Polar Crystals Research Articles

Emergent Antiferroelectric Ordering and the Coupling of Liquid Crystalline and Polar Order

Polar liquid crystals possess 3D orientational order coupled with unidirectional electric polarity, yielding fluid ferroelectrics. Such polar phases are generated by rod‐like molecules with large electric dipole moments. 2,5‐Disubstituted 1,3‐dioxane is commonly employed as a polar motif in said systems, and herein it is shown to suffer from thermal instability as a consequence of equatorial‐trans to axial‐trans isomerism at elevated temperatures. Isosteric building blocks are utilized as potential replacements for the 1,3‐dioxane unit, and in doing so new examples of fluid ferroelectric systems are obtained. For binary mixtures of certain composition, the emergence of a new fluid antiferroelectric phase, a finding not observed for either of the parent molecules, is observed. This study also reveals a critical tipping point for the emergence of polar order in otherwise apolar systems. These results hint at the possibility for uncovering new highly ordered polar liquid‐crystalline phases and delineate distinct transition mechanisms in orientational and polar ordering.

Binary and heterostructured microplates of iridium and ruthenium complexes: Preparation, characterization, and thermo-responsive emission

Thermo-responsive microcrystals exhibiting obvious emission intensity or color changes have great potentials in sensing, information encryption, and microelectronics. We report herein the binary assembly of a blue-emissive iridium complex and a red-emissive ruthenium complex into homogeneously-doped or optically-heterostructured microcrystals with thermo-responsive properties. Depending on the assembly conditions, lateral or longitudinal triblock heterostructures with a microplate shape are obtained, which display distinct emission pattern changes upon heating as a result of the decreased efficiency of energy transfer. In addition, branched heterostructures are prepared by a stepwise assembly. The luminescence polarization of the homogeneously-doped binary crystals and the waveguiding property of the longitudinal triblock heterostructure are further examined. This work evidences the versatility of transition metal complexes in the assembly into various luminescent nano/micro structures with potential applications in thermo-sensing and nanophotonics.

The Nature of Pyroelectric Polarity

The concept of spontaneous polarization in the pyroelectrics is called into a question, since omnipresent free electric charges make impossible to maintain any equilibrium and time-stable polarized state. We conjecture in this paper that pyroelectricity in polar crystals and piezoelectricity in polar-neutral crystals are due to hybridized ionic-covalent polarity-activating bonds. When they are in non-excited state, these bonds do not produce electric field, yet they are capable of generating the electric response to uniform non-electric influence, e.g., heat, pressure, etc. This response is described by some models of different electric moments. Different contributors to these moments can be measured using partial limitation of crystal thermal strain. In fact, the proposed approach modifies and extends the known concept of spontaneous polarization. In this context, ferroelectrics are distinguished by the fact that, in the electric field, they reorient their polarity-activating inter-atomic bonds with a non-linear response and hysteresis.

Structural, magnetic, magnetocaloric behavior and magneto-transport, electrical polarization study in 3d based bulk and nano-crystalline multiferroic double perovskite Dy2MnCoO6

In this paper, we report a detailed investigation of the crystal structure, magnetic, magnetocaloric, magneto-transport and electrical polarization properties of a new multiferroic material in the polycrystalline and nanocrystalline form of the Dy2MnCoO6 double perovskite. Both compounds crystallized in the monoclinic structure with P21/n space group. The magnetic properties of both systems are mainly dominant ferromagnetic (FM) and weak antiferromagnetic (AFM). The FM/AFM coupling is related by the competing and combining functions of the radius and the magnetic moments of rare earth ions (i.e. 3d–4f exchange interactions). The reduction of the saturation magnetization in the isothermal magnetization curves can be explained by the existence of anti-phase boundaries and local anti-site defects in the system. Moreover, these materials hold reasonable values of magnetocaloric parameters and the absence of hysteresis makes the system a potential candidate for magnetic refrigeration. These compounds revealed two magnetic phase transitions, according to the appearance of two peaks in the temperature dependence of magnetic entropy change curves. The temperature dependent resistivity data for both the systems display semiconductor nature near room temperature and insulating like behavior at low temperature regime. The variable-range hopping conduction mechanism is used to best understand their transport mechanism. In addition, the electrical polarization loop at low temperature confirms the presence of ferroelectricity for both the studied systems. The decreases polarization under an external magnetic field evidence the weak magnetoelectric coupling. The coexistence of FM ordering with insulating behavior and ferroelectricity at low temperature promises new opportunities and improvements in next generation applications for information storage, spintronic, and sensors.

