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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 379 records · Page 21
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Spin-optomechanical cavity interfaces by deep subwavelength phonon-photon confinement

A central goal of quantum information science is transferring qubits between space, time, and modality. Spin-based systems in solids are promising quantum memories, but high-fidelity transfer of their quantum states to telecom optical fields remains challenging. Here, we introduce a phonon-mediated interface between spins in a diamond nanobeam optomechanical crystal and telecom optical fields by a simultaneous deep-subwavelength confinement of optical and acoustic fields with mode volumes $V_{\textrm{mech}}$$/Λ^3_\textrm{p} ~ 10^{-5}$ and $V_{\textrm{opt}}$$/λ^3 ~ 10^{−3}$, respectively. This confinement boosts the spin-mechanical coupling rate of Group-IV silicon vacancy (SiV − ) centers by an order of magnitude to ~ 32 MHz while retaining high acousto-optical couplings. The optical cavity couples to the spin irrespective of the emitter’s native excited states, avoiding spectral diffusion. Using Quantum Monte Carlo simulations, we estimate heralded entanglement fidelities exceeding 0.96 between two such interfaces. We anticipate broad utility beyond diamond emitter-telecom systems to most solid-state quantum memories.

Raniwala, Hamza [Massachusetts Inst. of Technology↗
DOE OSTI2019

Quasicubic model for metal halide perovskite nanocrystals

In this work, we present an analysis of quantum confinement of carriers and excitons, and exciton fine structure, in metal halide perovskite (MHP) nanocrystals (NCs). Starting with coupled-band k · P theory, we derive a nonparabolic effective mass model for the exciton energies in MHP NCs valid for the full size range from the strong to the weak confinement limits. We illustrate the application of the model to CsPbBr 3 NCs and compare the theory against published absorption data, finding excellent agreement. We then apply the theory of electron-hole exchange, including both short- and long-range exchange interactions, to develop a model for the exciton fine structure. We develop an analytical quasicubic model for the effect of tetragonal and orthorhombic lattice distortions on the exchange-related exciton fine structure in CsPbBr 3 , as well as some hybrid organic MHPs of recent interest, including formamidinium lead bromide (FAPbBr 3 ) and methylammonium lead iodide (MAPbI3). Testing the predictions of the quasicubic model using hybrid density functional theory (DFT) calculations, we find qualitative agreement in tetragonal MHPs but significant disagreement in the orthorhombic modifications. Moreover, the quasicubic model fails to correctly describe the exciton oscillator strength and with it the long-range exchange corrections in these systems. Introducing the effect of NC shape anisotropy and possible Rashba terms into the model, we illustrate the calculation of the exciton fine structure in CsPbBr 3 NCs based on the results of the DFT calculations and examine the effect of Rashba terms and shape anisotropy on the calculated fine structure.

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

Atomistically resolved hot exciton relaxation dynamics in CdSe quantum dots: Experiment and theory

Semiconductor quantum dots (QDs) are well known to give rise to a quantum confined structure of excitons. Because of this quantum confinement, new physics of hot exciton relaxation dynamics arises. Decades of work using transient absorption (TA) spectroscopy have yielded initial simple observations, such as estimates of the cooling rate from single pump photon energy experiments. More detailed TA experiments employed variable pump photon energies to measure excitonic state-resolved transition rates. These TA measurements, usually the simplest form, have been employed to characterize QDs and their relaxation dynamics to this day. Yet, these TA measurements are fundamentally lacking in their ability to measure energy-resolved hot exciton cooling, which requires observation of the full cooling history through the real excitonic manifold. Here, we employ coherent multi-dimensional spectroscopy (CMDS) to perform an atomistically directed study of hot exciton cooling in CdSe QDs, revealing energy resolved relaxation dynamics. CMDS experiments are compared with simulations and prior TA measurements and simpler theories. Our findings reveal a hot exciton relaxation dynamics landscape. This relaxation dynamics landscape is a linear or sub-linear function of excess energy for different structures of QDs, with a strong size dependence. Our model simulations parameterized by the empirical pseudopotential model reproduces the experimental functional form and the dependence upon QD diameter and shell.

Atomistic simulations↗
DOE OSTI2022

X-ray free-electron laser based dark-field X-ray microscopy: a simulation-based study

Dark-field X-ray microscopy (DFXM) is a nondestructive full-field imaging technique providing three-dimensional mapping of microstructure and local strain fields in deeply embedded crystalline elements. This is achieved by placing an objective lens in the diffracted beam, giving a magnified projection image. So far, the method has been applied with a time resolution of milliseconds to hours. In this work, the feasibility of DFXM at the picosecond time scale using an X-ray free-electron laser source and a pump–probe scheme is considered. Thermomechanical strain-wave simulations are combined with geometrical optics and wavefront propagation optics to simulate DFXM images of phonon dynamics in a diamond single crystal. Using the specifications of the XCS instrument at the Linac Coherent Light Source as an example results in simulated DFXM images clearly showing the propagation of a strain wave.

