Polarization-dependent Spectra Research Articles

Spin chain orientation and magneto-optical coupling in twisted NiPS3 homostructures

Magnetic two-dimensional (2D) materials have garnered significant attention due to their unique electronic, magnetic, and optical properties and their potential applications in next-generation electronic and optoelectronic devices. However, the magneto-optical effects of oligolayer antiferromagnetic materials remain inadequately understood. Here, we investigate the magnetic properties of few-layer nickel phosphorus trisulfide (NiPS3) and its twisted heterostructures, emphasizing the observation of optical phenomena at low temperatures (1.65 K). By stacking few-layer NiPS3 to fabricate twisted homostructures, we probe their magnetic characteristics using photoluminescence (PL) spectroscopy. Our results reveal that sharp exciton peaks emerge at low temperatures and that the spin chain orientation in oligolayer NiPS3 can be discerned through the polarization dependence of exciton PL intensity. Notably, fewer-layered NiPS3 exhibits a significant magneto-optical effect under an applied magnetic field, allowing the modulation of the polarization angle of its exciton PL spectrum. Additionally, the polarization-dependent Raman spectrum of NiPS3 shows substantial changes under the influence of a magnetic field. These findings underscore the potential of few-layer NiPS3 for future magneto-optical device applications.

Polarization-Independent Perfect Absorption in Monolayer Black Phosphorus Metasurfaces at Terahertz Frequencies via Critical Coupling.

Two-dimensional (2D) materials, which possess rich underlying physical properties that can provide the potential for designing more efficient and compact optoelectronic devices, have attracted great interest among scientists. Due to the atomic-scale thickness and the anisotropy of in-plane conductivity, 2D black phosphorus (BP) exhibits a polarization-dependent absorption spectrum with low absorption, which limits its further development in polarization-independent applications such as light absorbers and sensors. In this paper, a polarization-independent perfect absorber in the terahertz band is proposed, which is composed of a patterned BP monolayer deposited on a lossless photonic crystal (PC) slab with a back reflection mirror. The absorption of the patterned BP monolayer can reach 100% at resonant frequencies through the critical coupling mechanism of guided resonance. Moreover, the absorber exhibits polarization-independent absorption characteristics for vertically incident light, which are attributed to the 4-fold rotational symmetry of the PC substrate and the patterned BP monolayer deposited on it. This work opens up the possibility of fabricating optically polarization-independent devices based on single-layer 2D anisotropic materials.

Quantifying Chemical Reactions and Interfacial Properties at Buried Polymer/Polymer Interfaces.

Maleic anhydride (MAH)-modified polymers are used as tie layers for binding dissimilar polymers in multilayer polymer films. The MAH chemistry which promotes adhesion is well characterized in the bulk; however, only recently has the interfacial chemistry been studied. Sum frequency generation vibrational spectroscopy (SFG) is an interfacial spectroscopy technique which provides detailed information on interfacial chemical reactions, species, and molecular orientations and has been essential for characterizing the MAH chemistry in both nylon and ethyl vinyl alcohol copolymer (EVOH) model systems and coextruded multilayer films. Here, we further characterize the interfacial chemistry between MAH-modified polyethylene tie layers and both EVOH and nylon by investigating the model systems over a range of MAH concentrations. We can detect the interfacial chemical reaction products between MAH and the barrier layer at MAH concentrations of ≥0.022 wt % for nylon and ≥0.077 wt % for EVOH. Additionally, from the concentration-dependent reaction reactant/product SFG peak positions and the product imide or ester/acid C═O group tilt angles extracted from the polarization-dependent SFG spectra, we quantitatively observe concentration-dependent changes to both the interfacial chemistry and interfacial structure. The interfacial chemistry and molecular orientation as a function of MAH concentration are well correlated with the adhesion strength, providing important quantitative information for the future design of MAH-modified tie layers for a variety of important applications.

