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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 199 records · Page 11
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Probing Surface Plasmon Dynamics in Periodic Nanostructures through Ultrafast Electron Microscopy

Surface plasmon polaritons (SPPs) can be manipulated to localize and guide light in subwavelength distances, enabling them to find applications in a wide range of areas, from sensing to quantum computing. Among several methods of SPP excitation, periodic arrays of nano- and microstructures are of particular interest, as they enable engineering SPP properties through structural parameters. Here, in this study, using the photon-induced near-field electron microscopy (PINEM) technique, we investigated the mode formation, coupling, interference, and decay of SPPs in square and hexagonal arrays of circular nanoholes under both visible and near-infrared excitation. Polarization-resolved analysis revealed the key factors governing SPP localization and interference patterns, showing that the periodicity and symmetry of the array primarily determine the SPP interference patterns and their orientation, while pump polarization mainly modulates their intensity. Time-resolved PINEM measurements demonstrated the spatial dependence of the SPP temporal characteristics. In addition, cathodoluminescence (CL) spectroscopy was employed to examine the intrinsic plasmonic characteristics of the structure. Finite difference time domain (FDTD) simulations showed strong agreement with both PINEM and CL measurements on the spatial and spectral behavior of SPPs. Understanding the spatiotemporal dynamics of SPPs on nanostructures beyond the diffraction limit is crucial for optimizing plasmonic structures for advanced photonic and quantum technologies.

Plasmonics↗
DOE OSTI2024

Ultrafast x-ray scattering and electronic coherence at avoided crossings: complete isotropic signals

Abstract Nonadiabatic transitions at conical intersections and avoided crossings play a pivotal role in shaping the outcomes of photochemical reactions. Using the photodissociation of LiF as a model, this theoretical study explores the application of gas phase nonresonant ultrafast x-ray scattering to map nonadiabatic transitions at an avoided crossing, utilizing the part of the scattering signal that probes electronic coherence directly. The presented scattering signals are rotationally averaged and calculated from two- rather than one-electron (transition) densities, which inherently accounts for all possible electronic transitions driven by the x-ray photon. This approach provides quantitative predictions of the experimental signals, thereby facilitating future experimental endeavors to observe nonadiabatic effects and coherent electron dynamics with ultrafast x-ray scattering.

Optics↗
DOE OSTI2020

Role of weak interlayer coupling in ultrafast exciton-exciton annihilation in two-dimensional rhenium dichalcogenides

Strong interactions between excitons are a characteristic feature of two-dimensional (2D) semiconductors, determining important excitonic properties, such as exciton lifetime, coherence, and photon-emission efficiency. Rhenium disulfide (ReS 2 ), a member of the 2D transition-metal dichalcogenide (TMD) family, has recently attracted great attention due to its unique excitons that exhibit excellent polarization selectivity and coherence features. However, an in-depth understanding of exciton-exciton interactions in ReS 2 is still lacking. In this work, we used ultrafast pump-probe spectroscopy to study exciton-exciton interactions in monolayer (1L), bilayer (2L), and triple layer ReS 2 . Additionally, we directly measure the rate of exciton-exciton annihilation, a representative Auger-type interaction between excitons. It decreases with increasing layer number, as observed in other 2D TMDs. However, while other TMDs exhibit a sharp weakening of exciton-exciton annihilation between 1L and 2L, such behavior was not observed in ReS 2 . We attribute this distinct feature in ReS 2 to the relatively weak interlayer coupling, which prohibits a substantial change in the electronic structure when the thickness varies. This work not only highlights the unique excitonic properties of ReS 2 but also provides novel insight into the thickness dependence of exciton-exciton interactions in 2D systems.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Controlling the helicity of light by electrical magnetization switching

