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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 991 records · Page 55
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Moisture-driven CO 2 pump for direct air capture

Direct Air Capture, the chemical separation of carbon dioxide (CO 2 ) from air, is considered a necessary approach to generate negative carbon emissions and in turn limit global warming, though energetic and monetary costs must continue to decline to meet the needed gigaton scale. The promise of energy-efficient and continuous carbon dioxide membrane separation has only recently been investigated with the development of facilitated chemical transport and novel electrochemically driven methods. This work demonstrates the potential for continuous pumping of CO 2 from air using commercial anion exchange membranes driven solely by a water vapor gradient. A reactive transport model that couples ionic transport with moisture sensitive bicarbonate chemistry in charged polymers, also termed moisture swing sorption, was developed alongside experimentally measured equilibrium and transport properties of CO 2 and water vapor in Fumasep FAA-3 to determine the mass transport limits of such a system. The results show that the commercial membrane is kinetically limited by the moisture sensitive chemistry, enabling a CO 2 current of 1.1 μmol/m 2 • s. In diffusion limited materials, a CO 2 pumping flux can reach 11 μmol/m 2 • s in and peak performance is expected with a dry air relative humidity around 50% pumping into a saturated water vapor permeate. In all configurations, water loss becomes the major cost in such a separation and must be managed through optimal polymer design or water recovery mechanisms. The work demonstrates the applicability of a new driving force, the evaporation of water, to meet the energetic demand of CO 2 separation from air.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Multi-octave-spanning supercontinuum generation through high-energy laser filaments in YAG and ZnSe pumped by a 2.4 μm femtosecond Cr:ZnSe laser

Abstract We present experimental and numerical investigations of high-energy mid-infrared filamentation with multi-octave-spanning supercontinuum generation (SCG), pumped by a 2.4 μm, 250 fs Cr:ZnSe chirped-pulse laser amplifier. The SCG is demonstrated in both anomalous and normal dispersion regimes with YAG and polycrystalline ZnSe, respectively. The formation of stable and robust single filaments along with the visible-to-mid-infrared SCG is obtained with a pump energy of up to 100 μJ in a 6-mm-long YAG medium. To the best of the authors’ knowledge, this is the highest-energy multi-octave-spanning SCG from a laser filament in a solid. On the other hand, the SCG and even-harmonic generation based on random quasi-phase matching (RQPM) are simultaneously observed from the single filaments in a 6-mm-long polycrystalline ZnSe medium with a pump energy of up to 15 μJ. The numerical simulations based on unidirectional pulse propagation equation and RQPM show excellent agreement with the measured multi-octave-spanning SCG and even-harmonic generation. They also reveal the temporal structure of mid-infrared filaments, such as soliton-like self-compression in YAG and pulse broadening in ZnSe.

Optics↗
DOE OSTI2019

Ab Initio Computation of Rotationally-Averaged Pump–Probe X-ray and Electron Diffraction Signals

We develop a new algorithm for the computation of the rotationally averaged elastic molecular diffraction signal for the cases of perpendicular or parallel pump–probe geometries. The algorithm first collocates the charge density from an arbitrary ab initio wave function onto a Becke quadrature grid [A. Becke, J. Chem. Phys. 1988, 88, 2457], providing a high-fidelity multiresolution representation of the charge density. A double sum is then performed over the Becke grid points, and the interaction between points computed using the scattering kernels of Williamson and Zewail [J. C. Williamson and A. H. Zewail, J. Phys. Chem. 1994, 98, 2766]. These kernels analytically average over the molecular orientations with the cos 2 γ selection factor appropriate for one-photon dipole absorption in a perpendicular pump–probe geometry. We demonstrate that the method is converged with small grids containing <500 points/atom. We implement the algorithm on a GPU for increased efficiency and emonstrate the algorithm for molecules with up to a few dozen atoms. We explore the accuracy of the independent atom model (IAM) by comparison with our new and more accurate method. We also investigate the possibility of detecting signatures of electronic transitions in polyatomic pump–probe diffraction experiments.

