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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 253 records · Page 14
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Spontaneous Exciton Collapse in a Strongly Flattened Ellipsoidal InSb Quantum Dot

Abstract Electronic and excitonic states in an InSb strongly flattened ellipsoidal quantum dot (QD) with complicated dispersion law are theoretically investigated within the framework of the geometric adiabatic approximation in the strong, intermediate, and weak quantum confinement regimes. For the lower levels of the spectrum, the square root dependence of energy on QD sizes is revealed in the case of Kane’s dispersion law. The obtained results are compared to the case of a parabolic (standard) dispersion law of charge carriers. The possibility of the accidental exciton instability is revealed for the intermediate quantum confinement regime. For the weak quantum confinement regime, the motion of the exciton's center-of-gravity is quantized, which leads to the appearance of additional Coulomb-like sub-levels. It is revealed that in the case of the Kane dispersion law, the Coulomb levels shift into the depth of the forbidden band gap, moving away from the quantum confined level, whereas in the case of the parabolic dispersion law, the opposite picture is observed. The corresponding selection rules of quantum transitions for the interband absorption of light are obtained. New selection rules of quantum transitions between levels conditioned by 2D exciton center of mass vertical motion quantization in a QD are revealed. The absorption threshold behavior characteristics depending on the QDs geometrical sizes are also revealed.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2026

Proposed framework for applying squeezed light to multi-photon absorption plasma diagnostics

We propose a quantum-enhanced plasma diagnostic based on squeezed states of light. Squeezed light can exhibit super-Poissonian photon statistics, leading to enhanced multiphoton absorption cross-sections compared to classical light. This effect enables improved sensitivity for two-photon excitation of high-energy atomic transitions such as ground-state excitation, and results in increased absorbed power and fluorescence in a plasma. We consider two methods of generating squeezed states and evaluate their advantages and limitations in the context of plasma absorption diagnostics. By comparing with and extending previous theoretical work, we predict an enhancement of the absorption signal by up to seven orders of magnitude at low intensities (10 1 W/m 2 ), with diminishing enhancement persisting up to high intensities (10 10 W/m 2 ). These results suggest that squeezed-light sources offer a viable pathway toward quantum-enhanced plasma diagnostics.

imaging↗
DOE OSTI2023

Chapter 14: Surface plasmon resonance enhanced artificial photosynthesis of chemical fuels for energy storage

Nanostructured noble metals such as Au, Ag, and Cu have interesting optical properties because of the oscillation motions of their surface electrons upon strong coupling with light under resonance conditions. This resonant oscillation motion of conduction electrons refers to surface plasmon resonance (SPR) and localized SPR (LSPR) when localized near the surface of a nanoparticle. The extinction spectrum of a solution of plasmonic nanoparticles has tunable wavelength responses from UV to NIR due to strong light scattering and absorption which are highly sensitive to the permittivity of the nanoparticles, their sizes and shapes, and chemical environment. Strong light scattering due to the LSPR of plasmonic nanoparticles creates a strong localized and far-field intensity capable of enhancing light absorption characteristics of a chromophore near a plasmonic surface. Engineering the chromophores’ radiative decay dynamics can be done by 1) increasing its radiative decay rate to increase its photoluminescence intensity and 2) increasing its nonradiative decay rates associated to direct charge transfer to the metal surface. Such interesting photophysical properties of a chromophore can be extended to other light-absorbing materials such as semiconductor thin films and nanostructures. This plasmonic effect on the photophysics of a light-absorbing material can be theoretically and experimentally validated. The phenomenon has also been applied to advanced optoelectronic devices such as organic light-emitting diodes (OLED)1 and organic photovoltaics (OPV).2-4 The local field created by the SPR can provide an intense EM field to enhance photoluminescence emission of an organic chromophore5-8 and Raman scattering of an organic molecule, and single-molecule Raman9-10 can be detected on specially designed LSPR substrate. (Figure 1 on SPR for energy) Recent studies suggest that LSPR can be incorporated in light-harvesting and conversion systems to increase energy conversion in a solar cell and photoelectrochemical cell and chemical transformations of CO2 to chemical fuels.11-12 Plasmonic active metals naturally exhibit catalytic activities for electrochemical fuel conversion that can be enhanced by engineering their structures to form unique catalytic structures such as symmetry-broken Au-Cu Janus nanocrystals.13 These studies are critical to addressing the global challenges of energy14-15 and CO2 emission from nonrenewable sources such as coal, petroleum, and natural gas.16-17 Electrochemical systems comprised of unique photonic structures and functions that enable efficient and affordable energy harvesting/conversion/storage are highly desired for providing safe and environment-friendly energy sources. This chapter reviews our recent work of LSPR enabled photoelectrochemical water splitting and recent advances in LSPR-enabled CO2 reduction and photochemical reactions reported in the literature. Scientific and technical challenges of applying LSPR to enhance these energy conversion and storage systems are discussed at the conclusion of this chapter.