Controlling the intensity of emitted light and charge current is the basis of transferring and processing information. By contrast, robust information storage and magnetic random-access memories are implemented using the spin of the carrier and the associated magnetization in ferromagnets. In this study, the missing link between the respective disciplines of photonics, electronics and spintronics is to modulate the circular polarization of the emitted light, rather than its intensity, by electrically controlled magnetization. Here we demonstrate that this missing link is established at room temperature and zero applied magnetic field in light-emitting diodes through the transfer of angular momentum between photons, electrons and ferromagnets. With spin-orbit torque a charge current generates also a spin current to electrically switch the magnetization. This switching determines the spin orientation of injected carriers into semiconductors, in which the transfer of angular momentum from the electron spin to photon controls the circular polarization of the emitted light. The spin-photon conversion with the nonvolatile control of magnetization opens paths to seamlessly integrate information transfer, processing and storage. Our results provide substantial advances towards electrically controlled ultrafast modulation of circular polarization and spin injection with magnetization dynamics for the next-generation information and communication technology, including space-light data transfer. The same operating principle in scaled-down structures or using two-dimensional materials will enable transformative opportunities for quantum information processing with spin-controlled single-photon sources, as well as for implementing spin-dependent time-resolved spectroscopies.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2025

Interfacial Strong Coupling and Negative Dispersion of Propagating Polaritons in Freestanding Oxide Membranes

Membranes of complex oxides like perovskite SrTiO3 extend the multi-functional promise of oxide electronics into the nanoscale regime of 2D materials. Here, it is demonstrated that freestanding oxide membranes supply a reconfigurable platform for nano-photonics based on propagating surface phonon polaritons. Infrared near-field imaging and spectroscopy enabled by a tunable ultrafast laser are applied to study pristine nano-thick SrTiO3 membranes prepared by hybrid molecular beam epitaxy. As predicted by coupled mode theory, it is found that strong coupling of interfacial polaritons realizes symmetric and antisymmetric hybridized modes with simultaneously tunable negative and positive group velocities. By resolving reflection of these propagating modes from membrane edges, defects, and substrate structures, their dispersion is quantified with position-resolved nano-spectroscopy. Remarkably, polariton negative dispersion is found to be both robust and tunable through choice of membrane dielectric environment and thickness, and proposes a novel design for in-plane Veselago lensing harnessing this control. This work lays the foundation for tunable transformation optics at the nanoscale using polaritons in a wide range of freestanding complex oxide membranes.

freestanding oxide membranes↗
DOE OSTI2026

Plasmonic Hybridization and Near-Field Localization in Gold “Dog Bone” Nanoparticles

Gold nanoparticles with complex anisotropic geometries offer unique opportunities for tailoring plasmonic near-fields beyond the limits of conventional nanorods. Here we combine photon-induced near-field electron microscopy (PINEM) and full-wave simulations to resolve plasmon hybridization and near-field localization in gold dog-bone nanoparticles and their dimers with and without conformal SiO 2 shells. We demonstrate that the dog-bone geometry drives unconventional polarization-dependent field confinement, including pronounced tip-localized near-fields under both longitudinal and transverse excitation. Conformal SiO 2 shells red-shift the plasmon resonances through dielectric screening and prevent charge-transfer coupling in adjacent dimers. Depending on the dimer orientation and excitation polarization, coupled structures exhibit distinct bonding- and antibonding-like hybridized modes as well as interparticle near-field channels. However, weakly interacting dimers retain largely independent particle responses with geometry-governed asymmetries. The close agreement between PINEM measurements and simulations establishes a direct picture of how shape, dielectric environment, and nanoscale coupling together define plasmonic modes in complex anisotropic nanoparticles. These findings provide design principles for engineering localized optical fields in plasmonic nanoscale structures.

hybridization↗
DOE OSTI2021

Toward Å-fs-meV Resolution in Electron Microscopy: Systematic Simulation of the Temporal Spread of Single-Electron Packets

