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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 73 records · Page 4
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Super-Large-Scale Hierarchically Porous Films Based on Self-Assembled Eye-Like Air Pores for High-Performance Daytime Radiative Cooling

Metal-free polymer daytime radiative cooling coatings with hierarchical eye-like air pores are proposed and fabricated with a super-large-scale film-stretching method. The hierarchically porous film (HPF) can be further coated with polymethyl methacrylate (PMMA) micro-hemispheres, forming coated HPF (cHPF), which do not dramatically change the optical or thermal properties. The cHPF is slightly better with a lower solar absorptivity (2.4%) and a higher thermal emissivity over the atmospheric transparency window (90.1%). The low solar absorptivity is due to the strong scattering of the hierarchical eye-like air pores, while the molecular vibrations and the focusing effect of the PMMA micro-hemispheres contribute to the high emissivity. Further, an average mid-day temperature reduction of 7.92 °C is achieved relative to the air temperature, and the average cooling power reaches 116.0 W m -2 , which are much better than the cooling performances of the commercial cooling cushion. During the day, the cHPF-covered simulated building is up to 6.47 and 4.84 °C cooler than the ambient and the white painted counterpart, respectively. The film is durable and resistant to chemical etching, and very promising to use globally, especially in warm and tropical regions.

36 MATERIALS SCIENCE↗
DOE OSTI2020

SuperCam Calibration Targets: Design and Development

Abstract SuperCam is a highly integrated remote-sensing instrumental suite for NASA’s Mars 2020 mission. It consists of a co-aligned combination of Laser-Induced Breakdown Spectroscopy (LIBS), Time-Resolved Raman and Luminescence (TRR/L), Visible and Infrared Spectroscopy (VISIR), together with sound recording (MIC) and high-magnification imaging techniques (RMI). They provide information on the mineralogy, geochemistry and mineral context around the Perseverance Rover. The calibration of this complex suite is a major challenge. Not only does each technique require its own standards or references, their combination also introduces new requirements to obtain optimal scientific output. Elemental composition, molecular vibrational features, fluorescence, morphology and texture provide a full picture of the sample with spectral information that needs to be co-aligned, correlated, and individually calibrated. The resulting hardware includes different kinds of targets, each one covering different needs of the instrument. Standards for imaging calibration, geological samples for mineral identification and chemometric calculations or spectral references to calibrate and evaluate the health of the instrument, are all included in the SuperCam Calibration Target (SCCT). The system also includes a specifically designed assembly in which the samples are mounted. This hardware allows the targets to survive the harsh environmental conditions of the launch, cruise, landing and operation on Mars during the whole mission. Here we summarize the design, development, integration, verification and functional testing of the SCCT. This work includes some key results obtained to verify the scientific outcome of the SuperCam system.

Manrique, J. A. (ORCID:0000000220532819)↗
DOE OSTI2026

Self-supervised and multi-fidelity learning for extended predictive soil spectroscopy

Infrared spectroscopy is a cost-effective, non-destructive, and environmentally benign technology that is increasingly recognized as an important solution for meeting the global demand for soil data. While both near-infrared (NIR) and mid-infrared (MIR) diffuse reflectance spectroscopy enable rapid estimation of soil properties, they present a significant trade-off: NIR offers superior scalability and lower operational costs, whereas MIR provides higher analytical fidelity by capturing fundamental molecular vibrations. In this study, we propose a self-supervised, multi-fidelity learning framework designed to bridge this gap. Our approach leverages large-scale MIR spectral libraries to learn a compact, transferable latent representation, into which NIR spectra are subsequently aligned for downstream prediction. The workflow consists of pretraining a latent model on a large MIR library, adapting the representation using a smaller paired NIR–MIR dataset, and evaluating generalization on an independent external test set. Across a range of chemical and physical soil properties, we found that MIR-derived embeddings improved prediction accuracy relative to baseline models that used raw MIR inputs. Predictions derived from the spectrum conversion (NIR to MIR) task did not match the performance of the original MIR spectra but were similar or superior to predictive performance of NIR-only models, suggesting the unified spectral latent space can effectively leverage the larger and more diverse MIR dataset for prediction of soil properties not well represented in current NIR libraries.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Excited State Intramolecular Proton Transfer with Nuclear-Electronic Orbital Ehrenfest Dynamics

