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At least 703 records · Page 39

All sources NASA NTRS DOE OSTI

DOE OSTI2025

ATR-SEIRAS Reveals Potential Inversion and Associated Electron Transfer Kinetics in the Reduction of Surface-Confined Anthraquinone

The detection of stable semiquinone radicals on an anthraquinone (AQ) layer chemically grafted to an electrode surface in aqueous electrolytes has been elucidated by using attenuated total reflection surface enhanced infrared absorption spectroscopy (ATR-SEIRAS). In very alkaline conditions (pH 13), the reduction of the AQ involves no proton transfer, but surface sensitive infrared spectroscopy reveals that the anthraquinone dianion forms a strong hydrogen bonding network with coadsorbed water, leading to irreversible features in the voltammetry. The potential dependence of the IR band assigned to the AQ radical is consistent with the enhanced hydrogen bonding network causing increased stabilization of the quinone radical and supports the predicted response of a system under mild potential inversion, whereby the formal potential for the reduction of the anthraquinone radical is positive of the reduction potential of the neutral AQ molecule. Time-resolved ATR-SEIRAS is used to measure the transient formation of the AQ •– radical, from which rate constant information can be extracted using the Butler–Volmer model involving two one-electron transfers without a direct disproportionation reaction. The potential dependence of the rate constants is consistent with the potential inversion and can be used to qualitatively simulate the measured cyclic voltammograms. In conclusion, the thermodynamic and kinetic analyses re-emphasize long established deficiencies associated with using one-electron reaction formalisms to characterize multi-electron systems.

37 - INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL C↗

DOE OSTI2021

Slow Auger Recombination of Trapped Excitons Enables Efficient Multiple Electron Transfer in CdS–Pt Nanorod Heterostructures

We report solar-to-fuel conversion reaction often requires multiple proton-coupled electron transfer (PCET) processes powered by the energetic electrons and/or holes generated by the absorption of multiple photons. The effective coupling of multiple electron transfer from the light absorber with the multiple PCET reactions at the catalytic center is one of the key challenges in efficient and selective conversion of solar energy to chemical fuels. In this paper, we examine the dynamics of multiple electron transfer in quantum confined CdS nanorods with a Pt tip, in which the CdS rod functions as the light absorber and the Pt tip the catalytic center. By excitation-fluence-dependent transient absorption spectroscopic measurements, we show that the multiexciton Auger recombination rate in CdS rods follows a carrier-collision model, k n A = n 2 (n – 1)/4k 2 A , with a biexciton lifetime (1/k 2 A ) of 2.0 ± 0.2 ns. In CdS–Pt nanorods, electron transfer kinetics from the CdS conduction band edge to the Pt show negligible dependence on the excitation fluence, occurring with a half-life time of 5.6 ± 0.6 ps. The efficiency of multiple exciton dissociation by multiple electron transfer to Pt decreases from 100% in biexciton states to ~41% at 22 exciton state due to the competition with Auger recombination. The half-lifetime of the n-charge separated state recombination (with n electrons in the Pt and n holes in the CdS) decreases from 10 μs in the single charge separated state to 42 ns in nine charge separated states. Our findings suggest the possibility of driving multielectron photocatalytic reactions under intense illumination and controlling product selectivity through multielectron transfer.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

The birth and evolution of solvated electrons in the water

The photo-induced radiolysis of water is an elementary reaction in biology and chemistry, forming solvated electrons, OH radicals, and hydronium cations on fast time scales. Here, we use an optical-pump terahertz-probe spectroscopy setup to trigger the photoionization of water molecules with optical laser pulses at ~400 nm and then time-resolve the transient solvent response with broadband terahertz (THz) fields with a ~90 fs time resolution. We observe three distinct spectral responses. The first is a positive broadband mode that can be attributed to an initial diffuse, delocalized electron with a radius of (22 ± 1) Å, which is short lived (<200 fs) because the absorption is blue-shifting outside of the THz range. The second emerging spectroscopic signature with a lifetime of about 150 ps is attributed to an intermolecular mode associated with a mass rearrangement of solvent molecules due to charge separation of radicals and hydronium cations. After 0.2 ps, we observe a long-lasting THz signature with depleted intensity at 110 cm -1 that is well reproduced by ab initio molecular dynamics. We interpret this negative band at 110 cm -1 as the solvent cage characterized by a weakening of the hydrogen bond network in the first and second hydration shells of the cavity occupied by the localized electron.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1996

Dynamic and Transient Performance of Turbofan/Turboshaft Convertible Engine With Variable Inlet Guide Vanes

