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At least 1,171 records · Page 65

Investigation of low-latitude hydrogen emission in terms of a two-component interstellar gas model

High-resolution 21-cm hydrogen line observations at low galactic latitude are analyzed to determine the large-scale distribution of galactic hydrogen. Distribution parameters are found by model fitting, optical depth effects are computed using a two-component gas model suggested by the observations, and calculations are made for a one-component uniform spin-temperature gas model to show the systematic departures between this model and data obtained by incorrect treatment of the optical depth effects. Synthetic 21-cm line profiles are computed from the two-component model, and the large-scale trends of the observed emission profiles are reproduced together with the magnitude of the small-scale emission irregularities. Values are determined for the thickness of the galactic hydrogen disk between half density points, the total observed neutral hydrogen mass of the galaxy, and the central number density of the intercloud hydrogen atoms. It is shown that typical hydrogen clouds must be between 1 and 13 pc in diameter and that optical thinness exists on large-scale despite the presence of optically thin gas.

Baker, P. L.↗

Contamination Observed on the Passive Optical Sample Assembly (POSA)-1 Experiment

The Passive Optical Sample Assembly-1 (POSA-1), part of the Mir Environmental Effects Payload (MEEP), was designed to study the combined effects of contamination, atomic oxygen, ultraviolet radiation, vacuum, thermal cycling, and other constituents of the space environment on spacecraft materials. The MEEP program is a Phase 1 International Space Station Risk Mitigation Experiment. The payload was attached by EVA to the exterior of the Mir docking module during the Space Shuttle mission STS-76. It was removed during STS-86 after exposure to the Mir environment for 18 months. POSA-1 consists of nearly 400 samples of thermal control paints, chemical conversion coatings, mirrors, optics, and other candidate materials for International Space Station Alpha (ISSA). POSA-1 also flew state-of-the-art materials, such as electrically conductive thermal control coatings developed under contract by IITRI and AZ Technology, and passive instruments for monitoring the atomic oxygen and ultraviolet radiation dose to the experiment. Contamination was detected on the POSA-1 experiment. On the side facing space (-Z(sub B) direction using the Mir coordinate system), visible contamination was observed. The contamination was uniform as would occur from a slow photodeposition process. A very definite film was deposited on the optical samples. The deposition appears to have directionality with definite shadowing effects. On the side facing the main Mr core (+ZB direction using the Mir coordinate system), no visible contamination was noted. Pre- and post-flight characterization of candidate spacecraft materials is discussed, particularly the effect of contamination on total hemispherical spectral reflectance (250 - 2500 nm), infrared emittance, the bi-directional reflectance distribution function (BRDF), and vacuum ultraviolet spectral reflectance. Extensive photography under normal and black light was performed. Results of electron spectroscopy for chemical analysis (ESCA) and Fourier Transform Infrared Analysis (FTIR) on selected samples are also discussed.

Zwiener, James M.↗

Light-Driven Charge Transport and Optical Sensing in Molecular Junctions

Probing charge and energy transport in molecular junctions (MJs) has not only enabled a fundamental understanding of quantum transport at the atomic and molecular scale, but it also holds significant promise for the development of molecular-scale electronic devices. Recent years have witnessed a rapidly growing interest in understanding light-matter interactions in illuminated MJs. These studies have profoundly deepened our knowledge of the structure–property relations of various molecular materials and paved critical pathways towards utilizing single molecules in future optoelectronics applications. In this article, we survey recent progress in investigating light-driven charge transport in MJs, including junctions composed of a single molecule and self-assembled monolayers (SAMs) of molecules, and new opportunities in optical sensing at the single-molecule level. We focus our attention on describing the experimental design, key phenomena, and the underlying mechanisms. Specifically, topics presented include light-assisted charge transport, photoswitch, and photoemission in MJs. Emerging Raman sensing in MJs is also discussed. Finally, outstanding challenges are explored, and future perspectives in the field are provided.