The recent development of the Ehrenfest dynamics approach in the nuclear-electronic orbital (NEO) framework provides a promising way to simulate coupled nuclear-electronic dynamics. Our previous study showed that the NEO-Ehrenfest approach with a semi- classical traveling proton basis method yields accurate predictions of molecular vibrational frequencies. In this work, we provide a more thorough analysis of the semiclassical traveling proton basis method to elucidate its validity and convergence behavior. We also conduct NEO-Ehrenfest dynamics simulations to study an excited state intramolecular proton transfer process. These simulations reveal that nuclear quantum effects influence the predictions of proton transfer reaction rates and kinetic isotope effects due to the intrinsic delocalized nature of the quantum nuclear wave function. This work illustrates the importance of nuclear quantum effects in coupled nuclear-electronic dynamical processes and shows that the NEO-Ehrenfest approach can be a powerful tool to provide insights and predictions for these processes.

Zhao, Luning↗
DOE OSTI2024

Spectroscopic Signatures of Phonon Character in Molecular Electron Spin Relaxation

Spin–lattice relaxation constitutes a key challenge for the development of quantum technologies, as it destroys superpositions in molecular quantum bits (qubits) and magnetic memory in single molecule magnets (SMMs). Gaining mechanistic insight into the spin relaxation process has proven challenging owing to a lack of spectroscopic observables and contradictions among theoretical models. Here, we use pulse electron paramagnetic resonance (EPR) to profile changes in spin relaxation rates (T 1 ) as a function of both temperature and magnetic field orientation, forming a two-dimensional data matrix. For randomly oriented powder samples, spin relaxation anisotropy changes dramatically with temperature, delineating multiple regimes of relaxation processes for each Cu(II) molecule studied. We show that traditional T 1 fitting approaches cannot reliably extract this information. Single-crystal T 1 anisotropy experiments reveal a surprising change in spin relaxation symmetry between these two regimes. We interpret this switch through the concept of a spin relaxation tensor, enabling discrimination between delocalized lattice phonons and localized molecular vibrations in the two relaxation regimes. Variable-temperature T 1 anisotropy thus provides a unique spectroscopic method to interrogate the character of nuclear motions causing spin relaxation and the loss of quantum information.

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

Operando Infrared Nanospectroscopy of the Silicon/Electrolyte Interface during Initial Stages of Solid-Electrolyte-Interphase Layer Formation

The solid electrolyte interphase (SEI) is a critical component in Li-ion batteries; however, its nanoscale structure and composition and unstable nature make it difficult to characterize and ascertain primary functional mechanisms. We use operando nanoscale Fourier transform infrared spectroscopy (nano-FTIR) with a broadband synchrotron IR source to study the SEI formation on a thin-film Si electrode at nanometer-scale spatial resolution as a function of time and voltage. By probing the Si/carbonate electrolyte interface through a 25 nm-thick amorphous Si window/electrode, we detect molecular vibrational modes within a 10s of nanometers region adjacent to the Si surface and observe that PF6 – anions react to form LiF at 0.5 V. Spatially resolved nano-FTIR spectra showcase subtle nanoscale heterogeneities in the initial solid/liquid interface and the resulting deposited LiF. With its nanoscale resolution and high chemical specificity, operando nano-FTIR provides unique insights into the dynamics and heterogeneous formation of SEIs and opens opportunities for connecting nanoscale interfacial properties to bulk performance metrics.

Dopilka, Andrew↗
DOE OSTI2026

Slow-Light Mid-IR Silicon Photonic Chips for NO 2 and CH 4 Gas Detection

A compact, chip-scale mid-infrared gas sensor is demonstrated, leveraging a two-dimensional photonic crystal waveguide (PCW) fabricated on a silicon-on-insulator (SOI) platform. The PCW comprises a hexagonal lattice with lattice constant a = 860 nm and hole radius r = 0.22a, incorporating a central line defect of reduced-radius holes (r s = 0.7r) to induce slow-light propagation near the photonic band edge with a group index of approximately 73, thereby enhancing light-matter interaction. The sensor operates at fundamental absorption wavelengths of 3.42 μm for nitrogen dioxide (NO 2 ) and 3.40 μm for methane (CH 4 ), utilizing the strongest molecular vibrational transitions for maximum sensitivity. Experimental validation was conducted using dynamically diluted gas mixtures generated by mass flow controllers, with signal acquisition performed by a liquid nitrogen-cooled InSb detector. For NO 2 , the sensor exhibited excellent linear response over 5–25 ppm (part per million) with coefficient of determination R 2 = 0.9934, achieving a detection limit of 210 ppb (part per billion)─representing the first reported silicon photonic-based NO 2 detection. For CH 4 , exposure to 25 ppm resulted in a 6.4% decrease in transmitted intensity, demonstrating multigas sensing capability. The CMOS-compatible fabrication process and compact 3 mm device footprint establish this SOI-PCW platform as a scalable, low-power solution for integrated mid-infrared gas sensing, with significant potential for environmental monitoring and industrial safety applications.

