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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 325 records · Page 18
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Controllable skyrmion chirality in ferroelectrics

Chirality, an intrinsic handedness, is one of the most intriguing fundamental phenomena in nature. Materials composed of chiral molecules find broad applications in areas ranging from nonlinear optics and spintronics to biology and pharmaceuticals. However, chirality is usually an invariable inherent property of a given material that cannot be easily changed at will. Here, we demonstrate that ferroelectric nanodots support skyrmions the chirality of which can be controlled and switched. We devise protocols for realizing control and efficient manipulations of the different types of skyrmions. Our findings open the route for controlled chirality with potential applications in ferroelectric-based information technologies.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2023

Performance characterization of freeform finished surfaces of potassium dihydrogen phosphate using fluid jet polishing with a nonaqueous slurry

Abstract Potassium dihydrogen phosphate (KDP) and its deuterated analog (DKDP) are unique nonlinear optical materials for high power laser systems. They are used widely for frequency conversion and polarization control by virtue of the ability to grow optical-quality crystals at apertures suitable for fusion-class laser systems. Existing methods for freeform figuring of KDP/DKDP optics do not produce surfaces with sufficient laser-induced–damage thresholds (LIDT’s) for operation in the ultraviolet portion of high-peak-power laser systems. In this work, we investigate fluid jet polishing (FJP) using a nonaqueous slurry as a sub-aperture finishing method for producing freeform KDP surfaces. This method was used to selectively polish surface areas to different depths on the same substrate with removals ranging from 0.16 μm to 5.13 μm. The finished surfaces demonstrated a slight increase in roughness as the removal depth increased along with a small number of fracture pits. Laser damage testing with 351 nm, 1 ns pulses demonstrated excellent surface damage thresholds, with the highest values in areas devoid of fracture pits. This work demonstrates, for the first time, a method that enables fabrication of a waveplate that provides tailored polarization randomization that can be scaled to meter-sized optics. Furthermore, this method is based on FJP technology that incorporates a nonaqueous slurry specially designed for use with KDP. This novel nonaqueous FJP process can be also used for figuring other types of materials that exhibit similar challenging inherent properties such as softness, brittleness, water-solubility, and temperature sensitivity.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Gradient-based optimization of complex nanoparticle heterostructures enabled by deep learning on heterogeneous graphs

Applications of deep learning (DL) to design nanomaterials are hampered by a lack of suitable data representations and training data. Here, in this study, we report efforts to overcome these limitations and leverage DL to optimize the nonlinear optical properties of core–shell upconverting nanoparticles (UCNPs). UCNPs, which have applications in fields such as biosensing, super-resolution microscopy and three-dimensional printing, can emit visible and ultraviolet light from near-infrared excitations. We report a large-scale dataset of UCNP emission spectra based on accurate but expensive kinetic Monte Carlo simulations (N > 6,000) and use these data to train a heterogeneous graph neural network using a physically motivated representation of UCNP nanostructure. Applying gradient-based optimization on the trained graph neural network, we identify structures with 6.5× higher predicted emission under 800-nm illumination than any UCNP in our training set. Our work reveals design principles for UCNP heterostructures and presents a roadmap for DL-based inverse design of nanomaterials.

