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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 307 records · Page 17
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Inverse Bremsstrahlung Absorption

Inverse bremsstrahlung absorption was measured based on transmission through a finite-length plasma that was thoroughly characterized using spatially resolved Thomson scattering. Expected absorption was then calculated using the diagnosed plasma conditions while varying the absorption model components. To match data, it is necessary to account for: (1) the Langdon effect; (2) laser-frequency (rather than plasma-frequency) dependence in the Coulomb logarithm, as is typical of bremsstrahlung theories but not transport theories; and (3) a correction due to ion screening. Radiation-hydrodynamic simulations of inertial confinement fusion implosions have to date used a Coulomb logarithm from the transport literature and no screening correction. Here, we anticipate that updating the model for collisional absorption will substantially revise our understanding of laser-target coupling for such implosions.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Effect of lattice excitations on transient near-edge x-ray absorption spectroscopy

Here, time-dependent and constituent-specific spectral changes in soft near-edge x-ray absorption spectroscopy (XAS) of an [Fe/MgO] 8 metal/insulator heterostructure after laser excitation are analyzed at the O K-edge with picosecond time resolution. The oxygen absorption edge of the insulator features a uniform intensity decrease of the fine structure at elevated phononic temperatures, which can be quantified by a simple simulation and fitting procedure presented here. Combining XAS with ultrafast electron diffraction measurements and ab initio calculations demonstrates that the transient intensity changes in XAS can be assigned to a transient lattice temperature. Thus, the sensitivity of transient near-edge XAS to phonons is demonstrated.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Mammalian complex III heme dynamics studied with pump-probe spectroscopy and red light illuminations

The electronic or molecular mechanisms which initiate photobiomodulation (PBM) in cells are not yet fully understood. Porcine complex III (C-III) of the electron transport chain was characterized with transient absorption spectroscopy (TAS). Then we applied our recently developed continuous wave laser coupled TAS procedure (CW-TAS) to investigate the effect of red light irradiances on the heme dynamics of C-III in its c 1 reduced state. The time constants associated with the axial ligand photodissociation were found to be 3.3 ± 0.3 ps for the oxidized state and 4.9 ± 0.4 ps for the c 1 reduced state. The analysis of the CW-TAS procedure yielded no significant changes in the C-III heme dynamics. We rule out the possibility of 635 nm CW light at 4.7 mW/cm 2 inducing a PBM effect on the heme dynamic of C-III, specifically with the photodissociation of its axial ligand.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2021

X-ray transient absorption reveals the 1Au (nπ*) state of pyrazine in electronic relaxation

Abstract Electronic relaxation in organic chromophores often proceeds via states not directly accessible by photoexcitation. We report on the photoinduced dynamics of pyrazine that involves such states, excited by a 267 nm laser and probed with X-ray transient absorption spectroscopy in a table-top setup. In addition to the previously characterized 1 B 2u (ππ*) (S 2 ) and 1 B 3u (nπ*) (S 1 ) states, the participation of the optically dark 1 A u (nπ*) state is assigned by a combination of experimental X-ray core-to-valence spectroscopy, electronic structure calculations, nonadiabatic dynamics simulations, and X-ray spectral computations. Despite 1 A u (nπ*) and 1 B 3u (nπ*) states having similar energies at relaxed geometry, their X-ray absorption spectra differ largely in transition energy and oscillator strength. The 1 A u (nπ*) state is populated in 200 ± 50 femtoseconds after electronic excitation and plays a key role in the relaxation of pyrazine to the ground state.