A convertible engine called the CEST TF34, using the variable inlet guide vane method of power change, was tested on an outdoor stand at the NASA Lewis Research Center with a waterbrake dynamometer for the shaft load. A new digital electronic system, in conjunction with a modified standard TF34 hydromechanical fuel control, kept engine operation stable and safely within limits. All planned testing was completed successfully. Steady-state performance and acoustic characteristics were reported previously and are referenced. This report presents results of transient and dynamic tests. The transient tests measured engine response to several rapid changes in thrust and torque commands at constant fan (shaft) speed. Limited results from dynamic tests using the pseudorandom binary noise technique are also presented. Performance of the waterbrake dynamometer is discussed in an appendix.

McArdle, Jack G.↗

NASA NTRS1983

Studies in electron phenomena in MOS structures: The pulsed C-V method

The pulse hysteresis capacitance voltage (C-V) provides a straight forward technique for measuring the change of various charges in MOS structures and a tool for investigating the kinetics of various electron phenomena is developed and described. The method can be used for measuring the energy distribution and kinetics of surface states with the resolution of about 1/5 x 10 to the -9 power cm eV. Some transients in an MOS structure, particularly, the thermal generation of minority charge carriers via surface states and the relaxation of minority charge carriers supplied from the inversion layer outside the MOS structure are theoretically investigated. Analytical expressions which clearly present the physics of those electron phenomena are derived.

Kaplan, G.↗

DOE OSTI2023

Spectral Deconvolution of Electron-Bifurcating Flavoproteins

Electron-bifurcating flavoproteins catalyze the tightly coupled reduction of high- and low-potential acceptors using a median-potential electron donor, and are invariably complex systems with multiple redox-active centers in two or more subunits. Methods are described that permit, in favorable cases, the deconvolution of spectral changes associated with reduction of specific centers, making it possible to dissect the overall process of electron bifurcation into individual, discrete steps.

electron bifurcation↗

DOE OSTI2025

Revealing the Phonon Bottleneck Limit in Negatively Charged CdS Quantum Dots

The capture of photoexcited hot electrons in semiconductors before they lose their excess energy to cooling is a long-standing goal in photon energy conversion. Semiconductor nanocrystals have large electron energy spacings that are expected to slow down electron relaxation by phonon emission, but hot electrons in photoexcited nanocrystals, nevertheless, cool rapidly by energy transfer to holes. This makes the intrinsic phonon-bottleneck-limited hot electron lifetime in nanocrystals elusive. For this work, we used a combination of theory and experiments to probe the hot-electron dynamics of negatively charged cadmium sulfide (CdS) colloidal quantum dots (QDs) in the absence of holes. Experiments found that these hot electrons cooled on a 100 ps time scale. Theoretical simulations predicted that pure phonon-bottleneck-limited hot electron cooling occurs on a similar time scale. This similarity suggests that the experimental measurements reflect the upper limit on the hot-electron lifetimes in these CdS QDs and the lower limit on the rates of processes that can harvest those hot electrons.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Can the Rate of a Catalytic Turnover Be Altered by Ligands in the Absence of Direct Binding Interactions?

Second sphere coordination effects ubiquitous in enzymatic catalysis occur through direct interactions, either covalent or non-covalent, with reaction intermediates and transition states. Here, we present herein evidence of indirect second sphere coordination effects in which ligation of water/alkanols far removed from the primary coordination sphere of the active site nevertheless alter energetic landscapes within catalytic redox cycles in the absence of direct physicochemical interactions with surface species mediating catalytic turnovers. Density functional theory, in situ X-ray absorption and infrared spectroscopy, and a wide array of steady-state and transient CO oxidation rate data suggest that the presence of peripheral water renders oxidation half-cycles within two-electron redox cycles over μ m -oxo-bridged trimers in MIL-100(M) more kinetically demanding. Communication between ligated water and the active site appears to occur through the Fe-O-Fe backbone, as inferred from spin density variations on the central μ m -oxygen 'junction'. Evidence is provided for the generality of these second sphere effects in that they influence different types of redox half-cycles or metals, and can be amplified or attenuated through choice of coordinating ligand. Specifically in the case of MIL-100(M) materials, the Cr isostructure can be made to kinetically mimic the Fe variant by disproportionately hindering oxidation half-cycles relative to the reduction half-cycles. Kinetic and spectroscopic inferences presented here significantly expand both the conceptual definition of second sphere effects as well as the palette of synthetic levers available for tuning catalytic redox performance through chemical ligation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Nonequilibrium charge-density-wave order beyond the thermal limit

