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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 181 records · Page 10
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Exciton–Polaritons in CsPbBr 3 Crystals Revealed by Optical Reflectivity in High Magnetic Fields and Two-Photon Spectroscopy

Cesium lead bromide (CsPbBr3) is a representative material of the emerging class of lead halide perovskite semiconductors that possess remarkable optoelectronic properties. Its optical properties in the vicinity of the bandgap energy are greatly contributed by excitons, which form exciton polaritons due to strong light–matter interactions. Exciton–polaritons in solution-grown CsPbBr 3 crystals are examined by means of circularly polarized reflection spectroscopy measured in high magnetic fields up to 60 T. The excited 2P exciton state is measured by two-photon absorption. Comprehensive modeling and analysis provides detailed quantitative information about the exciton–polariton parameters: exciton binding energy of 32.5 meV, oscillator strength characterized by longitudinal–transverse splitting of 5.3 meV, damping of 6.7 meV, reduced exciton mass of 0.18$m$ 0 , exciton diamagnetic shift of 1.6 μeV T -2 , and exciton Landé factor $g$ x = + 2.35. It is shown that the exciton states can be described within a hydrogen-like model with an effective dielectric constant of 8.7. From the measured exciton longitudinal–transverse splitting, Kane energy of E p = 15 eV is evaluated, which is in reasonable agreement with values of 11.8–12.5 eV derived from the carrier effective masses.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Differential holography

Differential Holography technology measures the amplitude and/or phase of, e.g., an incident linearly polarized spatially coherent quasi-monochromatic optical field by optically computing the first derivative of the field and linearly mapping it to an irradiance signal detectable by an image sensor. This information recorded on the image sensor is then recovered by a simple algorithm. In some embodiments, an input field is split into two or more beams to independently compute the horizontal and vertical derivatives (using amplitude gradient filters in orthogonal orientations) for detection on one image sensor in separate regions of interest (ROIs) or on multiple image sensors. A third unfiltered beam recorded in a third ROI directly measures amplitude variations in the input field to numerically remove its contribution as noise before recovering the original wavefront using a numerical in algorithm. When combined, the measured amplitude and phase constitute a holographic recording of the incident optical field.

Ravizza, Frank↗
DOE OSTI2024

Graviton topology

Over the past three decades, it has been shown that discrete and continuous media can support topologically nontrivial waves. Recently, it was shown that the same is true of the vacuum, in particular, right (R) and left (L) circularly polarized photons are topologically nontrivial. Here, we study the topology of another class of massless particles, namely gravitons. We show that the collection of all gravitons forms a topologically trivial vector bundle over the lightcone, allowing us to construct a globally smooth basis for gravitons. The graviton bundle also has a natural geometric splitting into two topologically nontrivial subbundles, consisting of the R and L gravitons. The R and L gravitons are unitary irreducible bundle representations of the Poincaré group, and are thus elementary particles; their topology is characterized by the Chern numbers ∓4. This nontrivial topology obstructs the splitting of graviton angular momentum into spin and orbital angular momentum.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2022

Nonequilibrium spintronic transport through Kondo impurities

In this work we analyze the nonequilibrium transport through a quantum impurity (quantum dot or molecule) attached to ferromagnetic leads by using a hybrid numerical renormalization group–time-dependent density matrix renormalization group thermofield quench approach. For this, we study the bias dependence of the differential conductance through the system, which shows a finite zero-bias peak, characteristic of the Kondo resonance and reminiscent of the equilibrium local density of states. In the nonequilibrium settings, the resonance in the differential conductance is also found to decrease with increasing the lead spin polarization. The latter induces an effective exchange field that lifts the spin degeneracy of the dot level. Therefore, as we demonstrate, the Kondo resonance can be restored by counteracting the exchange field with a finite external magnetic field applied to the system. Lastly, we investigate the influence of temperature on the nonequilibrium conductance, focusing on the split Kondo resonance. Our work thus provides an accurate quantitative description of the spin-resolved transport properties relevant for quantum dots and molecules embedded in magnetic tunnel junctions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Organic-to-inorganic structural chirality transfer in a 2D hybrid perovskite and impact on Rashba-Dresselhaus spin-orbit coupling