Tuning of the Berreman mode of GaN/AlxGa1-xN heterostructures on sapphire: The role of the 2D-electron gas in the mid-infrared

We investigated the mid-infrared optical properties of GaN/Al(x)Ga(1-x)N-type heterostructures on sapphire substrate grown by the Metal-Organic Chemical Vapor Deposition. We show how the polarization-dependent reflection spectrum is affected by the presence of the strain-induced 2D electron gas at the interfaces between Al(x)Ga(1-x)N and GaN layers. In particular, we show that the 2D electron gas contribution, modeled from its density and transport properties, can play a relevant role at the Berreman mode excitation condition. In this framework, our results offer an advanced approach for the optimization and design of GaN-based broadband optoelectronic and energy management devices.

Polarization-tuneable excitonic spectral features in the optoelectronic response of atomically thin ReS2

The low crystal symmetry of rhenium disulphide (ReS2) leads to the emergence of dichroic optical and optoelectronic response, absent in other layered transition metal dichalcogenides, which could be exploited for device applications requiring polarization resolution. To date, spectroscopy studies on the optical response of ReS2 have relied almost exclusively in characterization techniques involving optical detection, such as photoluminescence, absorbance, or reflectance spectroscopy. However, to realize the full potential of this material, it is necessary to develop knowledge on its optoelectronic response with spectral resolution. In this work, we study the polarization-dependent photocurrent spectra of few-layer ReS2 photodetectors, both in room conditions and at cryogenic temperature. Our spectral measurements reveal two main exciton lines at energies matching those reported for optical spectroscopy measurements, as well as their excited states. Moreover, we also observe an additional exciton-like spectral feature with a photoresponse intensity comparable to the two main exciton lines. We attribute this feature, not observed in earlier photoluminescence measurements, to a non-radiative exciton transition. The intensities of the three main exciton features, as well as their excited states, modulate with linear polarization of light, each one acquiring maximal strength at a different polarization angle. We have performed first-principles exciton calculations employing the Bethe-Salpeter formalism, which corroborate our experimental findings. Our results bring new perspectives for the development of ReS2-based nanodevices.

Anisotropic excitonic photocurrent in β−Ga2O3

Polarization-dependent photocurrent spectra are measured on a (001) $\ensuremath{\beta}\text{\ensuremath{-}}{\mathrm{Ga}}_{2}{\mathrm{O}}_{3}$ Schottky photodetector, where the linear polarization of light is rotated within the ab plane. Three spectral peaks at 4.92, 5.15, and 5.44 eV are observed that vary in intensity with the optical polarization direction. The peak transition energies are consistent with excitons previously reported in $\ensuremath{\beta}\text{\ensuremath{-}}{\mathrm{Ga}}_{2}{\mathrm{O}}_{3}$ due to interband transitions modified by the valence-band $p$-orbital anisotropy and the electron-hole Coulombic attraction. The measured polarization dependence of the photocurrent matches our predictions based on electromagnetic simulations of anisotropic absorption using the complex dielectric function tensor extracted from previous ellipsometry studies. These results illustrate the dominance of excitonic absorption and photocurrent in $\ensuremath{\beta}\text{\ensuremath{-}}{\mathrm{Ga}}_{2}{\mathrm{O}}_{3}$ both below and above the band gap, demonstrate a combined theoretical/experimental understanding of anisotropic photocarrier generation, and validate previous atomistic band-structure calculations in this low-symmetry ultrawide-band-gap semiconductor.

The impact of light polarization and the nature of modes in the formation of quasi-bound states in the continuum at near-normal incidence

Bound states in the continuum (BIC) is a peculiar resonant mode with an infinite radiative lifetime and quality factor (Q-factor) embedded within the radiation continuum, which find applications in sensing, lasing, and quantum photonics. While an ideal BIC with an infinite Q-factor can only occur in theory, observing quasi-BIC in realistic samples with finite sizes is possible. However, the robustness of quasi-BIC depends primarily on the trapped electromagnetic modes. Here, we discuss the polarization dependence and the nature of quasi-BIC mode in a two-dimensional array of gallium arsenide (GaAs) scatterers through finite difference time domain simulations and analytical calculations. The calculated angle- and polarization-dependent transmission spectra show quasi-BIC evolution with high Q-factor at near-normal incidence only for transverse magnetic polarization. The calculated total scattering cross-section implies the dominant contribution from electric dipole moments in generating the quasi-BIC. The evolution of quasi-BIC mode is discussed in terms of Mie or Fabry–Perot modes using geometry-dependent transmission and field intensity calculations. The proposed GaAs metasurfaces with quasi-BIC at 638 nm, corresponding to the zero phonon line of nitrogen-vacancy centers in diamond are useful for applications in photonic quantum technologies.

