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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 289 records · Page 16
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Tuning the Superconducting Transition Temperature of Co-sputtered Iridium and Platinum Films

A superconducting film with a tunable low transition temperature (Tc) is required in high-resolution Transition-Edge Sensor (TES) detectors, which have applications including dark matter detection, low threshold coherent elastic neutrino nucleus scattering measurement, and X-ray spectroscopy. We have been investigating a new approach to tune the Tc of superconducting thin films fabricated by co-sputtering Iridium and Platinum. The effects of Pt concentration and deposition parameters on the films' structural, electrical, and superconducting properties have been studied. AFM and XRD techniques and low temperature resistance measurements have been utilized for film characterization. By varying the Pt concentration and deposition parameters when co-sputtering, we have successfully achieved controllable tuning of Tc in the range of 30-200 mK. The experimental results demonstrate co-sputtering as a viable method for controlling the Tc of Ir-based thin films that can be applied to fabricating high-resolution TESs.

Yefremenko, V. G.↗
DOE OSTI2021

Revealing meso-structure dynamics in additive manufacturing of energy storage via operando coherent X-ray scattering

3D printing is an emerging technology for the fabrication of energy storage devices, offering advantages over traditional manufacturing methods. However, optimization and design of such devices requires an understanding of the meso-structure formation during the 3D printing process. This study utilizes operando coherent X-ray scattering, X-ray Photon Correlation Spectroscopy (XPCS), to study the spatiotemporally-resolved far-from-equilibrium dynamics during direct ink writing 3D printing. Here, Lithium Titanate (LTO) based ink is prepared and rheologically tested for its shear-thinning properties. Two-time intensity-intensity functions are calculated to be used in subsequent quantitative analysis, which allows for an overall characterization of the dynamics, description of an initial fast decorrelation and identification of sudden rearrangements of subdomains of the sample. The results show the dynamics to be anisotropic, spatiotemporally heterogenous and marked by distinct rearrangement events, all of which impact the electrochemical performance of energy storage devices. The studied 3D printing ink is used to fabricate electrodes which are then electrochemically tested, showing good performance in cycling and retaining structural integrity. This work furthers the understanding of the far-from-equilibrium material dynamics during 3D printing, giving quantitative characterization of this process, and highlights aspects of structure formation relevant to the electrochemical performance of the resultant energy storage device.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Developments in SRW Code and Sirepo Framework Supporting Simulation of Time-Dependent Coherent X-ray Scattering Experiments

Physical optics simulations for beamlines and experiments are essential for the effective use of synchrotron light source facilities such as NSLS-II at BNL. The SRW software package supports such source-to-detector simulations for coherent X-ray scattering and imaging experiments through its Python interface and Sirepo browser-based graphical user interface. This allows one to define custom sample models, assess the feasibility of an experiment, and estimate most appropriate beamline settings before using valuable beamtime. We discuss the recent use of general-purpose GPU resources and coherent mode decomposition algorithms in SRW to accelerate physical optics simulations with partially coherent X-rays. To illustrate these new capabilities, we describe simulations of typical time series of partially coherent scattering images used in X-ray Photon Correlation Spectroscopy (XPCS) experiments; aiming to characterize the nanoscale dynamics of a disordered sample, representing a solution of nanoparticles undergoing Brownian diffusion.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Towards Mitigating Electron Beam-Induced Damage in MOFs Using Low Dose Electron Microscopy for In-Situ Room-Temperature Measurements

Metal-Organic Frameworks (MOFs) have emerged as a versatile class of materials with applications in gas storage and separation, catalysis, and drug delivery [1]. Understanding their damage mechanisms in under various environmental conditions is crucial for optimizing performance and stability [2]. This study employs a combination of Length Structural Coherence (LSC) analysis in electron scattering and Electron Energy Loss Spectroscopy (EELS) to elucidate the damage mechanisms in two representative MOFs. MIL101(Fe), and MIL101(Cr). Here, the primary objective is to reveal structural and chemical changes that occur under electron beam irradiation in Scanning Transmission Electron Microscopy (STEM), both in the pristine state and during in-situ CO and CO 2 adsorption. By combining LSC in Radial Distribution Function (RDF) analysis with EELS, comprehensive insights into the nanoscale alterations are obtained and correlated to the electron dose rate.