Though efforts to improve the temporal resolution of transmission electron microscopes (TEMs) have waxed and waned for decades, with relatively recent advances routinely reaching sub-picosecond scales, fundamental and practical challenges have hindered the advance of combined Å-fs-meV resolutions, particularly for core-loss spectroscopy and real-space imaging. This is due in no small part to the complexity of the approach required to access timescales upon which electrons, atoms, molecules, and materials first begin to respond and transform – attoseconds to picoseconds. Here we present part of a larger effort devoted to systematically mapping the instrument parameter space of a TEM modified to reach ultrafast timescales. With General Particle Tracer, we studied the statistical temporal distributions of single-electron packets as a function of various fs pulsed-laser parameters and electron-gun configurations and fields for the exact architecture and dimensions of a Thermo Fisher Tecnai Femto ultrafast electron microscope. We focused on easily-adjustable parameters, such as laser pulse duration, laser spot size, photon energy, Wehnelt aperture diameter, and photocathode size. In addition to establishing trends and dispersion behaviors, we identify regimes within which packet duration can be 100s of fs and approach the 300-fs laser limit employed here. Overall, the results provide a detailed picture of the temporal behavior of single-electron packets in the Tecnai Femto gun region, forming the initial contribution of a larger effort.

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

Gallium oxide semiconductor-based large volume ultrafast radiation hard spectroscopic scintillators

We report on the development of the first-ever inorganic radiation-hard moisture-insensitive large volume spectroscopic semiconductor-based scintillator with less than 2 ns decay time and light yields as high as 8000 ph/MeV. Despite extensive research into scintillator materials, the quest for an ideal scintillator combining ultrafast decay times (akin to BaF 2 and Yb-doped scintillators such as Lu 2 O 3 :Yb), high light yields (exceeding 2000 photons per MeV), spectroscopic capabilities, and exceptional radiation hardness remain unfulfilled. In this study, we demonstrate and report for the first time the viability of large-volume (up to 20 mm thickness) gallium oxide (β-Ga 2 O 3 ) semiconductor-based scintillators for applications requiring these properties. These β-Ga 2 O 3 scintillators were grown using the fast turnaround (~2 days) crucible-free optical float zone (FZ) technique. The high light yield and ultrafast decay time of these high-purity n-type semiconductors with free carrier concentration of 6 × 10 17 cm –3 are attributed to native defects, specifically oxygen vacancies (V O ) and gallium–oxygen vacancy pairs (V Ga –V O ), generated during optimized FZ growth. The ultrafast decay, along with high light yield, enables excellent timing resolution and high count rate detection for applications like time-of-flight positron emission tomography, physics experiments, and nuclear safety. The radiation hardness of these devices has been documented in a separate publication.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2022

Observations on the deformation of metal microspheres in shock-driven polymer flows

We report that solid particles can be fragmented by a fast-moving fluid if their velocity difference is great enough, such as during the atmospheric entry of meteoroids or the shock compression of engineered particulate composites. The extent of particle deformation and breakup in such systems is poorly understood because the necessary extreme conditions make observation difficult and data scarce. To meet this need, experiments combining ultrafast synchrotron-based radiography with plate impact loading were performed at the dynamic compression sector at the advanced photon source. Metal microspheres of several densities and strengths (Au, Ta, and W) were placed inside a polymer matrix. A planar shock wave was then produced in the polymer by the impact of a gun-launched flyer plate. X-ray images of the resulting flow were collected at ~150ns intervals. These images document the progression of particle deformation across a range of flow conditions and particle materials. They show that the extent of deformation is sensitive to the ratio of drag stress to particle strength. The deforming particle's shape is determined by the initial shock–particle interaction, fluid stagnation pressure, and vorticity, each acting on its own timescale. A set of scaling relationships is presented to capture these observations and enable comparison with prior hydrodynamic data. The result is a framework for predicting the conditions under which strong particles are severely deformed by a shock-driven flow.

36 MATERIALS SCIENCE↗
DOE OSTI2024

UV-Induced Reaction Pathways in Bromoform Probed with Ultrafast Electron Diffraction