III-Nitride Magnetron Sputter Epitaxy on Si: Controlling Morphology, Crystal Quality, and Polarity Using Al Seed Layers.

Group III-nitride semiconductors have been subject of intensive research, resulting in the maturing of the material system and adoption of III-nitrides in modern optoelectronics and power electronic devices. Defined film polarity is an important aspect of III-nitride epitaxy as the polarity affects the design of electronic devices. Magnetron sputtering is a novel approach for cost-effective epitaxy of III-nitrides nearing the technological maturity needed for device production; therefore, control of film polarity is an important technological milestone. In this study, we show the impact of Al seeding on the AlN/Si interface and resulting changes in crystal quality, film morphology, and polarity of GaN/AlN stacks grown by magnetron sputter epitaxy. X-ray diffraction measurements demonstrate the improvement of the crystal quality of the AlN and subsequently the GaN film by the Al seeding. Nanoscale structural and chemical investigations using scanning transmission electron microscopy reveal the inversion of the AlN film polarity. It is proposed that N-polar growth induced by Al seeding is related to the formation of a polycrystalline oxygen-rich AlN interlayer partially capped by an atomically thin Si-rich layer at the AlN/Si interface. Complementary aqueous KOH etch studies of GaN/AlN stacks demonstrate that purely metal-polar and N-polar layers can be grown on a macroscopic scale by controlling the amount of Al seeding.

Dual-Core Photonic Crystal Fiber Polarization Beam Splitter Based on a Nematic Liquid Crystal with an Ultra-Short Length and Ultra-Wide Bandwidth

This paper presents a novel pentagonal structure dual-core photonic crystal fiber polarizing beam splitter (PS-DC-PCF PBS) filled with a nematic liquid crystal (NLC) in the central hole. Unlike previous designs with symmetric arrangements, the upper and lower halves of the structure have different air hole arrangements. The upper half consists of air holes arranged in a regular quadrilateral pattern, while the lower half features a regular hexagonal arrangement of air holes. By filling the central hole with birefringent liquid crystal, the birefringence of the structure is enhanced, reducing the coupling lengths along the x polarization and y polarization directions. The polarization properties, coupling characteristics, and the influence of different structural parameters on the extinction ratio of the polarizing beam splitter are analyzed using the full-vector finite element method. Simulation results demonstrate that the designed PS-DC-PCF PBS achieves a maximum extinction ratio (ER) of 72.94 dB with a splitting length of only 61.9 μm and a wide operating bandwidth of 423 nm (1.324–1.747 μm), covering most of the O, E, S, C, L, and U communication bands. It exhibits not only ultra-short splitting lengths and ultra-wide splitting bandwidth but also good manufacturing tolerances and anti-interference capabilities. The designed PS-DC-PCF PBS could provide crucial device support for future all-optical communication systems and has potential applications in fiber optic communication or fiber laser systems.

15‐3: Reflective Liquid Crystal Polarization Volume Grating for SWIR with High Diffraction Efficiency and Large Diffraction Angle and Sensor Application

We have developed a reflective polarization volume grating using liquid crystal polymer for SWIR with high efficiency and a large diffraction angle. By using this grating and a lightguide system, we demonstrated a sensor system that can capture identical images simultaneously in both visible and SWIR light.

75‐1: Invited Paper: Liquid Crystal Polarization Hologram for Eye Tracking Application

Eye‐tracking is vital in AR/VR/MR systems for display correction, rendering, accommodation, and more. However, existing eye‐tracking solutions fall short in accuracy, efficiency, form factor, and population coverage. Using Liquid crystal polarization hologram (LCPH) for eye‐tracking purposes offers a compact form‐factor with excellent performance.