Ultraviolet-C AlGaN Resonant-Cavity Light-Emitting Diodes with Thermal Stability Pipe-AlGaN-Distributed Bragg Reflectors.

Ultraviolet-C AlGaN resonant-cavity light-emitting diodes with top and bottom pipe-AlGaN-distributed Bragg reflectors (DBRs) have been demonstrated. For the top/bottom DBR structures, 20 pairs of n+-AlGaN:Si/n-AlGaN:Si stack structures were transformed into the pipe-AlGaN:Si/n-AlGaN:Si DBRs through a doping-selective electrochemical wet etching process. The reflectivity of the pipe-AlGaN DBR structure was measured as 90% at 276.7 nm with a 20.9 nm flat stopband width. The anisotropic optical properties of the pipe-AlGaN DBR structure had been analyzed through the polarization-dependent reflectance spectra. For temperature-dependent reflectance spectra, the central wavelengths were slightly redshifted from 275 nm (100 K) to 281 nm (600 K) due to thermal expansion, refractive index increase, and partial strain release phenomena in the pipe-DBR structure. High photoluminescence emission intensity and line-width reducing phenomena were observed at 10 K in the UVC-LED with the resonant-cavity structure, which has potential for high-efficiency UV-C light source applications.

Polarization-Dependent Selection Rules and Optical Spectrum Atlas of Twisted Bilayer Graphene Quantum Dots

Understanding how symmetries encode optical polarization information into selection rules in molecules and materials is important for their optoelectronic applications including spectroscopic analysis, display technology, and quantum computation. Here, we extend polarization-dependent selection rules from atoms to solid-state systems with various point groups with the help of the rotational operator for circular polarization and the twofold rotational operator (or reflection operator) for linear polarization. We use these new selection rules to study the optical properties of twisted bilayer graphene quantum dots (TBGQDs), which inherit advantages of graphene quantum dot including its ultrathin thickness, excellent biocompatibility, and shape- and size-tunable optical absorption or emission. We study how the electronic structures and optical properties of TBGQDs rely on size, shape, twist angle, and correlation effects for TBGQDs with 10 different point groups for which we obtain an optical selection rule database. We show how current operator matrix elements identify the generalized polarization-dependent selection rules. Our results show that both the electronic and optical band gaps follow power-law size scalings with a dominant role of the twist angle. We derive an atlas of optical conductivity spectra for both size and twist angle in TBGQDs. As a result of quantum confinement effects, in the atlas a new type of optical conductivity features emerges with multiple discrete absorption frequencies ranging from infrared to ultraviolet energy, allowing for applications in photovoltaic devices and photodetectors. The atlas and size scaling provide a full structure–symmetry-function interrelation and hence offer an excellent basis for the geometrical manipulation of optical properties of TBGQDs as building blocks for novel integrated carbon optoelectronics.2 MoreReceived 5 October 2021Revised 14 April 2022Accepted 3 May 2022DOI:https://doi.org/10.1103/PhysRevX.12.021055Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article’s title, journal citation, and DOI.Published by the American Physical SocietyPhysics Subject Headings (PhySH)Research AreasElectronic structureOptical conductivityPhysical SystemsGrapheneTechniquesGroup theoryMean field theorySymmetriesTight-binding modelCondensed Matter, Materials & Applied Physics

Two-Photon Absorption and Photoluminescence of Individual CsPbBr3 Nanocrystal Superlattices

