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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 91 records · Page 5
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Analyzing Custom Proof Masses and Quantum Limits of a Manufacturable Cavity Optical Levitation Solution

This report details results of a one-year LDRD to understand the dynamics, figures of merit, and fabrication possibilities for levitating a micro-scale, disk-shaped dielectric in an optical field. Important metrics are the stability, positional uncertainty, and required optical power to maintain levitation. Much of the results are contained in a publication written by our academic alliance collaborators. Initial structures were grown at Sandia labs and a test fabrication flow was executed. Owing to our strength in VCSEL lasers, we were particularly interested in calculations and fabrication flows that could be compatible with a VCSEL light source.

42 ENGINEERING↗
DOE OSTI2023

Uncovering extreme nonlinear dynamics in solids through time-domain field analysis

Time-domain analysis of harmonic fields with sub-cycle resolution is now experimentally viable due to the emergence of sensitive, on-chip techniques for petahertz-scale optical-field sampling. We demonstrate how such a time-domain, field-resolved analysis uncovers the extreme nonlinear electron dynamics responsible for high-harmonic generation within solids. Time-dependent density functional theory was used to simulate harmonic generation from a solid-state band-gap system driven by near- to mid-infrared waveforms. Particular attention was paid to regimes where both intraband and interband emission mechanisms play a critical role in shaping the nonlinear response. We show that a time-domain analysis of the harmonic radiation fields identifies the interplay between intra- and interband dynamical processes underlying the nonlinear light generation. With further analysis, we show that changes to the dominant emission regime can occur after only slight changes to the peak driving intensity and central driving wavelength. Furthermore, time-domain analysis of harmonic fields also reveals, for the first time, the possibility of rapid changes in the dominant emission mechanism within the temporal window of the driving pulse envelope. Finally, we examine the experimental viability of performing time-domain analysis of harmonic fields with sub-cycle resolution using realistic parameters.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2026

Terahertz‐Nanoscale Visualization of the Microscopic Spin‐Charge Architecture of Colossal Magnetoresistive Switching

Resolving sub-10 nm spin switching and the associated terahertz (THz) electrodynamics during the colossal magnetoresistance (CMR) transition is a definitive frontier in reaching the fundamental spatial, temporal, and energy-dissipation limits of spin-electronics. Yet, simultaneous control of high magnetic field, cryogenic environment, and nanometer resolution has remained an elusive benchmark for THz nanoscopy, leaving the local THz dynamics of these transitions largely unexplored. Here, we overcome these limitations by utilizing a custom-built cryogenic magneto-THz scattering-type scanning near-field optical microscopy (cm-THz-sSNOM) to resolve the near-field THz spectroscopic evolution of the magnetic field-driven CMR transition in a manganite single crystal. Our measurements provide a nanoscale visualization of the THz conductivity, capturing the moment that magnetic-field-induced spin switching triggers the transition from an antiferromagnetic insulator to a ferromagnetic metal. An ellipsoidal near-field model reveals a multi-scale transition initiated by 1–2 nm isolated spin-flip sites at low magnetic fields, which coalesce into ∼15 nm conducting regions as the threshold field is approached. These results provide an nano-THz view of CMR switching, establishing an analysis framework for mapping spin–charge–lattice–orbit–coupled dynamics at spatial scales that transcend the nominal sSNOM resolution.

Haeuser, Samuel [Iowa State University, Ames, IA (↗
DOE OSTI2025

Spontaneous Formation of Single-Crystalline Spherulites in a Chiral 2D Hybrid Perovskite

In two-dimensional (2D) chiral metal-halide perovskites (MHPs), chiral organic spacers induce structural chirality and chiroptical properties in the metal-halide sublattice. This structural chirality enables reversible crystalline-glass phase transitions in (S-NEA) 2 PbBr 4 , a prototypical chiral 2D MHP where NEA + represents 1-(1-naphthyl)ethylammonium. Here, in this study, we investigate two distinct spherulite states of (S-NEA) 2 PbBr 4 , exhibiting either radial-like or stripe-like banded patterns depending on the annealing conditions of the amorphous film. Despite similarities in optical absorption and photoluminescence, the stripe-like, banded spherulite exhibits higher crystallinity and improved optical transparency compared to those of radial-like spherulite. X-ray nanoprobe measurements reveal tilting-angle modulations in the octahedral plane of stripe-like spherulites, correlating with the film’s surface geometry. Transfer matrix calculations indicate that the optical contrast in stripe-like patterns, seen in bright-field optical microscopy, arises from optical interference effects, differing from the contrast mechanism observed in polymer spherulites. Ultrafast carrier dynamics experiments suggest that the stripe-like spherulites resemble single crystals more closely than radial-like spherulites, while electrical conductivity measurements show enhanced charge carrier transport in stripe-like spherulites. These findings offer insights into MHP spherulite states with a single composition but different morphologies, previously observed only in polymers, highlighting their potential for optoelectronic applications.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Multipolariton control in attosecond transient absorption of autoionizing states

