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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 991 records · Page 55
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Excited State Phenomena in Correlated Nanostructures: Transition Metal Oxide Clusters and Nanocrystals

The primary goal of our research program was to apply advanced computational techniques to predict electronic properties of molecular species. These include transition metal monoxide and dioxide clusters and negatively charged copper oxide clusters which are important systems for their utilization in a variety of technological applications. The enhanced electron-electron interactions inherent in these systems make it challenging to model their excited state properties within a parameter-free approach. The excited state properties in question include the interaction of light with these molecules which results in ejection of electrons from the system, or the absorption of light by the molecular system resulting in a molecule in a higher-energy state. Our overall goal was to investigate the impact of various computational and theoretical approaches on such electronic and optical excitations in these systems. Comparing several variants of theoretical approaches with available experimental data, and high-level quantum chemistry computations helped us identify the level of theory and approximations that are needed to achieve a reasonable balance between accuracy and computational demand.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

The Galactic Chemical Evolution of Chlorine

We measured {sup 35}Cl abundances in 52 M giants with metallicities in the range −0.5 < [Fe/H] < 0.12. Abundances and atmospheric parameters were derived using infrared spectra from CSHELL on the NASA Infrared Telescope Facility and from optical echelle spectra. We measured Cl abundances by fitting a H{sup 35}Cl molecular feature at 3.6985 μm with synthetic spectra. We also measured the abundances of O, Ca, Ti, and Fe using atomic absorption lines. We find that the [Cl/Fe] ratio for our stars agrees with chemical evolution models of Cl, and the [Cl/Ca] ratio is broadly consistent with the solar ratio over our metallicity range. Both indicate that Cl is primarily made in core-collapse supernovae with some contributions from Type Ia supernovae. We suggest that other potential nucleosynthesis processes, such as the ν-process, are not significant producers of Cl. Finally, we also find our Cl abundances are consistent with H ii and planetary nebular abundances at a given oxygen abundance, although there is scatter in the data.

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

Multi-frequency General Relativistic Radiation-hydrodynamics with M 1 Closure

We report on recent upgrades to our general relativistic radiation-magnetohydrodynamics code, Cosmos++ , which expands the two-moment, M 1 , radiation treatment from gray to multi-frequency transport, including Doppler and gravitational frequency shifts. The solver accommodates either photon (Bose–Einstein) or neutrino (Fermi–Dirac) statistical distribution functions with absorption, emission, and elastic scattering processes. An implicit scheme is implemented to simultaneously solve the primitive inversion problem together with the radiation–matter coupling source terms, providing stability over a broad range of opacities and optical depths where the interaction terms can be stiff. We discuss our formulations and numerical methods, and validate our methods against a wide variety of test problems spanning optically thin to thick regimes in flat, weakly curved, and strongly curved spacetimes.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2022

Semiconductor-dielectric-metal solar absorbers with high spectral selectivity

An ideal solar thermal absorber has a sharp transition between high and low absorptance at the wavelength where the blackbody emissive power begins to exceed the solar irradiance. However, most real selective absorbers have a fairly broad transition, leading to both solar absorption and thermal emission losses. Here, we model, fabricate, and characterize a highly selective semiconductor-dielectric-metal (Ga0.46In0.54As - MgF2 - Ag) solar absorber with an extremely sharp transition from high to low absorptance. The thin semiconductor serves as a selective filter, absorbing photons with wavelengths shorter than the bandgap and transmitting those with longer wavelengths. The highly reflective dielectric-metal rear mirror allows the structure to have very low emittance for longer wavelengths. These characteristics provide the absorber with a measured solar absorptance >91% below the bandgap wavelength and infrared emittance <5% at 100 degrees C above the bandgap wavelength. This transition wavelength can be tuned by modifying the semiconductor composition, and modeling indicates that the absorber's optical properties should be stable at high temperatures, making the structure a good candidate for unconcentrated to highly concentrated solar thermal energy conversion.