Nonlinear optical responses such as two-photon absorption and photoluminescence with halide perovskites are promising for the implications of fluorescence microscopy, high-density data storage, and microfabrication. Since a high degree of structural coherence can help improve the nonlinear optical responses, this study experimentally demonstrates that for individual CsPbBr3 nanocrystal superlattices, the two-photon luminescence is enhanced by about 16 times compared with that of randomly oriented nanocrystal films, and the polarization-dependent luminescence spectra reveal that the nanocrystal superlattices possess a 4-fold symmetry, which is similar to the single-crystal film structures. Due to their broad nonlinear absorption responses, wide-range interband photoluminescence is observed below the band gap. Furthermore, the intensity-dependent absorption results demonstrate that the two-photon absorption coefficient can be as large as 0.644 cm/MW, which is comparable with that of the semiconductor materials such as WS2 and ZnO. These superior performances make the CsPbBr3 nanocrystal superlattices promising for the implications of nonlinear devices such as optical power limiting and optical switches.

Silver-Coated 45° Radiated Tilted Fiber Grating Based Interferometer and Its Sensing Applications

We proposed a silver-coated 45° radiated tilted fiber grating (45° RTFG) based interferometer, in which the 45° RTFG is working as a beam splitter and a coupler, and the light transmitting in the fiber core is radiated out and resonant in the cladding radial cavity formed by the fully coated silver film, which forms multiple beam interference. We have theoretically and experimentally investigated the proposed fiber interferometer in terms of polarization-dependent transmission spectra, the free spectral range (FSR), spectral visibility and sensing characteristics. Due to the single polarization radiation feature of 45° RTFG, only S-polarized light could form the multiple beam interference and P-polarized light would pass through the grating with low loss. And the FSR of the proposed fiber interferometer is around 6.8 nm, which is determined by the 125 μm cladding diameter. The theoretical results show that the spectral visibility of interference is proportional to the coupling efficient of 45° RTFG and when the coupling efficient reaches 0.92, the spectral visibility is the maximum. In the experiment, the fiber interferometer formed by the 45° RTFG with 11 dB polarization extinction ratio has the spectral visibility of 26 dB. Moreover, we have also investigated the temperature, strain and twist characteristics of the proposed interferometer. The experimental results show that the transmission peak has a red shift with increasing temperature, with a sensitivity of 10 ± 0.1 pm/°C; The strain causes a blue shift for the transmission peak with −0.42 ± 0.01 pm/μϵ sensitivity, and the twist sensitivity reaches 22.408 ± 0.2 dB/rad. The proposed silver-coated 45° RTFG based interferometer has an in-fiber and compact structure, which can be potentially used for optical fiber sensing.

Polarization-controlled single-particle scattering imaging spectroscopy using waveguide excitation.

An imaging spectroscopic system that enables spatially-resolved detection of single-particle scattering with polarization-controlled waveguide excitation scheme is presented. The detected microscopic images of inhomogeneous nanostructures are recorded in a time sequence into a data cube based on a Michelson interferometer. The interferograms on selected pixels are Fourier-transformed into multiple spectra. The waveguide excitation scheme is presented for both transmission and reflection measurements while the dark-field excitation scheme is presented in transmission measurements for comparison. Gold nanoparticles, nanorods, and particles on film are utilized in the detection of polarization-dependent spectra. Measurement results are verified with the finite-difference time-domain (FDTD) simulations. The polarization-controlled coupling conditions in nanorods and particle-on-film systems are discussed with simulated field distributions around the nanostructures.

Revealing the Quantum-Confined Free Exciton A Anisotropic Emission in a CdS/CdS:SnS2 Superlattice Nanocone via Angle-Resolved Photoluminescence Spectroscopy

The nanostructures with exciton anisotropic emission are important in many applications due to the directionality of the flow of photons and the exciton confinement. Moreover, it is still a challenge to observe exciton anisotropic emission directly due to the limitation of measurement techniques and materials. Here, we observed the anisotropy of free exciton A (FXA) in a CdS/CdS:SnS2 superlattice nanocone by angle-resolved photoluminescence (ARPL) spectroscopy. Raman spectra and in situ spectral mapping indicate quasi-periodic SnS2 layers perpendicular to the nanocone within the CdS/CdS:SnS2 superlattice nanocone. Polarization-dependent ARPL spectra discriminated two exciton series, namely, FXA and free exciton B (FXB). By comparing different CdS nanostructures, FXA is found to be omniscient in different samples, but it is even significant in the CdS/CdS:SnS2 superlattice nanocone due to the local dielectric confinement of SnS2 layers in the nanocone and the enhanced anisotropic exciton–phonon coupling. Meanwhile, ARPL spectra indicated that the FXA emission blue shifts with reducing cross-sectional radius, while the FXB emission does not. The comprehensive understanding of the FXA anisotropic emission and quantum confinement effect in the CdS/CdS:SnS2 superlattice nanocone may trigger the potential applications in future anisotropy-polarized devices and wavelength-tuning lasers.