Pan, Shanlin↗
DOE OSTI2021

Light transport with weak angular dependence in fog

Random scattering and absorption of light by tiny particles in aerosols, like fog, reduce situational awareness and cause unacceptable down-time for critical systems or operations. Computationally efficient light transport models are desired for computational imaging to improve remote sensing capabilities in degraded optical environments. To this end, we have developed a model based on a weak angular dependence approximation to the Boltzmann or radiative transfer equation that appears to be applicable in both the moderate and highly scattering regimes, thereby covering the applicability domain of both the small angle and diffusion approximations. An analytic solution was derived and validated using experimental data acquired at the Sandia National Laboratory Fog Chamber facility. The evolution of the fog particle density and size distribution were measured and used to determine macroscopic absorption and scattering properties using Mie theory. A three-band (0.532, 1.55, and 9.68 µ m) transmissometer with lock-in amplifiers enabled changes in fog density of over an order of magnitude to be measured due to the increased transmission at higher wavelengths, covering both the moderate and highly scattering regimes. The meteorological optical range parameter is shown to be about 0.6 times the transport mean free path length, suggesting an improved physical interpretation of this parameter.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Photosynthetic adaptation to polar life: Energy balance, photoprotection and genetic redundancy

The persistent low temperature that characterize polar habitats combined with the requirement for light for all photoautotrophs creates a conundrum. The absorption of too much light at low temperature can cause an energy imbalance that decreases photosynthetic performance that has a negative impact on growth and can affect long-term survival. The goal of this review is to survey the mechanism(s) by which polar photoautotrophs maintain cellular energy balance, that is, photostasis to overcome the potential for cellular energy imbalance in their low temperature environments. Photopsychrophiles are photosynthetic organisms that are obligately adapted to low temperature (0⁰- 15 °C) but usually die at higher temperatures (≥20 °C). In contrast, photopsychrotolerant species can usually tolerate and survive a broad range of temperatures (5⁰- 40 °C). First, we summarize the basic concepts of excess excitation energy, energy balance, photoprotection and photostasis and their importance to survival in polar habitats. Second, we compare the photoprotective mechanisms that underlie photostasis and survival in aquatic cyanobacteria and green algae as well as terrestrial Antarctic and Arctic plants. We show that polar photopsychrophilic and photopsychrotolerant organisms attain energy balance at low temperature either through a regulated reduction in the efficiency of light absorption or through enhanced capacity to consume photosynthetic electrons by the induction of O 2 as an alternative electron acceptor. Finally, we compare the published genomes of three photopsychrophilic and one photopsychrotolerant alga with five mesophilic green algae including the model green alga, Chlamydomonas reinhardtii. We relate our genomic analyses to photoprotective mechanisms that contribute to the potential attainment of photostasis. Finally, we discuss how the observed genomic redundancy in photopsychrophilic genomes may confer energy balance, photoprotection and resilience to their harsh polar environment. Primary production in aquatic, Antarctic and Arctic environments is dependent on diverse algal and cyanobacterial communities. Although mosses and lichens dominate the Antarctic terrestrial landscape, only two extant angiosperms exist in the Antarctic. Furthermore, the identification of a single ‘molecular key’ to unravel adaptation of photopsychrophily and photopsychrotolerance remains elusive. Since these photoautotrophs represent excellent biomarkers to assess the impact of global warming on polar ecosystems, increased study of these polar photoautotrophs remains essential.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2020