14 SOLAR ENERGY↗
DOE OSTI2024

Resonant Multiple-Phonon Absorption Causes Efficient Anti-Stokes Photoluminescence in CsPbBr 3 Nanocrystals

Lead halide perovskite nanocrystals, such as CsPbBr 3 , exhibit efficient photoluminescence (PL) up-conversion, also referred to as anti-Stokes photoluminescence (ASPL). This is a phenomenon where irradiating nanocrystals up to 100 meV below gap results in higher energy band edge emission. Most surprising is that ASPL efficiencies approach unity and involve single-photon interactions with multiple phonons. This is unexpected given the statistically disfavored nature of multiple-phonon absorption. Here, in this study, we report and rationalize near-unity anti-Stokes photoluminescence efficiencies in CsPbBr 3 nanocrystals and attribute them to resonant multiple-phonon absorption by polarons. The theory explains paradoxically large efficiencies for intrinsically disfavored, multiple-phonon-assisted ASPL in nanocrystals. Moreover, the developed microscopic mechanism has immediate and important implications for applications of ASPL toward condensed phase optical refrigeration.

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

Unsymmetric Pentacene- and Pentacenequinone-Fused Porphyrins: Understanding the Effect of Cross- and Linear-Conjugation

Unsymmetric pentacenequinone-fused (cross-conjugated) and pentacene-fused (linear-conjugated) porphyrins were designed and synthesized. The cross-conjugated (AM 1 –AM 3 ) and linear-conjugated (AM 5 –AM 7 ) porphyrins displayed strikingly different sets of optical and electronic properties, both of which are unusual and nontypical of porphyrins. MCD, DFT, and TDDFT calculations suggest that multiple charge transfer states exist in both π-conjugated systems, which contributes to the complex absorption and MCD spectra of these molecular systems. The general Gouterman’s four-orbital model used to explain porphyrin spectroscopy led to contradicting theoretical and experimental data, and is thus not applicable for these molecular systems. The “2 + 4” and “3 + 3” active spaces have been deduced and have proven effective to interpret the absorption and MCD spectra of the pentacenequinone-fused (cross-conjugated) and pentacene-fused (linear-conjugated) porphyrins, respectively. Spectroelectrochemistry of AM 5 –AM 7 revealed broad and intense IR absorptions in the range of 1500–2500 nm, illustrating the exceptional ability of these pentacene-fused systems to accommodate positive charges. A pronounced metal effect was observed for pentacene-fused porphyrins. While pentacene-fused Ni(II) porphyrin (AM 6 ) demonstrated an abnormal ability to stabilize pentacene with a half-life of >28.3 days, the half-life of the free base and Zn(II) counterparts were normal, similar to those of pentacene analogues. This work provides important and useful information on guiding new material designs.

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

A new μ -high energy resolution fluorescence detection microprobe imaging spectrometer at the Stanford Synchrotron Radiation Lightsource beamline 6-2

In this report we describe a new synchrotron X-ray Fluorescence (XRF) imaging instrument with an integrated High Energy Fluorescence Detection X-ray Absorption Spectroscopy (HERFD-XAS) spectrometer at the Stanford Synchrotron Radiation Lightsource at beamline 6-2. The X-ray beam size on the sample can be defined via a range of pinhole apertures or focusing optics. XRF imaging is performed using a continuous rapid scan system with sample stages covering a travel range of 250 × 200 mm 2 , allowing for multiple samples and/or large samples to be mounted. The HERFD spectrometer is a Johann-type with seven spherically bent 100 mm diameter crystals arranged on intersecting Rowland circles of 1 m diameter with a total solid angle of about 0.44% of 4π sr. A wide range of emission lines can be studied with the available Bragg angle range of ~64.5°–82.6°. With this instrument, elements in a sample can be rapidly mapped via XRF and then selected features targeted for HERFD-XAS analysis. Furthermore, utilizing the higher spectral resolution of HERFD for XRF imaging provides better separation of interfering emission lines, and it can be used to select a much narrower emission bandwidth, resulting in increased image contrast for imaging specific element species, i.e., sparse excitation energy XAS imaging. This combination of features and characteristics provides a highly adaptable and valuable tool in the study of a wide range of materials.

