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At least 109 records · Page 6
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Spin-orbit–coupled exciton-polariton condensates in lead halide perovskites

Spin-orbit coupling (SOC) is responsible for a range of spintronic and topological processes in condensed matter. Here, we show photonic analogs of SOCs in exciton-polaritons and their condensates in microcavities composed of birefringent lead halide perovskite single crystals. The presence of crystalline anisotropy coupled with splitting in the optical cavity of the transverse electric and transverse magnetic modes gives rise to a non-Abelian gauge field, which can be described by the Rashba-Dresselhaus Hamiltonian near the degenerate points of the two polarization modes. With increasing density, the exciton-polaritons with pseudospin textures undergo phase transitions to competing condensates with orthogonal polarizations. Unlike their pure photonic counterparts, these exciton-polaritons and condensates inherit nonlinearity from their excitonic components and may serve as quantum simulators of many-body SOC processes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Magnetism Studies of Bis(acyl)phosphide-Supported Eu 3+ and Eu 2+ Complexes

A series of bis(acyl)phosphide-supported Eu complexes were synthesized (bis(acyl)phosphide = BAP). Here, in this study, BAP ligands proved to be excellent ligands for the synthesis of both Eu 3+ and Eu 2+ molecular complexes. Sodium bis(mesitoyl)phosphide (Na( mes BAP)) and sodium bis(2,4,6-triisopropylbenzoyl)phosphide (Na( tripp BAP)) were employed as ligand precursors for the synthesis of the Eu 3+ complexes Eu(bis(mesitoyl)phosphide) 3 (thf) 2 (Eu( mes BAP) 3 (thf) 2 ) and Eu(bis(2,4,6-triisopropylbenzoyl)phosphide) 3 (Eu( tripp BAP) 3 ), as well as the Eu 2+ complex, Eu(bis(2,4,6-triisopropylbenzoyl)phosphide) 2 (dme) 2 (Eu( tripp BAP) 2 (dme) 2 ) (thf = tetrahydrofuran, dme = 1,2-dimethoxyethane). All complexes were characterized using a combination of UV–vis–NIR–IR and NMR spectroscopies, and single-crystal X-ray diffraction (SC-XRD). The magnetic properties of these three monomeric Eu complexes were investigated by variable-temperature magnetic susceptibility. The magnetic data are typical for these ions, with Eu( tripp BAP) 2 (dme) 2 displaying Curie-type behavior. Both Eu( tripp BAP) 3 and Eu( mes BAP) 3 (thf) 2 possess similar 7 F 0 - 7 F 1 spin–orbit energy gaps and a similar zero-field splitting of the 7 F 1 state.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Heat conduction in magnetic insulators via hybridization of acoustic phonons and spin-flip excitations

We present a comprehensive study on the longitudinal magnetothermal transport in a paramagnetic effective spin-1/2 magnetic insulator CsYbSe 2 , by introducing a minimal model requiring only Zeeman splitting and magnetoelastic coupling. We use it to argue that hybridized excitations—formed from acoustic phonons and localized spin-flip-excitations across the Zeeman gap of the crystal electric field ground doublet—are responsible for a nonmonotonic field dependence of longitudinal thermal conductivity. Beyond highlighting a starring role for phonons, our results raise the prospect of universal magnetothermal transport phenomena in paramagnetic insulators that originate from simple features shared across many systems. Published by the American Physical Society 2025

Pocs, Christopher A.↗
DOE OSTI2022

Quantification of Exciton Fine Structure Splitting in a Two-Dimensional Perovskite Compound

Applications of two-dimensional (2D) perovskites have significantly outpaced the understanding of many fundamental aspects of their photophysics. The optical response of 2D lead halide perovskites is dominated by strongly bound excitonic states. However, a comprehensive experimental verification of the exciton fine structure splitting and associated transition symmetries remains elusive. Here we employ low temperature magneto-optical spectroscopy to reveal the exciton fine structure of (PEA) 2 PbI 4 (here PEA is phenylethylammonium) single crystals. We observe two orthogonally polarized bright in-plane free exciton (FX) states, both accompanied by a manifold of phonon-dressed states that preserve the polarization of the corresponding FX state. Introducing a magnetic field perpendicular to the 2D plane, we resolve the lowest energy dark exciton state, which although theoretically predicted, has systematically escaped experimental observation (in Faraday configuration) until now. These results corroborate standard multiband, effective-mass theories for the exciton fine structure in 2D perovskites and provide valuable quantification of the fine structure splitting in (PEA) 2 PbI 4 .

