Strong In-plane Optical Anisotropy Research Articles

Stabilized Synthesis of 2D Verbeekite: Monoclinic PdSe2 Crystals with High Mobility and In-Plane Optical and Electrical Anisotropy.

PdSe2 has a layered structure with an unusual, puckered Cairo pentagonal tiling. Its atomic bond configuration features planar 4-fold-coordinated Pd atoms and intralayer Se-Se bonds that enable polymorphic phases with distinct electronic and quantum properties, especially when atomically thin. PdSe2 is conventionally orthorhombic, and direct synthesis of its metastable polymorphic phases is still a challenge. Here, we report an ambient-pressure chemical vapor deposition approach to synthesize metastable monoclinic PdSe2. Monoclinic PdSe2 is shown to be synthesized selectively under Se-deficient conditions that induce Se vacancies. These defects are shown by first-principles density functional theory calculations to reduce the free energy of the metastable monoclinic phase, thereby stabilizing it during synthesis. The structure and composition of the monoclinic PdSe2 crystals are identified and characterized by scanning transmission electron microscopy imaging, convergent beam electron diffraction, and electron energy loss spectroscopy. Polarized Raman spectroscopy of the monoclinic PdSe2 flakes reveals their strong in-plane optical anisotropy. Electrical transport measurements show that the monoclinic PdSe2 exhibits n-type charge carrier conduction with electron mobilities up to ∼298 cm2 V-1 s-1 and a strong in-plane electron mobility anisotropy of ∼1.9. The defect-mediated growth pathway identified in this work is promising for phase-selective direct synthesis of other 2D transition metal dichalcogenides.

2D FeOCl: A Highly In-Plane Anisotropic Antiferromagnetic Semiconductor Synthesized via Temperature-Oscillation Chemical Vapor Transport.

2D van der Waals (vdW) transition-metal oxyhalides with low symmetry, novel magnetism, and good stability provide a versatile platform for conducting fundamental research and developing spintronics. Antiferromagnetic FeOCl has attracted significant interest owing to its unique semiconductor properties and relatively high Néel temperature. Herein, good-quality centimeter-scale FeOCl single crystals are controllably synthesized using the universal temperature-oscillation chemical vapor transport (TO-CVT) method. The crystal structure, bandgap, and anisotropic behavior of the 2D FeOCl are explored in detail. The absorption spectrum and electrical measurements reveal that 2D FeOCl is a semiconductor with an optical bandgap of ≈2.1eV and a resistivity of ≈10-1 Ω m at 295 K, and the bandgap increases with decreasing thickness. Strong in-plane optical and electrical anisotropies are observed in 2D FeOCl flakes, and the maximum resistance anisotropic ratio reaches 2.66 at 295 K. Additionally, the lattice vibration modes are studied through temperature-dependent Raman spectra and first-principles density functional calculations. A significant decrease in the Raman frequencies below the Néel temperature is observed, which results from the strong spin-phonon coupling effect in 2D FeOCl. This study provides a high-quality low-symmetry vdW magnetic candidate for miniaturized spintronics.

Polarization Conversion in MoS2 Flakes

We have studied experimentally a series of samples of layered MoS2 flakes with thicknesses varying from 1 to 10 μm and observed their strong in-plane optical anisotropy, which we attribute to the effects of strain in combination with fluctuations in the direction of the C-axis. This optical anisotropy allows us to convert the polarization of transmitted light from linear to circular with the degree up to 15%.

Anisotropic Optical Properties of 2D Silicon Telluride

ABSTRACTSilicon telluride (Si2Te3) is a silicon-based 2D chalcogenide with potential applications in optoelectronics. It has a unique crystal structure where Si atoms form Si-Si dimers to occupy the “metal” sites. In this paper, we report an ab initio computational study of its optical dielectric properties using the GW approximation and the Bethe-Salpeter equation (BSE). Strong in-plane optical anisotropy is discovered. The imaginary part of the dielectric constant in the direction parallel to the Si-Si dimers is found to be much lower than that perpendicular to the dimers. The optical measurement of the absorption spectra of 2D Si2Te3 nanoplates shows modulation of the absorption coefficient under 90-degree rotation, confirming the computational results. We show the optical anisotropy originates from the particular compositions of the wavefunctions in the valence and conduction bands. Because it is associated with the Si dimer orientation, the in-plane optical anisotropy can potentially be dynamically controlled by electrical field and strain, which may be useful for new device design. In addition, BSE calculations reduce GW quasiparticle band gap by 0.3 eV in bulk and 0.6 eV in monolayer, indicating a large excitonic effect in Si2Te3. Furthermore, including electron-hole interaction in bulk calculations significantly reduces the imaginary part of the dielectric constant in the out-of-plane direction, suggesting strong interlayer exciton effect in Si2Te3 multilayers.