47 OTHER INSTRUMENTATION↗
DOE OSTI2020

Phonon-induced near-field resonances in multiferroic BiFeO 3 thin films at infrared and THz wavelengths

Multiferroic BiFeO$_3$ (BFO) shows several phonon modes at infrared (IR) to THz energies, which are expected to carry information on any sample property coupled to crystal lattice vibrations. While macroscopic IR studies of BFO are often limited by single-crystal size, scattering-type scanning near-field optical microscopy (s-SNOM) allows for IR thin film spectroscopy of nanoscopic probing volumes with negligible direct substrate contribution to the optical signal. In fact, polaritons such as phonon polaritons of BFO introduce a resonant tip–sample coupling in s-SNOM, leading to both stronger signals and enhanced sensitivity to local material properties. Here in this paper, we explore the near-field response of BFO thin films at three consecutive resonances (centered around 5 THz, 13 THz, and 16 THz), by combining s-SNOM with a free-electron laser. We study the dependence of these near-field resonances on both the wavelength and tip–sample distance. Enabled by the broad spectral range of the measurement, we probe phonon modes connected to the predominant motion of either the bismuth or oxygen ions. Therefore, we propose s-SNOM at multiple near-field resonances as a versatile and very sensitive tool for the simultaneous investigation of various sample properties.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Ab initio ultrafast spin dynamics in solids

Spin relaxation and decoherence is at the heart of spintronics and spin-based quantum information science. Currently, theoretical approaches that can accurately predict spin relaxation of general solids including necessary scattering pathways and are capable of nanosecond to millisecond simulation time are urgently needed. We present a first-principles real-time density-matrix approach based on Lindblad dynamics to simulate ultrafast spin dynamics for general solid-state systems. Through the complete first-principles descriptions of pump, probe, and scattering processes including electron-phonon, electron-impurity, and electron-electron scatterings with self-consistent electronic spin-orbit couplings, our method can directly simulate the ultrafast pump-probe measurements for coupled spin and electron dynamics over nanoseconds at any temperatures and doping levels. We first apply this method to a prototypical system GaAs and obtain excellent agreement with experiments. We found that the relative contributions of different scattering mechanisms and phonon modes differ considerably between spin and carrier relaxation processes. In sharp contrast to previous work based on model Hamiltonians, we point out that the electron-electron scattering is negligible at room temperature but becomes dominant at low temperatures for spin relaxation in n-type GaAs. We further examine ultrafast dynamics in novel spin-valleytronic materials: monolayer and bilayer WSe 2 with realistic defects. We find that spin relaxation is highly sensitive to local symmetry and chemical bonds around defects. For the bilayer WSe 2 , we identify the scattering pathways in ultrafast dynamics and determine relevant dynamical properties, essential to its utilization of unique spin-valley-layer locking effects. In conclusion, our work provides a predictive computational platform for spin dynamics in solids, which has potential for designing new materials ideal for spintronics and quantum information technology.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Deep Optical Switching on Subpicosecond Timescales in an Amorphous Ge Metamaterial

Active nanostructured optical components show promise as potential building blocks for novel light-based computing and data processing architectures. However, nanoscale all-optical switches that have low activation powers and high-contrast ultrafast switching have been elusive so far. Here, pump–probe measurements performed on amorphous-Ge-based micro-resonator metasurfaces that exhibit strong resonant modes in the mid-infrared are reported. Relative change is observed in transmittance of ΔT/T ≈ 1 with picosecond (down to τ ≈ 0.5 ps) free carrier relaxation rates, obtained with very low pump fluences of 50 μJ cm –2 . In this work, these observations are attributed to efficient free carrier promotion, affecting light transmittance via high quality-factor optical resonances, followed by an increased electron–phonon scattering of free carriers due to the amorphous crystal structure of Ge. Full-wave simulations based on a permittivity model that describes free-carrier damping through crystal structure disorder find excellent agreement with the experimental data. These findings offer an efficient and robust platform for all-optical switching at the nanoscale.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Colossal Optical Anisotropy from Atomic-Scale Modulations