Sivonxay, Eric [Lawrence Berkeley National Laborat↗
DOE OSTI2022

Light–ferroelectric interaction in two-dimensional lead iodide perovskites

The unique physical properties of two-dimensional (2D) metal halide perovskites (MHPs) such as nonlinear optics, anisotropic charge transport, and ferroelectricity have made these materials promising candidates for multifunctional applications. Recently, fluorine derivatives such as 4,4-difluoropiperidinium lead iodide perovskite or (4,4-DFPD, C 5 H 10 F 2 N) 2 PbI 4 have shown strong ferroelectricity as compared to other 2D MHPs. Although it was previously addressed that the ferroelectricity in MHPs can be affected by illumination, the underlying physical mechanisms of light–ferroelectricity interaction in 2D MHPs are still lacking. Here, we explore the electromechanical responses in 4,4-(DFPD) 2 PbI 4 thin films using advanced scanning probe microscopy techniques revealing ferroelectric domain structures. In this work, hysteretic ferroelectric loops measured by contact-Kelvin probe force microscopy are dependent on domain structures under dark conditions, while ferroelectricity weakens under illumination. The X-ray diffraction patterns exhibit significant changes in preferential orientation of individual lattice planes under illumination. Particularly, the reduced intensity of the (1 1 1) lattice plane under illumination leads to transitioning from a ferroelectric to a paraelectric phase. The instability of positive ions, especially molecular organic cations, is observed under illumination by time-of-flight secondary ion mass spectrometry. The combination of crystallographic orientation and chemical changes under illumination clearly contributes to the origin of light–ferroelectricity interaction in 2D (4,4-DFPD, C 5 H 10 F 2 N) 2 PbI 4 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Advances in the photon avalanche luminescence of inorganic lanthanide-doped nanomaterials

Photon avalanche (PA)—where the absorption of a single photon initiates a ‘chain reaction’ of additional absorption and energy transfer events within a material—is a highly nonlinear optical process that results in upconverted light emission with an exceptionally steep dependence on the illumination intensity. Over 40 years following the first demonstration of photon avalanche emission in lanthanide-doped bulk crystals, PA emission has been achieved in nanometer-scale colloidal particles. The scaling of PA to nanomaterials has resulted in significant and rapid advances, such as luminescence imaging beyond the diffraction limit of light, optical thermometry and force sensing with (sub)micron spatial resolution, and all-optical data storage and processing. In this review, we discuss the fundamental principles underpinning PA and survey the studies leading to the development of nanoscale PA. Finally, we offer a perspective on how this knowledge can be used for the development of next-generation PA nanomaterials optimized for a broad range of applications, including mid-IR imaging, luminescence thermometry, (bio)sensing, optical data processing and nanophotonics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Incorporation of erbium ions into thin-film lithium niobate integrated photonics

As an active material with favorable linear and nonlinear optical properties, thin-film lithium niobate has demonstrated its potential in integrated photonics. Integration with rare-earth ions, which are promising candidates for quantum memories and transducers, will enrich the system with new applications in quantum information processing. In this work, we investigate the optical properties at 1.5 μm wavelengths of rare-earth ions (Er 3+ ) implanted in thin-film lithium niobate waveguides and micro-ring resonators. Optical quality factors near a million after post-annealing show that ion implantation damage can be repaired. The transition linewidth and fluorescence lifetime of erbium ions are characterized. The ion-cavity coupling is observed through a Purcell enhanced fluorescence from which a Purcell factor of 3.8 ± 0.5, compared with waveguide lifetime, is extracted. This platform is compatible with top-down lithography processes and leads to a scalable path for controlling spin-photon interfaces in photonic circuits.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Poling thin-film x-cut lithium niobate for quasi-phase matching with sub-micrometer periodicity

Quasi-phase-matched grating structures in lithium niobate waveguides with sub-micrometer periodicities will benefit the development of short-wavelength nonlinear optical devices. Here, we report on the reproducible formation of periodically poled domains in x-cut single-crystalline thin-film lithium niobate with periodicities as short as 600 nm. Shaped single-voltage poling pulses were applied to electrode structures that were fabricated by a combination of electron-beam and direct-writing laser lithography. Evidence of successful poling with good quality was obtained through second-harmonic microscopy and piezoresponse force microscopy imaging. For the sub-micrometer period structures, we observed patterns with a double periodicity formed by domain interactions and features with sizes <200 nm.