Crystals↗
DOE OSTI2024

Sub-100-fs energy transfer in coenzyme NADH is a coherent process assisted by a charge-transfer state

Excitation energy transfer (EET) is a key photoinduced process in biological chromophoric assemblies. Here we investigate the factors which can drive EET into efficient ultrafast sub-ps regimes. We demonstrate how a coherent transport of electronic population could facilitate this in water solvated NADH coenzyme and uncover the role of an intermediate dark charge-transfer state. High temporal resolution ultrafast optical spectroscopy gives a 54 ± 11 fs time constant for the EET process. Nonadiabatic quantum dynamical simulations computed through the time-evolution of multidimensional wavepackets suggest that the population transfer is mediated by photoexcited molecular vibrations due to strong coupling between the electronic states. The polar aqueous solvent environment leads to the active participation of a dark charge transfer state, accelerating the vibronically coherent EET process in favorably stacked conformers and solvent cavities. Our work demonstrates how the interplay of structural and environmental factors leads to diverse pathways for the EET process in flexible heterodimers and provides general insights relevant for coherent EET processes in stacked multichromophoric aggregates like DNA strands.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Ultrafast time-resolved x-ray absorption spectroscopy of ionized urea and its dimer through ab initio nonadiabatic dynamics

Investigating the early dynamics of chemical systems following ionization is essential for our understanding of radiation damage. However, experimental as well as theoretical investigations are very challenging due to the complex nature of these processes. Time-resolved x-ray absorption spectroscopy on a femtosecond timescale, in combination with appropriate simulations, is able to provide crucial insights into the ultrafast processes that occur upon ionization due to its element-specific probing nature. In this theoretical study, we investigate the ultrafast dynamics of valence-ionized states of urea and its dimer employing Tully's fewest switches surface hopping approach using Koopmans' theorem to describe the ionized system. We demonstrate that following valence ionization through a pump pulse, the time-resolved x-ray absorption spectra at the carbon, nitrogen, and oxygen K-edges reveal rich insights into the dynamics. Excited states of the ionized system give rise to time-delayed blueshifts in the x-ray absorption spectra as a result of electronic relaxation dynamics through nonadiabatic transitions. Moreover, our statistical analysis reveals specific structural dynamics in the molecule that induce time-dependent changes in the spectra. For the urea monomer, we elucidate the possibility to trace effects of specific molecular vibrations in the time-resolved x-ray absorption spectra. For the urea dimer, where ionization triggers a proton transfer reaction, we show how the x-ray absorption spectra can reveal specific details on the progress of proton transfer.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2025

Broadband coherent anti-Stokes Raman scattering (BCARS) microscopy for rapid, label-free biological imaging

Broadband coherent anti-Stokes Raman scattering (BCARS) microscopy is a label-free imaging approach that provides detailed chemical information at high spatial resolution in a sample through nonlinear, coherent excitation of molecular vibrations and detection of Raman spectra. While its utility for biological imaging has been demonstrated, many aspects of this technique must mature before it can be widely adopted. One of the areas of required improvement is imaging speed—most BCARS implementations involve sample rastering, which limits imaging speed. Beam scanning can provide faster BCARS imaging but presents some unique challenges. Here, we describe a beam-scanning BCARS microscopy system that improves spatial resolution twofold and imaging speed by fivefold over a previous beam-scanning implementation. These enhancements were enabled by an improvement in supercontinuum power and the use of a sCMOS camera for its high data transfer rate and low read noise. Implementation of the sCMOS camera required correction for the significant pixel-to-pixel background and photon response nonuniformity. Here, we report on the method that we implemented for calibrating and correcting the pixel-to-pixel differences in sCMOS camera noise.

Dixon, Jessica Z. [Georgia Institute of Technology↗
DOE OSTI2022

Enabling multiple intercavity polariton coherences by adding quantum confinement to cavity molecular polaritons

In this study, the “particle in a box” idea, which was broadly developed in semiconductor quantum dot research, was extended into mid-infrared (IR) cavity modes by applying lateral confinement in an optical cavity. The discrete cavity modes hybridized with molecular vibrational modes, resulting in a quartet of polariton states that can support multiple coherence states in the IR regime. We applied tailored pump pulse sequences to selectively prepare these coherences and verified the multi-coherence existence. The simulation based on Lindblad equation showed that because the quartet of polariton states resided in the same cavity, they were specifically robust toward decoherence caused by fluctuations in space. The multiple robust coherences paved the way for entangled states and coherent interactions between cavity polaritons, which would be critical for advancing polariton-based quantum information technology.