36 MATERIALS SCIENCE↗

Opto-Electronic Oscillator Stabilized By A Hyperfine Atomic Transition

Opto-electronic oscillator (OEO) is a closed-loop system with part of the loop is implemented by an optical beam, and the rest by RF circuitry. The technological advantage of this approach over traditional all-RF loops in the gigahertz range comes from the that frequency filtering can be done far more efficiently in the optical range with compact, low power, and have superior stability. In this work, we report our preliminary results on using the phenomenon of coherent population trapping in (87) Rb vapor as an optical filter. Such a filter allows us to stabilize the OEO at the hyperfine splitting frequency of rubidium, thus implementing a novel type of frequency standard.

OEO (OPTO-ELECTRONIC OSCILLATORS)↗

Atomically Flat Surfaces Developed for Improved Semiconductor Devices

New wide bandgap semiconductor materials are being developed to meet the diverse high temperature, -power, and -frequency demands of the aerospace industry. Two of the most promising emerging materials are silicon carbide (SiC) for high-temperature and high power applications and gallium nitride (GaN) for high-frequency and optical (blue-light-emitting diodes and lasers) applications. This past year Glenn scientists implemented a NASA-patented crystal growth process for producing arrays of device-size mesas whose tops are atomically flat (i.e., step-free). It is expected that these mesas can be used for fabricating SiC and GaN devices with major improvements in performance and lifetime. The promising new SiC and GaN devices are fabricated in thin-crystal films (known as epi films) that are grown on commercial single-crystal SiC wafers. At this time, no commercial GaN wafers exist. Crystal defects, known as screw defects and micropipes, that are present in the commercial SiC wafers propagate into the epi films and degrade the performance and lifetime of subsequently fabricated devices. The new technology isolates the screw defects in a small percentage of small device-size mesas on the surface of commercial SiC wafers. This enables atomically flat surfaces to be grown on the remaining defect-free mesas. We believe that the atomically flat mesas can also be used to grow GaN epi films with a much lower defect density than in the GaN epi films currently being grown. Much improved devices are expected from these improved low-defect epi films. Surface-sensitive SiC devices such as Schottky diodes and field effect transistors should benefit from atomically flat substrates. Also, we believe that the atomically flat SiC surface will be an ideal surface on which to fabricate nanoscale sensors and devices. The process for achieving atomically flat surfaces is illustrated. The surface steps present on the "as-received" commercial SiC wafer is also illustrated. because of the small tilt angle between the crystal "basal" plane and the polished wafer surface. These steps are used in normal SiC epi film growth in a process known as stepflow growth to produce material for device fabrication. In the new process, the first step is to etch an array of mesas on the SiC wafer top surface. Then, epi film growth is carried out in the step flow fashion until all steps have grown themselves out of existence on each defect-free mesa. If the size of the mesas is sufficiently small (about 0.1 by 0.1 mm), then only a small percentage of the mesas will contain an undesired screw defect. Mesas with screw defects supply steps during the growth process, allowing a rough surface with unwanted hillocks to form on the mesa. The improvement in SiC epi surface morphology achievable with the new technology is shown. An atomic force microscope image of a typical SiC commercial epilayer surface is also shown. A similar image of an SiC atomically flat epi surface grown in a Glenn laboratory is given. With the current screw defect density of commercial wafers (about 5000 defects/cm2), the yield of atomically free 0.1 by 0.l mm mesas is expected to be about 90 percent. This is large enough for many types of electronic and optical devices. The implementation of this new technology was recently published in Applied Physics Letters. This work was initially carried out in-house under a Director's Discretionary Fund project and is currently being further developed under the Information Technology Base Program.