Twist-Induced Hyperbolic Shear Metasurfaces

Following the discovery of moiré-driven superconductivity and density waves in twisted-graphene multilayers, twistronics has spurred a surge of interest in tailored broken symmetries through angular rotations enabling new properties, from electronics to photonics and phononics. Analogously, in monoclinic polar crystals a nontrivial angle between nondegenerate dipolar phonon resonances can naturally emerge due to asymmetries in their crystal lattice, and its variations are associated with intriguing polaritonic phenomena, including axial dispersion, i.e., the rotation of the optical axis with frequency, and microscopic shear effects that result in an asymmetric distribution of material loss. So far, these phenomena have been restricted to specific midinfrared frequencies difficult to access with conventional laser sources and fundamentally limited by the degree of asymmetry and by the strength of light-matter interactions available in natural crystals. Here, we leverage the twistronics concept to demonstrate maximal axial dispersion and loss redistribution of hyperbolic waves in elastic metasurfaces, achieved by tailoring the angle between coupled metasurface pairs featuring tailored anisotropy. We show extreme control over elastic wave dispersion and absorption via the twist angle and leverage the resulting phenomena to demonstrate enhanced propagation distance, in-plane reflection-free negative refraction and diffraction-free defect detection. Our work welds the concepts of twistronics, non-Hermiticity, and extreme anisotropy, demonstrating the powerful opportunities enabled by metasurfaces for tunable, highly directional surface-acoustic-wave propagation of great interest for a wide range of applications spanning from seismic mitigation to on-chip phononics and wireless communication systems, hence paving the way toward their translation into emerging photonic and polaritonic metasurface technologies. Published by the American Physical Society 2024

Transition Edge Sensors with Sub-eV Resolution And Cryogenic Targets (TESSERACT) at the underground laboratory of Modane (LSM)

The future TESSERACT experiment will search for individual galactic DM particles below the proton mass through interactions with advanced, ultra-sensitive detectors. Currently TESSERACT is in a design phase aiming to produce fully defined detector technologies that will explore DM masses down to 10 MeV. It is designed to be sensitive to DM candidates interacting with the detector target material in producing both nuclear recoil DM (NRDM) and electron recoil (ERDM). To do so, multiple target materials will be used with varying detection strategies to ensure the capability to both actively reject the so-called low-energy excess and discriminate nuclear recoils against electron recoils. In addition to maximizing sensitivity to a variety of DM interactions, this provides an independent handle on instrumental backgrounds. Nowadays, the TESSERACT project encompasses two US-based technologies, namely HeRALD using superfluid helium as a target material, and SPICE using polar crystals (Al2O3 and SiO2) and scintillating crystals such as GaAs. In these proceedings, we discuss the recent proposal to host the future TESSERACT experiment at the Modane Underground Laboratory (LSM) and add a third French-based cryogenic semiconducting (Ge, Si) detector technology to the TESSERACT payload.

Polarization Saturation in Multilayered Interfacial Ferroelectrics.

Van der Waals polytypes of broken inversion and mirror symmetries have been recently shown to exhibit switchable electric polarization even at the ultimate two-layer thin limit. Their out-of-plane polarization has been found to accumulate in a ladder-like fashion with each successive layer, offering 2D building blocks for the bottom-up construction of 3D ferroelectrics. Here, it is demonstrated experimentally that beyond a critical stack thickness, the accumulated polarization in rhombohedral polytypes of molybdenum disulfide saturates. The underlying saturation mechanism, deciphered via density functional theory and self-consistent Poisson-Schrödinger calculations, point to a purely electronic redistribution involving: 1.Polarization-induced bandgap closure that allows for cross-stack charge transfer and the emergence of free surface charge; 2. Reduction of the polarization saturation value, as well as the critical thickness at which it is obtained, by the presence of free carriers. The resilience of polar layered structures to atomic surface reconstruction, which is essentially unavoidable in polar 3D crystals, potentially allows for the design of new devices with mobile surface charges. The findings, which are of general nature, should be accounted for when designing switching and/or conductive devices based on ferroelectric layered materials.

