Temperature Dependence Of Birefringence Research Articles

Disentangling thermal birefringence and strain in the all-optical switching of ferroelectric polarization

Recent works have demonstrated that the optical excitation of crystalline materials with intense narrow-band infrared pulses, tailored to match the frequencies at which the crystal’s permittivity approaches close to zero, can drive a permanent reversal of magnetic and ferroelectric ordering. However, the physical mechanism that microscopically underpins this effect remains unclear, as well as the precise role of laser-induced heating and macroscopic strains. Here, we explore how infrared pulses can simultaneously give rise to strong temperature-dependent birefringence and strain in ferroelectric barium titanate. We develop a model of these two coexisting effects, allowing us to use polarization microscopy to disentangle them through their spatial distributions, temporal evolutions and spectral dependencies. We experimentally observe strain-induced patterns that are an order of magnitude larger than that which can be accounted for by laser-induced heating alone, suggesting that non-thermal effects must also play a role. Our results reveal the distinct fingerprints of heat- and strain-induced birefringence, shedding new light on the process of all-optical switching of order parameters in the epsilon-near-zero regime.

Mixing twist-bend and ferroelectric nematic liquid crystals.

Twist-bend (N_{tb}) and ferroelectric (N_{F}) nematic liquid crystals exhibit several novel effects and new physical properties. Here, we report experimental studies on the phase diagram and some physical properties of binary mixtures of CB9CB and RM734 mesogens. Both N-N_{tb} and N-N_{F} phase transition temperatures and the corresponding enthalpies decrease significantly and, eventually, these transitions disappear at some intermediate compositions, stabilizing wide nematic phase (N). Temperature-dependent birefringence several degrees above the N-N_{tb} phase transition shows strong director tilt fluctuations. The critical range of the fluctuations increases with the nematic range and the critical exponent is consistent with the mean field. The spontaneous polarization of RM734 decreases drastically with the addition of CB9CB mesogen. The temperature dependence of the splay elastic constant of the mixtures' high-temperature nematic (N) phase strikingly differs from that of the pristine CB9CB and RM734 mesogens. The study shows that a small inclusion of either compound has a substantial effect on the phase diagram and physical properties.

Enhanced Orientation of Liquid Crystals Inside Micropores of Metal-Organic Frameworks Having Thermoresponsivity.

With the aim of controlling the orientation of liquid crystals (LCs) toward realizing external stimuli-responsive materials with tunable functionalities, we synthesized a composite of LCs and metal-organic frameworks (MOFs) by filling LCs into the pores of MOFs (LC@MOFs) for the first time. The included LCs interact with the MOFs through coordination bonds between the cyano groups of the LCs and the metal ions of the MOFs, enabling the orientation of the LC molecules inside the pores of the MOFs and the realization of birefringence of LC@MOFs. The three-dimensional nanometer interstice frameworks maintained the LC orientation even at temperatures much higher than the isotropic phase transition temperature of bulk LCs. Furthermore, the orientational state changed upon heating or cooling, inducing temperature-dependent birefringence. This study provides a new approach to the development of stimuli-responsive optical materials and stimuli-responsive MOFs.

Novel properties of high-performance multi-component mixture for Vertically Aligned mode LCDs

ABSTRACT Vertically Aligned mode Liquid Crystal Displays (VALCDs) which have generated huge research interest due to their excellent contrast and wide viewing angle require materials with negative dielectric anisotropy. This work highlights the systematic development of a fifteen-component mixture from pure liquid crystalline compounds comprising laterally fluorinated bi-, tri- phenyl, tolane, bicyclohexane compounds and non-mesogenic compounds exhibiting negative dielectric anisotropy. The temperature dependence of birefringence (Δn), dielectric anisotropy (Δε), threshold voltage (Vth), bend elastic constant (K33), relaxation time (τ0) and rotational viscosity (γ1) as a function of temperature of this fifteen-component nematic mixture have been reported. This mixture exhibits a high Figure of Merit (FoM) which is desirable for reducing the device response time. Additionally, the orientational order parameter (OOP) values, activation energy (Ea), visco-elastic co-efficient (γ1/K33) and material parameters (A 0 ) have also been reported. The effect of pretilt angle in the alignment layers on the threshold voltage (Vth) and switching time (τ0) to ascertain the applicability of this material in Vertically Aligned mode Liquid Crystal Displays (VALCDs) have also been discussed.