Trifluoromethylated Phenanthroline Ligands Reduce Excited-State Distortion in Homoleptic Copper(I) Complexes

Herein, we report the synthesis and excited-state dynamics for a series of homoleptic copper(I) trifluoromethylated phenanthroline complexes with two, three, and four trifluoromethyl functional groups. Our analysis of the steady-state absorbance and emission, transient-absorption spectroscopy, and electronic-structure-theory calculations results enable in-depth analysis of the pseudo-Jahn–Teller distortion inhibition from increased steric hindrance of the trifluoromethyl functional group relative to the prototypical dimethyl phenanthroline complex. Surprisingly, our results demonstrate that the greatest degree of pseudo-Jahn–Teller distortion inhibition is achieved with trifluoromethylation of only the 2 and 9 positions by an unusual combination of steric hindrance and stabilization of a nondistorted 1 MLCT manifold observed by transient kinetic lifetimes and optimized excited-state structures. The intersystem-crossing (ISC) lifetime for the 2,9-bis(trifluoromethyl)-1,10-phenanthroline Cu(I) complex is 69 ps, while the triplet excited-state lifetime and emission quantum yield are 106 ns and 4 × 10 –3 , respectively. Further trifluoromethylation of the phenanthroline yields a greater σ bond inductive withdrawing force on the phenanthroline nitrogens, ultimately resulting in weaker coordination to the copper. Last, the surprising success of the 2,9-bis(trifluoromethyl)-1,10-phenanthroline Cu(I) complex by adjusting both ligand sterics and electronic properties outlines a new strategy for developing long-lived Cu(I) charge-transfer complexes.

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

Carrier and Phonon Dynamics in Multilayer WSe 2 Captured by Extreme Ultraviolet Transient Absorption Spectroscopy

Carrier and phonon dynamics in a multilayer WSe2 film are captured by extreme ultraviolet (XUV) transient absorption (TA) spectroscopy at the W N 6,7 , W O 2,3 , and Se M 4,5 edges (30–60 eV). After the broadband optical pump pulse, the XUV probe directly reports on occupations of optically excited holes and phonon-induced band renormalizations. Here, when compared with density functional theory calculations, XUV transient absorption due to holes is identified below the W O 3 edge whereas signals at the Se M 4,5 edges are dominated by phonon dynamics. Therein, 0.4 ps hole relaxation time, 1.5 ps carrier recombination time, and 1.7 ps phonon heating time are extracted. The acquisition of hole and phonon-induced signals in a single experiment can facilitate the investigation of the correlations between electron and phonon dynamics. Furthermore, the simultaneous observation of signals from different elements can be further extended to explore photochemical processes in multilayers and alloys, thereby providing key information for their applications in electronics, photocatalysts, and spintronics.

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

Differential absorption of circularly polarized light by a centrosymmetric crystal

Crystalline solids are governed by universal structure-property relationships derived from their crystal symmetry, leading to paradigmatic rules on what properties they can and cannot exhibit. A long-held structure-property relationship is that centrosymmetric crystals cannot differentially absorb circularly polarized light. In this study, we demonstrate the design, synthesis, and characterization of the centrosymmetric material Li 2 Co 3 (SeO 3 ) 4 , which violates this relationship not by defying symmetry-imposed selection rules but by invoking a photophysical process not previously characterized for crystalline solids. This process originates from an interference between linear dichroism and linear birefringence, referred to as LD-LB, and involves strong chiroptical signals that invert upon sample flipping. Here, in addition to enabling a chiroptical response under centrosymmetry, this process opens up photonic engineering opportunities based on crystalline solids.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Plasmon-Enhanced Greenhouse Selectivity for High-Temperature Solar Thermal Energy Conversion