Zhao, Jie (ORCID:0000000306230125)↗
DOE OSTI2021

Generating optical supercontinuum and frequency comb in tenuous plasmas

There are several mechanisms by which the frequency spectrum of a laser broadens when it propagates at near-relativistic intensity in a tenuous plasma. Focusing on one-dimensional effects, we identify two strong optical nonlinearities, namely, four-wave mixing (FWM) and forward Raman scattering (FRS), for creating octave-wide spectra. FWM dominates the interaction when the laser pulse is short and intense, and its combination with phase modulation produces a symmetrically broadened supercontinuum. FRS dominates when the laser pulse is long and relatively weak, and it broadens the laser spectrum mainly toward lower frequencies and produces a frequency comb. The frequency chirping combined with group velocity dispersion compresses the laser pulse, causing higher peak intensity.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Two-dimensional electronic–vibrational spectroscopy: Exploring the interplay of electrons and nuclei in excited state molecular dynamics

Two-dimensional electronic-vibrational spectroscopy (2DEVS) is an emerging spectroscopic technique which exploits two different frequency ranges for the excitation (visible) and detection (infrared) axes of a 2D spectrum. In contrast to degenerate 2D techniques, such as 2D electronic or 2D infrared spectroscopy, the spectral features of a 2DEV spectrum report cross correlations between fluctuating electronic and vibrational energy gaps rather than autocorrelations as in the degenerate spectroscopies. The center line slope of the spectral features reports on this cross correlation function directly and can reveal specific electronic-vibrational couplings and rapid changes in the electronic structure, for example. The involvement of the two types of transition moments, visible and infrared, makes 2DEVS very sensitive to electronic and vibronic mixing. 2DEV spectra also feature improved spectral resolution, making the method valuable for unraveling the highly congested spectra of molecular complexes. The unique features of 2DEVS are illustrated in this paper with specific examples and their origin described at an intuitive level with references to formal derivations provided. Although early in its development and far from fully explored, 2DEVS has already proven to be a valuable addition to the tool box of ultrafast nonlinear optical spectroscopy and is of promising potential in future efforts to explore the intricate connection between electronic and vibrational nuclear degrees of freedom in energy and charge transport applications.

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

Broadband 2DES detection of vibrational coherence in the S x state of canthaxanthin

The nonadiabatic mechanism that mediates nonradiative decay of the bright S 2 state to the dark S 1 state of carotenoids involves population of a bridging intermediate state, S x , in several examples. The nature of S x remains to be determined definitively, but it has been recently suggested that S x corresponds to conformationally distorted molecules evolving along out-of-plane coordinates of the isoprenoid backbone near a low barrier between planar and distorted conformations on the S 2 potential surface. Here, the electronic and vibrational dynamics accompanying the formation of S x in toluene solutions of the ketocarotenoid canthaxanthin (CAN) are characterized with broadband two-dimensional electronic spectroscopy (2DES) with 7.8 fs excitation pulses and detection of the linear polarization components of the third-order nonlinear optical signal. A stimulated-emission cross peak in the 2DES spectrum accompanies the formation of S x in <20 fs following excitation of the main absorption band. S x is prepared instantaneously, however, with excitation of hot-band transitions associated with distorted conformations of CAN’s isoprenoid backbone in the low frequency onset of the main absorption band. Vibrational coherence oscillation maps and modulated anisotropy transients show that S x undergoes displacements from the Franck–Condon S 2 state along out-of-plane coordinates as it passes to the S 1 state. The results are consistent with the conclusion that CAN’s carbonyl-substituted β-ionone rings impart an intramolecular charge-transfer character that frictionally slows the passage from S x to S 1 compared to carotenoids lacking carbonyl substitution. Despite the longer lifetime, the S 1 state of CAN is formed with retention of vibrational coherence after passing through a conical intersection seam with the S x state.

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

The polarized-signal density matrix: A practical way to recover molecular frame information from isotropic samples

We present a novel approach to model ultrafast time-dependent nonlinear optical polarization sensitive signals emitted from randomly oriented molecules. By projecting the laboratory-frame analyzer polarization axis into the molecular-frame and linking that axis with the density matrix through a tensor product, we demonstrate an approach to find a specific molecular orientation that yields a good approximation to simulated four-wave mixing signals produced by the same model but with averaging over molecular orientation.