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

The Influence of Air‐Sea CO 2 Disequilibrium on Carbon Sequestration by the Ocean's Biological Pump

Abstract The ocean's biological carbon pump (BCP) affects the Earth's climate by sequestering CO 2 away from the atmosphere for decades to millennia. One primary control on the amount of carbon sequestered by the biological pump is air‐sea CO 2 disequilibrium, which is controlled by the rate of air‐sea CO 2 exchange and the residence time of CO 2 in surface waters. Here, we use a data‐assimilated model of the soft tissue BCP to quantify carbon sequestration inventories and time scales from remineralization in the water column to equilibration with the atmosphere. We find that air‐sea CO 2 disequilibrium enhances the global biogenic carbon inventory by ∼35% and its sequestration time by ∼70 years compared to identical calculations made assuming instantaneous air‐sea CO 2 exchange. Locally, the greatest enhancement occurs in the subpolar Southern Ocean, where air‐sea disequilibrium increases sequestration times by up to 600 years and the biogenic dissolved inorganic carbon inventory by >100% in the upper ocean. Contrastingly, in deep‐water formation regions of the North Atlantic and Antarctic margins, where biological production creates undersaturated surface waters which are subducted before fully equilibrating with the atmosphere, air‐sea CO 2 disequilibrium decreases the depth‐integrated sequestration inventory by up to ∼150%. The global enhancement of carbon sequestration by air‐sea disequilibrium is particularly important for carbon respired in deep waters that upwell in the Southern Ocean. These results highlight the importance of accounting for air‐sea CO 2 disequilibrium when evaluating carbon sequestration by the biological pump and for assessing the efficacy of ocean‐based CO 2 removal methods.

Environmental Sciences & Ecology↗
DOE OSTI2016

Hetero-site-specific X-ray pump-probe spectroscopy for femtosecond intramolecular dynamics

New capabilities at X-ray free-electron laser facilities allow the generation of two-colour femtosecond X-ray pulses, opening the possibility of performing ultrafast studies of X-ray-induced phenomena. Specifically, the experimental realization of hetero-site-specific X-ray-pump/X-ray-probe spectroscopy is of special interest, in which an X-ray pump pulse is absorbed at one site within a molecule and an X-ray probe pulse follows the X-ray-induced dynamics at another site within the same molecule. In this paper, we show experimental evidence of a hetero-site pump-probe signal. By using two-colour 10-fs X-ray pulses, we are able to observe the femtosecond time dependence for the formation of F ions during the fragmentation of XeF 2 molecules following X-ray absorption at the Xe site.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2012

X-ray pump optical probe cross-correlation study of GaAs

Ultrafast dynamics in atomic, molecular and condensed-matter systems are increasingly being studied using optical-pump, X-ray probe techniques where subpicosecond laser pulses excite the system and X-rays detect changes in absorption spectra and local atomic structure. New opportunities are appearing as a result of improved synchrotron capabilities and the advent of X-ray free-electron lasers. These source improvements also allow for the reverse measurement: X-ray pump followed by optical probe. We describe here how an X-ray pump beam transforms a thin GaAs specimen from a strong absorber into a nearly transparent window in less than 100 ps, for laser photon energies just above the bandgap. We find the opposite effect - X-ray induced optical opacity - for photon energies just below the bandgap. This raises interesting questions about the ultrafast many-body response of semiconductors to X-ray absorption, and provides a new approach for an X-ray/optical cross-correlator for synchrotron and X-ray free-electron laser applications.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2017

Structures and transport dynamics of a Campylobacter jejuni multidrug efflux pump

Resistance-nodulation-cell division efflux pumps are integral membrane proteins that catalyze the export of substrates across cell membranes. Within the hydrophobe-amphiphile efflux subfamily, these resistance-nodulation-cell division proteins largely form trimeric efflux pumps. The drug efflux process has been proposed to entail a synchronized motion between subunits of the trimer to advance the transport cycle, leading to the extrusion of drug molecules. Here we use X-ray crystallography and single-molecule fluorescence resonance energy transfer imaging to elucidate the structures and functional dynamics of the Campylobacter jejuni CmeB multidrug efflux pump. We find that the CmeB trimer displays a very unique conformation. A direct observation of transport dynamics in individual CmeB trimers embedded in membrane vesicles indicates that each CmeB subunit undergoes conformational transitions uncoordinated and independent of each other. On the basis of our findings and analyses, we propose a model for transport mechanism where CmeB protomers function independently within the trimer.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2019

