-phase selective reflections in an electric field,” Phys. Rev. A 42, 3442–3448 (1990). [CrossRef] [PubMed]

, 24

24. H. J. Coles and H. F. Gleeson, “Electric field induced phase transitions and colour switching in the blue phases of chiral nematic liquid crystals,” Molecular Crystals and Liquid Crystals Incorporating Nonlinear Optics 167, 213–225 (1989). [CrossRef]

]. After the discovery of the polymer-stabilization technique to expand the temperature range of BPs [25

25. H. Kikuchi, M. Yokota, Y. Hisakado, H. Yang, and T. Kajiyama, “Polymer-stabilized liquid crystal blue phases,” Nature Mater. 1, 64–68 (2002). [CrossRef]

], many ‘engineered’ BPs such as those stabilized by nano-particles [26

26. H. Yoshida, Y. Tanaka, K. Kawamoto, H. Kubo, T. Tsuda, A. Fujii, S. Kuwabata, H. Kikuchi, and M. Ozaki, “Nanoparticle-stabilized cholesteric blue phases,” Appl. Phys. Express 2, 121501 (2009). [CrossRef]

28

28. J.-M. Wong, J.-Y. Hwang, and L.-C. Chien, “Electrically reconfigurable and thermally sensitive optical properties of gold nanorods dispersed liquid crystal blue phase,” Soft. Mat. 7, 7656–7659 (2011). [CrossRef]

] or tailor-made molecules [10

10. H. J. Coles and M. N. Pivnenko, “Liquid crystal ’blue phases’ with a wide temperature range,” Nature 436, 997–1000 (2005). [CrossRef] [PubMed]

, 29

29. A. Yoshizawa, Y. Kogawa, K. Kobayashi, Y. Takanishi, and J. Yamamoto, “A binaphthyl derivative with a wide temperature range of a blue phase,” J. Mater. Chem 19, 5759–5764 (2009). [CrossRef]

31

31. S. Shibayama, H. Higuchi, Y. Okumura, and H. Kikuchi, “Dendron-stabilized liquid crystalline blue phases with an enlarged controllable range of the photonic band for tunable photonic devices,” Adv. Funct. Mater. 23, 2387–2396 (2013). [CrossRef]

] have been proposed. It is therefore of much importance to understand the electro-optic response of pristine and engineered BPs.

Here, we investigate the electro-optic effects in pristine and polymer-stabilized (PS) BP I by simultaneously measuring the change in refractive index and the reflection spectrum. We first show that the slow secondary effect can contribute to as much as 20% of the total change in refractive index in a pristine BP, and, in an aim to shed light on the physical mechanism behind the secondary electro-optic effect, present a model which describes the observed phenomena through a coupling parameter between the primary Kerr effect and electrostriction. Secondly, and importantly for device applications, we show that the secondary effect can indeed be removed if electrostriction does not occur. The slow response is not observed in the PSBP, which has a fixed lattice structure that is stabilized by a polymer network. Our results show the importance of stabilizing the lattice structure to realize blue-phase devices with a fast response.

2. Methods

The BP sample used in this study was prepared by adding a chiral dopant [ISO-(6OBA)2, 7 wt%] to a nematic LC mixture (5CB, 46.5 wt% and JC-1041XX, 46.5 wt%) with positive dielectric anisotropy [31

31. S. Shibayama, H. Higuchi, Y. Okumura, and H. Kikuchi, “Dendron-stabilized liquid crystalline blue phases with an enlarged controllable range of the photonic band for tunable photonic devices,” Adv. Funct. Mater. 23, 2387–2396 (2013). [CrossRef]

]. We also prepared a PSBP by doping two types of monomers (dodecyl acrylate, 4.1 wt% and RM257, 4.2 wt%) and a photoinitiator (DMOAP, 0.8 wt%) in the aforementioned BP sample [25

25. H. Kikuchi, M. Yokota, Y. Hisakado, H. Yang, and T. Kajiyama, “Polymer-stabilized liquid crystal blue phases,” Nature Mater. 1, 64–68 (2002). [CrossRef]

, 32

32. Y. Haseba, H. Kikuchi, T. Nagamura, and T. Kajiyama, “Large electro-optic kerr effect in nanostructured chiral Liquid]Crystal composites over a wide temperature range,” Adv. Mater. 17, 2311–2315 (2005). [CrossRef]