Tunable attosecond transient absorption spectroscopy is an ideal tool for studying and manipulating autoionization dynamics in the continuum. We investigate near-resonant two-photon couplings between the bright 3s –1 4p and dark 3s –1 4f autoionizing states of argon that lead to Autler-Townes-like interactions, forming entangled light-matter states or polaritons. We observe that one-photon couplings with intermediate dark states play an important role in this interaction, leading to the formation of multiple polaritonic branches whose energies exhibit avoided crossings as a function of the dressing-laser frequency. Our experimental measurements and theoretical essential-state simulations show good agreement and reveal how the delay, frequency, and intensity of the dressing pulse govern the properties of autoionizing polariton multiplets. Furthermore, these results demonstrate new pathways for quantum control of autoionizing states with optical fields.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2024

Origins and consequences of asymmetric nano-FTIR interferograms

Infrared scattering-type near-field optical microscopy, IR s-SNOM, and its broadband variant, nano-FTIR, are pioneering, flagship techniques for their ability to provide molecular identification and material optical property information at a spatial resolution well below the far-field diffraction limit, typically less than 25 nm. While s-SNOM and nano-FTIR instrumentation and data analysis have been discussed previously, there is a lack of information regarding experimental parameters for the practitioner, especially in the context of previously developed frameworks. Like conventional FTIR spectroscopy, the critical component of a nano-FTIR instrument is an interferometer. However, unlike FTIR spectroscopy, the resulting interference patterns or interferograms are typically asymmetric. Here, we unambiguously describe the origins of asymmetric interferograms recorded with nano-FTIR instruments, give a detailed analysis of potential artifacts, and recommend optimal instrument settings as well as data analysis parameters.

47 OTHER INSTRUMENTATION↗
DOE OSTI2026

Field-resolved observation of exciton coherence in a van der Waals magnet

The emergence of coherence among electronic quasiparticles underlies collective quantum phenomena from superconductivity to superradiance. In semiconductors, exciton coherence is generally thought to decay rapidly due to scattering and dephasing, limiting its persistence on ultrafast timescales. Here, in this work, we demonstrate a light-field-driven mechanism that creates and stabilizes exciton coherence in the layered antiferromagnet CrSBr. We directly record the coherent optical field emitted by excitons and track in real time how a deterministic phase, imprinted by the excitation laser, drives incoherent excitons to synchronize into a collective state. This ensemble remains phase coherent for more than 2 ps, whereas its resonance energy undergoes an ultrafast modulation mediated by spin and lattice interactions. The time-resolved field evolution indicates that the multiple peaks seen in conventional spectra originate from a single excitonic resonance subject to dynamic energy modulation. Our findings establish optical phase imprinting as a mechanism to control and sustain collective order in semiconducting magnets, bridging light-driven dynamics with excitonic and magnetic correlations in layered quantum materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Probing dark exciton navigation through a local strain landscape in a WSe2 monolayer

Abstract In WSe 2 monolayers, strain has been used to control the energy of excitons, induce funneling, and realize single-photon sources. Here, we developed a technique for probing the dynamics of free excitons in nanoscale strain landscapes in such monolayers. A nanosculpted tapered optical fiber is used to simultaneously generate strain and probe the near-field optical response of WSe 2 monolayers at 5 K. When the monolayer is pushed by the fiber, its lowest energy states shift by as much as 390 meV (>20% of the bandgap of a WSe 2 monolayer). Polarization and lifetime measurements of these red-shifting peaks indicate they originate from dark excitons. We conclude free dark excitons are funneled to high-strain regions during their long lifetime and are the principal participants in drift and diffusion at cryogenic temperatures. This insight supports proposals on the origin of single-photon sources in WSe 2 and demonstrates a route towards exciton traps for exciton condensation.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Bolometric Superconducting Optical Nanoscopy (BOSON)

Superconducting transition-edge sensors are renowned for their extraordinary photon sensitivity and energy resolution, finding applications spanning quantum information, astronomy, and nanophotonics. Here, we report the development of bolometric superconducting optical nanoscopy (BOSON), a novel platform that integrates bolometric detection at the superconducting transition edges with near-field optical techniques. BOSON enables the mapping of photoinduced changes in superconductivity with unprecedented spatial resolution and photon sensitivity. By incorporating BOSON with low-dimensional materials, we achieved polariton imaging at nanowatt excitation levels—at least 4 orders of magnitude lower than the power typically required in prior near-field nanoscopy experiments. Our findings highlight the potential for BOSON to advance scanning-probe-based optical platforms to enable the detection of photons, polaritons, and Cooper pair dynamics at the nanoscale. This paves the way for quantum sensing applications using single-polariton detection and can offer deeper insights into quasiparticle dynamics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Applications of ultrafast nano-spectroscopy and nano-imaging with tip-based microscopy