dos Santos, Gabriel T. [Northwestern University, E↗
DOE OSTI2020

Quantum biology revisited

Photosynthesis is a highly optimized process from which valuable lessons can be learned about the operating principles in nature. Its primary steps involve energy transport operating near theoretical quantum limits in efficiency. Recently, extensive research was motivated by the hypothesis that nature used quantum coherences to direct energy transfer. This body of work, a cornerstone for the field of quantum biology, rests on the interpretation of small-amplitude oscillations in two-dimensional electronic spectra of photosynthetic complexes. This Review discusses recent work reexamining these claims and demonstrates that interexciton coherences are too short lived to have any functional significance in photosynthetic energy transfer. Instead, the observed long-lived coherences originate from impulsively excited vibrations, generally observed in femtosecond spectroscopy. These efforts, collectively, lead to a more detailed understanding of the quantum aspects of dissipation. Nature, rather than trying to avoid dissipation, exploits it via engineering of exciton-bath interaction to create efficient energy flow.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2026

TLS characterization using multilevel decay of a fixed-frequency transmon

Transmon qubits are a cornerstone of superconducting quantum computing platforms, yet their coherence times often exhibit temporal fluctuations that degrade processor performance. These variations are commonly attributed to shifts in the resonance frequencies of individual two-level systems (TLSs) near the qubit transition. In this study, we monitor the lifetimes of multiple energy levels of a fixed-frequency transmon and examine their temporal correlations. Our measurements reveal that one or more TLSs—detuned by more than 100 MHz from the qubit transition—can still significantly influence coherence. The proposed method provides a powerful tool for TLS spectroscopy without the need to tune the transmon frequency, either via a flux-tunable inductor or AC-Stark shifts.

Roy, Tanay [Fermilab] (ORCID:000000019442862X)↗
DOE OSTI2026

TLS characterization using multilevel decay of a fixed-frequency transmon

Transmon qubits are a cornerstone of superconducting quantum computing platforms, yet their coherence times often exhibit temporal fluctuations that degrade processor performance. These variations are commonly attributed to shifts in the resonance frequencies of individual two-level systems (TLSs) near the qubit transition. In this study, we monitor the lifetimes of multiple energy levels of a fixed-frequency transmon and examine their temporal correlations. Our measurements reveal that one or more TLSs—detuned by more than 100 MHz from the qubit transition—can still significantly influence coherence. The proposed method provides a powerful tool for TLS spectroscopy without the need to tune the transmon frequency, either via a flux-tunable inductor or AC-Stark shifts.

Roy, Tanay [Fermilab] (ORCID:000000019442862X)↗
NASA NTRS1986

Laser heterodyne spectrometer for helioseismology

The technique of laser heterodyne spectroscopy has been applied to the measurement of solar oscillations. Coherent mixing of solar radiation with the output of a frequency-stabilized CO2 laser permits the measurement of fully resolved profiles of solar absorption lines with high spectral purity and excellent frequency stability. This technique has been used to measure OH pure rotation lines in the infrared solar spectrum. Power spectra of these line frequency measurements show the well-known 5-min oscillations as well as significant velocity power at shorter periods.

Glenar, D. A.↗
DOE OSTI2024

Coherent Erbium Spin Defects in Colloidal Nanocrystal Hosts

We demonstrate nearly a microsecond of spin coherence in Er 3+ ions doped in cerium dioxide nanocrystal hosts, despite a large gyromagnetic ratio and nanometric proximity of the spin defect to the nanocrystal surface. The long spin coherence is enabled by reducing the dopant density below the instantaneous diffusion limit in a nuclear spin-free host material, reaching the limit of a single erbium spin defect per nanocrystal. We observe a large Orbach energy in a highly symmetric cubic site, further protecting the coherence in a qubit that would otherwise rapidly decohere. Spatially correlated electron spectroscopy measurements reveal the presence of Ce 3+ at the nanocrystal surface, which likely acts as extraneous paramagnetic spin noise. Even with these factors, defect-embedded nanocrystal hosts show tremendous promise for quantum sensing and quantum communication applications, with multiple avenues, including core-shell fabrication, redox tuning of oxygen vacancies, and organic surfactant modification, available to further enhance their spin coherence and functionality in the future.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2025

Correlating Superconducting Qubit Performance Losses to Sidewall Near-Field Scattering via Terahertz Nanophotonics

Elucidating dielectric losses, structural heterogeneity, and interface imperfections is critical for improving coherence in superconducting qubits. However, most diagnostics rely on destructive electron microscopy or low-throughput millikelvin quantum measurements. Here, we demonstrate noninvasive terahertz (THz) nano-imaging/-spectroscopy of encapsulated niobium transmon qubits, revealing sidewall near-field scattering that correlates with qubit coherence. We further employ a THz hyperspectral line scan to probe dielectric responses and field participation at Al junction interfaces. These findings highlight the promise of THz near-field methods as a high-throughput proxy characterization tool for guiding material selection and optimizing processing protocols to improve qubit and quantum circuit performance.