The greenhouse effect arises when thermal radiation is forced to undergo absorption and re-emission many times before escaping, while sunlight transmits largely unimpeded. Although this effect is responsible for global warming, it is generally weak in solid-state materials because radiation can be easily overpowered by other modes of heat transfer. Here, we report on the use of infrared plasmonic nanoparticles to enhance the greenhouse effect in transparent mesoporous materials. Local surface plasmon resonances in transparent conducting oxide nanoparticles (TCO NPs) selectively shorten the mean free path of thermal photons while maintaining high solar transmittance. The addition of a small amount of TCO NPs (<0.1% by volume) nearly halves the heat losses at 700 °C. This leads to an experimentally demonstrated effective thermal emittance of ~0.17 at 700 °C, which is the lowest reported value to date, among all selective surfaces and transparent insulating materials measured at 650 °C or above. Furthermore, our results show that plasmon-enhanced greenhouse selectivity (PEGS) is a promising mechanism for spectral control of radiative heat transfer, and more specifically, for conversion of minimally concentrated sunlight into high-temperature heat.

14 SOLAR ENERGY↗
DOE OSTI2020

Light scattering study of highly absorptive, non-fractal, hematite aggregates

In this paper, we present measurements of the scattered light intensity by aerosolized hematite aggregate particles. The measurements were made at a wavelength of 532 nm in the scattering angle range from 0.32° to 157°. Hematite has high values of the real and imaginary parts of the refractive index m = n + iκ = 3 + i0.5 at the studied wavelength. Scanning electron micrographs (SEM) indicated that the particles were aggregates whereas the optical microscope pictures showed that the aerosol had a bimodal distribution with effective mean diameters of roughly 1 and 10 µm. This is consistent with the light scattering results which displayed two Guinier regimes. The aggregates were composed of smaller grains with an approximate size of 200 nm. Ultra Small-Angle X-ray Scattering (USAXS) indicate that the aggregates were uniform and non-fractal. Mie calculations for a sphere equivalent to the aggregate size were compared to the experimentally observed results. The observed results showed an enhanced backscattering, whereas the Mie calculations did not due to the large imaginary part of the refractive index. Hematite aggregates were simulated by assuming they were composed of spherical monomers inside a spherical volume. Then the light scattering was calculated using the T-matrix method for these simulated aggregates. The calculated results show an enhanced backscattering. We present a dimensional analysis to estimate the extent of multiple scattering within the aggregate and find a correlation between the average number of scattering events within the aggregate and the enhancement in the backscattering.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Near-infrared spectra and molar absorption coefficients of trivalent lanthanides dissolved in molten LiCl–KCl eutectic

Determining the concentration of the dissolved lanthanide species in LiCl–KCl eutectic salt is important to the development of pyrochemical reprocessing of used nuclear fuel. In this process, lanthanide fission products are found dissolved in the electrorefiner electrolyte in their trivalent oxidation state. The presence of dissolved trivalent lanthanides increases the liquidus temperature of the electrolyte mixture and can lead to the formation of insoluble oxide or oxychloride phases and must therefore be continuously monitored and controlled during the operation. Absorbance spectroscopy is a promising method for continuous measurement of the concentration of lanthanides and other elements dissolved in the electrolyte. The absorption of light by elements is linearly proportional to the concentration of the element for relatively dilute solutions according to the Beer-Lambert law. Although measurement of the absorption of ultraviolet and visible range light by lanthanides in LiCl–KCl eutectic molten salt have been explored previously, near infrared (NIR) absorption spectroscopy has received far less attention. It may, however, provide a better analytical signal when insoluble phases are present due to less Raleigh scattering compared to shorter wavelength radiation. Additionally, it may allow for concentration determination for certain elements using NIR absorption features where UV and visible range features are overlapping with features from other species. In this study, we report the UV–Vis–NIR spectra of the trivalent lanthanide chlorides of neodymium, samarium, and dysprosium in LiCl–KCl eutectic. Molar absorption coefficients are reported for analytically useful absorption maxima, with a focus on the molar absorption coefficients for NIR absorption maxima which have not been reported previously. Additionally, we observe a NIR-range absorption band of Nd3+ which was previously predicted but never experimentally observed. Here, we compare the calculated crystal field levels to the newly observed absorbance band and find them to be in good agreement with previous predictions.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2020