36 MATERIALS SCIENCE↗
DOE OSTI2020

Single-Crystal X-Ray Spectropolarimeter

X-ray spectropolarimetry is a diagnostics technique suitable for measuring intense electron beams and strong magnetic fields in hot, dense plasmas. To increase the accuracy achievable, we investigated the possibility of measuring both orthogonal components of linear polarization simultaneously using a single crystal. We demonstrated experimentally for the first time that crystals with cubic symmetry can be used as polarizing beam splitters. We also found that the polarization-splitting planes in cubic crystals can be accessed in two crystal orientations, a property that can be used to decrease the clutter in polarized spectra. In parallel, we developed a ray-tracing code and are working to add the crystal reflectivity to instrument modeling codes, to help us interpret the spectra and to design spectroscopic and spectropolarimetric instruments. This work is motivated by the need to perform measurements of important quantities in difficult experimental conditions, such as the axial magnetic field at stagnation in magnetized liner inertial fusion loads.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
NASA NTRS1974

Separation of surface and bulk minority-carrier lifetimes in silicon

A photoexcitation technique is suggested which is direct and convenient, requiring little special equipment. No change in the dimensions of the crystal sample is necessary. Although related to the technique of interposing a filter between the light source and the sample, it differs in that the filter is part of the crystal itself. Basically, one of the electrodes is split into two electrodes, one collecting charge from carriers excited in the bulk. This phenomenon in which the carriers follow very closely the electric field lines has been used in position-sensitive semiconductor radiation detectors (Norbeck and Carlson, 1963) but has not been applied to lifetime measurements. In a sense, the split electrode creates a sample without a surface.

Carroll, K. A.↗
DOE OSTI2024

Determining the Effects of Zero-Field Splitting and Magnetic Exchange in Dimeric Europium(II) Complexes

Related BAP [BAP = bis(acyl)phosphide] and Acac (Acac = β-diketonate) molecules perform as robust supports for both lanthanide and actinide metals. Here, a molecular bimetallic Eu 2+ complex was successfully targeted and isolated by employing sodium bis(mesitoyl)phosphide [Na( mes BAP)] in a salt metathesis with EuI 2 , producing [Eu( mes BAP) 2 (et 2 o)] 2 (et 2 o = metal-coordinated diethyl ether). The corresponding Acac-Eu 2+ complex was targeted using mes Acac– (1,3-dimesityl-1,3-propanedione), generating [Eu( mes Acac) 2 (et 2 o)] 2 . Both complexes were characterized by single-crystal X-ray diffraction, UV–vis, IR, and NMR spectroscopies, and variable-temperature magnetic susceptibility. [Eu( mes BAP) 2 (et 2 o)] 2 was persistent under anaerobic, anhydrous conditions, whereas the analogous [Eu( mes Acac) 2 (et 2 o)] 2 showed evidence of decomposition under identical conditions. Finally, variable-temperature magnetic susceptibility and magnetization studies of [Eu( mes BAP) 2 (et 2 o)] 2 and [Eu( mes Acac) 2 (et 2 o)] 2 were performed, resulting in similar magnetic exchange coupling values of J ex = –0.018 and –0.023 cm –1 and axial zero-field-splitting D values of –0.38 and –0.51 cm –1 , respectively.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Quantum spin ice response to a magnetic field in the dipole-octupole pyrochlore Ce 2 Zr 2 O 7

The pyrochlore magnet Ce 2 Zr 2 O 7 has attracted much attention as a quantum spin ice candidate whose novelty derives in part from the dipolar-octupolar nature of the Ce 3+ pseudospin-1/2 degrees of freedom it possesses. We report heat capacity measurements on single crystal samples of Ce 2 Zr 2 O 7 down to T~0.1K in a magnetic field along the [$1,\bar{1},0$] direction. These measurements show that the broad hump in the zero-field heat capacity moves higher in temperature with increasing field strength and is split into two separate humps by the [$1,\bar{1},0$] magnetic field at ~2T. These separate features are due to the decomposition of the pyrochlore lattice into effectively decoupled chains for fields in this direction: One set of chains (α chains) is polarized by the field while the other (β chains) remains free. This situation is similar to that observed in the classical spin ices Ho 2 Ti 2 O 7 and Dy 2 Ti 2 O 7 , but with the twist that here the strong transverse exchange interactions produce substantial quantum effects. Our theoretical modeling suggests that the β chains are close to a critical state, with nearly-gapless excitations. We also report elastic and inelastic neutron scattering measurements on single crystal Ce 2 Zr 2 O 7 in [$1,\bar{1},0$] and [0,0,1] magnetic fields at temperatures down to T=0.03K. The elastic scattering behaves consistently with the formation of independent chains for a [$1,\bar{1},0$] field, while the [0,0,1] field produces a single field-induced elastic magnetic Bragg peak at (0,2,0) and equivalent wavevectors, indicating a polarized spin ice state for fields above ~3T. For both [$1,\bar{1},0$] and [0,0,1] magnetic fields, our inelastic neutron scattering results show an approximately dispersionless continuum of scattering that increases in both energy and intensity with increasing field strength. By modeling the complete set of experimental data using numerical linked cluster and semiclassical molecular dynamics calculations, we demonstrate the dominantly multipolar nature of the exchange interactions in Ce 2 Zr 2 O 7 and the smallness of the parameter θ, which controls the mixing between dipolar and octupolar degrees of freedom. Finally, these results support previous estimates of the microscopic exchange parameters and place strong constraints on the theoretical description of this prominent spin ice candidate.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRS1993