Abstract Translation of chirality and asymmetry across structural motifs and length scales plays a fundamental role in nature, enabling unique functionalities in contexts ranging from biological systems to synthetic materials. Here, we introduce a structural chirality transfer across the organic–inorganic interface in two-dimensional hybrid perovskites using appropriate chiral organic cations. The preferred molecular configuration of the chiral spacer cations, R -(+)- or S -(−)-1-(1-naphthyl)ethylammonium and their asymmetric hydrogen-bonding interactions with lead bromide-based layers cause symmetry-breaking helical distortions in the inorganic layers, otherwise absent when employing a racemic mixture of organic spacers. First-principles modeling predicts a substantial bulk Rashba-Dresselhaus spin-splitting in the inorganic-derived conduction band with opposite spin textures between R - and S -hybrids due to the broken inversion symmetry and strong spin-orbit coupling. The ability to break symmetry using chirality transfer from one structural unit to another provides a synthetic design paradigm for emergent properties, including Rashba-Dresselhaus spin-polarization for hybrid perovskite spintronics and related applications.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Comparison of spontaneous emission in trapped-ion multiqubit gates at high magnetic fields

Penning traps have been used for performing quantum simulations and sensing with hundreds of ions and provide a promising route toward scaling up trapped ion quantum platforms because of the ability to trap and control hundreds or thousands of ions in two- and three-dimensional crystals. In both Penning traps and the more common RF Paul traps, lasers are often used to drive multi-qubit entangling operations. A leading source of decoherence in these operations is off resonant spontaneous emission. While many trapped ion quantum computers or simulators utilize clock qubits, other systems, especially those with high magnetic fields such as Penning traps, rely on Zeeman qubits, which require a more complex calculation of this decoherence. We therefore examine theoretically the impacts of spontaneous emission on quantum gates performed with trapped-ion ground state Zeeman qubits in a high magnetic field. In particular, we consider two types of gates—light-shift ($\hat{σ}^z_i$ $\hat{σ}^z_j$) gates and Mølmer-Sørensen ($\hat{σ}^x_i$ $\hat{σ}^x_j$) gates—obtained with laser beams directed approximately perpendicular to the magnetic field (the quantization axis) and compare the decoherence errors in each. Within each gate type, we also compare different operating points with regards to the detunings, polarizations, and required intensity of the laser beams used to drive the gates. Here, we show that both gates can have similar performance at their optimal operating conditions at high magnetic fields and examine the experimental feasibility of various operating points. By examining the magnetic field dependence of each gate, we demonstrate that, when the P state fine structure splitting is large compared to the Zeeman splittings, the theoretical performance of the Mølmer-Sørensen gate is significantly better than that of the light-shift gate. Additionally, for the light-shift gate, we make an approximate comparison between the fidelities that can be achieved at high fields with the fidelities of state-of-the-art two-qubit trapped ion quantum gates. We show that, with regards to spontaneous emission, the achievable fidelity of the current NIST configuration is about an order of magnitude below that of the best low-field gates, but we also discuss several alternative configurations with potential error rates that are comparable with those for state-of-the art trapped ion gates.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2025

Quantum confining excitons with an electrostatic moiré superlattice

Quantum confining excitons has been a persistent challenge in the pursuit of strong exciton interactions and quantum light generation. Unlike electrons, which can be readily controlled via electric fields, imposing strong nanoscale potentials on excitons to enable quantum confinement has proven challenging. In this study, we utilize piezoelectric force microscopy to image the domain structures of twisted hexagonal boron nitride (h – BN), revealing evidence of strong in-plane electric fields at the domain boundaries. By placing a monolayer MoSe 2 only one to two nanometers away from the twisted h – BN interface, we observe energy splitting of neutral excitons and Fermi polarons by several millielectronvolts at the moiré domain boundaries. By directly correlating local structural and optical properties, we attribute such observations to excitons confined in a nanoscale one-dimensional electrostatic potential created by the strong in-plane electric fields at the moiré domain boundaries. Intriguingly, this 1D quantum confinement results in pronounced polarization anisotropy in the excitons’ reflection and emission, persistent to temperatures as high as ~80 Kelvins. Furthermore, these findings open new avenues for exploring and controlling strongly interacting excitons for classical and quantum optoelectronics.