Powell, J. Anthony↗

Giant Nonlinear Optical Response via Coherent Stacking of In-Plane Ferroelectric Layers

Thin ferroelectric materials hold great promise for compact nonvolatile memory and nonlinear optical and optoelectronic devices. Herein, an ultrathin in-plane ferroelectric material that exhibits a giant nonlinear optical effect, group-IV monochalcogenide SnSe, is reported. Nanometer-scale ferroelectric domains with ≈90°/270° twin boundaries or ≈180° domain walls are revealed in physical-vapor-deposited SnSe by lateral piezoresponse force microscopy. Atomic structure characterization reveals both parallel and antiparallel stacking of neighboring van der Waals ferroelectric layers, leading to ferroelectric or antiferroelectric ordering. Ferroelectric domains exhibit giant nonlinear optical activity due to coherent enhancement of second-harmonic fields and the as-resulted second-harmonic generation was observed to be 100 times more intense than monolayer WS 2 . This work demonstrates in-plane ferroelectric ordering and giant nonlinear optical activity in SnSe, which paves the way for applications in on-chip nonlinear optical components and nonvolatile memory devices.

36 MATERIALS SCIENCE↗

All-optical seeding of a light-induced phase transition with correlated disorder

Ultrafast manipulation of vibrational coherence is an emergent route to control the structure of solids. However, this strategy can only induce long-range correlations and cannot modify atomic structure locally, which is required in many technologically-relevant phase transitions. Here, we demonstrate that ultrafast lasers can generate incoherent structural fluctuations which are more efficient for material control than coherent vibrations, extending optical control to a wider range of materials. We observe that local, non-equilibrium lattice distortions generated by a weak laser pulse reduce the energy barrier to switch between insulating and metallic states in vanadium dioxide by 6%. In conclusion, seeding inhomogeneous structural-fluctuations presents an alternative, more energy efficient, route for controlling materials that may be applicable to all solids, including those used in data and energy storage devices.

36 MATERIALS SCIENCE↗

Wavelength conversion for single-photon polarization qubits through continuous-variable quantum teleportation

A quantum internet connects remote quantum processors that need to interact and exchange quantum signals over a long distance through photonic channels. However, these quantum nodes operate at the wavelength ranges unsuitable for long-distance transmission. Therefore, quantum wavelength conversion to telecom bands is crucial for long-distance quantum networks based on optical fiber. Here, we propose wavelength conversion devices for single-photon polarization qubits using continuous-variable quantum teleportation that can efficiently convert qubits between near-infrared (780–795 nm suitable for interacting with atomic quantum nodes) and telecom wavelength (1300–1500 nm suitable for long-distance transmission). The teleportation uses entangled photon fields (i.e., nondegenerate two-mode squeezed state) that can be generated by four-wave mixing in a rubidium atomic gas using a diamond configuration of atomic transitions. The entangled fields can be emitted in two orthogonal polarizations with locked relative phase, making them especially suitable for interfacing with single- photon polarization qubits. Furthermore, our work may pave the way for the realization of long-distance quantum networks.

74 ATOMIC AND MOLECULAR PHYSICS↗

The persistence of memory in ionic conduction probed by nonlinear optics

Predicting practical rates of transport in condensed phases enables the rational design of materials, devices and processes. This is especially critical to developing low-carbon energy technologies such as rechargeable batteries. For ionic conduction, the collective mechanisms, variation of conductivity with timescales and confinement, and ambiguity in the phononic origin of translation, call for a direct probe of the fundamental steps of ionic diffusion: ion hops. However, such hops are rare-event large-amplitude translations, and are challenging to excite and detect. Here we use single-cycle terahertz pumps to impulsively trigger ionic hopping in battery solid electrolytes. This is visualized by an induced transient birefringence, enabling direct probing of anisotropy in ionic hopping on the picosecond timescale. The relaxation of the transient signal measures the decay of orientational memory, and the production of entropy in diffusion. We extend experimental results using in silico transient birefringence to identify vibrational attempt frequencies for ion hopping. Using nonlinear optical methods, we probe ion transport at its fastest limit, distinguish correlated conduction mechanisms from a true random walk at the atomic scale, and demonstrate the connection between activated transport and the thermodynamics of information.