The interaction of many-body systems with intense light pulses may lead to novel emergent phenomena far from equilibrium. Recent discoveries, such as the optical enhancement of the critical temperature in certain superconductors and the photo-stabilization of hidden phases, have turned this field into an important research frontier. Here, we demonstrate nonthermal charge-density-wave (CDW) order at electronic temperatures far greater than the thermodynamic transition temperature. Using time- and angle-resolved photoemission spectroscopy and time-resolved X-ray diffraction, we investigate the electronic and structural order parameters of an ultrafast photoinduced CDW-to-metal transition. Tracking the dynamical CDW recovery as a function of electronic temperature reveals a behaviour markedly different from equilibrium, which we attribute to the suppression of lattice fluctuations in the transient nonthermal phonon distribution. A complete description of the system’s coherent and incoherent order-parameter dynamics is given by a time-dependent Ginzburg-Landau framework, providing access to the transient potential energy surfaces.

36 MATERIALS SCIENCE↗

DOE OSTI2023

The anisotropic nature of singlet fission in single crystalline organic semiconductors

The escalating global energy predicament implores for a revolutionary resolution—one that converts sunlight into electricity—holding the key to supreme conversion efficiency. This comprehensive review embarks on the exploration of the principle of generating multiple excitons per absorbed photon, a captivating concept that possesses the potential to redefine the fundamental confines of conversion efficiency, albeit its application remains limited in photovoltaic devices. At the nucleus of this phenomenon are two principal processes: multiple exciton generation (MEG) within quantum-confined environments, and singlet fission (SF) inside molecular crystals. The process of SF, characterized by the cleavage of a single photogenerated singlet exciton into two triplet excitons, holds promise to potentially amplify photon-to-electron conversion efficiency twofold, thereby laying the groundwork to challenge the detailed balance limit of solar cell efficiency. Our discourse primarily dissects the complex nature of SF in crystalline organic semiconductors, laying special emphasis on the anisotropic behavior of SF and the diffusion of the subsequent triplet excitons in single-crystalline polyacene organic semiconductors. We initiate this journey of discovery by elucidating the principles of MEG and SF, tracing their historical genesis, and scrutinizing the anisotropy of SF and the impact of quantum decoherence within the purview of functional mode electron transfer theory. We present an overview of prominent techniques deployed in investigating anisotropic SF in organic semiconductors, including femtosecond transient absorption microscopy and imaging as well as stimulated Raman scattering microscopies, and highlight recent breakthroughs linked with the anisotropic dimensions of Davydov splitting, Herzberg–Teller effects, SF, and triplet transport operations in single-crystalline polyacenes. Through this comprehensive analysis, our objective is to interweave the fundamental principles of anisotropic SF and triplet transport with the current frontiers of scientific discovery, providing inspiration and facilitating future ventures to harness the anisotropic attributes of organic semiconductor crystals in the design of pioneering photovoltaic and photonic devices.

Chemistry↗

DOE OSTI2024

Dual-comb spectroscopy in the deep ultraviolet

This Letter reports dual-frequency-comb spectroscopy in the deep ultraviolet used to characterize transient laser-produced plasmas. Dual-comb spectroscopy at these wavelengths enables access to a large number of strong electronic transitions in neutral and ionized atoms and molecules. This broadband dual-frequency-comb system at 265 nm measures multiple transitions in neutral and singly ionized iron atoms in a laser-produced plasma. Analysis of absorption spectra yields time-resolved ion and neutral column densities, excitation temperatures, and electron densities, which are measured down to 10 14 cm —3 levels. The results provide insights into low-temperature plasma properties.

47 OTHER INSTRUMENTATION↗

NASA NTRS1975

The sources of material comprising a mass ejection coronal transient

The origin of the material ejected during a white-light coronal transient on August 26 and 27, 1973, is investigated using simultaneous observations of a slowly ascending prominence and the more rapid accompanying coronal transient. Nearly identical simultaneous images of the prominence were obtained over a six-hour period in the H-alpha and He II (304 A) emission lines; contemporaneous Skylab coronograph observations over approximately 1.5 hours showed that the mass-ejection coronal transient rose above the ascending prominence. Based on analysis of these observations, it is concluded that: (1) the bulk of the ejected material originated in the lower corona, despite the lack of an observed depletion there; (2) the material in the transient was at coronal temperature and was visible in polarized radiation due to Thomson scattering of photospheric light by free electrons; and (3) the total event was far larger, more energetic, and longer lasting than would have been inferred from the prominence observations alone.