Dipole-dipole correlations in the nematic phases of symmetric cyanobiphenyl dimers and their binary mixtures with 5CB.

We report on the temperature dependence of birefringence and of the static dielectric permittivity tensor in a series of binary mixtures between the symmetric, bent-shaped, 1'',9''-bis(4-cyanobiphenyl-4'-yl)nonane (CB9CB) dimer and the monomeric nematogen 5CB. In the studied composition range the mixtures exhibit two nematic phases with distinct birefringence and dielectric features. Birefringence measurements are used to estimate the temperature dependence of the tilt between the axis defining the nanoscale helical modulation of the low temperature nematic phase with the (local) direction of the maximal alignment of the cyanobiphenyl units. Planar as well as magnetically and/or electrically aligned samples are used to measure the perpendicular and parallel components of the dielectric permittivity in both nematic phases. A self-consistent molecular field theory that takes into account flexibility and symmetry of the constituent mesogens is introduced for the calculation of order parameters and intra-molecular orientational dipolar correlations of the flexible dimers as a function of temperature/concentration. Utilising the tilt angle, as calculated from the birefringence measurements, and the predictions of the molecular theory, dielectric permittivity is modelled in the framework of the anisotropic version of the Kirkwood-Fröhlich theory. Using the inter-molecular Kirkwood correlation factors as adjustable parameters, excellent agreement between theory and permittivity measurements across the whole temperature range and composition of the mixtures is obtained. The importance of the orientational, intra- and inter-molecular, dipolar correlations, their relative impact on the static dielectric properties, as well as their connection with the local structure of the nematic phases of bent-shaped bimesogens, is discussed.

A Panda fiber temperature sensor up to 900°C

The use of Panda-type polarization-maintaining (PM) fiber for the localized sensing of high temperatures was analyzed with simulations and experiments up to 900°C. Accuracy and repeatability of the results started to decline above 800°C. Fused silica optical fiber melts at 1700°C, which sets an ultimate limit for measurable temperatures. In practice, optical fiber birefringence restricts the maximum temperature to 1060°C where PM fiber loses its ability to maintain polarization. Three sensor fibers (4, 5 and 10 cm long) were spliced at 45° angles to input/output fibers and calibrated in an oven from room temperature to 850–900°C temperature range. Two superluminescent light-emitting diodes (SLEDs) were coupled together as a broadband light source. Birefringence-induced change of the polarization in the sensor fiber was measured with a polarization splitter and an optical spectrum analyzer (OSA) as a function of the wavelength. Temperature-dependent birefringence generates a sinusoidal reflection spectrum from the input polarization mode to the orthogonal output polarization mode. Temperature changes could be concluded from variations in these spectra. Finally, a small fusion device, NORTH, at DTU, Denmark was successfully used as a testbed to make sure that the sensors can handle transportation and the instrumentation required for vacuum operation and still produce sensible data from a harsh environment.

Determination of optical birefringence and orientational order parameter of octyloxycyanobiphenyl from a voltage-dependent optical transmission technique

ABSTRACT Measurements of optical birefringence have been performed on mesogen 4-cyano-4′-n-octyloxybiphenyl (8OCB) from a voltage-dependent optical transmission technique. The temperature dependence of birefringence has been determined from the voltage dependence of transmitted intensity through homogeneously aligned (planar) plane-parallel liquid crystal-filled cells of different cell-thicknesses. At a particular temperature, a systematic increase of birefringence has been observed with a decrease in cell-thickness. From the optical birefringence data, related orientational order parameter values have also been calculated. The outcomes for orientational order parameter are compared with those reported from other well-known techniques for the similar mesogen. Close agreement among the temperature dependence of orientational order parameter from this study and those from other techniques validates the reliability of the present optical method in precise investigation of physical characteristics of liquid crystalline materials.