Spin-current-mediated rapid magnon localisation and coalescence after ultrafast optical pumping of ferrimagnetic alloys

Sub-picosecond magnetisation manipulation via femtosecond optical pumping has attracted wide attention ever since its original discovery in 1996. Furthermore, the spatial evolution of the magnetisation is not yet well understood, in part due to the difficulty in experimentally probing such rapid dynamics. Here, we find evidence of rapid magnetic order recovery in materials with perpendicular magnetic anisotropy via nonlinear magnon processes. We identify both localisation and coalescence regimes, whereby localised magnetic textures nucleate and subsequently evolve in accordance with a power law formalism. Coalescence is observed for optical excitations both above and below the switching threshold. Simulations indicate that the ultrafast generation of noncollinear magnetisation via optical pumping establishes exchange-mediated spin currents with an equivalent 100% spin polarised charge current density of 108 A/cm 2 . Such large spin currents precipitate rapid recovery of magnetic order after optical pumping. These processes suggest an ultrafast optical route for the stabilization of desired meta-stable states, e.g., isolated skyrmions.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Revealing core-valence interactions in solution with femtosecond X-ray pump X-ray probe spectroscopy

Abstract Femtosecond pump-probe spectroscopy using ultrafast optical and infrared pulses has become an essential tool to discover and understand complex electronic and structural dynamics in solvated molecular, biological, and material systems. Here we report the experimental realization of an ultrafast two-color X-ray pump X-ray probe transient absorption experiment performed in solution. A 10 fs X-ray pump pulse creates a localized excitation by removing a 1 s electron from an Fe atom in solvated ferro- and ferricyanide complexes. Following the ensuing Auger–Meitner cascade, the second X-ray pulse probes the Fe 1 s → 3 p transitions in resultant novel core-excited electronic states. Careful comparison of the experimental spectra with theory, extracts +2 eV shifts in transition energies per valence hole, providing insight into correlated interactions of valence 3 d with 3 p and deeper-lying electrons. Such information is essential for accurate modeling and predictive synthesis of transition metal complexes relevant for applications ranging from catalysis to information storage technology. This study demonstrates the experimental realization of the scientific opportunities possible with the continued development of multicolor multi-pulse X-ray spectroscopy to study electronic correlations in complex condensed phase systems.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2024

Experimental demonstration of attosecond pump–probe spectroscopy with an X-ray free-electron laser

Pump–probe experiments with subfemtosecond resolution are the key to understanding electronic dynamics in quantum systems. Here we demonstrate the generation and control of subfemtosecond pulse pairs from a two-colour X-ray free-electron laser. By measuring the delay between the two pulses with an angular streaking diagnostic, we characterize the group velocity of the X-ray free-electron laser and show control of the pulse delay down to 270as. Here, we confirm the application of this technique to a pump–probe measurement in core-ionized para-aminophenol. These results reveal the ability to perform pump–probe experiments with subfemtosecond resolution and atomic site specificity.

47 OTHER INSTRUMENTATION↗
DOE OSTI2016

Tracking reaction dynamics in solution by pump–probe X-ray absorption spectroscopy and X-ray liquidography (solution scattering)