25 ENERGY STORAGE↗

Mixed excitonic nature in water-oxidized BiVO 4 surfaces with defects

BiVO 4 is a promising photocatalyst for efficient water oxidation, with surface reactivity determined by the structure of active catalytic sites. Surface oxidation in the presence of oxygen vacancies induces electron localization, suggesting an atomistic route to improve the charge transfer efficiency within the catalytic cycle. In this paper, we study the effect of oxygen vacancies on the electronic and optical properties at BiVO 4 surfaces upon water oxidation. We use density functional theory and many-body perturbation theory to explore the change in the electronic and quasiparticle energy levels and to evaluate the electron-hole coupling as a function of the underlying structure. Further we show that while the presence of defects alters the atomic structure and largely modifies the wave-function nature, leading to defect-localized states at the quasiparticle gap region, the optical excitations remain largely unchanged due to the substantial hybridization of defect and nondefect electron-hole transitions. Our findings suggest that defect-induced surface oxidation supports improved electron transport, both through bound and tunable electronic states and via a mixed nature of the optical transitions, expected to reduce electron-hole defect trapping.

36 MATERIALS SCIENCE↗

Ground-Based Testing of Replacement Thermal Control Materials for the Hubble Space Telescope

The mechanical and optical properties of the metallized Teflon FEP thermal control materials on the Hubble Space Telescope (HST) have degraded over the nearly seven years the telescope has been in orbit. Given the damage to the outer layer of the multi-layer insulation (MLI) that was apparent during the second servicing mission (SM2), the decision was made to replace the outer layer during subsequent servicing missions. A Failure Review Board was established to investigate the damage to the MLI and identify a replacement material. The replacement material had to meet the stringent thermal requirements of the spacecraft and maintain mechanical integrity for at least ten years. Ten candidate materials were selected and exposed to ten-year HST-equivalent doses of simulated orbital environments. Samples of the candidates were exposed sequentially to low and high energy electrons and protons, atomic oxygen, x-ray radiation, ultraviolet radiation and thermal cycling. Following the exposures, the mechanical integrity and optical properties of the candidates were investigated using Optical Microscopy, Scanning Electron Microscopy (SEM), a Laboratory Portable Spectroreflectometer (LPSR) and a Lambda 9 Spectroreflectometer. Based on the results of these simulations and analyses, the Failure Review Board selected a replacement material and two alternates that showed the highest likelihood of providing the requisite thermal properties and surviving for ten years in orbit.

Townsend, Jacqueline A.↗

Secured Optical Communications Using Quantum Entangled Two-Photon Transparency Modulation

A system and method is disclosed wherein optical signals are coded in a transmitter by tuning or modulating the interbeam delay time (which modulates the fourth-order coherence) between pairs of entangled photons. The photon pairs are either absorbed or not absorbed (transparent) by an atomic or molecular fluorescer in a receiver, depending on the inter-beam delay that is introduced in the entangled photon pairs. Upon the absorption, corresponding fluorescent optical emissions follow at a certain wavelength, which are then detected by a photon detector. The advantage of the disclosed system is that it eliminates a need of a coincidence counter to realize the entanglement-based secure optical communications because the absorber acts as a coincidence counter for entangled photon pairs.