Performance and compensation method of first-order liquid crystal beam-steering system under continuous wave laser irradiation

The effects of laser irradiation thermal deposition on the performance degradation of liquid crystal (LC) devices in high-power laser systems are extremely vital. In this study, the first-order beam-steering system (FBS) was developed using a passive liquid crystal polarization grating (LCPG) and liquid crystal adjustable wave-plate (LCAW). The LCPG was prepared by holographic exposure technology, and the LCAW was prepared using the standard LC cell preparation process. We investigated the influences of diffraction efficiency of FBS under a 1070-nm continuous-wave (CW) laser irradiation. The energy is concentrated in the −1st order at first. When the half-wave retardation was reached, all the energy is concentrated in the +1st order (∼97 %), and the beam is deflected. Once the phase retardation decreases below the half-wave retardation, the energy gradually reconcentrates in the −1st order. When the LCAW fails, the diffraction the energy is refocused to the −1st order by the LCPG. The results indicated that both thermal deposition and driving voltage reduce the phase retardation of the LCAW, generating a variation of energy between in ±1st orders. By reducing the driving voltage, this half-wave retardation can be recovered under a certain half-wave voltage and laser power density, and the diffraction efficiency of the +1st order can be compensated to ∼97 %. If the reduced phase retardation is not less than half-wave, the FBS can still be modulated in high-power continuous lasers. Our research provides a reference for the development of beam-steering technology based on LC materials in high-power laser systems.

A design approach to obtaining highly polar liquid crystal dimers

ABSTRACT The synthesis and characterisation of 10 members of the [4[(E)-[4-[4-[ω-(4-cyanophenyl)phenoxy]alkyloxy]-3-nitrophenyl]methylideneamino]phenyl] 2,4-dimethoxybenzoates is reported in which the number of methylene units in the flexible spacer is increased from three to twelve. The mesogenic units are based on cyanobiphenyl and 3-nitrobenzylideneaniline benzoate and linked by the spacer such that their dipoles are parallel giving rise to a large longitudinal dipole moment. All 10 members of the series show a nematic phase, and the nematic-isotropic transition temperatures, TNI, and associated entropy changes show a strong dependence on the length and parity of the spacer. This behaviour is attributed to the average shapes of the molecules and their flexibility. The heptyl member was further characterised using dielectric spectroscopy revealing a high value of dielectric permittivity reflecting the large dipole moment of the molecules and possibly indicating local short-range ferroelectric order. The synthesis and characterisation of two members of the [4[(E)-[4-[4-[3-(ω-cyanophenyl)phenoxy]alkyloxy]-4-nitrophenyl]methylideneamino]phenyl] 2,4-dimethoxybenzoates are also described for which the difference in shape between odd and even members is reduced. Both dimers are exclusively nematogenic and the difference between TNI for the odd and even member is smaller reflecting the more similar molecular shapes. The potential for developing dimers that exhibit the ferroelectric nematic phase is discussed.

Nd:YVO4/YVO4 cascaded Raman laser pumped dual-wavelength signal wave MgO:PPLN-OPO with wide range adjustable wavelength interval

This article presents a dual-wavelength signal wave output system capable of generating a broad range of adjustable wavelength intervals. The setup involved the creation of a dual-wavelength cascaded Raman laser featuring composite cavities operating at 1176 nm and 1313 nm. Experimental investigations were carried out on an external cavity MgO:PPLN-OPO driven by the cascaded Raman laser. By setting the crystal polarization period to 27.6-34.4 µm and the temperature to 50-130°C, adjustable tunable output of dual-wavelength signal wave at 1176 nm-MgO:PPLN-OPO (1550-2294 nm) and 1313 nm-MgO:PPLN-OPO (1768-2189 nm) was achieved with a wavelength interval of 0-218 nm. Under the conditions of a period of 34.4 µm, temperature of 90°C, and an incident Raman power of 2.6 W, the highest conversion efficiency of Raman to dual-wavelength signal wave (2212, 2182 nm) was 34.2%. Furthermore, the maximum output power of dual-wavelength signal wave was recorded at 1.02 W with an incident Raman power of 3.33 W.

