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DOE OSTI2024

Mechanochromic Palettes of Cholesteric Liquid Crystal Elastomers for Visual Signaling

Mechanochromic photonic materials present promising prospects for enhancing diverse facets of human life. Cholesteric liquid crystal elastomers (CLCEs) present immediate mechanochromic properties, allowing their utility in various fields, including camouflages, textiles, and anticounterfeiting. Nonetheless, it is essential to provide differentiated color information corresponding to diverse types and degrees of deformation for practical use in real life. Herein, we investigate the mechanochromic responses of CLCEs using their optical rotation under compression and uniaxial stretching. The CLCEs exhibit the same reflection colors indistinguishable for compression and uniaxial stretching due to their contracted pitches. In contrast, the linearly polarized light passing through deformed CLCEs can be modulated by optical rotation, resulting in distinct transmission colors that can be discerned through mechanical deformations. We demonstrate a visual signaling system with color information derived from optical rotation. By comprehending and manipulating the mechanoresponsive behavior of CLCEs, we can advance these materials into innovative solutions with enhanced functionality and performance, thereby broadening their applications for human life enhancement.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Novel Technology of Non-Contact Real-Time Radiation Damage Sensor for High Power Targets

High-power proton beams planned for forthcoming long-baseline neutrino experiments will subject solid targets to unprecedented radiation damage, threatening reliability and increasing costs. To address this challenge, we are building a real-time, non-contact sensor that tracks damage by measuring broadband laser reflectivity changes from the target surface. A low-power super-continuum Class 3B laser illuminates the sample inside a vacuum test chamber while a high-resolution fiber-coupled spectrometer captures S- and P-polarized light; spectral shifts reveal defect-driven variations in optical constants. My internship goal is to design, build, and commission this prototype by implementing a laser-safety interlock and light shield, integrating remote-operation cameras, and fabricating modular 3-D-printed mounts that enable tool-free swaps without disturbing alignment. The laser, spectrometer, and vacuum chamber have been delivered; interlock hardware, cameras, and mounts are in final assembly, and leak testing of the chamber is underway. Upcoming work will focus on initial calibration of the sensor and executing first beam-irradiation studies.

Pumarino, Rafael↗

DOE OSTI2023

Vaterite Optical Petrography in Lake Sturgeon Otoliths

Vaterite occurring in fish otoliths exhibits plumose and spherulitic habits, the latter being like those grown from aqueous solutions. Vaterite spherulites are known to have sheaf-like texture and can be up to 100 μm in size. In thin section, the spherulites typically show uniaxial positive interference figures between cross-polarizers using a polarizing light microscope but without conoscopic or Bertrand lenses because the spherulites mimic the effect of these lenses. Plumose vaterite can show both uniaxial (+) and biaxial (+) interference figures with a small 2V, which suggests that crystal structural models for vaterite should have the plane of the carbonate group parallel to the optic axis or acute bisectrix. Finally, vaterite spherulites grown from aqueous solution exhibit similar structure and growth habits.

58 GEOSCIENCES↗

DOE OSTI2025

Reexamining Circular Dichroism in Photoemission From a Topological Insulator

The orbital angular momentum (OAM) of electron states is an essential ingredient for topological and quantum geometric quantities in solids. For example, Dirac surface states with helical spin- and orbital-angular momenta are a hallmark of a 3D topological insulator. Angle-resolved photoemission spectroscopy (ARPES) with variable circular light polarization, known as circular dichroism (CD), has been assumed to be a direct probe of OAM and, by proxy, of the Berry curvature of electronic bands in energy- and momentum-space. Indeed, topological surface states have been shown to exhibit angle-dependent CD (CDAD), and more broadly, CD is often interpreted as evidence of spin-orbit coupling. Meanwhile, it is well-established that CD originates from the photoemission matrix elements, which can have extrinsic contributions related to the experimental geometry and the inherently broken inversion symmetry at the sample surface. Therefore, it is important to broadly examine CD-ARPES to determine the scenarios in which it provides a robust probe of intrinsic material physics. We performed CD-ARPES on the canonical topological insulator $\mathrm{Bi}_2\mathrm{Se}_3$ over a wide range of incident photon energies. Not only do we observe angle-dependent CD in the surface states, as expected, but we also find CD of a similar magnitude in virtually all bulk bands. Since OAM is forbidden by inversion symmetry in the bulk, we conclude this originates from symmetry-breaking in the photoemission process. Comparison with theoretical calculations supports this view and suggests that $\textit{hidden}$ OAM - localized to atomic sites within each unit cell - contributes significantly. Additional effects, including inter-atomic interference and final-state resonances, are responsible for the rapid variation of the CDAD signal with photon energy.