Calculated phonon modes, infrared and Raman spectra in orthorhombic α − MoO3 and monolayer MoO3

Orthorhombic α−MoO3 is a layered oxide with various applications and with excellent potential to be exfoliated as a 2D ultra-thin film or monolayer. In this paper, we present a first-principles computational study of its vibrational properties. Our focus is on the zone center modes, which can be measured by a combination of infrared and Raman spectroscopy. The polarization dependent spectra are simulated. Calculations are also performed for a monolayer form in which “double layers” of Mo2O6, which are weakly van der Waals bonded in the α-structure, are isolated. Shifts in phonon frequencies are analyzed.

Simultaneous Measurement of pH and Temperature with Phase-Shifted Long-Period Fiber Grating Inscribed on High-Birefringence Fiber by CO₂ Laser Pulses.

We propose an optical fiber grating sensor capable of simultaneously measuring pH and temperature based on a phase-shifted long-period fiber grating (PS-LPFG) inscribed on high-birefringence fiber (HBF). The PS-LPFG was fabricated on HBF with CO₂ laser pulses, and a phase shift π was induced by inserting a grating-free fiber region (GFFR) between two identical LPFGs with a grating period of ˜510 μm. The length of the GFFR was set as half of the grating period to induce a π phase shift. With the spectral characteristics of a π-PS-LPFG exhibiting two split attenuation bands, the PS-LPFG written on HBF, which is referred to as the HB-PS-LPFG, can create two polarization-dependent transmission spectra with dual-resonance dips at different wavelengths according to two orthogonal input polarization states, e.g., linear horizontal polarization (LHP) and linear vertical polarization (LVP). For simultaneous measurement of pH and temperature with the fabricated HB-PS-LPFG as a sensor head, the inter-resonance wavelength separation of the dual-resonance dips in each transmission spectrum obtained for an LHP or LVP input signal was exploited as a sensor indicator. By investigating the wavelength changes of the two sensor indicators, which were induced by pH and temperature variations, linear and independent spectral responses to both pH and temperature variations were experimentally confirmed in a pH range from 1 to 11 and a temperature range from 25 to 65 °C. Owing to the unique pH and temperature responses of the fabricated HB-PS-LPFG, ambient variations in pH and temperature could be simultaneously estimated from the measured wavelength changes and sensitivities of the two sensor indicators.

Polarization of hard X-ray dielectronic satellite lines from Na-like W ions

One of the important signatures of non-thermal high-atomic-number multiply ionized plasmas is polarization of hard x-ray line emission. Atomic processes in laboratory and astrophysical plasmas with anisotropic electron distribution that can lead to such polarization include dielectronic recombination. All previous research on x-ray line polarization of dielectronic satellite lines was mostly focused on K-shell radiation. Here we present one of the first studies of polarization of L-shell dielectronic satellite lines using the hard x-ray spectra of Na-like W produced by dielectronic recombination. Polarization of dielectronic satellites is calculated using two approaches: density matrix formalism and the FAC code. The most intense dielectronic satellite lines of Na-like W appeared to be positively polarized with the maximum degree of polarization between 0.4545 and 0.6. Polarization-dependent dielectronic satellite spectra of Na-like W are calculated with a gaussian electron distribution function centered at the beam energies from 2400 eV to 4100 eV. Such spectra cover the spectral range from 1.19 Å to 1.38 Å with each spectrum including two traces of line intensities associated with the parallel polarization and perpendicular polarization state. The polarization-dependent spectra were found to be strongly dependent on the energy of the electron beam which can be used for the development of x-ray plasma polarization spectroscopy to study non-thermal multiply ionized W plasmas. Radiative and polarization properties of W radiation studied in this paper are important for fusion research.