Optical beam forming techniques for phased array antennas

Conventional phased array antennas using waveguide or coax for signal distribution are impractical for large scale implementation on satellites or spacecraft because they exhibit prohibitively large system size, heavy weight, high attenuation loss, limited bandwidth, sensitivity to electromagnetic interference (EMI) temperature drifts and phase instability. However, optical beam forming systems are smaller, lighter, and more flexible. Three optical beam forming techniques are identified as applicable to large spaceborne phased array antennas. They are (1) the optical fiber replacement of conventional RF phased array distribution and control components, (2) spatial beam forming, and (3) optical beam splitting with integrated quasi-optical components. The optical fiber replacement and the spatial beam forming approaches were pursued by many organizations. Two new optical beam forming architectures are presented. Both architectures involve monolithic integration of the antenna radiating elements with quasi-optical grid detector arrays. The advantages of the grid detector array in the optical process are the higher power handling capability and the dynamic range. One architecture involves a modified version of the original spatial beam forming approach. The basic difference is the spatial light modulator (SLM) device for controlling the aperture field distribution. The original liquid crystal light valve SLM is replaced by an optical shuffling SLM, which was demonstrated for the 'smart pixel' technology. The advantages are the capability of generating the agile beams of a phased array antenna and to provide simultaneous transmit and receive functions. The second architecture considered is the optical beam splitting approach. This architecture involves an alternative amplitude control for each antenna element with an optical beam power divider comprised of mirrors and beam splitters. It also implements the quasi-optical grid phase shifter for phase control and grid amplifier for RF power. The advantages are no SLM is required for this approach, and the complete antenna system is capable of full monolithic integration.

Wu, Te-Kao↗
NASA NTRS1992

Fast optical switch having reduced light loss

An electrically controlled optical switch uses an electro-optic crystal of the type having at least one set of fast and slow optical axes. The crystal exhibits electric field induced birefringence such that a plane of polarization oriented along a first direction of a light beam passing through the crystal may be switched to a plane of polarization oriented along a second direction. A beam splitting polarizer means is disposed at one end of the crystal and directs a light beam passing through the crystal whose plane of polarization is oriented along the first direction differently from a light beam having a plane of polarization oriented along the second direction. The electro-optic crystal may be chosen from the crystal classes 43m, 42m, and 23. In a preferred embodiment, the electro-optic crystal is a bismuth germanium oxide crystal or a bismuth silicon oxide crystal. In another embodiment of the invention, polarization control optics are provided which transmit substantially all of the incident light to the electro-optic crystal, substantially reducing the insertion loss of the switch.

Nelson, Bruce N.↗
DOE OSTI2026

On-Chip Cavity Electroacoustics Using Lithium Niobate Phononic Crystal Resonators

Mechanical systems are pivotal in quantum technologies because of their long coherent time and versatile coupling to qubit systems. So far, the coherent and dynamic control of gigahertz-frequency mechanical modes mostly relies on optomechanical coupling and piezoelectric coupling to superconducting qubits. Here, we demonstrate on-chip cavity electroacoustic dynamics using our microwave-frequency electrically modulated phononic crystal resonators on lithium niobate. Leveraging the high dispersion of phononic crystal, our acoustic modes space unevenly in the frequency spectrum, emulating atomic energy levels. Atomiclike transitions between different acoustic modes are selectively achieved by applying electrical fields to modulate acoustic modes via the nonlinear piezoelectricity of lithium niobate. Among two modes, we demonstrate Autler-Townes splitting, ac Stark shift, and Rabi oscillation with a maximum cooperativity of 4.18. Extending to three modes, we achieve nonreciprocal frequency conversions with an isolation up to 20 dB. Nonreciprocity can be tuned by the time delay between the two modulating pulses. Finally, our cavity electroacoustic platform could find broad applications in sensing, microwave signal processing, acoustic computing, and quantum acoustics.