Two-Dimensional Palladium Diselenide with Strong In-Plane Optical Anisotropy and High Mobility Grown by Chemical Vapor Deposition.

Two-dimensional (2D) palladium diselenide (PdSe2 ) has strong interlayer coupling and a puckered pentagonal structure, leading to remarkable layer-dependent electronic structures and highly anisotropic in-plane optical and electronic properties. However, the lack of high-quality, 2D PdSe2 crystals grown by bottom-up approaches limits the study of their exotic properties and practical applications. In this work, chemical vapor deposition growth of highly crystalline few-layer (≥2 layers) PdSe2 crystals on various substrates is reported. The high quality of the PdSe2 crystals is confirmed by low-frequency Raman spectroscopy, scanning transmission electron microscopy, and electrical characterization. In addition, strong in-plane optical anisotropy is demonstrated via polarized Raman spectroscopy and second-harmonic generation maps of the PdSe2 flakes. A theoretical model based on kinetic Wulff construction theory and density functional theory calculations is developed and described the observed evolution of "square-like" shaped PdSe2 crystals into rhombus due to the higher nucleation barriers for stable attachment on the (1,1) and (1,-1) edges, which results in their slower growth rates. Few-layer PdSe2 field-effect transistors reveal tunable ambipolar charge carrier conduction with an electron mobility up to ≈294 cm2 V-1 s-1 , which is comparable to that of exfoliated PdSe2 , indicating the promise of this anisotropic 2D material for electronics.

Highly Sensitive Polarization Photodetection Using a Pseudo-One-Dimensional Nb(1- x)Ti xS3 Alloy.

Low-symmetry layered two-dimensional (2D) materials with strong in-plane optical anisotropy can potentially be applied for polarization photodetection. This is especially true for those 2D materials with a direct band gap, which can efficiently absorb light with specific axial polarization. However, discovering such new anisotropic 2D materials with a direct band structure is still extremely challenging. Here, we fabricate a photodetector using a pseudo-one-dimensional (pseudo-1D) Nb(1- x)Ti xS3 alloy device and demonstrate that it is highly sensitive to the polarized light because of the strong in-plane optical anisotropy and direct band gap of the alloy by combining angle-resolved polarization Raman spectroscopy, azimuth-dependent reflectance difference microscopy, polarization-dependent absorption spectroscopy, and hybrid functional theory calculations. As a consequence, the polarization photodetector of the Nb(1- x)Ti xS3 alloy shows a large photocurrent anisotropic ratio and a high photoresponse. The choice of a low-symmetry layered pseudo-1D Nb(1- x)Ti xS3 alloy in polarization photodetection might open up new functionalities for novel optoelectronic device applications.

Structural and Optical Properties of Single- and Few-Layer Magnetic Semiconductor CrPS4.

Atomically thin binary two-dimensional (2D) semiconductors exhibit diverse physical properties depending on their composition, structure, and thickness. By adding another element in these materials, which will lead to formation of ternary 2D materials, the property and structure would greatly change and significantly expanded applications could be explored. In this work, we report structural and optical properties of atomically thin chromium thiophosphate (CrPS4), a ternary antiferromagnetic semiconductor. Its structural details were revealed by X-ray and electron diffraction. Transmission electron microscopy showed that preferentially cleaved edges are parallel to diagonal Cr atom rows, which readily identified their crystallographic orientations. Strong in-plane optical anisotropy induced birefringence that also enabled efficient determination of crystallographic orientation using polarized microscopy. The lattice vibrations were probed by Raman spectroscopy and exhibited significant dependence on thickness of crystals exfoliated down to a single layer. Optical absorption determined by reflectance contrast was dominated by d-d-type transitions localized at Cr3+ ions, which was also responsible for the major photoluminescence peak at 1.31 eV. The spectral features in the absorption and emission spectra exhibited noticeable thickness dependence and hinted at a high photochemical activity for single-layer CrPS4. The current structural and optical investigation will provide a firm basis for future study and application of this kind of atomically thin magnetic semiconductors.

Aligned silver nanowire-based transparent electrodes for engineering polarisation-selective optoelectronics.

We herein report on a remarkably simple, fast, and economic way of fabricating homogeneous and well oriented silver nanowires (AgNWs) that exhibit strong in-plane electrical and optical anisotropies. Using a small quantity of AgNW suspension, the horizontal-dip (H-dip) coating method was applied, in which highly oriented AgNWs were deposited unidirectionally along the direction of coating over centimetre-scale lengths very rapidly. In applying the H-dip-coating method, we adjusted the shear strain rate of the capillary flow in the Landau-Levich meniscus of the AgNW suspension, which induced a high degree of uniaxial orientational ordering (0.37–0.43) of the AgNWs, comparable with the ordering seen in archetypal nematic liquid crystal (LC) materials. These AgNWs could be used to fabricate not only transparent electrodes, but also LC-alignment electrodes for LC devices and/or polarising electrodes for organic photovoltaic devices, having the potential to revolutionise the architectures of a number of polarisation-selective opto-electronic devices for use in printed/organic electronics.

