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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 595 records · Page 33
All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

Field-resolved observation of exciton coherence in a van der Waals magnet

The emergence of coherence among electronic quasiparticles underlies collective quantum phenomena from superconductivity to superradiance. In semiconductors, exciton coherence is generally thought to decay rapidly due to scattering and dephasing, limiting its persistence on ultrafast timescales. Here, in this work, we demonstrate a light-field-driven mechanism that creates and stabilizes exciton coherence in the layered antiferromagnet CrSBr. We directly record the coherent optical field emitted by excitons and track in real time how a deterministic phase, imprinted by the excitation laser, drives incoherent excitons to synchronize into a collective state. This ensemble remains phase coherent for more than 2 ps, whereas its resonance energy undergoes an ultrafast modulation mediated by spin and lattice interactions. The time-resolved field evolution indicates that the multiple peaks seen in conventional spectra originate from a single excitonic resonance subject to dynamic energy modulation. Our findings establish optical phase imprinting as a mechanism to control and sustain collective order in semiconducting magnets, bridging light-driven dynamics with excitonic and magnetic correlations in layered quantum materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Chapter 8: Time-Resolved Photoluminescence Characterization of Polycrystalline Thin-Film Solar Cells

This chapter describes some photoluminescence (PL) approaches to characterize thin film solar cells with emphasis on time-resolved methods. Spectral PL analysis is complementary and was recently reviewed. Since TRPL is not very commonly used in PV characterization, we consider interface and bulk recombination in the test structures and in devices, briefly describe charge-carrier transport and recombination microscopy, and finally, summarize and compare some CdTe, CdSeTe, CIGS, kesterite, and perovskite EO characteristics.

bulk recombination↗
DOE OSTI2018

Single-shot frequency-resolved optical gating for retrieving the pulse shape of high energy picosecond pulses

Accurate characterization of laser pulses used in experiments is a crucial step to the analysis of their results. In this paper, a novel single-shot frequency-resolved optical gating (FROG) device is described, one that incorporates a dispersive element which allows it to fully characterize pulses up to 25 ps in duration with a 65 fs per pixel temporal resolution. Hera, a newly developed phase retrieval routine based on memetic algorithms is implemented and shown to circumvent the stagnation problem that often occurs with traditional FROG analysis programs when they encounter a local minimum.

47 OTHER INSTRUMENTATION↗
DOE OSTI2019

Solvent-dependent complex reaction pathways of bromoform revealed by time-resolved X-ray solution scattering and X-ray transient absorption spectroscopy

The photochemical reaction pathways of CHBr3 in solution were unveiled using two complementary X-ray techniques, time-resolved X-ray solution scattering (TRXSS) and X-ray transient absorption spectroscopy, in a wide temporal range from 100 ps to tens of microseconds. By performing comparative measurements in protic (methanol) and aprotic (methylcyclohexane) solvents, we found that the reaction pathways depend significantly on the solvent properties. In methanol, the major photoproducts are CH3OCHBr2 and HBr generated by rapid solvolysis of iso-CHBr2-Br, an isomer of CHBr3. In contrast, in methylcyclohexane, iso-CHBr2-Br returns to CHBr3 without solvolysis. In both solvents, the formation of CHBr2 and Br is a competing reaction channel. From the structural analysis of TRXSS data, we determined the structures of key intermediate species, CH3OCHBr2 and iso-CHBr2-Br in methanol and methylcyclohexane, respectively, which are consistent with the structures from density functional theory calculations.

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

Low-pass spectral analysis of time-resolved serial femtosecond crystallography data

Low-pass spectral analysis (LPSA) is a recently developed dynamics retrieval algorithm showing excellent retrieval properties when applied to model data affected by extreme incompleteness and stochastic weighting. In this work, we apply LPSA to an experimental time-resolved serial femtosecond crystallography (TR-SFX) dataset from the membrane protein bacteriorhodopsin (bR) and analyze its parametric sensitivity. While most dynamical modes are contaminated by nonphysical high-frequency features, we identify two dominant modes, which are little affected by spurious frequencies. The dynamics retrieved using these modes shows an isomerization signal compatible with previous findings. We employ synthetic data with increasing timing uncertainty, increasing incompleteness level, pixel-dependent incompleteness, and photon counting errors to investigate the root cause of the high-frequency contamination of our TR-SFX modes. By testing a range of methods, we show that timing errors comparable to the dynamical periods to be retrieved produce a smearing of dynamical features, hampering dynamics retrieval, but with no introduction of spurious components in the solution, when convergence criteria are met. Using model data, we are able to attribute the high-frequency contamination of low-order dynamical modes to the high levels of noise present in the data. Finally, we propose a method to handle missing observations that produces a substantial dynamics retrieval improvement from synthetic data with a significant static component. Reprocessing of the bR TR-SFX data using the improved method yields dynamical movies with strong isomerization signals compatible with previous findings.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2020