Observation of "de Vries-like" properties in bent-core molecules.

“de Vries” liquid crystals, defined by a maximum layer shrinkage of ≤1% from the smectic A to C phase transition, are an integral component of ferroelectric liquid crystal (FLC) displays. Bona fide de Vries materials described in the literature are primarily perfluorinated, polysiloxane and polysilane-terminated rod-like (or calamitic) LCs. Herein, for the first time, we report a series of newly designed achiral unsymmetrical bent-core molecules with terminal alkoxy chains exhibiting similar properties to “de Vries” LCs. The new molecular structure is based on the systematic distribution of four phenyl rings attached via ester and imine linkers having 3-amino-2-methylbenzoic acid as the central core with a bent angle of 147°. Detailed microscopic investigations in differently aligned (planar as well as homeotropic) cells along with SAXS/WAXS studies revealed that the materials exhibited a SmA–SmC phase sequence along with the appearance of the nematic phase at higher temperatures. SAXS measurements divulged the layer spacings (d-spacings) and hence, the layer shrinkage was calculated ranging from 0.19% to 0.68% just below the SmA–SmC transition. The variation of the calculated molecular tilt angle (α) derived from the temperature-dependent SAXS data, followed the power law with exponent values 0.29 ± 0.01 and 0.25 ± 0.01 for compounds 1/10 and 1/12, respectively. The experimental values obtained were very close to the theoretically predicted values for the materials with de Vries-like properties. The analysis of temperature-dependent birefringence studies based on the prediction of the Landau theory, showed a dip across the SmA–SmC phase transition typical of compounds exhibiting the de Vries characteristics. The collective results obtained suggest “de Vries” SmA as a probable model for this bent-core system which may find applications in displays.

Ferroelectric phase-transition frustration near a tricritical composition point

Phase transition describes a mutational behavior of matter states at a critical transition temperature or external field. Despite the phase-transition orders are well sorted by classic thermodynamic theory, ambiguous situations interposed between the first- and second-order transitions were exposed one after another. Here, we report discovery of phase-transition frustration near a tricritical composition point in ferroelectric Pb(Zr1-xTix)O3. Our multi-scale transmission electron microscopy characterization reveals a number of geometrically frustrated microstructure features such as self-assembled hierarchical domain structure, degeneracy of mesoscale domain tetragonality and decoupled polarization-strain relationship. Associated with deviation from the classic mean-field theory, dielectric critical exponent anomalies and temperature dependent birefringence data unveil that the frustrated transition order stems from intricate competition of short-range polar orders and their decoupling to long-range lattice deformation. With supports from effective Hamiltonian Monte Carlo simulations, our findings point out a potentially universal mechanism to comprehend the abnormal critical phenomena occurring in phase-transition materials.

Performance improvement of a resonant fiber optic gyroscope with a hybrid photonic crystal fiber ring resonator.

The photonic crystal fiber (PCF) with better thermal stability and polarization-maintaining performance is applied to the resonant fiber optic gyroscope (RFOG). A hybrid fiber ring resonator is fabricated using the conventional polarization-maintaining fiber (PMF) and PCF with close mode field diameters (MFDs) to reduce MFD-mismatch-induced splicing loss. Furthermore, the temperature-dependent birefringence coefficients of the PMF and the PCF are measured to differ almost four times in absolute value and be opposite in sign. The polarization stability of the hybrid PCF-PMF ring resonator is improved by a factor of 7 compared with the PMF ring resonator with the same length of PMF. The RFOG equipped with this hybrid PCF-PMF ring resonator achieves a bias stability of 1.67°/h.