Materials with large birefringence (Δn, where n is the refractive index) are sought after for polarization control (e.g., in wave plates, polarizing beam splitters, etc.), nonlinear optics, micromanipulation, and as a platform for unconventional light–matter coupling, such as hyperbolic phonon polaritons. Layered 2D materials can feature some of the largest optical anisotropy; however, their use in most optical systems is limited because their optical axis is out of the plane of the layers and the layers are weakly attached. This work demonstrates that a bulk crystal with subtle periodic modulations in its structure—Sr 9/8 TiS 3 —is transparent and positive-uniaxial, with extraordinary index n e = 4.5 and ordinary index n o = 2.4 in the mid- to far-infrared. The excess Sr, compared to stoichiometric SrTiS 3 , results in the formation of TiS 6 trigonal-prismatic units that break the chains of face-sharing TiS 6 octahedra in SrTiS 3 into periodic blocks of five TiS 6 octahedral units. The additional electrons introduced by the excess Sr form highly oriented electron clouds, which selectively boost the extraordinary index n e and result in record birefringence (Δn > 2.1 with low loss). The connection between subtle structural modulations and large changes in refractive index suggests new categories of anisotropic materials and also tunable optical materials with large refractive-index modulation.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Nanometer-Thick Sr 2 IrO 4 Freestanding Films for Flexible Electronics

In this article, we report the structural and optical properties of nanoscale Sr 2 IrO 4 freestanding thin-films fabricated using a water-soluble Sr 3 Al 2 O 6 layer. The coherent lattice structure, phonon modes, two-magnon Raman scattering, and optical absorption spectra of the Sr 2 IrO 4 nanomembrane are analogous to those of the layered iridate epitaxial thin-films and single crystals. Remarkably, the formation of 3-unit-cell-thick SrIrO 3 and interfacial composite layers alleviates the antiphase boundaries at the Sr 2 IrO 4 /Sr 3 Al 2 O 6 interface, resulting in structurally-robust nanomembranes. Our experimental results show that this freestanding thin-film approach of layered oxides can provide techniques for tuning or realizing unprecedented states beyond conventional thin-film methods, suggesting a pathway in achieving flexible layered-oxide electronics.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Landau-phonon polaritons in Dirac heterostructures

Polaritons are light-matter quasiparticles that govern the optical response of quantum materials at the nanoscale, enabling on-chip communication and local sensing. Here, we report Landau-phonon polaritons (LPPs) in magnetized charge-neutral graphene encapsulated in hexagonal boron nitride (hBN). These quasiparticles emerge from the interaction of Dirac magnetoexciton modes in graphene with the hyperbolic phonon polariton modes in hBN. Using infrared magneto-nanoscopy, we reveal the ability to completely halt the LPP propagation in real space at quantized magnetic fields, defying the conventional optical selection rules. The LPP-based nanoscopy also tells apart two fundamental many-body phenomena: the Fermi velocity renormalization and field-dependent magnetoexciton binding energies. Our results highlight the potential of magnetically tuned Dirac heterostructures for precise nanoscale control and sensing of light-matter interaction.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Phonon softening near topological phase transitions

Topological phase transitions occur when the electronic bands change their topological properties, typically featuring the closing of the band gap. While the influence of topological phase transitions on electronic and optical properties has been extensively studied, its implication on phononic properties and thermal transport remains unexplored. In this paper, we use first-principles simulations to show that certain phonon modes are significantly softened near topological phase transitions, leading to increased phonon-phonon scattering and reduced lattice thermal conductivity. We demonstrate this effect using two model systems: pressure induced topological phase transition in ZrTe 5 and chemical composition induced topological phase transition in Hg 1-x Cd x Te. We attribute the phonon softening to emergent Kohn anomalies associated with the closing of the band gap. Our paper reveals the strong connection between electronic band structures and lattice instabilities, and opens up a potential direction towards controlling heat conduction in solids.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

An experimental and computational investigation of the structure and spectroscopic signatures of α -UO 3

α-UO 3 is a common intermediate compound found in the nuclear fuel cycle, yet the exact crystal structure of this material has long been debated. Inconsistent computational and experimental data in previous works has led to varying conclusions between authors. Furthermore, to ensure the validity of our results in this work, the structural and spectroscopic signatures of pure phase α-UO 3 are investigated using powder X-ray diffraction and optical vibrational spectroscopy (infrared and Raman). Rietveld refinement of powder X-ray diffraction data on pure phase α-UO 3 collected in this work allows us to propose an alteration to the currently accepted C2mm structure (a = 3.9705 Å, b = 6.8553 Å, c = 4.15955 Å, α = β = γ = 90°) for α-UO 3 with no uranyl [UO 2 2+ ] bonds. Raman spectra collected using two excitation wavelengths (two instruments using 532 nm and one 785 nm) are presented, and differences with recently published results are discussed. Infrared spectra from two instruments used here agree well with recently published results, but the spectral range encompassed in our data extends past what has been reported with modern techniques. Additionally, we provide tentative vibrational mode assignments based on density functional perturbation theory calculations and resulting phonon eigenvector visualizations. Unexpected features in the optical vibrational spectra of α-UO 3 are explained by unique features in the structure we present.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2020