47 OTHER INSTRUMENTATION↗
DOE OSTI2024

Intercalation of quaternary ammonium cations as a key factor of electron storage in MoS2 thin films

Electrochemical intercalation of cations within two-dimensional transition metal dichalcogenides presents a promising route for tailoring their optoelectronic properties. We have now succeeded in modulating the optical properties of MoS2 thin films through electrochemical intercalation of quaternary ammonium cations. The spectroelectrochemical experiments conducted with varying sizes of the intercalant revealed the size-dependent stability of the intercalated MoS2 nanosheets. The observed absorption change of the exciton bands is reversible and arises from the storage of electrons in MoS2 nanosheets and the subsequent weakening of interlayer van der Waals interactions following cation intercalation. This structural change is evidenced by the emergence of A*1g out-of-plane Raman mode. Additionally, the photoelectron spectroscopy reveals the emergence of a lower binding energy component of Mo 3d and the shift in Fermi level to higher energies, confirming the presence of stored electrons in cation intercalated-MoS2. The underlying mechanism of intercalation-induced property modifications in MoS2 discussed in the present study is useful in developing strategies for energy conversion devices.

Physics↗
DOE OSTI2023

How do supernova remnants cool? – I. Morphology, optical emission lines, and shocks

ABSTRACT Supernovae (SNe) inject ∼1051 erg in the interstellar medium, thereby shocking and heating the gas. A substantial fraction of this energy is later lost via radiative cooling. We present a post-processing module for the flash code to calculate the cooling radiation from shock-heated gas using collisional excitation data from mappings v. When applying this tool to a simulated SN remnant (SNR), we find that most energy is emitted in the EUV. However, optical emission lines ([O iii], [N ii], [S ii], H α, H β) are usually best observable. Our shock detection scheme shows that [S ii] and [N ii] emissions arise from the thin shell surrounding the SNR, while [O iii], H $\rm \alpha$, and H $\rm \beta$ originate from the volume-filling hot gas inside the SNR bubble. We find that the optical emission lines are affected by the SNR’s complex structure and its projection on to the plane of the sky because the escaping line luminosity can be reduced by 10–80 per cent due to absorption along the line of sight. Additionally, the subtraction of contaminating background radiation is required for the correct classification of an SNR on the oxygen or sulphur BPT diagrams. The electron temperature and density obtained from our synthetic observations match well with the simulation but are very sensitive to the assumed metallicity.

Astronomy & Astrophysics↗
DOE OSTI2020

The Spectacular Ultraviolet Flash from the Peculiar Type Ia Supernova 2019yvq

Early observations of Type Ia supernovae (SNe Ia) provide essential clues for understanding the progenitor system that gave rise to the terminal thermonuclear explosion. Here, we present exquisite observations of SN 2019yvq, the second observed SN Ia, after iPTF 14atg, to display an early flash of emission in the ultraviolet (UV) and optical. Our analysis finds that SN 2019yvq was unusual, even when ignoring the initial flash, in that it was moderately underluminous for a SN Ia ($M_g \approx -18.5$ mag at peak) yet featured very high absorption velocities ($v \approx 15,0000$ km s -1 for Si II λ6355 at peak). We find that many of the observational features of SN 2019yvq, aside from the flash, can be explained if the explosive yield of radioactive 56 Ni is relatively low (we measure $M_{^{56}\mathrm{Ni}} = 0.31 \pm 0.05\,M_\odot$) and it and other iron-group elements are concentrated in the innermost layers of the ejecta. To explain both the UV/optical flash and peak properties of SN 2019yvq we consider four different models: interaction between the SN ejecta and a nondegenerate companion, extended clumps of 56 Ni in the outer ejecta, a double-detonation explosion, and the violent merger of two white dwarfs. Each of these models has shortcomings when compared to the observations; it is clear additional tuning is required to better match SN 2019yvq. In closing, we predict that the nebular spectra of SN 2019yvq will feature either H or He emission, if the ejecta collided with a companion, strong [Ca II] emission, if it was a double detonation, or narrow [O I] emission, if it was due to a violent merger.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2025