Optical anisotropy of interface-bound exciton emission in a-plane ZnO/Zn1-xMgxO MQWs with Zn1-yMgyO buffer layer

The anisotropic exciton emission in a-plane nonpolar ZnO/ZnMgO MQWs offers opportunity for anisotropic photonic devices. By introducing Zn1-yMgyO buffer layer between r-plane sapphire substrate and MQWs, we investigated the structural and optical properties of ten-period a-plane ZnO/Zn1−xMgxO (ZnO/ZnMgO) multiple quantum wells (MQWs) with different widths of Zn1−xMgxO barrier layers grown by pulsed-laser deposition on Zn1-yMgyO buffered r-plane sapphire. Polarization-dependent photoluminescence spectra reveal that two additional linear polarizations of interface-bound exciton emission with E⊥c orienting at ~± 50° with respect to the regular a-plane MQWs are attributed to the generation of (0 0 0 2)-oriented nano-domains (NDs). As evidenced by XRD and TEM, we found four sets of (0 0 0 2)-oriented MQWs NDs are embedded in regular a-plane ZnO/ZnMgO MQWs with 90° in-plane rotation from one another which are inclined by 27.6° towards the [1 1 2¯ 0]-direction of the ZnO/ZnMgO MQWs. The existence of (0 0 0 2)-oriented NDs is further confirmed by the phase-contrast atomic force microscopy that modulates the optical anisotropy of interface-bound exciton emission in a-plane nonpolar ZnO/ZnMgO MQWs.

Anisotropic band structure of TiS3 nanoribbon revealed by polarized photocurrent spectroscopy

A re-discovered member of the layered material family, Titanium Trisulfide (TiS3), has attracted intense research interest recently for the possibility of realizing an exciton insulator in the monolayer limit. However, due to their quasi-one-dimensional nature, thin TiS3 flakes are typically in the form of nanoribbons that are challenging to characterize by optical absorption spectra, due to their small cross section. Here, we employ a sensitive photocurrent spectroscopy technique to probe the absorption of a thin TiS3 nanoribbon in a field-effect transistor configuration. We have found a significant modification of the band structure of the thin TiS3 nanoribbon, compared to its bulk counterpart. In addition, the polarization-dependent photocurrent spectra of thin TiS3 nanoribbons exhibit greatly enhanced anisotropy compared to that of a thick TiS3 device. The atomically thin TiS3 flake, thus, not only provides an exciting platform for investigating many-body physics but also enables anisotropic quantum optoelectronics.

Polarization dependent cladding modes coupling and spectral analyses of excessively tilted fiber grating.

We report on the detailed analyses of mode coupling from fiber core to cladding in excessively tilted fiber gratings (ETFGs). Cladding modes responsible for the typical dual peak pairs in the transmission spectrum of ETFGs are identified with phase matching condition, which suggests two set of dual peak pairs generated from coupling to cladding modes with even and odd azimuthal order. The polarization dependence of those dual peak pairs are also investigated by calculating the coupling coefficients of cladding modes for two orthogonal polarizations. With the calculated coupling coefficients, the measured polarization dependent spectra can be reproduced numerically.

Anisotropic properties of pipe-GaN distributed Bragg reflectors.

We report here a simple and robust process to convert periodic Si-doped GaN/undoped-GaN epitaxial layers into a porous-GaN/u-GaN distributed Bragg reflector (DBR) structure and demonstrate its material properties in a high-reflectance epitaxial reflector. Directional pipe-GaN layers with anisotropic optical properties were formed from n+-GaN : Si layers in a stacked structure through a lateral and doping-selective electrochemical etching process. Central wavelengths of the polarized reflectance spectra were measured to be 473 nm and 457 nm for the pipe-GaN reflector when the direction of the linear polarizer was along and perpendicular to the pipe-GaN structure. The DBR reflector with directional pipe-GaN layers has the potential for a high efficiency polarized light source and vertical cavity surface emitting laser applications.