FOS: Physical sciences↗

DOE OSTI2023

Probing Majorana wavefunctions in Kitaev honeycomb spin liquids with second-order two-dimensional spectroscopy

Two-dimensional coherent terahertz spectroscopy (2DCS) emerges as a valuable tool to probe the nature, couplings, and lifetimes of excitations in quantum materials. It thus promises to identify unique signatures of spin liquid states in quantum magnets by directly probing properties of their exotic fractionalized excitations. Here, we calculate the second-order 2DCS of the Kitaev honeycomb model and demonstrate that distinct spin liquid fingerprints appear already in this lowest-order nonlinear response $\chi^{(2)}_{yzx}(\omega_1, \omega_2)$ when using crossed light polarizations. We further relate the off-diagonal 2DCS peaks to the localized nature of the matter Majorana excitations trapped by $\mathbb{Z}_2$ flux excitations and show that 2DCS thus directly probes the inverse participation ratio of Majorana wavefunctions. By providing experimentally observable features of spin liquid states in the 2D spectrum, our work can guide future 2DCS experiments on Kitaev magnets.

Qiang, Yihua↗

DOE OSTI2022

System and method for determining absolute carrier-envelope phase of ultrashort laser pulses

A system for determining an absolute carrier-envelope phase (CEP) of ultrashort laser pulses includes a laser system for generating a laser beam including ultrashort optical pulses of a duration of less than 10 fs, an ultrabroadband quarter-wave plate configured to polarize the laser beam, and a gas jet emitting a continuous jet stream into the laser beam. The system includes focusing optics to adjust a focal spot of the laser beam to the gas jet, and a detector arrangement including a beam block and a microchannel plate (MCP) imaging detector, wherein the laser beam is directed to the detector arrangement. The method involves using angular streaking to determine the absolute CEP of both elliptically and linearly polarized light.

Li, Wen↗

DOE OSTI2024

Field-induced spin polarization in the lightly Cr-substituted layered antiferromagnet NiP S 3

Tuning magnetic properties in layered magnets is an important route to realize novel phenomenon related to two-dimensional (2D) magnetism. Recently, tuning antiferromagnetic (AFM) properties through substitution and intercalation techniques has been widely studied in MPX 3 compounds. Interesting phenomena, such as diverse AFM structures and even the signatures of ferrimagnetism, have been reported. However, long-range ferromagnetic (FM) ordering has remained elusive. Here, in this work, we explored the magnetic properties of the Cr-substituted NiP S 3 . We found that Cr substitution is extremely efficient in controlling spin orientation in NiP S 3 . Our study reveals a field-induced spin polarization in lightly (9%) Cr-substituted NiP S 3 , which is likely attributed to the attenuation of AFM interactions and magnetic anisotropy due to Cr doping. Our work provides a possible strategy to achieve FM phase in AFM MPX 3 , which could be useful for investigating 2D magnetism as well as potential device applications.

2-dimensional systems↗

DOE OSTI2020

Study of light nuclei by polarization observables in electron scattering

Electron-induced proton, neutron and deuteron knock-out remains the most versatile probe of the electro-magnetic properties and spin structure of light nuclei. The advent of highly polarized beams and targets and improvements in recoil polarization methods, as well as analysis and simulation techniques, have enabled us to study the static and dynamical properties of few-body systems with unprecedented precision. Recent experiments at Jefferson Lab and MAMI are presented and put into perspective of state-of-the art Faddeev calculations, with focus on the ^\mathbf{3}\mathbf{He} 3 𝐇 𝐞 nucleus.

Sirca, Simon↗

DOE OSTI2023

Thermodynamics of Light-Induced Nanoscale Polar Structures in Ferroelectric Superlattices

Here we study the thermodynamics of nanoscale polar structures in PbTiO 3 /SrTiO 3 ferroelectric superlattices induced by above-bandgap optical excitation using a phase-field model explicitly considering both structural and electronic processes. We demonstrate that the light-excited carriers provide the charge compensation of polarization bound charges and the lattice thermal energy, both of which are key to the thermodynamic stabilization of a previously observed supercrystal, a three dimensionally periodic nanostructure, within a window of substrate strains, while different mechanical and electrical boundary conditions can stabilize a number of other nanoscale polar structures by balancing the competing short-range exchange interactions responsible for the domain wall energy and longrange electrostatic and elastic interactions. The insights into the light-induced formation and richness of nanoscale structures from this work offer theoretical guidance for exploring and manipulating the thermodynamic stability of nanoscale polar structures employing a combination of thermal, mechanical, and electrical stimuli as well as light.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Light-Driven Ultrafast Polarization Manipulation in a Relaxor Ferroelectric