Thurston, Richard L↗
DOE OSTI2022

Shifts in valence states in bimetallic MXenes revealed by electron energy-loss spectroscopy (EELS)

MXenes are an emergent class of two-dimensional materials with a very wide spectrum of promising applications. The synthesis of multiple MXenes, specifically solid-solution MXenes, allows fine tuning of their properties, expands their range of applications, and leads to enhanced performance. The functionality of solid-solution MXenes is closely related to the valence state of their constituents: transition metals, oxygen, carbon, and nitrogen. However, the impact of changes in the oxidation state of elements in MXenes is not well understood. In this work, three interrelated solid-solution MXene systems (Ti$_{2–y}$Nb$_y$CT$_x$, Nb$_{2–y}$V$_y$CT$_x$, and Ti$_{2–y}$V$_y$CT$_x$) were investigated with scanning transmission electron microscopy and electron energy-loss spectroscopy to determine the localized valence states of metals at the nanoscale. The analysis demonstrates changes in the electronic configuration of V upon modification of the overall composition and within individual MXene flakes. These shifts of oxidation state can explain the nonlinear optical and electronic features of solid-solution MXenes. Vanadium appears to be particularly sensitive to modification of the valence state, while titanium maintains the same oxidation state in Ti–Nb and Ti–V MXenes, regardless of stoichiometry. Here, the study also explains Nb's influential role in the previously observed electronic properties in the Nb–V and Nb–Ti systems.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Driven-dissipative phase transition in a Kerr oscillator: From semiclassical PT symmetry to quantum fluctuations

We study a minimal model that has a driven-dissipative quantum phase transition, namely a Kerr non-linear oscillator subject to driving and dissipation. Using mean-field theory, exact diagonalization, and the Keldysh formalism, we analyze the critical phenomena in this system, showing which aspects can be captured by each approach and how the approaches complement each other. Then critical scaling and finite-size scaling are calculated analytically using the quantum Langevin equation. Furthermore, the physics contained in this simple model is surprisingly rich: it includes a continuous phase transition, Z 2 symmetry breaking, PT symmetry, state squeezing, and critical fluctuations. Due to its simplicity and solvability, this model can serve as a paradigm for exploration of open quantum many-body physics.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Improved Heralded Single-Photon Source with a Photon-Number-Resolving Superconducting Nanowire Detector

Deterministic generation of single photons is essential for many quantum information technologies. A bulk optical nonlinearity emitting a photon pair, where the measurement of one of the photons heralds the presence of the other, is commonly used with the caveat that the single-photon emission rate is constrained due to a trade-off between multiphoton events and pair emission rate. Using an efficient and low noise photon-number-resolving superconducting nanowire detector we herald, in real time, a single photon at telecommunication wavelength. We perform a second-order photon correlation g 2 ( 0 ) measurement of the signal mode conditioned on the measured photon number of the idler mode for various pump powers and demonstrate an improvement of a heralded single-photon source. We develop an analytical model using a phase-space formalism that encompasses all multiphoton effects and relevant imperfections, such as loss and multiple Schmidt modes. We perform a maximum-likelihood fit to test the agreement of the model to the data and extract the best-fit mean photon number μ of the pair source for each pump power. A maximum reduction of 0.118 ± 0.012 in the photon g 2 ( 0 ) correlation function at μ = 0.327 ± 0.007 is obtained, indicating a strong suppression of multiphoton emissions. For a fixed g 2 ( 0 ) = 7 × 10 − 3 , we increase the single pair generation probability by 25%. Our experiment, built using fiber-coupled and off-the-shelf components, delineates a path to engineering ideal sources of single photons.