Rabi model↗
DOE OSTI2023

Haldane topological spin-1 chains in a planar metal-organic framework

Haldane topological materials contain unique antiferromagnetic chains with symmetry-protected energy gaps. Such materials have potential applications in spintronics and future quantum computers. Haldane topological solids typically consist of spin-1 chains embedded in extended three-dimensional (3D) crystal structures. Here, we demonstrate that [Ni(μ-4,4'-bipyridine)(μ-oxalate)] n (NiBO) instead adopts a two-dimensional (2D) metal-organic framework (MOF) structure of Ni 2+ spin-1 chains weakly linked by 4,4'-bipyridine. NiBO exhibits Haldane topological properties with a gap between the singlet ground state and the triplet excited state. The latter is split by weak axial and rhombic anisotropies. Several experimental probes, including single-crystal X-ray diffraction, variable-temperature powder neutron diffraction (VT-PND), VT inelastic neutron scattering (VT-INS), DC susceptibility and specific heat measurements, high-field electron spin resonance, and unbiased quantum Monte Carlo simulations, provide a detailed, comprehensive characterization of NiBO. Vibrational (also known as phonon) properties of NiBO have been probed by INS and density-functional theory (DFT) calculations, indicating the absence of phonons near magnetic excitations in NiBO, suppressing spin-phonon coupling. The work here demonstrates that NiBO is indeed a rare 2D-MOF Haldane topological material.

36 MATERIALS SCIENCE↗
NASA NTRS1971

Surface field analysis of splitting of orbitals of atoms and ions approaching a metal surface.

The splitting of p- and d-orbitals of an atom or an ion which is caused by the locally varying potential near the surface of a realistic metal has been studied for bcc and fcc substrates. A quasi-ionic model is reasonable at close distance, inasmuch as the electron gas does not completely screen the ionic cores. The arrangement of ion cores near the surface causes the potential to vary in three dimensions. Expressions for energy levels were derived for an unsymmetric group using the quasi-ionic model and techniques used in the treatment of crystal field of nearest neighbors. A number of cases involving ions, as well as atoms in the vicinity of a metal substrate were numerically evaluated.

Rao, P. V. S.↗
DOE OSTI2023

Optically Active Spin Defects in Few-Layer Thick Hexagonal Boron Nitride

Optically active spin defects in hexagonal boron nitride (hBN) are promising quantum systems for the design of two-dimensional quantum sensing units offering optimal proximity to the sample being probed. In this Letter, we first demonstrate that the electron spin resonance frequencies of boron vacancy centers ($V$$^{–}_{B}$) can be detected optically in the limit of few-atomic-layer thick hBN flakes despite the nanoscale proximity of the crystal surface that often leads to a degradation of the stability of solid-state spin defects. We then analyze the variations of the electronic spin properties of $V$$^{–}_{B}$ centers with the hBN thickness with a focus on (i) the zero-field splitting parameters, (ii) the optically induced spin polarization rate and (iii) the longitudinal spin relaxation time. Furthermore, this Letter provides important insights into the properties of $V$$^{–}_{B}$ centers embedded in ultrathin hBN flakes, which are valuable for future developments of foil-based quantum sensing technologies.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Rashba splitting in organic–inorganic lead–halide perovskites revealed through two-photon absorption spectroscopy

Abstract The Rashba splitting in hybrid organic–inorganic lead–halide perovskites (HOIP) is particularly promising and yet controversial, due to questions surrounding the presence or absence of inversion symmetry. Here we utilize two-photon absorption spectroscopy to study inversion symmetry breaking in different phases of these materials. This is an all-optical technique to observe and quantify the Rashba effect as it probes the bulk of the materials. In particular, we measure two-photon excitation spectra of the photoluminescence in 2D, 3D, and anionic mixed HOIP crystals, and show that an additional band above, but close to the optical gap is the signature of new two-photon transition channels that originate from the Rashba splitting. The inversion symmetry breaking is believed to arise from ionic impurities that induce local electric fields. The observation of the Rashba splitting in the bulk of HOIP has significant implications for the understanding of their spintronic and optoelectronic device properties.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

All-optical reconfiguration of single silicon-vacancy centers in diamond for non-volatile memories