Characterization of transient molecular structures formed during chemical and biological processes is essential for understanding their mechanisms and functions. Over the last decade, time-resolved X-ray liquidography (TRXL) and time-resolved X-ray absorption spectroscopy (TRXAS) have emerged as powerful techniques for molecular and electronic structural analysis of photoinduced reactions in the solution phase. Both techniques make use of a pump–probe scheme that consists of (1) an optical pump pulse to initiate a photoinduced process and (2) an X-ray probe pulse to monitor changes in the molecular structure as a function of time delay between pump and probe pulses. TRXL is sensitive to changes in the global molecular structure and therefore can be used to elucidate structural changes of reacting solute molecules as well as the collective response of solvent molecules. On the other hand, TRXAS can be used to probe changes in both local geometrical and electronic structures of specific X-ray-absorbing atoms due to the element-specific nature of core-level transitions. These techniques are complementary to each other and a combination of the two methods will enhance the capability of accurately obtaining structural changes induced by photoexcitation. Here we review the principles of TRXL and TRXAS and present recent application examples of the two methods for studying chemical and biological processes in solution. Furthermore, we briefly discuss the prospect of using X-ray free electron lasers for the two techniques, which will allow us to keep track of structural dynamics on femtosecond time scales in various solution-phase molecular reactions.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2019

Hydrodynamic and Structural Response Modeling of a Prototype Floating Membrane Reservoir System for Pumped Storage Hydropower

Hydrodynamic, computational fluid dynamics, and finite-element modeling were performed for a novel floating membrane reservoir system design for closed-loop pumped storage hydropower application. The conceptual design, which is now protected under an invention disclosure with a patent pending, offers a potential low-cost, low-impact solution to address the high costs, long investment return periods, and environmental disruptions encountered with traditional pumped storage development while offering modularity to enable replication at many locations. Prior to physical tests on a prototype, this paper documents the response analysis and modeling completed to simulate hydraulic and structural performance under different reservoir deployment and alignment arrangements, evaluate system stability, and refine the conceptual design. The results indicate that the excitation frequency from vortex shedding is at least an order of magnitude lower than the water sloshing frequencies in the reservoir, the structural natural frequency of the entire reservoir, and the vibrational frequencies of the side membranes, although excitation frequencies from other sources could cause mechanical resonance under certain conditions. To control destabilizing effects and prevent rocking motion and vibration, the authors conclude that the design could be improved by including a support structure around the floating reservoir, which could also provide floating-membrane containment, improve safety, and facilitate vertical reservoir movement. These conclusions, based on hydrodynamic and structural response modeling, help define specifications for upcoming full-scale prototype construction, deployment, and testing. This study demonstrates standard modeling technique application to an innovative design for which similar applications have not been previously evaluated. As a result, the refined design is capable of improving the scalability and feasibility of pumped storage hydropower in the United States and will be considered for commercialization following prototype testing.

13 HYDRO ENERGY↗
DOE OSTI2010

Surface pump-probe femtosecond-laser mass spectrometry: Time-, mass-, and velocity-resolved detection of surface reaction dynamics

A detailed account of the experimental methodology of surface pump-probe femtosecond-laser mass spectrometry is presented. This recently introduced technique enables the direct time-resolved investigation of surface reaction dynamics by monitoring the mass and the relative velocity of intermediates and products of a photoinduced surface reaction via multiphoton ionization. As a model system, the photodissociation dynamics of methyl iodide adsorbed at submonolayer coverage on magnesia ultrathin films is investigated. The magnesia surface preparation and characterization as well as the pulsed deposition of methyl iodide are described. The femtosecond-laser excitation (pump) and, in particular, the resonant multiphoton ionization surface detection (probe) schemas are discussed in detail. Results of pump-probe time-resolved methyl and iodine atom detection experiments are presented and the potential of this method for velocity-resolved photofragment analysis is evaluated.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2011

Distinguishing Between Relaxation Pathways by Combining Dissociative Ionization Pump Probe Spectroscopy and Ab Initio Calculations: A Case Study of Cytosine

We present a general method for tracking molecular relaxation along different pathways from an excited state down to the ground state. We follow the excited state dynamics of cytosine pumped near the S0-S1 resonance using ultrafast laser pulses in the deep ultraviolet and probed with strong field near infrared pulses which ionize and dissociate the molecules. The fragment ions are detected via time of flight mass spectroscopy as a function of pump probe delay and probe pulse intensity. Our measurements reveal that different molecular fragments show different timescales, indicating that there are multiple relaxation pathways down to the ground state. We interpret our measurements with the help of ab initio electronic structure calculations of both the neutral molecule and the molecular cation for different conformations en route to relaxation back down to the ground state. Our measurements and calculations show passage through two seams of conical intersections between ground and excited states and demonstrate the ability of dissociative ionization pump probe measurements in conjunction with ab initio electronic structure calculations to track molecular relaxation through multiple pathways.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Molecular alignment effect on the photoassociation process via a pump-dump scheme