Davis, Samantha I.↗
DOE OSTI2021

Harmonic generation predominantly from a single spin channel in a half metal

Harmonic generation in atoms and molecules has reshaped our understanding of ultrafast phenomena beyond the traditional nonlinear optics and has launched attosecond physics. Harmonics from solids represent a new frontier, where both majority and minority spin channels contribute to harmonics. This is true even in a ferromagnet whose electronic states are equally available to optical excitation. In this work, we demonstrate that harmonics can be generated {mostly} from a single spin channel in half metallic chromium dioxide. An energy gap in the minority channel greatly reduces the harmonic generation, so harmonics predominantly emit from the majority channel, with a small contribution from the minority channel. However, this is only possible when the incident photon energy is well below the energy gap in the minority channel, so all the transitions in the minority channel are virtual. The onset of the photon energy is determined by the transition energy between the dipole-allowed transition between the O-$2p$ and Cr-$3d$ states. Harmonics mainly from a single spin channel can be detected, regardless of laser field strength, as far as the photon energy is below the minority band energy gap. This prediction should be tested experimentally

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Flexosensitive polarization vortices in thin ferroelectric films

In this work, we present a theoretical study on the influence of the flexoelectric coupling on the spatial distribution and temperature behavior of the spontaneous polarization for several types of stable domain structure in thin ferroelectric films, such as stripe domains and vortices. Finite-element modeling (FEM) for BaTiO 3 films and analytical calculations within the Landau-Ginzburg-Devonshire approach reveals that an out-of-plane polarization component can be very sensitive to the flexoelectric coupling for periodic quasi-2D stripe domains and 3D vortex-antivortex structures. However, the influence is rather different for these structures. The flexoelectric coupling increases significantly the amplitude of a small out-of-plane polarization component in the stripe domains, and the “up” or “down” direction of the component is defined by the sign of the flexoelectric coefficients. Concerning the vortex-antivortex pairs, their antivortices with in-plane antiсirculation have smooth wide dipolar cores through the entire film, whose shape and other features are almost insensitive to the coupling. The vortices with in-plane vorticity have spikelike cores with an out-of-plane quadrupolar moment induced by the flexoelectric coupling. The cores are located near the film–dead-layer interfaces. FEM results corroborated by analytical calculations prove that a change of the flexoelectric coefficient sign leads to a reorientation of the core axial polarization, making the flexosensitive 3D vortices similar to the recently introduced “flexons” in cylindrical nanoparticles. The relatively wide temperature range (from 200 to 400 K) of the flexosensitive vortices' existence gives us confidence that they can be observed experimentally in thin ferroelectric films by scanning-probe and nonlinear optical microscopy methods.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Magnetic bulk photovoltaic effect: Strong and weak field

Shift current and ballistic current have been proposed to explain the bulk photovoltaic effect (BPVE), and there have been experiments designed to separate the two mechanisms. These experiments are based on the assumption that under magnetic field, ballistic current can have a Hall effect while the shift current cannot, which is from some energy-scale arguments and has never been proven. A recent work [D. Hornung and R. von Baltz, Phys. Rev. B 103, 195203 (2021)] using quantum transport formalism achieves a conclusion that shift current indeed has a Hall current, seemingly contradicting the previous assumption and making the situation more confusing. Moreover, the behavior of BPVE under strong magnetic field is still unexplored. In this Letter, using a minimal two-dimensional tight-binding model, we carry out a systematic numerical study of the BPVE under weak and strong magnetic field by treating the field in a nonperturbative way. Further, our model clearly shows the appearance of the magnetically induced ballistic current along the transverse direction, which agrees with the previous predictions, and interestingly a sizable longitudinal response of the shift current is also observed, a phenomenon that is not captured by any existing theories where the magnetic field is treated perturbatively. More surprisingly, drastically different shift current is found in the strong-field regime, and the evolution from weak to strong field resembles a phase transition. We hope that our work could resolve the debate over the behavior of BPVE under magnetic field, and the strong-field behavior of shift current is expected to inspire more studies on the relation between nonlinear optics and quantum geometry.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