2-dimensional systems↗
DOE OSTI2025

Xylanolytic metabolism is regulated by coordination of transcription factors XynR and XylR in extremely thermophilic Caldicellulosiruptorales

ABSTRACT Global transcription factors (TFs) control metabolic processes in bacteria to efficiently utilize available carbon. The orderCaldicellulosiruptoraleshas drawn interest due to the ability of its members to degrade components of lignocellulosic biomass. Regulatory reconstruction ofAnaerocellum (f. Caldicellulosiruptor) besciiidentified two major global transcription factors for xylan utilization, XynR and XylR, and the corresponding putative transcription factor binding sites. Recombinant versions of XynR (LacI family) and XylR (ROK family) were subjected to fluorescence polarization (FP) and biolayer interferometry (BLI) analysis to confirm the predicted binding sites. Four XynR sites and two XylR sites were validated, accounting for 20 of 26 genes regulated by XynR and six of seven genes regulated by XylR. Bioinformatic analysis of the individual genes controlled by the two regulators showed an inter-dependent scheme for xylan conversion; the transport of xylooligosaccharides (XOS) is dependent on XylR, while enzymes responsible for hydrolysis are controlled by both regulators. For xylose catabolism by the xylose isomerase-xylulose kinase pathway, regulation is also split, with XylR controlling xylose isomerase and XynR controlling xylokinase. The XynR/XylR regulator pair withinA. besciiis conserved in all sequenced species ofCaldicellulosiruptorales, suggesting similarities in regulating linear xylan conversion. In other xylanolytic thermophiles, XylR homologs control xylan degradation, compared to just 6 out of 26 genes forA. bescii. These results show that two separate regulatory schemes (dual repression) are coordinated byA. besciito effectively regulate the hemicellulose inventory and xylan catabolism. IMPORTANCE To take full advantage of extreme thermophiles as platform metabolic engineering microorganisms, the tools for genetic manipulation must be further developed, and strategies that exploit a better understanding of metabolic regulation need to be discerned.Anaerocellum bescii, the most studied of the extremely thermophilic fermentative anaerobic bacteria that can utilize microcrystalline cellulose, can degrade microcrystalline cellulose and hemicellulose and has been metabolically engineered to convert the resulting sugars to products such as ethanol and acetone. For xylan, in particular, two major global transcription factors (TFs), XynR and XylR, play a role in sugar metabolism, although their predicted regulatory interdependence from bioinformatics analysis has not been elucidated experimentally. Here, fluorescence polarization (FP) and biolayer interferometry (BLI) were used to explore this issue to support metabolic engineering efforts aimed at improving carbohydrate processing to industrial chemicals.

Biotechnology & Applied Microbiology↗
DOE OSTI2021

All-Dielectric Meta-Optics for High-Efficiency Independent Amplitude and Phase Manipulation

Optical metasurfaces, composed of subwavelength scattering elements, demonstrate remarkable control over the transmitted amplitude, phase, and polarization of light. However, manipulating the amplitude upon transmission, without the use of surface waves, requires loss if a single metasurface is used. Herein, high-efficiency independent manipulation of the amplitude and phase of a beam is described using two lossless phase-only metasurfaces separated by a distance. With this configuration, optical components such as combined beam-forming and splitting devices are experimentally demonstrated, as well as those for forming complex-valued, 3D holograms. The compound meta-optic platform provides a promising approach for achieving high-performance holographic displays and compact optical components, while exhibiting a high overall efficiency.

42 ENGINEERING↗
DOE OSTI2021

Strong Rashba-Dresselhaus Effect in Nonchiral 2D Ruddlesden-Popper Perovskites

Chirality transfer from organic chiral molecules to lead halides is theorized as the origin of the strong Rashba-Dresselhaus effect causing large circular dichroism (CD) and circularly polarized luminescence (CPL) in metal halide perovskites (MHPs). In this report a concrete empirical evidence is provided that such strong CD and CPL can occur even in nonchiral 2D Ruddlesden-Popper perovskites (RPPs) (BA) 2 (MA) n-1 Pb n I 3n+1 (where MA = CH 3 NH 3 and BA = CH 3 (CH 2 ) 3 NH 3 ). The CD and CPL responses occurring at the excitonic transition of the MHPs are strongest (≈100 mdeg and 4.8%, respectively) when a single lead halide octahedral [PbI 6 ] 4- layer is repeatedly stacked between two nonchiral molecules BA + (n = 1). However, they are rapidly quenched as n increases. It is hypothesized that strong Rashba-Dresselhaus splitting in the 2D RPPs originates the strong CD and CPL signatures. Density functional theory calculations reveal that the large interlayer distortions in the inorganic layers at the organic/inorganic interface give rise to the strong Rashba-Dresselhaus splitting. A Rashba-Dresselhaus field of ≈600 and ≈50 mT for n = 1 and 2, respectively, is estimated by magnetic circular dichroism spectroscopy. The studies may have significant impact on designing 2D RPPs with large Rashba-Dresselhaus effects at room temperature for spintronic applications.