Relaxor ferroelectrics have been intensely studied for decades based on their unique electromechanical responses which arise from local structural heterogeneity involving polar nanoregions or domains. Here, we report first studies of the ultrafast dynamics and reconfigurability of the polarization in freestanding films of the prototypical relaxor 0.68PbMg 1/3 Nb 2/3 O 3 -0.32PbTiO 3 (PMN-0.32PT) by probing its atomic-scale response via femtosecond-resolution, electron-scattering approaches. By combining these structural measurements with dynamic phase-field simulations, we show that femtosecond light pulses drive a change in both the magnitude and direction of the polarization vector within polar nanodomains on few-picosecond time scales. This study defines new opportunities for dynamic reconfigurable control of the polarization in nanoscale relaxor ferroelectrics.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2021

Chiral-induced spin selectivity enables a room-temperature spin light-emitting diode

In traditional optoelectronic approaches, control over spin, charge, and light requires the use of both electrical and magnetic fields. In a spin-polarized light-emitting diode (spin-LED), charges are injected, and circularly polarized light is emitted from spin-polarized carrier pairs. Typically, the injection of carriers occurs with the application of an electric field, whereas spin polarization can be achieved using an applied magnetic field or polarized ferromagnetic contacts. We used chiral-induced spin selectivity (CISS) to produce spin-polarized carriers and demonstrate a spin-LED that operates at room temperature without magnetic fields or ferromagnetic contacts. The CISS layer consists of oriented, self-assembled small chiral molecules within a layered organic-inorganic metal-halide hybrid semiconductor framework. The spin-LED achieves ±2.6% circularly polarized electroluminescence at room temperature.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2025

Precision gyroscope from the helicity of light

We describe a gyroscope that measures rotation based on the effects of the rotation on the polarization of light. Rotation induces a differential phase shift in the propagation of left- and right-circularly polarized light and this phase shift can be measured in suitably designed interferometric setups. The signal in this setup is independent of the frequency of light, unlike various sources of noise such as vibrations, which cause phase shifts that depend on the frequency. Such vibrations are the practical limit on the sensitivity of conventional Sagnac-style optical interferometers that are typically used as gyroscopes. In the proposed setup, one can potentially mitigate this source of noise by simultaneously using two (or more) sources of light that have different frequencies. The signal in this setup scales with the total storage time of the light. Due to its frequency independence, it is thus most optimal to measure the signal using superconducting radio-frequency systems where the high finesse of the available cavities enables considerably longer storage times than is possible in an optical setup.

47 OTHER INSTRUMENTATION↗

DOE OSTI2021

Optical current monitor

An optical current monitor for detecting a current traveling through conductive material. The optical current monitor comprises a light source for emitting light at an output level; a lens configured to receive the light; Faraday material positioned near the conductive material and configured to receive light that has passed through the lens, thereby producing rotated light; a polarizer configured to polarize the rotated light; a photodetector configured to receive the rotated light and output a signal as a function of the rotated light; and a feedback system. The feedback system is configured to receive the signal from the photodetector and modify the output level of the light source based on the signal so that the signal remains at a reference level when the current is not traveling through the conductive material.

Laughlin, Daric Gray↗

DOE OSTI2025

Polarization-resolved core exciton dynamics in LiF using attosecond transient absorption spectroscopy

The ability to control absorption by modifying the polarization of light presents an exciting opportunity to experimentally determine the orbital alignment of absorption features. Here, attosecond extreme ultraviolet (XUV) transient absorption spectroscopy is used to investigate the polarization dependence of core exciton dynamics in LiF thin films at the Li + K edge. XUV pulses excite electrons from the Li 1s core level into the conduction band, allowing for the formation of a p-orbital-like core exciton, aligned along the XUV light polarization axis. A sub-5 fs near-infrared (NIR) probe pulse then arrives at variable time delays, perturbing the XUV-excited states and allowing the coherence decay of the core exciton to be mapped. The coherence lifetimes are found to be ≈ 2.4 ± 0.4 fs, which is attributed to a phonon-mediated dephasing mechanism as in previous core exciton studies. The differential absorption features are also shown to be sensitive to the relative polarization of the XUV and NIR fields. The parallel NIR probe induces couplings between the initial XUV-excited p-like bright exciton and s-like dark excitons. When crossed pump and probe polarizations are used, the coupling between the bright and dark states is no longer dipole-allowed, and the transient absorption signal associated with the coupling is suppressed by approximately 90%. This interpretation is supported by simulations of a few-level model system, as well as analysis of the calculated band structure. Here, the results indicate that laser polarization can serve as a powerful experimental tool for exploring the orbital alignment of core excitonic states in solid-state materials.