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

Approaching the Lower Temporal Limit of Laser‐Produced Plasma Sources for Table‐Top Soft X‐Ray NEXAFS Measurements

Abstract The increasing popularity of time‐resolved X‐ray absorption measurements for understanding dynamics in molecular and material systems has led to many advances in table‐top sources for pulsed X‐rays. We report on a table‐top laser‐produced plasma (LPP) source that can perform soft X‐ray (SXR), near‐edge X‐ray absorption fine structure (NEXAFS) measurements using a laser source with 23 ps pulse duration. The spectrometer's key specifications, such as brilliance, resolution, and stability, are characterized against the more commonly used longer‐pulse‐duration LPP sources. The 23 ps laser produced approximately an order of magnitude weaker SXR flux than the 8 ns laser for a higher power density due to the smaller total energy absorbed by the plasma. The increased repetition rate, as well as the use of a high line‐density X‐grating, and a self‐referencing scheme still allowed for NEXAFS measurements of Si 3 N 4 and TiO 2 thin films with 2.5 minute acquisition times, a resolving power of E/ΔE=424, and a signal‐to‐noise ratio of 100. It was observed that degradation of the gas jet nozzle led to long‐term instability of the source, which can be remediated using alternative nozzle designs. This work demonstrates the feasibility of achieving higher temporal resolution in future time‐resolved X‐ray absorption measurements using table‐top LPP sources.

Nimlos, Danika [Division of Chemistry and Chemical↗
DOE OSTI2023

High-Resolution Thermal Profiling of a High-Power Diode Laser Facet During Aging

Here, we study the facet temperature distribution of a high-power diode laser over its lifetime using a noncontact, high spatial resolution CCD-based thermoreflectance technique. Based on the known correlation between non-radiative defects and heating, thermal maps can provide valuable information regarding the formation and evolution of small point defects that are at or near the facet during aging. In the laser under study in this work we measure the appearance of local hot spots on the facet, including concentrated hot spots that appear just before or just after COD and are correlated with loss of local light emission. The locations of these hot spots do not exhibit morphology changes in high-resolution SEM imaging of the facet, indicating that the related defects are too small to be observable in SEM or are located at some depth under the facet. Prior to COD, we measure a gradual facet temperature increase accompanied by a gradual optical power decrease and gradual facet optical absorption increase, indicating gradual degradation of the laser.

47 OTHER INSTRUMENTATION↗
DOE OSTI2024

Broadband rapid-scanning phase-modulated Fourier transform electronic spectroscopy

We present a phase-modulated approach for ultrabroadband Fourier transform electronic spectroscopy. To overcome the bandwidth limitations and spatial chirp introduced by acousto-optic modulators (AOMs), pulses from a 1 µm laser are modulated using AOMs prior to continuum generation. This phase modulation is transferred to the continuum generated in a yttrium aluminum garnet crystal. Separately generated phase-modulated continua in two arms of a Mach-Zehnder interferometer interfere with the difference of their modulation frequencies, enabling physical under-sampling of the signal and the suppression of low-frequency noise. By interferometrically tracking the relative time delay of the continua, we perform continuous, rapid-scanning Fourier transform electronic spectroscopy with a high signal-to-noise ratio and spectral resolution. As proof of principle, we measure the linear absorption and fluorescence excitation spectra of a laser dye and various biological samples.

Javed, Ariba↗
DOE OSTI2022

Gamma-radiation-induced negative nonlinear absorption in quartz glass

The effect of ionizing radiation on the nonlinear optical properties of materials needs to be considered for applications that employ high-power laser pulses in extreme radiation environments. The Heraeus Infrasil302 optical quartz glass was irradiated by gamma rays, and its nonlinear absorption was measured using the open-aperture Z-scan technique with nanosecond laser pulses. Irradiation results in a negative nonlinear absorption coefficient whose magnitude increases with irradiation dose. Nonlinear absorption coefficients of -0.78, -1.14, -1.29, and -1.88~ × ~10 -13 m/W are measured for gamma doses of 600 krad, 1.2 Mrad, 3.6 Mrad, and 10 Mrad, respectively. Thermal annealing restores the optical properties of quartz-glass to their unirradiated values. It is suggested that metallic impurities introduced by the manufacturing process have a role in inducing saturated absorption in irradiated quartz glass, which manifests as negative nonlinear absorption coefficient, and is demonstrated by comparing Infrasil302 quartz results to equivalent irradiated measurements for Spectrosil2000 quartz.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2022