Innovation in microscopy has often been critical in advancing both fundamental science and technological progress. Notably, the evolution of ultrafast near-field optical nano-spectroscopy and nano-imaging has unlocked the ability to image at spatial scales from nanometers to ångströms and temporal scales from nanoseconds to femtoseconds. This approach revealed a plethora of fascinating light-matter states and quantum phenomena, including various species of polaritons, quantum phases, and complex many-body effects. This review focuses on the working principles and state-of-the-art development of ultrafast tip-enhanced and near-field microscopy, integrating diverse optical pump-probe methods across the terahertz (THz) to ultraviolet (UV) spectral ranges. It highlights their utility in examining a broad range of materials, including two-dimensional (2D), organic molecular, and hybrid materials. The review concludes with a spatio-spectral-temporal comparison of ultrafast nano-imaging techniques, both within already well-defined domains, and offering an outlook on future developments of ultrafast tip-based microscopy and their potential to address a wider range of materials.

Zhao, Zhichen [Tongji University, Shanghai (China)↗
DOE OSTI2024

Strong-Field Bloch Electron Interferometry for Band-Structure Retrieval

When Bloch electrons in a solid are exposed to a strong optical field, they are coherently driven in their respective bands where they acquire a quantum phase as the imprint of the band shape. If an electron approaches an avoided crossing formed by two bands, it may be split by undergoing a Landau-Zener transition. We here employ subsequent Landau-Zener transitions to realize strong-field Bloch electron interferometry (SFBEI), allowing us to reveal band structure information. In particular, we measure the Fermi velocity (band slope) of graphene in the vicinity of the K points as 1.07±0.04 nm fs –1 . As a result, we expect SFBEI for band structure retrieval to apply to a wide range of material systems and experimental conditions, making it suitable for studying transient changes in band structure with femtosecond temporal resolution at ambient conditions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Compound Meta-Optics for Complete and Loss-Less Field Control

Optical metasurfaces offer a compact platform for manipulation of the amplitude, phase, and polarization state of light. Independent control over these properties, however, is hindered by the symmetric transmission matrix associated with single-layer metasurfaces. Here, we utilize multilayer birefringent meta-optics to realize high-efficiency, independent control over the amplitude, phase, and polarization state of light. In this work, high-efficiency control is enabled by redistributing the wavefront between cascaded metasurfaces, while end-to-end inverse design is used to realize independent complex-valued functions for orthogonal polarization states. Based on this platform, we demonstrate spatial mode division multiplexing, optical mode conversion, and universal vectorial holograms, all with diffraction efficiencies over 80%. This meta-optic platform expands the design space of flat optics and could lead to advances in optical communications, quantum entanglement, and information encryption.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Nano-spectroscopy of excitons in atomically thin transition metal dichalcogenides

Abstract Excitons play a dominant role in the optoelectronic properties of atomically thin van der Waals (vdW) semiconductors. These excitons are amenable to on-demand engineering with diverse control knobs, including dielectric screening, interlayer hybridization, and moiré potentials. However, external stimuli frequently yield heterogeneous excitonic responses at the nano- and meso-scales, making their spatial characterization with conventional diffraction-limited optics a formidable task. Here, we use a scattering-type scanning near-field optical microscope (s-SNOM) to acquire exciton spectra in atomically thin transition metal dichalcogenide microcrystals with previously unattainable 20 nm resolution. Our nano-optical data revealed material- and stacking-dependent exciton spectra of MoSe 2 , WSe 2 , and their heterostructures. Furthermore, we extracted the complex dielectric function of these prototypical vdW semiconductors. s-SNOM hyperspectral images uncovered how the dielectric screening modifies excitons at length scales as short as few nanometers. This work paves the way towards understanding and manipulation of excitons in atomically thin layers at the nanoscale.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Femtosecond exciton dynamics in WSe 2 optical waveguides

Van-der Waals (vdW) atomically layered crystals can act as optical waveguides over a broad range of the electromagnetic spectrum ranging from Terahertz to visible. Unlike common Si-based waveguides, vdW semiconductors host strong excitonic resonances that may be controlled using non-thermal stimuli including electrostatic gating and photoexcitation. Here, we utilize waveguide modes to examine photo-induced changes of excitons in the prototypical vdW semiconductor, WSe 2 , prompted by femtosecond light pulses. Using time-resolved scanning near-field optical microscopy we visualize the electric field profiles of waveguide modes in real space and time and extract the temporal evolution of the optical constants following femtosecond photoexcitation. By monitoring the phase velocity of the waveguide modes, we detect incoherent A-exciton bleaching along with a coherent optical Stark shift in WSe 2 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Sharp, high numerical aperture (NA), nanoimprinted bare pyramid probe for optical mapping