For many chemical reactions, it remains notoriously difficult to predict and experimentally determine the rates and branching ratios between different reaction channels. This is particularly the case for reactions involving short-lived intermediates, whose observation requires ultrafast methods. The UV photochemistry of bromoform (CHBr 3 ) is among the most intensely studied photoreactions. Yet, a detailed understanding of the chemical pathways leading to the production of atomic Br and molecular Br 2 fragments has proven challenging. In particular, the role of isomerization and/or roaming and their competition with direct C–Br bond scission has been a matter of continued debate. Here, in this work, gas-phase ultrafast megaelectronvolt electron diffraction (MeV-UED) is used to directly study structural dynamics in bromoform after single 267 nm photon excitation with femtosecond temporal resolution. The results show unambiguously that isomerization contributes significantly to the early stages of the UV photochemistry of bromoform. In addition to direct C–Br bond breaking within <200 fs, formation of iso-CHBr 3 (Br-CH-Br-Br) is observed on the same time scale and with an isomer lifetime of >1.1 ps. The branching ratio between direct dissociation and isomerization is determined to be 0.4 ± 0.2:0.6 ± 0.2, i.e., approximately 60% of molecules undergo isomerization within the first few hundred femtoseconds after UV excitation. The structure and time of formation of iso-CHBr 3 compare favorably with the results of an ab initio molecular dynamics simulation. The lifetime and interatomic distances of the isomer are consistent with the involvement of a roaming reaction mechanism.

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

An Exceptionally Powerful, Radiatively Driven Ultrafast Outflow in the Rapidly Accreting AGN RE J1034+396

We report the analysis of ∼1 Ms of XMM-Newton observations of the rapidly accreting active galactic nucleus RE J1034+396. The 0.3–9 keV EPIC-pn spectra are well described by a model consisting of steep continuum emission from the corona accompanied by relativistically blurred reflection from a highly ionized accretion disk. The source is known to exhibit strong excess soft X-ray emission, which we show is well represented by thermal disk photons Comptonized by a warm plasma spanning the inner accretion flow. Additionally, the EPIC-pn data provide compelling evidence (ΔC ∼ 60 for four additional parameters) for the presence of an ultrafast outflow (UFO) with a line-of-sight velocity v/c = 0.307$^{+0.001}_{-0.005}$, and an emission signature consistent with reflection of the corona from modestly ionized, outflowing gas. The simultaneous 0.5–2.5 keV RGS spectra show clear absorption lines. Modelling of these data confirms the presence of the UFO and constrains its equivalent hydrogen column density, log N H /(atom cm −2 ) = 21.7$^{+0.1}_{-0.2}$. The RGS data also reveal at least two warm absorber components with a modest outflow velocity (1680$^{+40}_{-50}$ km s -1 ). The measured properties and time evolution of the UFO in RE J1034+396 suggest that it is formed from collisionally ionized plasma, launched from the disk surface and accelerated by radiation pressure. The high terminal velocity and substantial absorbing column density imply that the outflow carries sufficient momentum and energy to transform its environment, being capable of driving out essentially all dust and gas it interacts with along the line of sight, even if the AGN were initially surrounded by a Compton-thick absorber.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2021

Ultrafast optical switching and power limiting in intersubband polaritonic metasurfaces

Highly nonlinear optical materials with fast third-order nonlinear optical response are crucial for the operation of all-optical photonic devices, such as switches for signal processing and computation, power limiters, and saturable absorbers. The nonlinear response of traditional optical materials is weak, thus requiring large light intensities to induce significant changes in their properties. Here we show that optical control of the coupling rate in subwavelength patch antennas coupled to intersubband transitions in multi-quantum-well semiconductor heterostructures can provide a giant third-order nonlinear response, on the order of 3.4 × <#comment/> 10 − <#comment/> 13 m 2 / V 2 , with a response time < <#comment/> 2 p s . We utilize this effect to realize intersubband polaritonic metasurfaces and demonstrate their operation as highly nonlinear saturable and reverse saturable absorbers, enabling optical power limiters and other elements for all-optical modulation and control. Our approach enables a plethora of compact, low-power, highly nonlinear devices with spectral, temporal, and structured wavefront responses tailored by design.