Attosecond laser spectroscopy↗

DOE OSTI2024

Light-induced transitions of polar state and domain morphology of photoferroelectric nanoparticles

Using the Landau-Ginzburg-Devonshire approach, we study light-induced phase transitions, evolution of polar state and domain morphology in photo-ferroelectric nanoparticles (NPs). Light exposure increases the free carrier density near the NP surface and may in turn induce phase transitions from the nonpolar paraelectric to the polar ferroelectric phase. Using the uniaxial photo-ferroelectric Sn 2 P 2 S 6 as an example, here we show that visible light exposure induces the appearance and vanishing of striped, labyrinthine or curled domains and changes in the polarization switching hysteresis loop shape from paraelectric curves to double, pinched and single loops, as well as the shifting in the position of the tricritical point. Furthermore, we demonstrate that an ensemble of non-interacting photo-ferroelectric NPs may exhibit superparaelectric-like features at the tricritical point, such as strongly frequency-dependent giant piezoelectric and dielectric responses, which can potentially be exploited for piezoelectric applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2022

Multiple-polarization-sensitive photodetector based on a perovskite metasurface

Most polarization-sensitive photodetectors detect either linearly polarized (LP) or circularly polarized (CP) light. Here, we experimentally demonstrate a multiple-polarization photodetector based on a hybrid organic–inorganic perovskite (HOIP) metasurface, which is sensitive to both LP and CP light simultaneously. The perovskite metasurface is composed of a HOIP antenna array on a single-crystal HOIP film. Owing to the antenna anisotropy, the absorption of linearly polarized light at the metasurface depends on the polarization angle; also, due to the mirror asymmetry of the antenna elements, the metasurface is also sensitive to different circular polarizations. Polarization-dependent photocurrent responses to both LP and CP light are detected. Our results highlight the potential of perovskite metasurfaces for integrated photoelectric applications.

47 OTHER INSTRUMENTATION↗

DOE OSTI2020

Femtosecond photocurrents at the FeRh/Pt interface

Femtosecond laser excitations of FeRh/Pt bilayers launch an ultrafast pulse of electric photocurrents in the Pt-layer and subsequently result in the emission of electromagnetic radiation in the THz spectral range. Analysis of the THz emission as a function of the polarization of the femtosecond laser pulse, external magnetic field, sample temperature, and sample orientation shows that the photocurrent can emerge due to vertical spin pumping and photo-induced inverse spin–orbit torque at the FeRh/Pt interface. Additionally, the vertical spin pumping from FeRh into Pt does not depend on the polarization of light and originates from ultrafast laser-induced demagnetization of the ferromagnetic phase of FeRh. The photo-induced inverse spin–orbit torque at the FeRh/Pt interface can be described in terms of a helicity-dependent effect of circularly polarized light on the magnetization of the ferromagnetic FeRh and the subsequent generation of a photocurrent.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2026

Photogalvanic Effects in Surface States of Topological Insulators under Perpendicular Magnetic Fields

We present a theoretical study of the nonlinear magneto-optical shift conductivity in the surface states of the prototypical topological insulator Bi$_2$Se$_3$ under a perpendicular quantizing magnetic field. By describing the electronic states as Landau levels and using a perturbative approach, we derive the microscopic expression for the shift conductivity $\sigma^{(2);\alpha\beta\gamma}(-\omega,\omega)$, where $\alpha,\beta,\gamma=\pm$ stand for the circular polarization of light and $\omega$ is the light frequency; the spectra are further decomposed into contributions from the interband and intraband optical transitions, for which the selection rules are identified. Considering that the system possesses $C_3$ point group of symmetry, the nonzero components of the conductivity tensor are $\sigma^{(2);-++}=[\sigma^{(2);+--}]^\ast$. Therefore, a pure circularly polarized light generates zero shift current. In the clean limit, the conductivities are nonzero only for discrete photon energies because of the discrete Landau levels and energy conservation, and they become Lorentzian lineshapes with the inclusion of damping, which relaxes the condition of energy conservation. The dependence of the spectra on the damping parameters, the magnetic fields, and the chemical potentials is investigated in detail. Our results reveal that the shift current is highly tunable by the chemical potential and the magnetic field. Furthermore, these results underscore the potential of topological insulators for tunable, strong nonlinear magneto-optical applications.

Landau level↗