Excited state dynamics of cis , cis -1,3-cyclooctadiene: UV pump VUV probe time-resolved photoelectron spectroscopy

We present UV pump, vacuum ultraviolet probe time-resolved photoelectron spectroscopy measurements of the excited state dynamics of cis,cis-1,3-cyclooctadiene. A 4.75 eV deep UV pump pulse launches a vibrational wave packet on the first electronically excited state, and the ensuing dynamics are probed via ionization using a 7.92 eV probe pulse. The experimental results indicate that the wave packet undergoes rapid internal conversion to the ground state in under 100 fs. Comparing the measurements with electronic structure and trajectory surface hopping calculations, we are able to interpret the features in the measured photoelectron spectra in terms of ionization to several states of the molecular cation.

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

Time-resolved broadband impulsive stimulated Brillouin scattering in single crystal hematite

Impulsive stimulated Brillouin scattering (ISBS) has emerged as a noninvasive means to determine the elastic properties of transparent materials. Here, we report on time-resolved broadband ISBS reflectivity measurements in single crystal hematite, α-Fe 2 O 3 . We found that the observed transient reflectivity changes are best described by the known strain propagation model (SPM) and introduced a simple derivation of the ISBS-SPM formula based on ray tracing, which accounts for the presence of the interface. Additionally, measurements at different incident probe beam angles illustrate a plausible approach toward determining the speed of sound in transparent media without any prior knowledge of their dielectric properties and vice versa.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Diverse simulations of time-resolved photoluminescence in thin-film solar cells: A SnO 2 /CdSe y Te 1-y case study

Time-resolved photoluminescence (TRPL) is widely used to measure carrier lifetime in thin-film solar cell absorbers. However, the injection dependence of data and frequent non-exponential decay shapes complicate the interpretation. Here, we develop a numerical model to simulate injection-dependent TRPL measurements in a SnO 2 /CdSe y Te 1-y case study solar cell structure, considering parameters of interest to researchers in industry and academia. Previous simulations have shown that, in low injection, excess electrons and holes injected by the laser pulse are rapidly separated in the electric field formed by the pn junction. As a result, at early times, the PL signal can decay faster than the Shockley-Read-Hall lifetime in the absorber bulk (t_bulk). Prior simulations have shown that the charge stored in the junction can slowly leak out to affect decays at late times. However, it has not been clear if and to what degree charge storage can affect the slopes extracted from TRPL decays - t_2 - commonly cited as the TRPL-measured lifetime. Here, we show that charge storage can, in some cases, result in t_2 values that substantially overestimate t_bulk. Previous simulations indicate that high injection conditions can screen the junction field and minimize charge separation. Here, we show that continued injection increases can drive down t_2 below t_bulk as radiative recombination becomes dominant. We catalog charge storage and radiative recombination impacts for a diverse set of material parameters and compare results to double-heterostructure models.

CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS,S↗
DOE OSTI2021

A time-resolved imaging system for the diagnosis of x-ray self-emission in high energy density physics experiments

A diagnostic capable of recording spatially and temporally resolved x-ray self-emission data was developed to characterize experiments on the MAGPIE pulsed-power generator. The diagnostic used two separate imaging systems: a pinhole imaging system with two-dimensional spatial resolution and a slit imaging system with one-dimensional spatial resolution. The two-dimensional imaging system imaged light onto the image plate. The one-dimensional imaging system imaged light onto the same piece of image plate and a linear array of silicon photodiodes. This design allowed the cross-comparison of different images, allowing a picture of the spatial and temporal distribution of x-ray self-emission to be established. The design was tested in a series of pulsed-power-driven magnetic-reconnection experiments.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2022

Growth of PdCoO 2 films with controlled termination by molecular-beam epitaxy and determination of their electronic structure by angle-resolved photoemission spectroscopy