Kojima, Jun↗

Evaluation and Selection of Replacement Thermal Control Materials for the Hubble Space Telescope

The mechanical and optical properties of the metallized Teflon(Registered Trademark) FEP thermal control materials on the Hubble Space Telescope (HST) have degraded over the nearly seven years the telescope has been in orbit. Given the damage to the outer layer of the multi-layer insulation (MLI) that was apparent during the second servicing mission (SM2), the decision was made to replace the outer layer during subsequent servicing missions. A Failure Review Board was established to investigate the damage to the MLI and identify a replacement material. The replacement material had to meet the stringent thermal requirements of the spacecraft and maintain structural integrity for at least ten years. Ten candidate materials were selected and exposed to ten-year HST-equivalent doses of simulated orbital environments. Samples of the candidates were exposed sequentially to low and high energy electrons and protons, atomic oxygen, x-ray radiation, ultraviolet radiation and thermal cycling. Following the exposures, the mechanical integrity and optical properties of the candidates were investigated using Optical Microscopy, Scanning Electron Microscopy (SEM), and a Laboratory Portable Spectroreflectometer (LPSR). Based on the results of these simulations and analyses, the FRB selected a replacement material and two alternates that showed the highest likelihood of providing the requisite thermal properties and surviving for ten years in orbit.q

Townsend, Jacqueline A.↗

The atomic gas sequence and mass–metallicity relation from dwarfs to massive galaxies

Galaxy scaling relations provide insights into the processes that drive galaxy evolution. The extension of these scaling relations into the dwarf galaxy regime is of particular interest. This is because dwarf galaxies represent a crucial stage in galaxy evolution, and understanding them could also shed light on their role in reionizing the early Universe. There is currently no consensus on the processes that dominate the evolution of dwarfs. In this work, we constrain the atomic gas sequence (stellar mass versus atomic gas fraction) and mass–metallicity relation (stellar mass versus gas-phase metallicity) from dwarf (⁠10 6.5 M ⊙ ⁠) to massive (⁠10 11.5 M ⊙ ) galaxies in the local Universe. The combined optical and 21-cm spectroscopic observations of the Dark Energy Spectroscopic Instrument and Arecibo Legacy Fast ALFA surveys allow us to constrain both scaling relations simultaneously. We find a slope change of the atomic gas sequence at a stellar mass of ~10 9 M ⊙ ⁠. We also find that the shape and scatter of the atomic gas sequence and mass–metallicity relation are strongly linked for both dwarfs and more massive galaxies. Consequently, the low-mass slope change of the atomic gas sequence is imprinted onto the mass–metallicity relation of dwarf galaxies. The mass scale of the measured slope change is consistent with a predicted escape velocity threshold below which low-mass galaxies experience significant supernova-driven gas loss, as well as with a reduction in cold gas accretion onto more massive galaxies.

79 ASTRONOMY AND ASTROPHYSICS↗

Accelerating Quantum Materials Development with Advances in Transmission Electron Microscopy

Quantum materials are driving a technology revolution in sensing, communication, and computing, while simultaneously testing many core theories of the past century. Materials such as topological insulators, complex oxides, superconductors, quantum dots, color center-hosting semiconductors, and other types of strongly correlated materials can exhibit exotic properties such as edge conductivity, multiferroicity, magnetoresistance, superconductivity, single photon emission, and optical-spin locking. These emergent properties arise and depend strongly on the material’s detailed atomic-scale structure, including atomic defects, dopants, and lattice stacking. In this review, we describe how progress in the field of electron microscopy (EM), including in situ and in operando EM, can accelerate advances in quantum materials and quantum excitations. We begin by describing fundamental EM principles and operation modes. We then discuss various EM methods such as (i) EM spectroscopies, including electron energy loss spectroscopy (EELS), cathodoluminescence (CL), and electron energy gain spectroscopy (EEGS); (ii) four-dimensional scanning transmission electron microscopy (4D-STEM); (iii) dynamic and ultrafast EM (UEM); (iv) complementary ultrafast spectroscopies (UED, XFEL); and (v) atomic electron tomography (AET). We describe how these methods could inform structure–function relations in quantum materials down to the picometer scale and femtosecond time resolution, and how they enable precision positioning of atomic defects and high-resolution manipulation of quantum materials. For each method, we also describe existing limitations to solve open quantum mechanical questions, and how they might be addressed to accelerate progress. Among numerous notable results, our review highlights how EM is enabling identification of the 3D structure of quantum defects; measuring reversible and metastable dynamics of quantum excitations; mapping exciton states and single photon emission; measuring nanoscale thermal transport and coupled excitation dynamics; and measuring the internal electric field and charge density distribution of quantum heterointerfaces- all at the quantum materials’ intrinsic atomic and near atomic-length scale. Finally, we conclude by describing open challenges for the future, including achieving stable sample holders for ultralow temperature (below 10K) atomic-scale spatial resolution, stable spectrometers that enable meV energy resolution, and high-resolution, dynamic mapping of magnetic and spin fields. With atomic manipulation and ultrafast characterization enabled by EM, quantum materials will be poised to integrate into many of the sustainable and energy-efficient technologies needed for the 21st century.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Hybrid Molecular Beam Epitaxy for Single-Crystalline Oxide Membranes with Binary Oxide Sacrificial Layers