Insight into the Chemistry of PETN Under Shock Compression Through Ultrafast Broadband Mid-Infrared Absorption Spectroscopy

In this study, thin films of pentaerythritol tetranitrate (PETN) were shock compressed using the laser driven shock apparatus at Los Alamos National Laboratory (LANL). Two spectroscopic probes were available to this apparatus: visible white light transient absorption spectroscopy (VIS) from 400 to 700 nm and mid-infrared transient absorption spectroscopy (MIR) from 1150 to 3800 cm –1 . Important PETN vibrational modes are the symmetric and antisymmetric NO 2 stretches at 1280 and 1650 cm –1 , respectively, as well as CH stretches at ~2900 cm –1 . Shock strength was varied from approximately 3 to 55 GPa to span from the chemically unreactive regime to the regime in which fast chemical reaction took place on the 250 ps time scale of the measurements. VIS and MIR results suggest irreversible chemistry was induced in PETN at pressures above 30 GPa. At lower shock pressures, the spectroscopy showed minimal changes attributable to pressure induced effects. Under the higher-pressure reactive conditions, the frequency region at the antisymmetric NO 2 stretch mode had a significantly increased absorption while the region around the symmetric NO 2 stretch did not. No observable increased absorption occurred in the higher frequency regions where CH-, NH-, and OH- bond absorptions would be observed. A broad absorption appeared on the shoulder at the red-edge of the CO 2 vibrational band around 2200 cm –1 . In addition to the experiments, reactive molecular dynamics were carried out under equivalent shock conditions to correlate the evolution of the infrared spectrum to molecular processes. The simulations show results consistent to experiments up to 30 GPa but suggest that NO and NO 2 related features provided the strongest contributions to the shocked infrared changes. Proposed mechanisms for shocked PETN chemistry are analyzed as consistent or inconsistent with the data presented here. Our experimental data suggests C≡O or N 2 O bond formation, nitrite formation, and absence of significant hydroxyl or amine concentrations in the initial chemistry steps in PETN shocked above 30 GPa.

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

Ab initio theory of free-carrier absorption in semiconductors

The absorption of light by free carriers in semiconductors results in optical loss for all photon wavelengths. Since free-carrier absorption competes with optical transitions across the band gap, it also reduces the efficiency of optoelectronic devices such as solar cells because it does not generate electron-hole pairs. In this work, we develop a first-principles theory of free-carrier absorption taking into account both single-particle excitations and the collective Drude term, and we demonstrate its application to the case of doped Si. Here, we determine the free-carrier absorption coefficient as a function of carrier concentration and we obtain excellent agreement with experimental data. We identify the dominant processes that contribute to free-carrier absorption at various photon wavelengths, and analyze the results to evaluate the impact of this loss mechanism on the efficiency of Si-based optoelectronic devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Picoseconds-Limited Exciton Recombination in Metal–Organic Chalcogenides Hybrid Quantum Wells

Metal-organic species can be designed to self-assemble in large-scale, atomically defined, supramolecular architectures. Hybrid quantum wells, where inorganic two-dimensional (2D) planes are separated by organic ligands, are a particular example. The ligands effectively provide an intralayer confinement for charge carriers resulting in a 2D electronic structure, even in multilayered assemblies. Air-stable metal organic chalcogenides hybrid quantum wells have recently been found to host tightly bound 2D excitons with strong optical anisotropy in a bulk matrix. Here, we investigate the excited carrier dynamics in the prototypical metal organic chalcogenide [AgSePh] ∞ , disentangling three excitonic resonances by low temperature transient absorption spectroscopy. Our analysis suggests a complex relaxation cascade comprising ultrafast screening and renormalization, inter-exciton relaxation, and self-trapping of excitons within few picoseconds. Finally, the ps-decay provided by the self-trapping mechanism may be leveraged to unlock the material's potential for ultrafast optoelectronic applications.

2D excitons↗