Thermal transport across nanoscale damage profile in sapphire irradiated by swift heavy ions

In this work, we studied the degradation of thermal conductivity in single crystal sapphire (α-Al 2 O 3 ) irradiated by 167 MeV Xe swift heavy ions (SHIs) over the multiple fluences in the range of 10 12 –10 14 ions/cm 2 . Thermal conductivity was measured primarily in the cross-plane direction using a noncontact ultrafast optical pump-probe technique called picosecond time domain thermoreflectance (TDTR). Multiple samples with variable ion fluences allowed us to probe distinct regions resulting from different regimes of microstructure evolution caused by electronic energy loss. By tuning the penetration depth of the thermal waves using different modulation frequencies, two regions with distinct conductivities were identified and the values of which were found to be consistent with phonon-mediated thermal transport models while the microstructure was confirmed by electron microscopy characterization. These damaged regions were determined to be a several micrometer thick ion track region and several tens of nanometer-thick amorphous layer present only above 5.0 × 10 13 ions/cm 2 . These results demonstrate the applicability of TDTR to resolve thermal transport behavior in SHI irradiated oxides having nonhomogeneous damage profile on a nanometer scale. The presented approach facilitates future studies aiming at resolving the impact of distinct damage resulting from electronic and nuclear stopping regimes under irradiation.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2021

Thermal conductivity of the quasi-one-dimensional materials TaSe 3 and ZrTe 3

The high breakdown current densities and resilience to scaling of the metallic transition metal trichalcogenides TaSe 3 and ZrTe 3 make them of interest for possible interconnect applications, and it motivates this study of their thermal conductivities and phonon properties. These crystals consist of planes of strongly bonded one-dimensional chains more weakly bonded to neighboring chains. Phonon dispersions and the thermal conductivity tensors are calculated using density functional theory combined with an iterative solution of the phonon Boltzmann transport equation. The phonon velocities and the thermal conductivities of TaSe 3 are considerably more anisotropic than those of ZrTe 3 . The maximum LA velocity in ZrTe 3 occurs in the cross-chain direction, and this is consistent with the strong cross-chain bonding that gives rise to large Fermi velocities in that direction. The thermal conductivities are similar to those of other metallic two-dimensional transition metal dichalcogenides. At room temperature, a significant portion of the heat is carried by the optical modes. In the low frequency range, the phonon lifetimes and mean free paths in TaSe 3 are considerably shorter than those in ZrTe 3 . Here, we find that the shorter lifetimes in TaSe 3 are consistent with the presence of lower frequency optical branches and zone-folding features in the acoustic branches that arise due to the doubling of the TaSe 3 unit cell within the plane.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Critical role of magnetic moments in the lattice dynamics of YBa 2 Cu 3 O 6

The role of lattice dynamics in unconventional high-temperature superconductivity is still vigorously debated. Theoretical insights into this problem have long been prevented by the absence of an accurate first-principles description of the combined electronic, magnetic, and lattice degrees of freedom. Utilizing the recently constructed r 2 SCAN density functional that stabilizes the antiferromagnetic (AFM) state of the pristine oxide YBa 2 ⁢Cu 3 ⁢O 6 , we faithfully reproduce the experimental dispersion of key phonon modes. Here we further find significant magnetoelastic coupling in numerous high-energy Cu-O bond stretching optical branches, where the AFM results improve over the soft nonmagnetic phonon bands.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2026

At Extreme Strain Rates, Pure Metals Thermally Harden while Alloys Thermally Soften

When materials are deformed at extreme strain rates, >10 6 s -1 , a counterintuitive mechanical response is seen where the strength and hardness of pure metals increases with increasing temperature. This anti-thermal hardening is due to dislocations meeting resistance to their motion from phonons in the crystal lattice. However, here, using optically-driven microballistic impact testing to measure dynamic strength and hardness, we show that when the composition is systematically varied away from high purity, the mechanical response of metals transitions from phonon drag of dislocations back to thermally activated pinning of dislocations, even at the highest strain rates. This boundary from “hotter-is-stronger” to “hotter-is-softer” is observed and mapped for nickel, titanium and gold. Furthermore, the ability to tune between deformation mechanisms with very different temperature dependencies speaks to new directions for alloy design in extreme conditions.

Ballistic transport↗