Diffraction enhanced imaging utilizing a laser produced x-ray source

Image formation by Fresnel diffraction utilizes both absorption and phase-contrast to measure electron density profiles. The low spatial and spectral coherence requirements allow the technique to be performed with a laser-produced x-ray source coupled with a narrow slit. This makes it an excellent candidate for probing interfaces between materials at extreme conditions, which can only be generated at large-scale laser or pulsed power facilities. Here, we present the results from a proof-of-principle experiment demonstrating an effective ~2 μm laser-generated source at the OMEGA Laser Facility. This was achieved using slits of 1 × 30 μm 2 and 2 × 40 μm 2 geometry, which were milled into 30 μm thick Ta plates. Combining these slits with a vanadium He-like 5.2 keV source created a 1D imaging system capable of micrometer-scale resolution. The principal obstacles to achieving an effective 1 μm source are the slit tilt and taper—where the use of a tapered slit is necessary to increase the alignment tolerance. We demonstrate an effective source size by imaging a 2 ± 0.2 μm radius tungsten wire.

3D printing↗
DOE OSTI2022

Laser spot welding of additive manufactured 304L stainless steel

Here, the goal of this work is to understand if an additively manufactured 304L stainless steel exhibits similar spot-welding behavior as wrought 304L stainless steel. Due to the many differences between an additively manufactured component and wrought product, it is important to determine how the material interacts with the laser and how it affects the weld bead morphology. In this paper, the laser coupling efficiency, weld size, and solidification of spot welds produced in wrought and additively manufactured 304L stainless steel were investigated. The coupling efficiency of wrought and additively manufactured 304L stainless steel of similar surface condition were approximately the same over a range of applied laser energies. Laser welding of the untreated (rougher) surface of additively manufactured 304L, however, showed improved coupling efficiency ranging between 3.3 and 100%. The rougher surface traps the incoming light and increases the coupling efficiency at lower laser energies, while at higher energy, the absorption efficiency is dominated by intrinsic absorption from the keyhole formation rather than surface roughness. The resulting spot weld microstructures differed from welds made in wrought 304L and additively manufactured 304L. Welds made in wrought 304L were fully austenitic containing what is suspected to be massive austenite, which suggests that these welds solidified as primary ferrite. Welds made in additively manufactured 304L were also fully austenitic and contained both cellular austenite and what is suspected to be massive austenite. These observations mean that welds made in additively manufactured 304L solidified as primary ferrite and primary austenite. The differences in weld microstructures made in wrought and AM 304L can be attributed to differences in the composition and solidification rate.

304L stainless steel↗
DOE OSTI2021

Extremely Bright, Near-IR Emitting Spontaneously Blinking Fluorophores Enable Ratiometric Multicolor Nanoscopy in Live Cells

New bright, photostable, emission-orthogonal fluorophores that blink without toxic additives are needed to enable multicolor, live-cell, single-molecule localization microscopy (SMLM). Here we report the design, synthesis, and biological evaluation of Yale676sb, a photostable, near-IR-emitting fluorophore that achieves these goals in the context of an exceptional quantum yield (0.59). When used alongside HMSiR, Yale676sb enables simultaneous, live-cell, two-color SMLM of two intracellular organelles (ER + mitochondria) with only a single laser and no chemical additives.

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

Direct Observation of the ππ* to nπ* Transition in 2-Thiouracil via Time-Resolved NEXAFS Spectroscopy

The photophysics of nucleobases has been the subject of both theoretical and experimental studies over the past decades due to the challenges posed by resolving the steps of their radiationless relaxation dynamics, which cannot be described in the framework of the Born–Oppenheimer approximation (BOA). In this context, the ultrafast dynamics of 2-thiouracil has been investigated with a time-resolved NEXAFS study at the Free Electron Laser FLASH. Near Edge X-ray Absorption Fine Structure spectroscopy (NEXAFS) can be used to observe electronic transitions in ultrafast molecular relaxation. We performed time-resolved UV-pump/X-ray probe absorption measurements at the sulfur 2s (L1) and 2p (L2/3) edges. We are able to identify absorption features corresponding to the S2 (ππ*) and S1 (nπ*) electronic states. We observe a delay of 102 ± 11 fs in the population of the nπ* state with respect to the initial optical excitation and interpret the delay as the time scale for the S2 → S1 internal conversion. We furthermore identify oscillations in the absorption signal that match a similar observation in our previous X-ray photoelectron spectroscopy study on the same molecule.