The photoassociation processes via the pump-dump scheme for the heternuclear (Na + H → NaH) and the homonuclear (Na + Na → Na{sub 2}) molecular systems are studied, respectively, using the time-dependent quantum wavepacket method. For both systems, the initial atom pair in the continuum of the ground electronic state (X{sup 1}Σ{sup +}) is associated into the molecule in the bound states of the excited state (A{sup 1}Σ{sup +}) by the pump pulse. Then driven by a time-delayed dumping pulse, the prepared excited-state molecule can be transferred to the bound states of the ground electronic state. It is found that the pump process can induce a superposition of the rovibrational levels |v, j〉 on the excited state, which can lead to the field-free alignment of the excited-state molecule. The molecular alignment can affect the dumping process by varying the effective coupling intensity between the two electronic states or by varying the population transfer pathways. As a result, the final population transferred to the bound states of the ground electronic state varies periodically with the delay time of the dumping pulse.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Pump-probe Kelvin-probe force microscopy: Principle of operation and resolution limits

Knowledge on surface potential dynamics is crucial for understanding the performance of modern-type nanoscale devices. We describe an electrical pump-probe approach in Kelvin-probe force microscopy that enables a quantitative measurement of dynamic surface potentials at nanosecond-time and nanometer-length scales. Also, we investigate the performance of pump-probe Kelvin-probe force microscopy with respect to the relevant experimental parameters. We exemplify a measurement on an organic field effect transistor that verifies the undisturbed functionality of our pump-probe approach in terms of simultaneous and quantitative mapping of topographic and electronic information at a high lateral and temporal resolution.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Focal overlap gating in velocity map imaging to achieve high signal-to-noise ratio in photo-ion pump-probe experiments

We demonstrate a technique in velocity map imaging (VMI) that allows spatial gating of the laser focal overlap region in time resolved pump-probe experiments. This significantly enhances signal-to-noise ratio by eliminating background signal arising outside the region of spatial overlap of pump and probe beams. This enhancement is achieved by tilting the laser beams with respect to the surface of the VMI electrodes which creates a gradient in flight time for particles born at different points along the beam. By suitably pulsing our microchannel plate detector, we can select particles born only where the laser beams overlap. Furthermore, this spatial gating in velocity map imaging can benefit nearly all photo-ion pump-probe VMI experiments especially when extreme-ultraviolet light or X-rays are involved which produce large background signals on their own.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2020

High sensitivity pump–probe measurements of magnetic, thermal, and acoustic phenomena with a spectrally tunable oscillator

We describe an optical pump/probe system for sensitive measurements of time-resolved optical measurements of material dynamics. The instrument design is optimized for time-resolved magneto-optic Kerr effect (TR-MOKE) measurements of dynamics in magnetic materials. The system also allows for time-domain thermoreflectance (TDTR) measurements of thermal transport properties and picosecond acoustic measurements of film thickness and/or elastic constants. The system has several advantages over the conventional designs for TRMOKE and/or TDTR systems. Measurements of pump-induced changes to the probe beam intensity are shot-noise limited. The system’s design allows for MOKE and/or thermoreflectance measurements of both sides of a sample. Pumping and probing the sample on opposite sides allows nanoscale flash diffusivity measurements of transport properties. The wavelengths of the pump and probe beams are straightforward to tune between 350–525 nm and 690–1050 nm. A tunable wavelength allows for optical resonances in a wide array of materials to be excited and/or probed. Finally, the setup is calibrated to allow for the real and imaginary components of Kerr signals to be separately quantified.

47 OTHER INSTRUMENTATION↗