]. Sandwich cells with an approximate thickness of 27 μm, assembled from two pre-cleaned, indium tin oxide- (ITO-) coated glass substrates were filled with the samples. The phase sequences of the samples were determined from polarized optical microscopy to be cholesteric (45.4 °C)/BP I (45.9 °C)/BP II (46.9 °C)/isotropic for the BP (on heating the sample at a rate of 0.1 °C/min) and cholesteric (30.0 °C)/BP I (33.5 °C)/BPII (35.5 °C)/isotropic for the PSBP (on cooling the sample at a rate of 0.2 °C/min). The PSBP sample was polymerized at 32.5 °C by irradiation with UV light (1.66 mW/cm2, 365 nm) for 20 min, after which BP I was stabilized to below −60 °C [25

25. H. Kikuchi, M. Yokota, Y. Hisakado, H. Yang, and T. Kajiyama, “Polymer-stabilized liquid crystal blue phases,” Nature Mater. 1, 64–68 (2002). [CrossRef]

]. Electro-optic measurements were performed at 45.7 °C for BP I and 27.5 °C for PSBP.

A two-beam interference microscope was built on a commercially available upright microscope (Olympus, BX-51), using a He-Ne laser (λ = 632.8 nm) as the probe light source. The setup was also equipped with a white light source and a beam-splitter to enable simultaneous acquisition of polarized reflection spectra [33

33. H. Yoshida, S. Yabu, H. Tone, H. Kikuchi, and M. Ozaki, “Electro-optics of cubic and tetragonal blue phase liquid crystals investigated by two-beam interference microscopy,” Appl. Phys. Express 6, 062603 (2013). [CrossRef]

]. The sample was observed at the edge of the ITO electrodes so that regions both subject to and not subject to the field could be observed: the change in the refractive index was evaluated from the difference in the phase between the two regions. This configuration was employed to reduce errors introduced in the experiment, such as field-induced narrowing of the cell-gap. The resolution of the setup, limited by fluctuations in the fringe originating from environmental vibrations, was δnmin ∼ 10−4. The diameter of the measured spot for spectroscopy was ∼130 μm, and measurement was performed on the (110) platelet of BP I, which was confirmed by Kossel line observations. Application of an electric field oriented the (110) plane of the BP lattice along the electric field, but the azimuthal orientation was random, with domain sizes approximately 100 μm [33

33. H. Yoshida, S. Yabu, H. Tone, H. Kikuchi, and M. Ozaki, “Electro-optics of cubic and tetragonal blue phase liquid crystals investigated by two-beam interference microscopy,” Appl. Phys. Express 6, 062603 (2013). [CrossRef]

]. The experiment was computer-controlled to acquire the interference fringe and the reflection spectrum at 200 ms intervals for 60 s. A rectangular electric field (1 kHz) was applied for 30 s and then removed, and the voltage was incremented after a rest period of 60 s. At this temperature, BP I showed a field-induced transition to the centered-tetragonal BP X at an applied fields above 2.7 V/μm [33

33. H. Yoshida, S. Yabu, H. Tone, H. Kikuchi, and M. Ozaki, “Electro-optics of cubic and tetragonal blue phase liquid crystals investigated by two-beam interference microscopy,” Appl. Phys. Express 6, 062603 (2013). [CrossRef]

]: data were analyzed below this transition threshold.

3. Results and Discussion

Figure 2 shows the transient response of the Bragg wavelength and relative refractive index of the BP sample. The Bragg wavelength shows a slow response with characteristic times of 10 s or more: this is because the shift in the Bragg wavelength is due to an elastic deformation of the lattice involving a large number of LC molecules, and also because we have used a thick cell to obtain a phase difference that is large enough to be detected. The refractive index, on the other hand, shows a fast response because it is caused mainly by reorientation of the nematic director on a scale smaller than the lattice constant. As reported previously in many studies, the response time is on the submillisecond scale and is observed as a step-like response near 0 and 30 s in the time resolution of this measurement [14

14. P. R. Gerber, “Electro-optical effects of a small-pitch blue-phase system,” Mol. Cryst. Liq. Cryst. 116, 197–206 (1985). [CrossRef]

, 16

16. S. Yabu, H. Yoshida, G. Lim, K. Kaneko, Y. Okumura, N. Uehara, H. Kikuchi, and M. Ozaki, “Dual frequency operation of a blue phase liquid crystal,” Opt. Mater. Express 1, 1577–1584 (2011). [CrossRef]