Old and New Insights into Structure and Properties of Eu2[SiO4

Lemon-yellow single crystals of Eu2[SiO4] were obtained by reaction of elemental europium with Eu2O3 in the presence of SiO2 carried out in evacuated silica ampules at 1373 K for 48 h followed by constant cooling to room temperature with 120 K per hour. Eu2[SiO4] crystallizes at room temperature in the larnite-type structure of β-Ca2[SiO4] (monoclinic, P21/n) with parameters a = 565.02(5), b = 709.15(6), c = 975.84(8) pm, β = 92.614(3)° for Z = 4. At 452 K it undergoes a reversible phase transition to an incommensurate structure similar to the isotypic compounds Sr2[SiO4] and K2[SeO4]. The phase transition energy was determined to 0.54(2) J·g–1 by DSC measurements and temperature dependent birefringence measurements show that the phase transition exhibits a significant hysteresis. Refinements of the structure of Eu2[SiO4] based on single crystal X-ray diffraction data show that the high temperature modification crystallizes in the orthorhombic space group Pnma(α00)0ss with a = 710.16(6), b = 566.93(5), c ...

New fabrication approach to develop a high birefringence photo-crosslinked film based on a sulfur-containing liquid crystalline molecule with large temperature dependence of birefringence

ABSTRACTWe present a new fabrication approach to achieve a high birefringence film by means of photopolymerization based on an alkylthio-containing rod-like liquid crystalline molecule exhibiting large temperature dependence of birefringence. We designed a new reactive mesogen having alkylthio linkages (BPM–S). It was found that BPM–S had a larger increment of birefringence with decreasing temperature, relative to commercially available alkoxy analog LC242. This result could be thought to be due to enhanced intermolecular attractive interaction for an alkylthio mesogen implied by the proximity of laterally neighboring molecules and cybotactic nematic tendency based on wide-angle X-ray measurement. The uniaxially-aligned photo-polymerized film for BPM–S showed higher birefringence than that for LC 242.

Reduced thermal sensitivity of hybrid air-core photonic band-gap fiber ring resonator

A novel hybrid air-core photonic band-gap fiber (PBF) ring resonator with twin 90° polarization-axis rotated splices is proposed and demonstrated. Frist, we measure the temperature dependent birefringence coefficient of air-core PBF and Panda fiber. Experimental results show that the relative temperature dependent birefringence coefficient of air-core PBF is 1.42×10-8/°C, which is typically ~16 times less than that of Panda fiber. Then, we extract the geometry profile of air-core PBF from scanning electron microscope (SEM) images. Numerical modal is built to distinguish the fast axis and slow axis in the fiber. By precisely setting the length difference in air-core PBF and Panda fiber between two 90° polarization-axis rotated splicing points, the hybrid air-core PBF ring resonator is constructed, and the finesse of the resonator is 8.4. Environmental birefringence variation induced by temperature change can be well compensated, and experimental results show an 18-fold reduction in thermal sensitivity, compared with resonator with twin 0° polarization-axis rotated splices.

Synthesis, phase transitions and birefringence of novel liquid crystalline 1,4-phenylene bis(4-alkylthio benzoates) and insights into the cybotactic nematic behaviour

ABSTRACTWe synthesised a novel family of liquid crystalline 1,4-phenylene bis(4-alkylthio benzoates), of which homologues with different alkyl chain lengths of 1–8 were designed, to investigate the structure–property relationship. The mesogenic incidence and tendency were found to be strongly dependent on the carbon numbers in the terminal alkyl chains. Even members formed widely monotropic or enantiotropic nematic (N) phases compared to odd members that showed either none or monotropic-narrower ones. The temperature dependence of birefringence (Δn) for the hexylthio homologue was evaluated and compared to that for a hexyloxy counterpart. It was found that the hexylthio homologue exhibited higher Δn values than the hexyloxy counterpart over the entire range of near TIN–T. In addition, wide-angle X-ray diffraction measurements, using magnetically aligned specimens, found enhanced cybotactic nematic tendency with smectic (Sm) A-like temperature dependence for the hexylthio analogue, due to the intermolecular attractive S···S interaction, in comparison with the hexyloxy analogue exhibiting N phase with clear Sm C-type clusters. We revealed the actual benefits of alkylthio groups in the fluid N phase.