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

Spectroscopy of atoms in an optical dipole trap using spectrally selective heating by a probe laser field

Spectral properties of atoms localised in an optical dipole trap are studied using the method of spectrally selective heating by a probe field. The method is based on measuring the number of atoms in a trap after they interact with a probe field. The dependence of the number of atoms on the frequency of the probe field fully characterises the shift and width of the spectral absorption line of trapped atoms. (paper)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Ligand Desorption and Fragmentation in Oleate-Capped CdSe Nanocrystals under High-Intensity Photoexcitation

Semiconductor nanocrystals (NCs) offer prospective use as active optical elements in photovoltaics, light-emitting diodes, lasers, and photocatalysts due to their tunable optical absorption and emission properties, high stability, and scalable solution processing, as well as compatibility with additive manufacturing routes. Over the course of experiments, during device fabrication, or while in use commercially, these materials are often subjected to intense or prolonged electronic excitation and high carrier densities. The influence of such conditions on ligand integrity and binding remains underexplored. Here, in this study, we expose CdSe NCs to laser excitation and monitor changes in oleate that is covalently attached to the NC surface using nuclear magnetic resonance as a function of time and laser intensity. Higher photon doses cause increased rates of ligand loss from the particles, with upward of 50% total ligand desorption measured for the longest, most intense excitation. Surprisingly, for a range of excitation intensities, fragmentation of the oleate is detected and occurs concomitantly with formation of aldehydes, terminal alkenes, H 2 , and water. After illumination, NC size, shape, and bandgap remain constant although low-energy absorption features (Urbach tails) develop in some samples, indicating formation of substantial trap states. The observed reaction chemistry, which here occurs with low photon to chemical conversion efficiency, suggests that ligand reactivity may require examination for improved NC dispersion stability but can also be manipulated to yield desired photocatalytically accessed chemical species.

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

Plutonium Co-precipitation with Calcite

The mobility of plutonium (Pu) in the environment is affected by Pu–mineral interactions, such as adsorption–desorption and structural incorporation. Calcite (CaCO 3 ) is a common secondary phase in near surface environments and a major component of many rocks and soils and is expected to form as an alteration product of cement-based materials planned for use in geological repositories. The reactivity of the calcite surface and its ability to tolerate significant variations in its chemical composition through substitution of Ca for other cations make calcite a potentially important sink for environmental contaminants. Here, single crystals of calcite were synthesized from aqueous solutions in equilibrium with air containing Pu as either Pu(VI) or Pu(IV) and characterized using a combination of laser ablation inductively coupled plasma mass spectrometry (LA–ICP–MS) and X-ray absorption spectroscopy (XAS). These data are used to assess the amount, structure, and oxidation state of Pu co-precipitated into calcite, providing insight into the potential for Pu sequestration in calcite precipitates. Overall, the XAS and LA–ICP–MS data support the co-precipitation of plutonyl [Pu(VI/V)] in the bulk calcite, although the exact nature of the co-precipitated Pu complex is difficult to elucidate in the synthesized material. Co-precipitated plutonyl could be incorporated in either distorted Ca lattice sites or defect sites, and we provide evidence to suggest that Pu(VI) is reduced mainly to Pu(V) in the precipitated solid. LA–ICP–MS additionally shows that the co-precipitation of Pu(VI/V) is favored over the co-precipitation of Pu(IV). Altogether, our results suggest that Pu sequestration in calcite under environmental conditions could immobilize Pu and isolate it from groundwater interactions in contaminated environments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Leveraging the redox activities of cerium and dibenzotetrathiafulvalene to discover a photo-responsive magnetic material