2D IR↗
DOE OSTI2020

Coupling of organic cation and inorganic lattice in methylammonium lead halide perovskites: Insights into a pressure-induced isostructural phase transition

Organic-inorganic hybrid metal-halide perovskite (OIHP) materials provide a tunable platform for engineering their optoelectronic properties. Although several high-pressure studies have been conducted from the OIHP family of single crystals and films, the exact nature of the dynamic coupling of the CH 3 NH 3 (MA) cation with the octahedral lattice framework and the mechanisms responsible for the structural phase transformation under pressure are not well captured. By combined photoluminescence (PL), synchrotron-based x-ray diffraction, and Raman-scattering studies as a function of pressure from methylammonium lead bromide (MAPbBr 3 ), we shed light on an isostructural phase transition due to the coupling of the MA cation and the PbBr 6 lattice through hydrogen bonding. The sharp discontinuities at ~ 1 GPa and ~ 3 GPa in the PL peak positions correlate with the structural changes observed in high-pressure XRD and Raman-scattering studies. The electronic band edge as a function of pressure is calculated within density-functional theory. The PL peak position, intensity and width of the excitonic peak show significant changes at 2 GPa, which corroborate the changes observed in high-pressure Raman-scattering studies. The frequencies of the lattice modes and the C-H/N-H bending and stretching modes of the MA cation show anomalous changes and other nuances at 2 GPa. The suppression of rotational and orientational disorder of the organic moiety is initiated at 2 GPa and the ordering is completed by 3.0 GPa, leading to an order-disorder type cubic II (Im$\overline{3}$) to orthorhombic ( Pnma ) phase transition. Along with the revelation of an isostructural transformation at 2 GPa, this paper highlights the impact of molecular vibrations on the electronic properties of MAPbBr 3 under pressure.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Isotopic Signatures of Lithium Carbonate and Lithium Hydroxide Monohydrate Measured Using Raman Spectroscopy

Lithium isotopic ratios have wide ranging applications as chemical signatures, including improved understanding of geochemical processes and battery development. Measurement of isotope ratios using optical spectroscopies would provide an alternative to traditional mass spectrometric methods, which are expensive and often limited to a chemical laboratory. In this work, Raman spectra of 7 Li 2 CO 3 , 6 Li 2 CO 3 , 7 LiOH*H 2 O and 6 LiOH*H 2 O have been measured to determine the effect of lithium isotope substitution on the Raman molecular vibrations. Thirteen peaks were observed in the spectrum of lithium carbonate, with discernable isotopic shifts occurring in eleven of the thirteen vibrations, two of which have not been previously reported in the literature. The spectrum of lithium hydroxide monohydrate contained nine peaks, with discernable isotopic shifts occurring in eight of the nine vibrations, four of which have not been previously reported in the literature. The Raman spectral data reported here for lithium carbonate and lithium hydroxide monohydrate are in agreement with the previously reported works in the literature, in which the Raman active modes of these molecules were first identified and assigned. However, due to the stability and resolution of the detection system used in this work, isotopic shifts with a magnitude less than one wavenumber have been identified. Principal Component Regression was used to evaluate the sensitivity to isotopic content of small Raman peak shifts in Li 2 CO 3 and indicates differences greater than 2 atom-% could be reliably determined. These measurements add to the body of work on lithium isotope Raman spectroscopy for these two compounds and increases the number of Raman bands which could be used for lithium isotope content analysis.

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

Hyperspectral acquisition with ScanImage at the single pixel level: application to time domain coherent Raman imaging

We present a comprehensive strategy and its practical implementation using the commercial ScanImage software platform to perform hyperspectral point scanning microscopy when a fast time-dependent signal varies at each pixel level. In the proposed acquisition scheme, the scan along the X-axis is slowed down while the data acquisition is maintained at a high pace to enable the rapid acquisition of the time-dependent signal at each pixel level. The ScanImage generated raw 2D images have a very asymmetric aspect ratio between X and Y, the X axis encoding both for space and time acquisition. The results are X-axis macro-pixel where the associated time-dependent signal is sampled to provide hyperspectral information. We exemplified the proposed hyperspectral scheme in the context of time-domain coherent Raman imaging, where a pump pulse impulsively excites molecular vibrations that are subsequently probed by a time-delayed probe pulse. In this case, the time-dependent signal is a fast acousto-optics delay line that can scan a delay of 4.5ps in 25 μ s at each pixel level. With this acquisition scheme, we demonstrate ultra-fast hyperspectral vibrational imaging in the low frequency range [10 cm −1 , 150 cm −1 ] over a 500 μm field of view (64 x 64 pixels) in 130ms (∼ 7.5 frames/s). The proposed acquisition scheme can be readily extended to other applications requiring the acquisition of a fast-evolving signal at each pixel level.