Kim, Richard H.J. [Ames Lab]↗
DOE OSTI2021

Broadband 2DES detection of vibrational coherence in the S x state of canthaxanthin

The nonadiabatic mechanism that mediates nonradiative decay of the bright S 2 state to the dark S 1 state of carotenoids involves population of a bridging intermediate state, S x , in several examples. The nature of S x remains to be determined definitively, but it has been recently suggested that S x corresponds to conformationally distorted molecules evolving along out-of-plane coordinates of the isoprenoid backbone near a low barrier between planar and distorted conformations on the S 2 potential surface. Here, the electronic and vibrational dynamics accompanying the formation of S x in toluene solutions of the ketocarotenoid canthaxanthin (CAN) are characterized with broadband two-dimensional electronic spectroscopy (2DES) with 7.8 fs excitation pulses and detection of the linear polarization components of the third-order nonlinear optical signal. A stimulated-emission cross peak in the 2DES spectrum accompanies the formation of S x in <20 fs following excitation of the main absorption band. S x is prepared instantaneously, however, with excitation of hot-band transitions associated with distorted conformations of CAN’s isoprenoid backbone in the low frequency onset of the main absorption band. Vibrational coherence oscillation maps and modulated anisotropy transients show that S x undergoes displacements from the Franck–Condon S 2 state along out-of-plane coordinates as it passes to the S 1 state. The results are consistent with the conclusion that CAN’s carbonyl-substituted β-ionone rings impart an intramolecular charge-transfer character that frictionally slows the passage from S x to S 1 compared to carotenoids lacking carbonyl substitution. Despite the longer lifetime, the S 1 state of CAN is formed with retention of vibrational coherence after passing through a conical intersection seam with the S x state.

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

Complete spectroscopy in the attosecond regime

Harnessing light waveforms at attosecond time scales provides information of the structure and dynamics of matter on it's natural time scales. For this reason attosecond metrology has been at the forefront of the optical sciences for more than a decade, and it represents the latest time-domain frontier of the quantum world. Attosecond light pulses are commonly generated using higher-order harmonic generation (HHG) , a process capable of generating XUV coherent pulses. In addition to generate attosecond pulses, HHG can be used to study the structure and dynamics of atoms and molecules by analyzing the spectral content of the XUV pulses. This approach is known as HHG spectroscopy and it provides a coherent, time-dependent approach to study structure and dynamics in the quantum world. In this proposal we will generate harmonics from two optical foci produced by a system of a two-dimensional spatial light modulator (SLM) and a lens. In the far eld the train of attosecond pulses will interfere creating harmonic-dependent fringes. The position of such fringes is a direct measurement of the relative phase between the two foci and they also carry information about the quantum state of the target atom or molecule. Therefore, by measuring the amplitude and relative phase of the emitted harmonics we will have access to both, the amplitude and phase of the dipole moments of the studied target. Because the two beams are completely indistinguishable from each other up to a few millimeters from the focus, both driving pulses share the exact beam path. So far we have measured a jitter of 700 zeptoseconds with a 12.5 attosecond resolution in the delay control of the two foci. These two time scales represent some of the best time controls ever achieved to date.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

Towards full surface Brillouin zone mapping by coherent multi-photon photoemission

Abstract We report a novel approach for coherent multi-photon photoemission in the entire Brillouin zone with infrared light that is readily implemented in a laboratory setting. We excite a solid state material, Ag(110), with intense femtosecond laser pulses to excite higher-order multi-photon photoemission; angle-resolved electron spectroscopic acquisition records photoemission at large in-plane momenta involving optical transitions from the occupied to unoccupied bands of the sample that otherwise might remain hidden by the photoemission horizon. We propose this as a complementary ultrafast method to time- and angle-resolved two-color, e.g. infrared pump and extreme ultraviolet probe, photoemission spectroscopy, with the advantage of being able to measure and control the coherent electron dynamics.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Hund's superconductor Li(Fe,Co)As

We combine transport, angle-resolved photoemission spectroscopy, and scanning tunneling spectroscopy to investigate several low-energy manifestations of the Hund's coupling in a canonical FeSC family Li(Fe,Co)As. We determine the doping dependence of the coherent-incoherent crossover temperature and the quasiparticle effective mass enhancement in the normal state. Furthermore, our tunneling spectroscopy result in the superconducting state supports the idea that superconductivity emerging from Hund's metal state displays a universal maximal superconducting gap vs transition temperature (2Δ max /k B T c ) value, which is independent of doping level and T c .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Light-induced electron spin qubit coherences in the purple bacteria reaction center protein