Utilizing the powerful combination of molecular-beam epitaxy (MBE) and angle-resolved photoemission spectroscopy (ARPES), we produce and study the effect of different terminating layers on the electronic structure of the metallic delafossite PdCoO 2 . Attempts to introduce unpaired electrons and synthesize new antiferromagnetic metals akin to the isostructural compound PdCrO 2 have been made by replacing cobalt with iron in PdCoO 2 films grown by MBE. Using ARPES, we observe similar bulk bands in these PdCoO 2 films with Pd-, CoO 2 -, and FeO 2 -termination. Nevertheless, Pd- and CoO 2 -terminated films show a reduced intensity of surface states. Additionally, we are able to epitaxially stabilize PdFe x Co 1– x O 2 films that show an anomaly in the derivative of the electrical resistance with respect to temperature at 20 K, but do not display pronounced magnetic order.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Lattice and electronic structure of ScN observed by angle-resolved photoemission spectroscopy measurements

Scandium nitride (ScN) has recently attracted much attention for its potential applications in thermoelectric energy conversion, as a semiconductor in epitaxial metal/semiconductor superlattices, as a substrate for GaN growth, and alloying it with AlN for 5G technology. This study was undertaken to better understand its stoichiometry and electronic structure. ScN (100) single crystals 2 mm thick were grown on a single crystal tungsten (100) substrate by a physical vapor transport method over a temperature range of 1900–2000 °C and a pressure of 20 Torr. The core level spectra of Sc 2p 3/2,1/2 and N 1s were obtained by x-ray photoelectron spectroscopy (XPS). The XPS core levels were shifted by 1.1 eV toward higher values as the [Sc]:[N] ratio varied from 1.4 at 1900 °C to ~1.0 at 2000 °C due to the higher binding energies in stoichiometric ScN. Angle-resolved photoemission spectroscopy measurements confirmed that ScN has an indirect bandgap of ~1.2 eV.

42 ENGINEERING↗
DOE OSTI2025

Time-resolved vacuum-ultraviolet photoelectron spectroscopy of the à 1 A u state of acetylene

Ultrafast time-resolved photoelectron spectra are reported for the vacuum-ultraviolet (VUV) photoionization of acetylene following excitation to the à 1 A u state via UV absorption at 200 nm. The excitation energy lies above the lowest dissociation threshold to C 2 H X̃ 2 Σ + + H, as well as above the threshold for adiabatic dissociation of the à 1 A u state to form C 2 H (à 2 Π) + H. The time-dependent mass spectra and photoelectron spectra provide insight into the intramolecular decay processes of the à 1 A u state. In addition, photoelectron spectra of the à 1 A u state with VUV light access both the X̃ 2 Π u and à 2 Σ g + states of the ion, as well as the predicted, but previously unobserved, 1 2 Π g state, which corresponds to a two-hole, one-particle configuration that lies in close proximity to the à 2 Σ g + state. The 1 2 Π g state is split into 2 A 2 + 2 B 2 and 2 A g + 2 B g states in the cis and trans configurations, respectively. In conclusion, electronic structure calculations, along with trajectory calculations, reproduce the principal features of the experimental data and confirm the assignment of the 1 2 Π g state.

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

Protein folding from heterogeneous unfolded state revealed by time-resolved X-ray solution scattering

One of the most challenging tasks in biological science is to understand how a protein folds. In theoretical studies, the hypothesis adopting a funnel-like free-energy landscape has been recognized as a prominent scheme for explaining protein folding in views of both internal energy and conformational heterogeneity of a protein. Despite numerous experimental efforts, however, comprehensively studying protein folding with respect to its global conformational changes in conjunction with the heterogeneity has been elusive. Here we investigate the redox-coupled folding dynamics of equine heart cytochrome c (cyt-c) induced by external electron injection by using time-resolved X-ray solution scattering. A systematic kinetic analysis unveils a kinetic model for its folding with a stretched exponential behavior during the transition toward the folded state. With the aid of the ensemble optimization method combined with molecular dynamics simulations, we found that during the folding the heterogeneously populated ensemble of the unfolded state is converted to a narrowly populated ensemble of folded conformations. These observations obtained from the kinetic and the structural analyses of X-ray scattering data reveal that the folding dynamics of cyt-c accompanies many parallel pathways associated with the heterogeneously populated ensemble of unfolded conformations, resulting in the stretched exponential kinetics at room temperature. This finding provides direct evidence with a view to microscopic protein conformations that the cyt-c folding initiates from a highly heterogeneous unfolded state, passes through still diverse intermediate structures, and reaches structural homogeneity by arriving at the folded state.