(NH 3 (CH 2 ) 7 NH 3 ) 2 Sn 3 I 10 , a Vacancy-Ordered Three-Dimensional Tin(II) Perovskite-Derived Semiconductor

Ordering vacancies in hybrid Sn(II) halide semiconductors provides a strategy for preventing uncontrolled oxidation and formation of mobile holes. In this study, we report the structure and optical and electronic properties of (NH 3 (CH 2 ) 7 NH 3 ) 2 Sn 3 I 10 , a vacancy-ordered perovskite derivative with three-dimensional inorganic connectivity. The crystal structure resembles that of a Dion–Jacobson layered perovskite derivative, but with [SnI 5 ] square pyramids bridging the layers. UV–vis diffuse reflectance spectroscopy reveals a sharp onset of light absorption at 1.86(1) eV with the photoluminescence emission maximum at 1.90(1) eV. However, the maximum excitation occurs from 3.42 to 3.81 eV (325 to 370 nm), revealing a significant Stokes shift of 1.3 eV. The electronic properties determined from dark and time-resolved microwave conductivity measurements reveal a minimum carrier mobility of 4.3 × 10 –2 cm 2 V –1 s –1 and a maximum carrier density of 5.96 × 10 16 cm –3 , a uniquely low value for a hybrid Sn(II) halide semiconductor. The transport behavior in combination with first-principles calculations of the electronic band structure and dielectric permittivity suggest polaron-mediated electronic transport, yet the photogenerated carriers have a fast and fluence-dependent nonradiative recombination rate, suggestive of localized “defect-like” states at the band edge. The observed photoluminescence is most consistent with single-ion-like behavior of an asymmetric Sn(II) environment. Together, these results suggest that defect ordering presents a strategy for the reduction of mobile charge carriers at equilibrium.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Strongly Correlated Exciton-Magnetization System for Optical Spin Pumping in CrBr 3 and CrI 3 .

Ferromagnetism in van der Waals systems, preserved down to a monolayer limit, attracted attention to a class of materials with general composition CrX 3 (X=I, Br, Cl), which are treated now as canonical two-dimensional ferromagnets. Their diverse magnetic properties, such as different easy axes or varying and controllable character of in-plane or interlayer ferromagnetic coupling, make them promising candidates for spintronic, photonic, optoelectronic, and other applications. Still, significantly different magneto-optical properties between the three materials, have been presenting a challenging puzzle for researchers over the last few years. Herewith, we demonstrate that despite similar structural and magnetic configurations, the coupling between excitons and magnetization is qualitatively different in CrBr 3 and CrI 3 films. Through a combination of the optical spin pumping experiments with the state-of-the-art theory describing bound excitonic states in the presence of magnetization, we concluded that the hole-magnetization coupling has the opposite sign in CrBr 3 and CrI 3 and also between the ground and excited exciton state. Consequently, we demonstrate efficient spin pumping capabilities in CrBr 3 driven by magnetization via spin-dependent absorption and unraveled the different origins of the magnetic hysteresis in CrBr 3 and CrI 3 are unraveled

36 MATERIALS SCIENCE↗
DOE OSTI2025

Synthesis, Crystal Structure, and Optical Properties of the Barium meta -Pertechnetate Ba[TcO 4 ] 2