Stimuli-responsive changes in lanthanide-based materials are a promising research direction. In this study, [DBTTF] 4 [Ce 2 Cl 10 ] DBTTF = dibenzotetrathiafulvalene (1) was synthesized by a light-induced crystallization, where photo-oxidation of DBTTF enables formation of the cerium dimer [Ce 2 Cl 10 ] 4− . Intermolecular interactions between the stacked organic units of the crystal result in charge transfer bands in the visible-NIR (near-infrared) region, evident in the solid-state absorption spectrum upon comparison with the solution spectrum. The assignments of the sublattice oxidation states were made with single-crystal X-ray diffraction (SC-XRD) structural characterization, Raman spectroscopy, X-ray absorption spectroscopy, and magnetometry. Continuous 532 nm laser irradiation of the microcrystalline solid modulates the redox states in 1, leading to ∼40% reduction in the observed magnetization at 2 K. Density functional theory PBE+U/HSE06 band structure calculations predict Mott insulating behavior in 1, with a bandgap of 0.54/0.81 eV, and further support the conjecture that the observed photo-induced change in magnetization results from electron transfer from the [Ce 2 Cl 10 ] 4− anions to the π-stacked [DBTTF] 2 2+ organic dimer subunits. An enhancement in conductivity is similarly observed upon 532 nm irradiation, determined by single-crystal transport measurements. The findings reveal that photo-responsive lanthanide-based materials can be achieved by integration of redox-active organic moieties with redox-active lanthanide cations for the realization of switchable, photo-magnetic materials.

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

Pathways to excitation of atoms with bicircular laser pulses

We study the excitation of the hydrogen atom by bichromatic circularly polarized laser pulses using numerical solutions of the time-dependent Schrödinger equation. The results are in agreement with the selection rules for multiphoton processes in such fields, namely, excited states are populated in which orbital angular momentum and magnetic quantum numbers are either both odd or both even, independent of the relative helicity, peak intensity, and pulse duration of the pulses. For co-rotating pulses the results show that excitation predominantly proceeds to states with magnetic quantum number of the same helicity as the laser pulses. Besides pathways via direct photon absorption from the ground state our results indicate that a transfer of population among the Rydberg states occurs via Λ-type transitions. In the case of counter-rotating pulses the largest excitation probability is found for Rydberg states that differ in magnetic quantum number by Δm=±3. This pattern allows us to estimate how many photons from each of the two bichromatic fields have been absorbed. Finally, we confirm that a population in Rydberg states beyond a maximum orbital angular quantum number is unlikely.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2025

High-precision monitoring of outgassing species in model extreme ultraviolet photoresists with a cavity ring-down spectrometer

Background Extreme ultraviolet (EUV) photoresists play a pivotal role in advancing nanopatterning technologies by balancing image quality and sensitivity. The outgassing behavior of photoresist thin films under EUV and deep ultraviolet (DUV) exposure reveals chemical details relevant to their performance. Aim Here, we focus on utilizing an analytical technique not previously used in photolithography, the tabletop cavity ring-down spectrometer, to investigate outgassing dynamics in EUV photoresists, enabling precise chemical identification and deeper insights into resist processing. Approach The spectrometer’s enhanced laser path length (∼ 20 km) and broadband absorption capabilities in the C–H overtone region allow for sensitive and temporally resolved detection of mixtures of outgassed species. Using a model resist comprising a polymer matrix with a photoacid generator and quencher, we analyzed the influence of time delays between exposure and post-exposure bake (PEB) as well as storage under varying environmental conditions. Results Suppression of isobutylene outgassing and thickness loss was observed with extended delays between exposure and PEB, potentially linked to water absorption and acid deactivation. The technique proved highly effective in distinguishing subtle chemical differences between processing stages. Conclusions Delay times and their environmental conditions, particularly humidity, reduce outgassing and thickness loss of photoresists during PEB, suggesting decreased acid-driven deprotection. This can potentially impact sensitivity, defectivity, and roughness of resist patterns, necessitating precise monitoring and control.

Extreme ultraviolet photoresists↗