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

Electronic coherences in nonadiabatic molecular photophysics revealed by time-resolved photoelectron spectroscopy

Significance Time-resolved photoelectron spectroscopy (TRPES) is a promising technique for the study of ultrafast molecular processes, such as the nonadiabatic dynamics taking place at conical intersections. Directly accessing the evolution of the coherences generated at the conical intersection should provide most valuable dynamical information. However, the signals are dominated by background contributions due to state populations, and most theoretical treatments completely neglect the role of the coherences. Here we show that distinguishable signatures of molecular coherences appear in TRPES. These can be recorded using currently available ultrashort pulses and unambiguously extracted at the postprocessing stage. The technique thus provides direct access to nonadiabatic coherence dynamics.

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

Time-resolved experiments on gas-phase atoms and molecules with XUV and X-ray free-electron lasers

Over the last 20 years, XUV and X-ray free-electron lasers have enabled a wide variety of time-resolved experiments that have dramatically advanced our understanding of ultra-fast molecular dynamics on atomic length scales and femto-second time scales. This review focuses on experimental studies of ultrafast dynamics of atoms and molecules in the gas phase, tracing the development of the field from early proof-of-principle studies to recent pump-probe experiments that elucidate the coupled electronic and nuclear dynamics during photochemical reactions with a temporal resolution that is now extending into the attosecond domain.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Ultrafast dynamics of 2-thiouracil investigated by time-resolved Auger spectroscopy

In this paper, we present time-resolved ultraviolet-pump x-ray probe Auger spectra of 2-thiouracil. An ultraviolet induced shift towards higher kinetic energies is observed in the sulfur 2p Auger decay. The difference Auger spectra of pumped and unpumped molecules exhibit ultrafast dynamics in the shift amplitude, in which three phases can be recognized. In the first 100 fs, a shift towards higher kinetic energies is observed, followed by a 400 fs shift back to lower kinetic energies and a 1 ps shift again to higher kinetic energies. We use a simple Coulomb-model, aided by quantum chemical calculations of potential energy states, to deduce a C-S bond expansion within the first 100 fs. The bond elongation triggers internal conversion from the photoexcited S 2 to the S 1 state. Based on timescales, the subsequent dynamics can be interpreted in terms of S 1 nuclear relaxation and S 1 -triplet internal conversion.

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

Robust two-colour pyrometry uncertainty analysis to acquire spatially-resolved measurements

Two-colour pyrometry (2CP) has been used over several decades to study engine-relevant combustion processes, but results are generally regarded as qualitative or semi-quantitative. In many current 2CP systems, large measurement errors are introduced by parallax because the two measured wavelengths are not from the same line of sight. Here this work presents a spatially-resolved 2CP system with the objective of quantifying and reducing measurement uncertainty. An optical setup that eliminates parallax in 2CP is used together with pixel-by-pixel calibration of the camera sensor to increase measurement accuracy. Primary uncertainty terms are identified, and an error propagation analysis is performed to compute uncertainties in the final results of soot temperature, soot concentration parameter, KL, and soot mass. These methodologies are applied to investigate an auto-igniting fuel spray in a constant pressure flow rig at diesel-like conditions of high ambient pressure and temperature. Results show bias uncertainty of around 200 K (≈10%) for temperature and about 40%–60% for KL. High uncertainty was found to occur on the diffusion flame front where both optical thickness and soot concentrations are small. However, these uncertain measurement zones with relatively low soot concentrations contribute minimally to the total soot mass present in the reacting jet during the temporal evolution of the flame.

42 ENGINEERING↗
DOE OSTI2023

Spatially-resolved dynamic sampling of different phasic magnetic resonances of nanoparticle ensembles in a magnetotactic bacterium Magnetospirillum magnetotacticum

Abstract Nanoscaled magnetic particle ensembles are promising building blocks for realizing magnon based binary logic. Element-specific real-space monitoring of magnetic resonance modes with sampling rates in the GHz regime is imperative for the experimental verification of future complex magnonic devices. Here we present the observation of different phasic magnetic resonance modes using the element-specific technique of time-resolved scanning transmission x-ray microscopy within a chain of dipolarly coupled Fe 3 O 4 nanoparticles (40–50 nm particle size) inside a single cell of a magnetotactic bacterium Magnetospirillum magnetotacticum . The particles are probed with 25 nm resolution at the Fe L 3 x-ray absorption edge in response to a microwave excitation of 4.07 GHz. A plethora of resonance modes is observed within multiple particle segments oscillating in- and out-of-phase, well resembled by micromagnetic simulations.

time-resolved scanning transmission x-ray microsco↗