Direct programming of confined surface phonon polariton resonators with the plasmonic phase-change material In3SbTe2

Tailoring light-matter interaction is essential to realize nanophotonic components. It can be achieved with surface phonon polaritons (SPhPs), an excitation of photons coupled with phonons of polar crystals, which also occur in 2d materials such as hexagonal boron nitride or anisotropic crystals. Ultra-confined resonances are observed by restricting the SPhPs to cavities. Phase-change materials (PCMs) enable non-volatile programming of these cavities based on a change in the refractive index. Recently, the plasmonic PCM In3SbTe2 (IST) was introduced which can be reversibly switched from an amorphous dielectric state to a crystalline metallic one in the entire infrared to realize numerous nanoantenna geometries. However, reconfiguring SPhP resonators to modify the confined polaritons modes remains elusive. Here, we demonstrate direct programming of confined SPhP resonators by phase-switching IST on top of a polar silicon carbide crystal and investigate the strongly confined resonance modes with scanning near-field optical microscopy. Reconfiguring the size of the resonators themselves result in enhanced mode confinements up to a value of λ/35.\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$${{{{{\\boldsymbol{\\lambda }}}}}}{{{{{\\boldsymbol{/}}}}}}{{{{{\\boldsymbol{35}}}}}}{{{{{\\boldsymbol{.}}}}}}$$\\end{document} Finally, unconventional cavity shapes with complex field patterns are explored as well. This study is a first step towards rapid prototyping of reconfigurable SPhP resonators that can be easily transferred to hyperbolic and anisotropic 2d materials.

Investigation of Crystallization Growth Characteristics of Mg(OH)2 Crystals under Unconstrained Conditions.

Utilizing MgO as the precursor and deionized water as the solvent, this study synthesized nanoparticles of Mg(OH)2 via hydrothermal methods, aiming to control its purity, particle size, and morphology by understanding its growth under non-uniform nucleation. Characterization of crystal morphology and structure was conducted through scanning electron microscopy and X-ray diffraction, while laser particle size detection assessed the secondary particle size distribution. The study focused on how MgO's hydrothermal process conditions influence Mg(OH)2 crystal growth, particularly through ion concentration and release rate adjustments to direct crystal growth facets. These adjustments shifted the dominant growth plane, enhancing the peak intensity ratio I001/I101 from 1.03 to 2.14, thereby reducing surface polarity and secondary aggregation of crystals. The study of the physicochemical properties of the same sample at different times revealed the pattern of crystal dissolution and recrystallization. A 2 h hydrothermal reaction notably altered the particle size distribution, with a decrease in particles sized 0.2~0.4 μm and an increase in those sized 0.4~0.6 μm, alongside new particles over 1 μm, indicating a shift toward uniformity through dissolution and recrystallization. Optimal conditions (6% magnesium oxide concentration, 160 °C, 2 h) led to the synthesis of highly dispersed, uniformly sized magnesium hydroxide, showcasing a simple, eco-friendly, and high-yield process.

Freeform Liquid–Crystal Polarization Imaging Optics: A Practical Approach from Design to Fabrication

AbstractFreeform liquid–crystal polarization imaging optics (LPIOs) have vast potential for application in next‐generation interactive displays like augmented reality and virtual reality. However, tailoring the phase profile of a freeform LPIO for flexible aberration correction and diffraction efficiency control is still a big challenge due to the difficulties arising from the non‐zero étendue of an imaging system and the finite bandwidth of LPIOs. Here, a practical approach to creating freeform LPIOs from design to fabrication is proposed. A freeform polarization exposure is developed to produce a flexible, precise, and ultra‐high‐resolution photoalignment pattern for a freeform LPIO. A cooperative optimization is performed between the freeform LPIO and the freeform polarization exposure system to find the optimal phase of the freeform LPIO and the optimal surface profiles of the freeform lenses employed in the exposure system to produce freeform wavefronts. The optimal phase of the freeform LPIO is then achieved by superposition interference of the engineered freeform wavefronts via freeform polarization exposure. The effectiveness of the approach and the advantages of freeform LPIOs is experimentally demonstrated. The proposed approach will significantly promote the widespread applications of freeform LPIOs in the field of optics and photonics.

Polar Crystals Using Molecular Chirality: Pseudosymmetric Crystallization toward Polarization Switching Materials.