Temperature-dependent birefringence of lithium triborate, LBO in the THz regime

Optical properties of lithium triborate (LBO) in the terahertz regime (0.2–2 THz) were characterized using broadband terahertz time-domain spectroscopy. The frequency dependence of refractive index and absorption coefficient of the LBO crystal was experimentally investigated over the temperature range of 77–297 K, which the experimental results indicated that LBO has very low optical absorption coefficient at terahertz frequencies especially for the beam polarization along the crystal’s principal dielectric axis X. Moreover, a giant birefringence was observed, and the refractive index difference between the axis X and Z gradually decreased with decreasing temperature, which is attributed to the behavior of the TO phonon modes of B1 and B2 symmetries at low frequencies at different temperatures. As potential applications, LBO can be exemplarily used as terahertz wave shapers, beam splitters, terahertz wave plates, circular polarizers and other polarization devices.

A crystalline molecular gyrotop with a biphenylene dirotor and its temperature-dependent birefringence

A crystalline molecular gyrotop with a biphenylene dirotor showed a reduction in the birefringence with increasing temperature.

Temperature dependence of birefringence in ethanol-filled suspended core fiber.

The temperature dependence of the birefringence in a suspended core fiber (SCF) has been experimentally analyzed by using a polarimetric setup. The used configuration consists of two linear polarizers and the SCF as birefringent medium. A theoretical study based on Jones matrices has been carried out to analyze the experimental observed behavior. For this, a polarimetric all-fiber configuration was used whose sensitivity depends on the wavelength variation with temperature. Results obtained show that it is strongly affected when the air holes of SCF are partially filled with ethanol.

Development of birefringence imaging analysis method for observing cubic crystals in various phase transitions.

Optical birefringence imaging systems demonstrate a high potential for comprehensively investigating various phase transitions. To completely demonstrate such abilities, the temperature dependence of birefringence (Δn) was measured in Δn ≃ 0 materials (i.e., cubic crystals with imperfect crystallization) via a background subtraction method. As a result, highly accurate birefringence imaging at 384 × 288 pixels was obtained using phase transition processes as well as varying temperatures visually characterized by the spatial distribution of not only the retardance level but also the optical fast-axis azimuth.

Active cancellation of residual amplitude modulation in a frequency-modulation based Fabry-Perot interferometer.

Residual amplitude modulation (RAM) is one of the most common noise sources known to degrade the sensitivity of frequency modulation spectroscopy. RAM can arise as a result of the temperature dependent birefringence of the modulator crystal, which causes the orientation of the crystal's optical axis to shift with respect to the polarization of the incident light with temperature. In the fiber-based optical interferometer used on the National Institute of Standards and Technology calculable capacitor, RAM degrades the measured laser frequency stability and correlates with the environmental temperature fluctuations. We have demonstrated a simple approach that cancels out excessive RAM due to polarization mismatch between the light and the optical axis of the crystal. The approach allows us to measure the frequency noise of a heterodyne beat between two lasers individually locked to different resonant modes of a cavity with an accuracy better than 0.5 ppm, which meets the requirement to further determine the longitudinal mode number of the cavity length. Also, this approach has substantially mitigated the temperature dependency of the measurements of the cavity length and consequently the capacitance.

Studies of optical texture, birefringence, order parameter, normalized polarizability and validation of the four-parameter model of a thermotropic mesogen 7OAOB

Study of optical texture of different mesophases and phase transition temperatures of the liquid crystal compound 4,4′-di-n-heptyloxy-azoxy benzene has been carried out by using optical polarizing microscope. Enthalpy values and the phase transition temperatures have also been conducted by DSC studies. The variation of refractive indices with temperature has been measured by a thin prism technique using He–Ne laser and temperature dependent birefringence is calculated which shows a moderate value. Validation of the modified four-parameter model based on Vuks approximation has been carried out and reported in this article. The most important characteristics of LC compound namely macroscopic and microscopic order parameter have been evaluated by using direct extrapolation method and modified Vuks method based on Haller's extrapolation respectively. Temperature gradients of refractive indices have also been calculated. Further the normalized polarizabilities for extraordinary and ordinary rays and their ratio have been reported in this paper.