Metais, Samuel↗
DOE OSTI2021

Enskog Transport Calculations with Magpie

he revised Enskog theory for mixtures has been implemented, as a library, in the LANL institutional thermochemical code Magpie. This report provides the necessary physical background and several representative examples of transport calculations with this library. The particular attention is paid to how the contributions of non-translational degrees of freedom (molecular vibrations, rotations, electronic excitations) to the energy transport can be consistently accounted for via the so called Eucken correction.

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

Quantum Computing for Energy-Related Applications

Growing interest in quantum computing and simulations have created opportunities for its deployment to improve processes pertaining to energy production, distribution, and consumption. While quantum computing is considered as a paradigm shift in our basic understanding of physical computation, effective implementation of quantum computing in energy applications also depends on progress and development in the dimensions of both quantum computing hardware and quantum computing algorithms. To fully address the status and future challenges of quantum information science (QIS) applied within the energy sector, in this presentation, we firstly summarize recent advancements on the applications of quantum computing to energy infrastructure and materials, complex energy system processes, advanced manufacturing, and energy system security. Then, we will demonstrate the results of quantum computing both on a simulator and a quantum device accessing from OLCF. Our first example is to use the variational quantum eigensolver (VQE) with a unitary coupled cluster with singles and doubles (UCCSD) ansatz to simulate a series of LixHyq molecules (q=-1, 0, +1). The obtained results showed that the quantum computing VQE-UCCSD is comparable to classical CCSD for small systems like LiH with respect to full configuration interaction (FCI). Targeting on CO2 capture application, our second example is to use VQE to quantify molecular vibrational energies and reaction pathways between CO2 and a simplified amine-based solvent model—NH3 to form H2NCOOH. This research showcases quantum computing applications in the study of CO2 capture reactions.

Duan, Yuhua↗
DOE OSTI2024

HamLib: A library of Hamiltonians for benchmarking quantum algorithms and hardware

In order to characterize and benchmark computational hardware, software, and algorithms, it is essential to have many problem instances on-hand. This is no less true for quantum computation, where a large collection of real-world problem instances would allow for benchmarking studies that in turn help to improve both algorithms and hardware designs. To this end, here we present a large dataset of qubit-based quantum Hamiltonians. The dataset, called HamLib (for Hamiltonian Library), is freely available online and contains problem sizes ranging from 2 to 1000 qubits. HamLib includes problem instances of the Heisenberg model, Fermi-Hubbard model, Bose-Hubbard model, molecular electronic structure, molecular vibrational structure, MaxCut, Max- k -SAT, Max- k -Cut, QMaxCut, and the traveling salesperson problem. The goals of this effort are (a) to save researchers time by eliminating the need to prepare problem instances and map them to qubit representations, (b) to allow for more thorough tests of new algorithms and hardware, and (c) to allow for reproducibility and standardization across research studies.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2023

Probing Complex Chemical Processes at the Molecular Level with Vibrational Spectroscopy and X-ray Tools

Understanding the origins of structure and bonding at the molecular level in complex chemical systems spanning magnitudes in length and time is of paramount interest in physical chemistry. Here, we have coupled vibrational spectroscopy and X-ray based techniques with a series of microreactors and aerosol beams to tease out intricate and sometimes subtle interactions, such as hydrogen bonding, proton transfer, and noncovalent interactions. This allows for unraveling the self-assembly of arginine-oleic acid complexes in an aqueous solution and growth processes in a metal–organic framework. Terahertz and infrared spectroscopy provide an intimate view of the hydrogen-bond network and associated phase changes with temperature in neopentyl glycol. The hydrogen-bond network in aqueous glycerol aerosols and levels of protonation of nicotine in aqueous aerosols are visualized. Future directions in probing the hydrogen-bond networks in deep eutectic solvents and organic frameworks are described, and we suggest how X-ray scattering coupled to X-ray spectroscopy can offer insight into the reactivity of organic aerosols.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