circular dichroism↗
DOE OSTI2024

Large exchange-driven intrinsic circular dichroism of a chiral 2D hybrid perovskite

Abstract In two-dimensional chiral metal-halide perovskites, chiral organic spacers endow structural and optical chirality to the metal-halide sublattice, enabling exquisite control of light, charge, and electron spin. The chiroptical properties of metal-halide perovskites have been measured by transmissive circular dichroism spectroscopy, which necessitates thin-film samples. Here, by developing a reflection-based approach, we characterize the intrinsic, circular polarization-dependent complex refractive index for a prototypical two-dimensional chiral lead-bromide perovskite and report large circular dichroism for single crystals. Comparison with ab initio theory reveals the large circular dichroism arises from the inorganic sublattice rather than the chiral ligand and is an excitonic phenomenon driven by electron-hole exchange interactions, which breaks the degeneracy of transitions between Rashba-Dresselhaus-split bands, resulting in a Cotton effect. Our study suggests that previous data for spin-coated films largely underestimate the optical chirality and provides quantitative insights into the intrinsic optical properties of chiral perovskites for chiroptical and spintronic applications.

25 ENERGY STORAGE↗
DOE OSTI2025

Electrical switching of a p-wave magnet

Magnetic states with zero magnetization but non-relativistic spin splitting are outstanding candidates for the next generation of spintronic devices. Their electronvolt (eV)-scale spin splitting, ultrafast spin dynamics and nearly vanishing stray fields make them particularly promising for several applications. A variety of such magnetic states with non-trivial spin textures have been identified recently, including even-parity d-wave, g-wave or i-wave altermagnets and odd-parity p-wave magnets. Achieving voltage-based control of the non-uniform spin polarization of these magnetic states is of great interest for realizing energy-efficient and compact devices for information storage and processing. Spin-spiral type II multiferroics are optimal candidates for such voltage-based control, as they exhibit an inversion-symmetry-breaking magnetic order that directly induces ferroelectric polarization, allowing for symmetry-protected cross-control between spin chirality and polar order. Here we combine photocurrent measurements, first-principles calculations and group-theory analysis to provide direct evidence that the spin polarization of the spin-spiral type II multiferroic NiI 2 exhibits odd-parity character connected to the spiral chirality. The symmetry-protected coupling between chirality and polar order enables electrical control of a primarily non-relativistic spin polarization. Our findings represent an observation of p-wave magnetism in a spin-spiral type II multiferroic, which may lead to the development of voltage-based switching of non-relativistic spin polarization in compensated magnets.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2025

Orbital-spin locking and its optical signatures in altermagnets

Altermagnets, magnetic materials with zero magnetization and spin-split band structure, have gained tremendous attention recently for their rich physics and potential applications. Here, we report on a microscopic tight-binding model that unveils a unique coupling between orbitals and spins in d-wave altermagnets, which gives rise to momentum-dependent and spin-selective optical absorption. This coupling promotes the controlled optical excitation of up or down spins depending on the polarization direction of linearly polarized light. Such an effect originates from the coupling of orbitals to the sublattice degree of freedom through the crystal field, which is then coupled to spins through the antiferromagnetic interaction. Our crystal field analysis, which is general to any type of altermagnet, helps understand the onset of altermagnetism from a microscopic point of view, and we use our results to propose clear magneto-optical signatures of our predictions. Our findings shine light on the interplay between orbitals and spins in altermagnets, thus paving the way towards novel orbitronic and optospintronic devices.