Strain engineering is vital for tuning the optical and spin properties of solid-state color centers, enhancing spin coherence and compensating emission wavelength shift. Here, we develop an all-optical approach to directly modify the local strain of color centers at the nanoscale by migrating the nearby defect. High-power pulsed optical irradiation triggers defect migration, which subsequently leads to the redistribution of the local crystal lattice of the host material. This redistribution alters the strain experienced by nearby color centers. Using silicon-vacancy centers in diamond, we validate this method and demonstrate a ground state splitting enhancement of up to 1.8 THz. Unlike conventional methods, our approach requires no external fields or nanostructure modifications, enabling non-volatile strain control and optical memory functionality across wide temperature ranges. Its local, permanent nature offers a scalable path for enhancing spin coherence in large-scale quantum systems and has potential applications in photonic machine learning.

Nanoscale devices↗
NASA NTRS2011

Multi-Wavelength, Multi-Beam, and Polarization-Sensitive Laser Transmitter for Surface Mapping

A multi-beam, multi-color, polarized laser transmitter has been developed for mapping applications. It uses commercial off-the-shelf components for a lowcost approach for a ruggedized laser suitable for field deployment. The laser transmitter design is capable of delivering dual wavelengths, multiple beams on each wavelength with equal (or variable) intensities per beam, and a welldefined state of polarization. This laser transmitter has been flown on several airborne campaigns for the Slope Imaging Multi-Polarization Photon Counting Lidar (SIMPL) instrument, and at the time of this reporting is at a technology readiness level of between 5 and 6. The laser is a 1,064-nm microchip high-repetition-rate laser emitting energy of about 8 microjoules per pulse. The beam was frequency-doubled to 532 nm using a KTP (KTiOPO4) nonlinear crystal [other nonlinear crystals such as LBO (LiB3O5) or periodically poled lithium niobiate can be used as well, depending on the conversion efficiency requirements], and the conversion efficiency was approximately 30 percent. The KTP was under temperature control using a thermoelectric cooler and a feedback monitoring thermistor. The dual-wavelength beams were then spectrally separated and each color went through its own optical path, which consisted of a beam-shaping lens, quarterwave plate (QWP), and a birefringent crystal (in this case, a calcite crystal, but others such as vanadate can be used). The QWP and calcite crystal set was used to convert the laser beams from a linearly polarized state to circularly polarized light, which when injected into a calcite crystal, will spatially separate the circularly polarized light into the two linear polarized components. The spatial separation of the two linearly polarized components is determined by the length of the crystal. A second set of QWP and calcite then further separated the two beams into four. Additional sets of QWP and calcite can be used to further split the beams into multiple orders of two. The spatially separated beams had alternating linearly polarization states; a half-wave plate (HWP) array was then made to rotate the alternating states of A multi-beam, multi-color, polarized laser transmitter has been developed for mapping applications. It uses commercial off-the-shelf components for a lowcost approach for a ruggedized laser suitable for field deployment. The laser transmitter design is capable of delivering dual wavelengths, multiple beams on each wavelength with equal (or variable) intensities per beam, and a welldefined state of polarization. This laser transmitter has been flown on several airborne campaigns for the Slope Imaging Multi-Polarization Photon Counting Lidar (SIMPL) instrument, and at the time of this reporting is at a technology readiness level of between 5 and 6. The laser is a 1,064-nm microchip high-repetition-rate laser emitting energy of about 8 microjoules per pulse. The beam was frequency-doubled to 532 nm using a KTP (KTiOPO4) nonlinear crystal [other nonlinear crystals such as LBO (LiB3O5) or periodically poled lithium niobiate can be used as well, depending on the conversion efficiency requirements], and the conversion efficiency was approximately 30 percent. The KTP was under temperature control using a thermoelectric cooler and a feedback monitoring thermistor. The dual-wavelength beams were then spectrally separated and each color went through its own optical path, which consisted of a beam-shaping lens, quarterwave plate (QWP), and a birefringent crystal (in this case, a calcite crystal, but others such as vanadate can be used). The QWP and calcite crystal set was used to convert the laser beams from a linearly polarized state to circularly polarized light, which when injected into a calcite crystal, will spatially separate the circularly polarized light into the two linear polarized components. The spatial separation of the two linearly polarized components is determined by the length of the crystal. A cond set of QWP and calcite then further separated the two beams into four. Additional sets of QWP and calcite can be used to further split the beams into multiple orders of two. The spatially separated beams had alternating linearly polarization states; a half-wave plate (HWP) array was then made to rotate the alternating states of

Yu, Anthony W.↗