The ability to correlate optical hyperspectral mapping and high resolution topographic imaging is critically important to gain deep insight into the structure–function relationship of nanomaterial systems. Scanning near-field optical microscopy can achieve this goal, but at the cost of significant effort in probe fabrication and experimental expertise. To overcome these two limitations, we have developed a low-cost and high-throughput nanoimprinting technique to integrate a sharp pyramid structure on the end facet of a single-mode fiber that can be scanned with a simple tuning-fork technique. The nanoimprinted pyramid has two main features: (1) a large taper angle (~70°), which determines the far-field confinement at the tip, resulting in a spatial resolution of 275 nm, an effective numerical aperture of 1.06, and (2) a sharp apex with a radius of curvature of ~20 nm, which enables high resolution topographic imaging. Optical performance is demonstrated through evanescent field distribution mapping of a plasmonic nanogroove sample, followed by hyperspectral photoluminescence mapping of nanocrystals using a fiber-in-fiber-out light coupling mode. Through comparative photoluminescence mapping on 2D monolayers, we also show a threefold improvement in spatial resolution over chemically etched fibers. These results show that the bare nanoimprinted near-field probes provide simple access to spectromicroscopy correlated with high resolution topographic mapping and have the potential to advance reproducible fiber-tip-based scanning near-field microscopy.

47 OTHER INSTRUMENTATION↗
DOE OSTI2020

Cathodoluminescence of Ultrathin Twisted Ge 1–x Sn x S van der Waals Nanoribbon Waveguides

Ultrathin van der Waals semiconductors have shown extraordinary optoelectronic and photonic properties. Propagating photonic modes make layered crystal waveguides attractive for photonic circuitry and for studying hybrid light-matter states. Accessing guided modes by conventional optics is challenging due to limited spatial resolution and poor out-of-plane far field coupling. Scanning near-field optical microscopy (SNOM) can overcome these issues and can characterize waveguide modes down to tens of nm resolution, albeit for planar samples or nanostructures with moderate height variations. Electron microscopy provides atomic-scale localization also for more complex geometries, and recent advances extended the accessible excitations from interband transitions to phonons. In this work, bottom-up synthesized layered semiconductor (Ge 1-x Sn x S) nanoribbons with axial twist and deep sub-wavelength thickness are demonstrated as a platform for realizing waveguide modes, and cathodoluminescence (CL) spectroscopy is introduced as a tool to characterize them. Combined experiments and simulations show the excitation of guided modes by the electron beam and their efficient detection via photons emitted in the ribbon plane, which enables measuring key properties such as the evanescent field into the vacuum cladding with nanometer resolution. The results identify van der Waals waveguides operating in the infrared and highlight an electron microscopy-based approach for probing complex-shaped nanophotonic structures.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Phonon-enhanced nonlinearities in hexagonal boron nitride

Abstract Polar crystals can be driven into collective oscillations by optical fields tuned to precise resonance frequencies. As the amplitude of the excited phonon modes increases, novel processes scaling non-linearly with the applied fields begin to contribute to the dynamics of the atomic system. Here we show two such optical nonlinearities that are induced and enhanced by the strong phonon resonance in the van der Waals crystal hexagonal boron nitride (hBN). We predict and observe large sub-picosecond duration signals due to four-wave mixing (FWM) during resonant excitation. The resulting FWM signal allows for time-resolved observation of the crystal motion. In addition, we observe enhancements of third-harmonic generation with resonant pumping at the hBN transverse optical phonon. Phonon-induced nonlinear enhancements are also predicted to yield large increases in high-harmonic efficiencies beyond the third.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Scanless laser waveform measurement in the near-infrared

Field-resolved measurements of few-cycle laser waveforms allow access to ultrafast electron dynamics in light–matter interactions and are key to future lightwave electronics. Recently, sub-cycle gating based on nonlinear excitation in active pixel sensors has allowed the first single-shot measurements of mid-infrared optical fields. Extending the techniques to shorter wavelengths, however, is not feasible using silicon-based detectors with bandgaps in the near-infrared. Here, we demonstrate an all-optical sampling technique for near-infrared laser fields, wherein an intense fundamental field generates a sub-cycle gate through nonlinear excitation of a wide-bandgap crystal, in this case, ZnO, which can sample the electric field of a weak perturbing pulse. By using a crossed-beam geometry, the temporal evolution of the perturbing field is mapped onto a transverse spatial axis of the nonlinear medium, and the waveform is captured in a single measurement of the spatially resolved fluorescence emission from the crystal. The technique is demonstrated through field-resolved measurements of the field reshaping during nonlinear propagation in the ZnO detection crystal.

Truong, Tran-Chau (ORCID:0000000348940635)↗