]. Interestingly, for electric field intensities between 2.11 and 2.57 V/μm, a very slow change in the refractive index is observed, with characteristic times similar to that of electrostriction. The presence of this response was confirmed by making at least five measurements, and was found to be on the order of 10−4, which was as large as 20 % of the total shift in the refractive index (Note that a similar slow response is also observed for 2.72 V/μm at which the sample has turned to BP X. The applied field dependence of the slow response in BP X was found to be different from that of BP I and is out of scope of this paper). In Fig. 2(b), the applied field dependence of the response time of the slow response fitted to a single exponential function, τ, the amount of the slow change in the refractive index, δnslow, and the ratio of the slow change to the total change in refractive index, δnslow/δn, are shown: although the effect was not observable at low fields because of the limitation of our setup, δnslow shows a monotonic increase between applied fields of 2.1 and 2.6 V/μm.

Fig. 2 (a) Transient response of Bragg wavelength and change in refractive index for BP I sample, and (b) applied field dependence of the time constant of the slow response fitted to an exponential function, slow change in refractive index and ratio of the slow change to the total change in refractive index.

The slow mode in the refractive index has a response time similar to that of electrostriction and can therefore be attributed to the secondary electro-optic effect of BPs. In a BP where the crystal structure is formed by the distribution of the nematic director, the mechanism of the effect can be described physically as follows. The Kerr coefficient has been shown to have a cubic dependence on the BP lattice constant [15

15. H. Choi, H. Higuchi, and H. Kikuchi, “Electrooptic response of liquid crystalline blue phases with different chiral pitches,” Soft Matter 7, 4252–4256 (2011). [CrossRef]

]. Thus, the extent to which the local nematic director can reorient is limited by the three-dimensional structure of the BP. As the lattice deforms under an applied field, the director is able to reorient further in the direction of the field, which in turn deforms the lattice further, until equilibrium is reached. The extra reorientation of the LC molecules enabled by lattice deformation contributes to an extra change in the refractive index with a characteristic response time similar to that of electrostriction. Interestingly, the slow response is observed only when the field is applied to the sample and not when the field is removed. This does not contradict the description above, since there is no directional torque acting in the off-switching process. This indicates that the molecules can return instantaneously to a configuration similar to the initial orientation (even though the lattice may be deformed), such that the difference in the refractive index is negligible.

The response of BPs has been modeled theoretically by different groups. The analytical approach that had been employed in earlier studies [3

3. H. S. Kitzerow, “The effect of electric fields on blue phases,” Mol. Cryst. Liq. Cryst. 202, 51–83 (1991). [CrossRef]

, 20

20. V. E. Dmitrienko, “Electro-optic effects in blue phases,” Liq. Cryst. 5, 847–851 (1989). [CrossRef]

, 34

34. R. M. Hornreich and S. Shtrikman, “Dynamic response of a helicoidal cholesteric phase to an applied field,” Phys. Rev. A 44, R3430–R3433 (1991). [CrossRef] [PubMed]

] is now rare and the trend of theoretical BP research has shifted to performing numerical simulations, in both free and confined geometries [5

5. G. P. Alexander and D. Marenduzzo, “Cubic blue phases in electric fields,” Europhys. Lett. 81, 66004 (2008). [CrossRef]

8

8. A. Tiribocchi, G. Gonnella, D. Marenduzzo, E. Orlandini, and F. Salvadore, “Bistable defect structures in blue phase devices,” Phys. Rev. Lett. 107, 237803 (2011). [CrossRef] [PubMed]

, 35

35. J.-i. Fukuda, M. Yoneya, and H. Yokoyama, “Simulation of cholesteric blue phases using a Landau

OCIS Codes
(160.2100) Materials : Electro-optical materials
(160.3710) Materials : Liquid crystals
(160.1585) Materials : Chiral media

ToC Category:
Liquid Crystals

History
Original Manuscript: February 28, 2014
Revised Manuscript: April 1, 2014
Manuscript Accepted: April 1, 2014
Published: April 10, 2014

Virtual Issues
Optical Materials for Flat Panel Displays (2013) Optical Materials Express

Citation
Hiroyuki Yoshida, Shuhei Yabu, Hiroki Tone, Yuto Kawata, Hirotsugu Kikuchi, and Masanori Ozaki, "Secondary electro-optic effect in liquid crystalline cholesteric blue phases," Opt. Mater. Express 4, 960-968 (2014)
http://www.opticsinfobase.org/ome/abstract.cfm?URI=ome-4-5-960


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References

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