The advancement in thin-film exfoliation for synthesizing oxide membranes has led to possibilities for creating artificially assembled heterostructures with structurally and chemically incompatible materials. The sacrificial layer method is a promising approach to exfoliate as-grown films from a compatible material system, allowing for their integration with dissimilar materials. Nonetheless, the conventional sacrificial layers often possess an intricate stoichiometry, thereby constraining their practicality and adaptability, particularly when considering techniques such as molecular beam epitaxy (MBE). This is where easy-to-grow binary alkaline-earth-metal oxides with a rock salt crystal structure are useful. These oxides, which include (Mg, Ca, Sr, Ba)O, can be used as a sacrificial layer covering a much broader range of lattice parameters compared to conventional sacrificial layers and are easily dissolvable in deionized water. In this study, we show the epitaxial growth of the single-crystalline perovskite SrTiO 3 (STO) on sacrificial layers consisting of crystalline SrO, BaO, and Ba 1–x Ca x O films, employing a hybrid MBE method. Our results highlight the rapid (≤5 min) dissolution of the sacrificial layer when immersed in deionized water, facilitating the fabrication of millimeter-sized STO membranes. Using high-resolution X-ray diffraction, atomic-force microscopy, scanning transmission electron microscopy, impedance spectroscopy, and scattering-type near-field optical microscopy (SNOM), we demonstrate single-crystalline STO membranes with bulk-like intrinsic dielectric properties. The employment of alkaline earth metal oxides as sacrificial layers is likely to simplify membrane synthesis, particularly with MBE, thus expanding the research and application possibilities.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Ultrafast solvent-to-solute proton transfer mediated by intermolecular coherent vibrations

Ultrafast photoinduced excited-state proton transfer (ESPT) plays a crucial role in protecting biomolecules and functional materials from photodamage. However, the influence of solute-solvent interactions on ESPT dynamics remains under active investigation. Here, we present an ultrafast spectroscopic study of ESPT in the photobase 2-(2´-pyridyl)benzimidazole (PBI) in methanol. Ultrafast absorption spectroscopy, supported by quantum chemical calculations, reveals three distinct kinetic steps: (1) a 2.2 ps solvent-to-solute proton transfer, (2) subsequent nonradiative relaxation to the ground state within 31 ps, producing a vibrationally hot ensemble with substantial excess kinetic energy, and (3) equilibration as this energy dissipates into the surrounding solvent bath over 186 ps. Femtosecond-resolved dynamics exhibit oscillatory signals indicative of coherent wavepacket motion on the S 1 potential energy surface. A phase flip in the excited-state absorption maximum confirms this assignment. Fourier analysis resolves two dominant periods (∼117 fs and ∼340 fs), corresponding to in-plane and out-of-plane vibrational modes coupled between PBI and the hydrogen-bonded methanol molecule. The rapid dephasing ( < 300 fs) suggests that the nuclear wavefunction evolves on an anharmonic potential energy surface while traversing the ESPT reaction coordinate.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