Vila, Marc↗
DOE OSTI2024

Pressure–Temperature–Magnetic Field Phase Diagram of Multiferroic (NH 4 ) 2 FeCl 5 ·H 2 O

We combined synchrotron-based infrared absorbance and Raman scattering spectroscopies with diamond anvil cell techniques and a symmetry analysis to explore the properties of multiferroic (NH 4 ) 2 FeCl 5 ·H 2 O under extreme pressure–temperature conditions. Compression-induced splitting of the Fe–Cl stretching, Cl–Fe–Cl and Cl–Fe–O bending, and NH 4 + librational modes defines two structural phase transitions, and a group–subgroup analysis reveals space group sequences that vary depending upon proximity to the unexpectedly wide order–disorder transition. Here, we bring these findings together with prior high-field work to develop the pressure–temperature–magnetic field phase diagram uncovering competing polar, chiral, and magnetic phases in this system.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Total Angular Momentum Dichroism of the Terahertz Vortex Beams at the Antiferromagnetic Resonances

Here, terahertz vortex beams with different superposition of the orbital angular momentum $\textit{l}$ = ± 1, ±2, ±3, and ±4 and spin angular momentum σ = ±1 were used to study antiferromagnetic (AFM) resonances in TbFe 3 (BO 3 ) 4 and Ni 3 TeO 6 single crystals. In both materials we observed a strong vortex beam dichroism for the AFM resonances that are split in external magnetic field. The magnitude of the vortex dichroism is comparable to that for conventional circular dichroism due to σ. The selection rules at the AFM resonances are governed by the total angular momentum of the vortex beam: $\textit{j}$ = σ + $\textit{l}$. In particular, for $\textit{l}$ = ±2, ±3, and ±4 the sign of $\textit{l}$ is shown to dominate over that for conventional circular polarization σ.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Switchable planar chirality and spin texture in highly ordered ferroelectric hybrid perovskite domains

Chiral organic-inorganic hybrid perovskites offer a promising platform for developing non-linear chiro-optical applications and chiral-induced spin selectivity. Here, we show that achiral hybrid perovskites that have highly ordered ferroelectric domains with orthogonal polarization exhibit planar chirality, as manifested by second harmonic generation with strong circular dichroism. Interestingly, the handedness of the second harmonic generation circular dichroism response can be alternatingly switched between orthogonally polarized domains and domain walls. To correlate the origin of planar chirality in these domains, atom-resolved atomic force microscopy is used to reveal distinct arrangements of atomic rows in these ferroelectric crystals that indicate planar symmetry breaking. Remarkably, a large SHG anisotropy factor of 0.41 is measured at the domain wall. Additionally, spatially resolved two-photon photoluminescence excitation measurement provide evidence of larger Rashba spin-splitting in these chiral ferroelectric domains compared to domain-free areas. Our discoveries of domain-dependent planar chirality and spin texture hold great promise for advancement of domain-specific chiro-optical applications.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Time-resolved magneto-optical effects in the altermagnet candidate MnTe

α -MnTe is an antiferromagnetic semiconductor with above room temperature T N = 310 K, which is promising for spintronic applications. Recently, it was reported to be an altermagnet, containing bands with momentum-dependent spin splitting; time-resolved experimental probes of MnTe are, therefore, important both for understanding novel magnetic properties and potential device applications. Here, we investigate ultrafast spin dynamics in epitaxial MnTe(001)/InP(111) thin films using pump-probe magneto-optical measurements in the Kerr configuration. At room temperature, we observe an oscillation mode at 55 GHz that does not appear at zero magnetic field. Combining field and polarization dependence, we identify this mode as a magnon, likely originating from inverse stimulated Raman scattering. Magnetic field-dependent oscillations persist up to at least 335 K, which could reflect coupling to known short-range magnetic order in MnTe above T N . Additionally, we observe two optical phonons at 3.6 and 4.2 THz, which broaden and redshift with increasing temperature.

Gray, Isaiah↗
DOE OSTI2021

Chemical bonding and Born charge in 1T-HfS 2

We combine infrared absorption and Raman scattering spectroscopies to explore the properties of the heavy transition metal dichalcogenide 1T-HfS 2 . We employ the LO–TO splitting of the E u vibrational mode along with a reevaluation of mode mass, unit cell volume, and dielectric constant to reveal the Born effective charge. We find $Z$$^{*}_{B}$ = 5.3e, in excellent agreement with complementary first-principles calculations. In addition to resolving the controversy over the nature of chemical bonding in this system, we decompose Born charge into polarizability and local charge. We find α = 5.07 Å 3 and Z* = 5.2e, respectively. Polar displacement-induced charge transfer from sulfur p to hafnium d is responsible for the enhanced Born charge compared to the nominal 4+ in hafnium. 1T-HfS 2 is thus an ionic crystal with strong and dynamic covalent effects. Taken together, our work places the vibrational properties of 1T-HfS 2 on a firm foundation and opens the door to understanding the properties of tubes and sheets.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