High-quality single crystals of the colorless title compound Ba[ 99 TcO 4 ] 2 were prepared from radioactive, isotope-pure 99 TcO 2 by oxidation with H 2 O 2 in an aqueous ammonia solution and subsequent cation metathesis using an ion-exchange column. Single-crystal X-ray diffraction revealed Ba[TcO 4 ] 2 to crystallize isotopically to Ba[MnO 4 ] 2 in the orthorhombic space group Fddd with the lattice parameters a = 747.34(5) pm, b = 1244.08(7) pm, and c = 1511.23(9) pm for Z = 8. Its crystal structure features [BaO 12 ] 22- icosahedra surrounded by ten [TcO 4 ] - tetrahedra connected via two edges and eight corners. The optical properties of Ba[TcO 4 ] 2 investigated by UV-vis spectroscopy show the broad O 2- → Tc 7+ ligand-to-metal charge transfer (2p → 4d) process within these discrete [TcO 4 ]- anions at an absorption maximum of around 350 nm.

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

Generalised hyper-Ramsey spectroscopy of two-level atoms in an optically dense medium

The peculiarities of Ramsey resonance and its sensitivity to the light shift from an optically dense medium of cold atoms are investigated. Different composite pulse protocols for clock spectroscopy, including hyper-Ramsey, modified and generalised hyper-Ramsey schemes, are compared. Error signals change significantly due to the processes of absorption and dispersion in the atomic medium. The dependence of the position of the central fringe resonance with a residual uncompensated light shift of the atomic transition is studied with the attenuation of the radiation intensity in the medium taken into account. It is shown that using a combination of generalised hyper-Ramsey error signals allows one to suppress the sensitivity to the light shift for any length of the medium. (laser cooling of atoms)

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Insulation or Irradiance: Exploring Why Bifacial Photovoltaics Run Hot

Bifacial photovoltaics are predicted to become the dominant device architecture over the next couple of years, but their thermal performance is not yet well understood. In this study, we model the thermal effects of different backside lamination materials on the performance of bifacial PERC cells. Glass-glass laminated cells were found to operate hotter than equivalent glass-polymer backsheet packed cells. This was solely due to the increased absorption of rear side incident light.

bifacial↗
DOE OSTI2020

In situ temperature profile measurements with high-energy X-rays as a probe of optical floating zone crystal growth environment

The ability of optical floating zone (OFZ) furnaces to rapidly produce large single crystals of complex emerging materials has had a transformative effect on many scientific fields that require samples of this type. However, the crystal growth process within the OFZ furnace is not well understood owing to the challenges involved in monitoring the high-temperature crystal growth process. Novel beamline-compatible optical furnaces that approximate the inhomogeneous growth environment within an OFZ furnace have been fabricated and tested in high-energy synchrotron beamlines. In this paper, it is demonstrated that temperature profiles can be effectively extracted from powder diffraction data collected on polycrystalline ceramic rods heated at their tip. Furthermore, these measured temperature profiles can be accurately reproduced using a heat-transfer model that accounts for solid-state thermal conduction, partial sample lamp power absorption, convective air cooling and radiative cooling, allowing key thermal parameters such as thermal conductivity to be extracted from experimental data.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Outlook for active plasma spectroscopy with entangled two-photon absorption

Entangled two-photon absorption (ETPA) exhibits a quantum-enhanced two-photon absorption cross-section and a linear scaling with incident power that exceeds classical two-photon absorption (TPA) at low photon flux. Here, we assess the feasibility and applications of ETPA for active plasma spectroscopy. The ETPA-absorbed power for an Ar + species in a helicon plasma scenario is calculated to be as high as 0.6 nW cm −1 along the incident beam path for nondegenerate-entangled photon pairs that are near-resonant with an intermediate level. The ETPA absorption power exceeds classical TPA and Bremsstrahlung emission, a necessary condition for a feasible fluorescence measurement. Applications of ETPA plasma spectroscopy may include trace impurity detection, ground-state excitation, and continuous-wave pumping for high-bandwidth turbulence measurements. Possible benefits of plasma measurements are less harm to optical components with lower incident flux and reduced stray light that can contaminate optical diagnostics.

active plasma spectroscopy↗