Engineering optical properties of a graphene oxide metamaterial assembled in microfluidic channels.

The dense packing of two dimensional flakes by van der Waals forces has enabled the creation of new metamaterials with desirable optical properties. Here we assemble graphene oxide sheets into a three dimensional metamaterial using a microfluidic technique and confirm their ordering via measurements of ellipsometric parameters, polarized optical microscopy, polarized transmission spectroscopy, infrared spectroscopy and scanning electron microscopy. We show that the produced metamaterials demonstrate strong in-plane optical anisotropy (Δn≈0.3 at n≈1.5-1.8) combined with low absorption (k<0.1) and compare them with as-synthesized samples of graphene oxide paper. Our results pave the way for engineered birefringent metamaterials on the basis of two dimensional atomic crystals including graphene and its derivatives.

Optical properties of ZnO/(Zn, Mg)O quantum wells

This paper reviews the optical properties of ZnO/(Zn, Mg)O single quantum wells grown by molecular beam epitaxy. Both heteroepitaxial quantum well growth along the polar c-direction and homoepitaxial quantum well growth on the nonpolar M plane cases are considered. The optical properties of these quantum wells are investigated by using reectance, continuous wave photoluminescence, and time-resolved photoluminescence spectroscopies. The quantum-conned Stark eect dominates the properties of the excitons for polar quantum wells. The magnitude of the internal electric eld that is induced by both spontaneous and piezoelectric polarizations is determined by comparing the experimental results with a variational calculation of excitonic energies and lifetimes. For nonpolar quantum wells, the optical spectra reveal strong in-plane optical anisotropies, as predicted by the group theory. Moreover, the radiative recombination of free excitons is dominating the quantum well photoluminescence even at room temperature.

Ultraviolet true zero-order wave plate made of birefringent porous silica

Porous Si made from (110) Si wafers exhibits strong in-plane optical anisotropy (birefringence) in the visible and near-IR ranges. Oxidation of the birefringent porous Si results in the formation of birefringent porous silica. We demonstrate that the degree of the birefringence of porous silica can be controlled by the oxidation condition, and very small birefringence can be achieved. The smallest anisotropy of the refractive index (Δn) is 0.001, which is about ten times smaller than that of quartz. The small birefringence allows us to produce true zero-order wave plates operating in the UV range.

Low temperature reflectivity study of nonpolar ZnO/(Zn,Mg)O quantum wells grown on M-plane ZnO substrates

We report growth of high quality ZnO/Zn0.8Mg0.2O quantum well on M-plane oriented ZnO substrates. The optical properties of these quantum wells are studied by using reflectance spectroscopy. The optical spectra reveal strong in-plane optical anisotropies, as predicted by group theory, and marked reflectance structures, as an evidence of good interface morphologies. Signatures ofc onfined excitons built from the spin-orbit split-off valence band, the analog of exciton C in bulk ZnO are detected in normal incidence reflectivity experiments using a photon polarized along the c axis of the wurtzite lattice. Experiments performed in the context of an orthogonal photon polarization, at 90^{\circ}; of this axis, reveal confined states analogs of A and B bulk excitons. Envelope function calculations which include excitonic interaction nicely account for the experimental report.

In-plane optical anisotropy in GaAsN/GaAs single-quantum well investigated by reflectance-difference spectroscopy

The interface properties of GaNxAs1−x/GaAs single-quantum well is investigated at 80 K by reflectance difference spectroscopy. Strong in-plane optical anisotropies (IPOA) are observed. Numerical calculations based on a 4 band K⋅P Hamiltonian are performed to analyze the origin of the optical anisotropy. It is found that the IPOA can be mainly attributed to anisotropic strain effect, which increases with the concentration of nitrogen. The origin of the strain component ϵxy is also discussed.

Stimulated emission at 474nm from an InGaN laser diode structure grown on a (112¯2) GaN substrate

The stimulated emissions from semipolar InGaN laser diode (LD) structures grown on (112¯2) GaN substrates are observed at room temperature under photopumped conditions. The measured emission peaks are in the photon energy range from 2.62eV (474nm)to3.05eV (405nm), and the emission intensity has a threshold behavior with respect to the pumping power. A strong in-plane optical anisotropy is observed between the two perpendicular directions, [1¯1¯23] and [11¯00], due to anisotropic matrix elements, which depend on the crystal orientation; the stimulated emission measured along the [1¯1¯23] direction occurs with a lower threshold pumping power at a lower energy compared to that obtained along the [11¯00] direction. The experimental results and the valence band calculations indicate that the transverse-electric mode with an electric vector along the [11¯00] direction is dominant for gain formation in semipolar and nonpolar InGaN LDs. Compared to c-plane InGaN LDs, semipolar InGaN LDs have comparable or less threshold pumping powers.