Mann, Sander A. (ORCID:0000000277420615)↗
DOE OSTI2021

Quantum Nature of Dielectric Laser Accelerators

Dielectric laser accelerators (DLAs) hold great promise for producing economic and compact on-chip radiation sources. On-chip DLAs benefit from fabrication capabilities of the silicon industry and from breakthroughs in silicon-photonic nanostructures to enhance the interaction between particles and laser fields. Seemingly unrelated recent advances in the quantum interactions of electrons and light have raised interest in the underlying classical-quantum correspondence principle at the foundations of electron acceleration. Here, we present the observation of the underlying quantum nature of DLAs: observing quantized peaks in the electron-energy spectra. Our findings demonstrate quasi-phase-matching between an electron wave function and a light wave, which also demonstrates the role of the quantum wave function in the inverse Smith-Purcell effect. We harness the capabilities of an ultrafast transmission electron microscope (UTEM) to maintain a long electron-light interaction length extending over hundreds of periods of the laser pulse, mediated by a silicon-photonic nanograting DLA. The UTEM is shown as a new platform for characterization of future DLA concepts. The results raise fundamental questions regarding the role of quantum mechanics in DLA design, and more generally about the prospects of manipulating particles’ quantum wave functions in accelerator physics.

43 PARTICLE ACCELERATORS↗
DOE OSTI2025

Ultrastable Gold Nanostars via Bottlebrush-like Block Copolymers

Gold (Au) nanostars are plasmonic nanostructures possessing potentials for small molecule detection, photocatalytic activities, and photothermal therapy. However, Au nanostars synthesized in the traditional way are often plagued by poor photo, thermal, and chemical stabilities. Here, we report an unconventional route to the synthesis of ultrastable colloidal Au nanostars enabled by bottlebrush-like block copolymers (BBCPs), dispensing with the need for Au seeds. Crafting of Au nanostars using BBCPs is rendered by bridging the latter with Au 3+ ions as cross-linkers that have multiple coordination sites. Notably, the presence of a covalently tethered polymer shell on the surface of Au nanostars (i.e., polymer-ligated Au nanostars) imparts remarkably high stability under high temperature and laser excitation over conventional cetyltrimethylammonium bromide (CTAB)-mediated Au nanostars. Due to enhanced laser stability, plasmonic fields near Au nanostars can be visualized under high laser fluence by ultrafast electron microscopy (UEM) without morphological degradation. Notably, the presence of insulating polystyrene chains does not compromise the plasmonic field distribution, with the highest field intensity observed along the star arms. In conclusion, the greatly improved long-term photo, thermal, and chemical stabilities make Au nanostars a prospective noble metal nanomaterial for a range of sensing applications.

Cellulose↗
DOE OSTI2025

Ultrafast optical modulation of vibrational strong coupling in ReCl(CO) 3 (2,2-bipyridine)

Polaritons – hybrid light-matter states formed from the strong coupling of a bright molecular transition with a confined photonic mode – may offer new opportunities for optical control of molecular behavior. Vibrational strong coupling (VSC) has been reported to impact ground-state chemical reactivity, but its influence on electronic excited-state dynamics remains unexplored. Here, we take a first step towards excited-state VSC by demonstrating optical modulation of the ReCl(CO) 3 (bpy), (bpy = 2,2-bipyridine) complex under VSC using femtosecond ultraviolet (UV)-pump/infrared (IR)-probe spectroscopy. We establish ground-state VSC of ReCl(CO) 3 (bpy) in a microfluidic Fabry-Pérot cavity equipped with indium tin oxide (ITO)-coated mirrors. ITO is effectively dichroic as it is reflective in the IR and transmissive in the UV-visible and therefore minimizes optical interference. Excitation with UV pump light drives ReCl(CO) 3 (bpy) into a manifold of electronic excited states that subsequently undergo non-radiative relaxation dynamics. We probe the transient response of the strongly-coupled system in the mid-IR, observing both Rabi contraction and cavity-filtered excited-state absorption signatures. We reconstruct the intrinsic response of intracavity molecules from the transient cavity transmission spectra to enable quantitative comparison with extracavity control experiments. We report no changes in the excited-state dynamics of ReCl(CO) 3 (bpy) under ground-state VSC. However, we do observe significant amplification of transient vibrational signals due to classical cavity-enhanced optical effects. This effort lays the groundwork to pursue direct excited-state VSC aimed at modulating photochemical reactivity.

cavity-enhanced spectroscopy↗