Photosynthetic reaction center proteins (RCs) provide ideal model systems for studying quantum entanglement between multiple spins, a quantum mechanical phenomenon wherein the properties of the entangled particles become inherently correlated. Following light-generated sequential electron transfer, RCs generate spin-correlated radical pairs (SCRPs), also referred to as entangled spin qubit (radical) pairs (SQPs). Understanding and controlling coherence mechanisms in SCRP/SQPs is important for realizing practical uses of electron spin qubits in quantum sensing applications. The bacterial RC (bRC) provides an experimental system for exploring quantum effects in the SCRP P 865 + Q A − , where P 865 , a special pair of bacteriochlorophylls, is the primary donor, and Q A is the primary quinone acceptor. In this study, we focus on understanding how local molecular environments and isotopic substitution, particularly deuteration, influence spin coherence times (T M ). Using high-frequency electron paramagnetic resonance (EPR) spectroscopy, we observed that the local environment surrounding P 865 and Q A plays a significant role in determining T M . Our findings show that while deuteration led to a modest increase in T M , particularly at low temperatures, but the effect was substantially smaller than predicted by classical nuclear spin diffusion alone. This result is in contrast to our previous study of the photosystem I (PSI) RC, where no increase in T M was observed upon deuteration. Theoretical modeling identified several methyl groups at key distances from the spin centers of both bRC and PSI, and methyl group tunneling at low temperatures has been previously suggested as a mechanism for enhanced spin decoherence. Additionally, our study revealed a strong dependence of spin coherence on the orientation of the external magnetic field, highlighting the influence of the protein microenvironment on spin dynamics. In conclusion, these results offer new insights for optimizing coherence times in quantum system design for quantum information science and sensing applications.

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

Encapsulation Enhances the Quantum Coherence of a Solid‐State Molecular Spin Qubit

Spins within molecules benefit from the atomistic control of synthetic chemistry for the realization of qubits. One advantage is that the quantum superpositions of the spin states encoding the qubit can be coherently manipulated using electromagnetic radiation. The main challenge is the fragility of these superpositions when qubits are to partake of solid-state devices. We address this issue with a supramolecular approach for protecting molecular spin qubits against decoherence. The molecular qubit [Cr(ox)3]3- has been encapsulated inside the diamagnetic triple-stranded helicate [Zn2L3]4+ (L is a bis-pyrazolylpyridine ligand). The quantum coherence of the protected qubit is then analyzed with pulsed EPR spectroscopy and compared with the unprotected qubit, both in solution and in the solid state. Crucially, the spin-spin relaxation in the solid state has been examined within diamagnetic crystal lattices of the isostructural ([Al(ox)3]@[Zn2L3])+ or [Al(ox)3]3- assemblies, respectively, doped with the Cr3+ qubit in two different (<10%) concentrations. The study unveils a surprising increase of the phase memory time of the qubit upon encapsulation only in the solid. Spin-lattice relaxation times also exhibit a significant enhancement, as established from inversion recovery pulse sequences and from slow relaxation of the magnetization of the protected qubit, not featured by the free qubit.

Swain, Abinash↗
DOE OSTI2020

Investigation of a Lignin-Based Deep Eutectic Solvent Using p -Hydroxybenzoic Acid for Efficient Woody Biomass Conversion

Deep eutectic solvents (DESs) are effective solvents for biomass conversion and have been proposed as alternatives to ionic liquids (ILs). In this paper, we first report an effective pretreatment of woody biomass using a novel hardwood lignin-based DES prepared from p -hydroxybenzoic acid (PB) and choline chloride (ChCl), which are used as the hydrogen bond donor and acceptor, respectively. The impacts of the ChCl-PB DES on structural properties and enzymatic hydrolysis of poplar wood were comprehensively evaluated. The performance of ChCl-PB DES was also compared with two other DESs with p -coumaric acid (PCA) and 4-hydroxybenzaldehyde (PHA) as the hydrogen bond donors, which have been successfully applied to herbaceous biomass conversion in previous studies. The results showed that hemicellulose and lignin were effectively fractionated during the proposed ChCl-PB DES pretreatment under a relatively mild temperature. The ChCl-PB DES pretreatment resulted in up to 69% of delignification, and the pretreated poplar residues had over 90% of glucose yield by a 72 h-enzymatic hydrolysis. Transformation of poplar biomass during the DES pretreatment was evaluated by gel permeation chromatography (GPC), two-dimensional heteronuclear single quantum coherence (2D-HSQC), and 31 P nuclear magnetic resonance (NMR) spectroscopies. The recovered lignin showed relatively high purity, narrow molecular weight distribution (PDI < 1.6), and relatively low molecular weight (~1400 g/mol for M w ). A sustainable process was achieved by recycling DES as well as the utilization of PB, which is a producible aromatic compound from hardwood lignin, for the proposed DES formation in the system. This study indicates that the proposed novel DES with a hardwood lignin-based PB compound is a promising pretreatment solvent to achieve an economically feasible biomass conversion process.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