Effect of Fluorination of the Hydrophilic Heads on Morphology and Molecular Structure of Langmuir Monolayers of Long-Chain Ethers

Brewster angle microscopy (BAM) and grazing incidence X-ray diffraction (GIXD) were used to compare morphology and molecular structure of Langmuir monolayers of docosyl trifluoroethyl ether (DFEE) and docosyl ethyl ether (DEE) on water. When spread at a molecular area of 70 Å2/molecule both substances form islands of condensed phase and suspension of small 2D microcrystals attaching at the borderlines under compression. The DEE islands and the DEE monolayer at low surface pressure exhibit strong in-plane optical anisotropy, while the DFEE islands and the compact DFEE film are isotropic. The anisotropy of the DEE monolayer disappears at 10 mN/m, and above this surface pressure the monolayers with fluorinated and nonfluorinated heads are visually the same. The GIXD analysis identifies a L2‘ phase with NNN molecular tilt and NN lattice distortion in the DEE islands and DEE monolayer at low surface pressure. The maximum tilt angle at zero compression is 22.6°. The islands and the compact DFEE film consist of closely packed upright molecules forming an S phase. At high surface pressure both monolayers have the same upright molecular arrangement with centered rectangular lattice and practically the same unit cell parameters and lattice distortion. Under such conditions the DFEE and DEE molecules occupy the same area of the water surface Axy = A0 = 19.1 Å2. Since the van der Waals radius of the CF3 group is by 16% larger as compared to that of the CH3 group, the same A0 value of the two films means a significantly thinner hydration shell of the fluorinated head. Substitution of the terminal CH3 group in the DEE head by the CF3 group in the DFEE head removes the low-pressure tilted phase and causes formation of the condensed phase of upright fluorinated molecules even at no compression. The decreased headgroup hydration of DFEE could be responsible for the upright versus tilted orientation of the DFEE and DEE molecules at low surface pressure. We suppose that the mechanism of the continuous tilting transition causing erection of the DEE chains is related to an increasing dehydration of the headgroups under compression.

Polarization properties of nonpolar GaN films and (In,Ga)N/GaN multiple quantum wells

We have grown GaN films and (In,Ga)N/GaN multiple quantum wells (MQWs) by plasma-assisted molecular-beam epitaxy on γ-LiAlO2(100) substrates. Due to the crystal symmetry of γ-LiAlO2(100), GaN films and (In,Ga)N/GaN MQWs can be realized in a nonpolar (M-plane) configuration, i.e., the c axis of the wurtzite unit cell lies in the growth plane. For compressively, anisotropically strained M-plane GaN films, the band structure of the valence band changes in such a way that the optical transmittance becomes 100% linearly polarized for two orthogonal in-plane directions, where one of these directions is parallel to the c axis of the GaN film. The photoluminescence properties of M-plane In0.1Ga0.9N/GaN MQWs exhibit a strong in-plane optical anisotropy for linear polarization with an energy-dependent polarization degree of up to 96%, which is presumably also due to a large valence-band splitting induced by the large compressive strain in the QWs.

Polarization anisotropy of the photoluminescence of M-plane (In,Ga)N/GaN multiple quantum wells

We investigate the polarization anisotropy of the photoluminescence of an M-plane (11̄00) In0.1Ga0.9N/GaN multiple quantum well grown on γ-LiAlO2 (100) by molecular-beam epitaxy. In contrast to C-plane (0001) structures, a strong in-plane optical anisotropy with an energy-dependent polarization degree of up to 96% is observed for this M-plane sample. An apparent spectral shift of the emission with polarization angle is attributed to the impact of exciton localization on the polarization degree. The presence of localized states manifests itself further in the anomalous temperature dependence of the photoluminescence linewidth.

Polishing-related optical anisotropy of semi-insulating GaAs studied by reflectance difference spectroscopy

The strong in-plane optical anisotropy of (001) semi-insulating GaAs, which comes from the submicron region under the surface, has been observed by reflectance difference spectroscopy. The optical anisotropy can be explained by the anisotropic strain that is introduced by the asymmetric distribution of 60° dislocations during surface polishing. The simulated spectra reproduce the line shape of the experimental ones. The simulations show that the anisotropic strain is typically about 2.3×10−4.