Polar compounds with switchable polarization properties are applicable in various devices such as ferroelectric memory and pyroelectric sensors. However, a strategy to prepare polar compounds has not been established. We report a rational synthesis of a polar CoGa crystal using chiral cth ligands (SS-cth and RR-cth, cth = 5,7,7,12,14,14-hexamethyl-1,4,8,11-tetraazacyclotetradecane). Both the original homo metal Co crystal and Ga crystal exhibit a centrosymmetric isostructure, where the dipole moment of metal complexes with the SS-cth ligand and those with the RR-cth ligand are canceled out. To obtain a polar compound, the Co valence tautomeric complex with SS-cth in the homo metal Co crystal is replaced with the Ga complex with SS-cth by mixing Co valence tautomeric complexes with RR-cth and Ga complexes with SS-cth. The CoGa crystal exhibits polarization switching between the pseudononpolar state at a low temperature and the polar state at a high temperature because only Co complexes exhibit changes in electric dipole moment due to metal-to-ligand charge transfer. Following the same strategy, the polarization-switchable CoZn complex was synthesized. The CoZn crystal exhibits polarization switching between the polar state at a low temperature and the pseudononpolar state at a high temperature, which is the opposite temperature dependence to that of the CoGa crystal. These results revealed that the polar crystal can be synthesized by design, using a chiral ligand. Moreover, our method allows for the control of temperature-dependent polarization changes, which contrasts with typical ferroelectric compounds, in which the polar ferroelectric phase typically occurs at low temperatures.

Enhanced high-power behaviors of Mn-doped Pb (In1/2Nb1/2) O3-Pb(Mg1/3Nb2/3) O3-PbTiO3 piezoelectric crystals through combining direct and alternating current polarization

Elevating both the mechanical quality factor and piezoelectric properties is pivotal for enhancing the efficiency of high-power piezoelectric devices. Mn-doped Pb (In1/2Nb1/2) O3-Pb(Mg1/3Nb2/3) O3-PbTiO3 (Mn: PIN-PMN-PT) single crystals have previously exhibited a notable mechanical quality factor, yet encountered a substantial decline in piezoelectric coefficient. In pursuit of the concurrent optimization of these parameters, we explored the co-enhancement of mechanical quality factor and piezoelectric coefficient in [001]-oriented Mn: PIN-PMN-PT single crystals by employing a synergistic approach (DCP-ACP) involving direct-current poling (DCP) and alternating-current poling (ACP). Our investigation reveals a remarkable improvement, with the piezoelectric coefficient and mechanical quality factor experiencing a notable surge of 53% and 118%, respectively, compared to the outcomes achieved with DCP alone. Compared to the ACP method, the piezoelectric coefficient and the mechanical quality factor were improved more than 7% and 18%, respectively. Moreover, the coercive field and remnant polarization of the single crystals witnessed a substantial upswing post DCP-ACP. The results are attributed to the elimination of the 71° domain walls, as observed through polarized light microscopy. Here we demonstrate Mn: PIN-PMN-PT single crystals are expected to has high mechanical quality factor and strong piezoelectric constants through DCP-ACP, thus suggesting a new route to high performance ferroelectrics.

Wide-angle and Fano-shape contrast between emission and absorption in hybrid polariton-involved planar structure

Nonreciprocal light propagation in planar structure has become a hot topic because of the pattern-free fabrication process and the potentials for exploring heat transfer and energy management. An effective strategy incorporated with natural van der Waals material (α-phase molybdenum trioxide, α-MoO3), ultra-thin polar crystal (silicon carbide, SiC) thin film and a Weyl semimetal interlayer sitting on a metal (silver, Ag) substrate is proposed. The emission and absorption of the suggested device is explored with electromagnetic simulations that utilize the 4×4 transfer matrix method. Angular-resolved emission shows that the Fano-shape of nonreciprocity can be maintained within wide angle range. Tunable Fano resonances with different line shapes are demonstrated by varying the structural parameters. Moreover, the enhanced nonreciprocal radiation effect can be observed for both s- and p-polarized incidence waves. The proposal allows simultaneous control of spectral distribution and polarization of radiation, which will facilitate the active design and application of mid-infrared emitters.