Hildner, E.↗

NASA NTRS1979

Effects of space environment on composites: An analytical study of critical experimental parameters

A generalized methodology currently employed at JPL, was used to develop an analytical model for effects of high-energy electrons and interactions between electron and ultraviolet effects. Chemical kinetic concepts were applied in defining quantifiable parameters; the need for determining short-lived transient species and their concentration was demonstrated. The results demonstrates a systematic and cost-effective means of addressing the issues and show qualitative and quantitative, applicable relationships between space radiation and simulation parameters. An equally important result is identification of critical initial experiments necessary to further clarify the relationships. Topics discussed include facility and test design; rastered vs. diffuse continuous e-beam; valid acceleration level; simultaneous vs. sequential exposure to different types of radiation; and interruption of test continuity.

Gupta, A.↗

NASA NTRS1987

In-circuit fault injector user's guide

A fault injector system, called an in-circuit injector, was designed and developed to facilitate fault injection experiments performed at NASA-Langley's Avionics Integration Research Lab (AIRLAB). The in-circuit fault injector (ICFI) allows fault injections to be performed on electronic systems without special test features, e.g., sockets. The system supports stuck-at-zero, stuck-at-one, and transient fault models. The ICFI system is interfaced to a VAX-11/750 minicomputer. An interface program has been developed in the VAX. The computer code required to access the interface program is presented. Also presented is the connection procedure to be followed to connect the ICFI system to a circuit under test and the ICFI front panel controls which allow manual control of fault injections.

Padilla, Peter A.↗

NASA NTRS1992

Carrier removal and defect behavior in p-type InP

A simple expression, obtained from the rate equation for defect production, was used to relate carrier removal to defect production and hole trapping rates in p-type InP after irradiation by 1-MeV electrons. Specific contributions to carrier removal from defect levels H3, H4, and H5 were determined from combined deep-level transient spectroscopy (DLTS) and measured carrier concentrations. An additional contribution was attributed to one or more defects not observed by the present DLTS measurements. The high trapping rate observed for H5 suggests that this defect, if present in relatively high concentration, could be dominant in p-type InP.

Weinberg, I.↗

DOE OSTI2020

Nonlinear fluorescence spectroscopy of layered perovskite quantum wells

Interest in layered organohalide perovskites is motivated by their potential for use in optoelectronic devices. In these systems, the smallest and largest quantum wells are primarily concentrated near the glass and air interfaces of a film, thereby establishing a gradient in the average values of the bandgaps. It has been suggested that this layered architecture promotes the funneling of electronic excitations through space in a manner similar to light-harvesting processes in photosynthetic antennae. Whereas energy and charge transfer are difficult to distinguish by conventional transient absorption techniques, it has recently been shown that these competing relaxation mechanisms may be separately targeted with nonlinear fluorescence (NLFL) and photocurrent “action spectroscopies.” Here, we present perturbative rate functions to describe NLFL experiments conducted on layered perovskite systems. The formulas reproduce the patterns of resonances observed in experimental measurements and show how signatures of energy transfer manifest in two-dimensional spectra. Overall, this work suggests that NLFL spectroscopy may be used to fully reveal the trajectories of electronic excitations by correlating ultrafast energy transfer pathways to fluorescence emission from the thickest quantum wells.

Ouyang, Zhenyu↗

DOE OSTI2024

A High-Fidelity Electromagnetic Transient Model of Inverter-based Resources Integrated to an IEEE-9 Bus System for Benchmarking Studies

An inverter-based resource (IBR) is a source of electricity that is asynchronously connected to the electrical grid via an electronic power converter. These power sources lack the intrinsic behaviors of the standard power plants, presenting specific challenges to system stability. These power sources lack the intrinsic behaviors of the standards power plants and their features are almost entirely defined by the control strategy used on them, presenting specific challenges to system stability as their penetration increases into the already fragile Bulk Power System (BPS). Utilizing renewable energy has a great upside but the electrical industry needs to understand the requirements like performing electromagnetic transient (EMT) simulation studies in planning and/or in interconnection studies. This paper presents the development of a high-fidelity EMT model based on commercial equipment and field parameters, which at the same time aims to study the increasing penetration of IBRs and their impact on the actual BPS. The open-source EMT model developed will be a benchmarking example that can be used to evaluate algorithms in the power grid (including evaluating grid-forming controls, power system monitoring and operation, etc.).

Martinez Montejano, Misael↗

DOE OSTI2020

Transient Lattice Response upon Photoexcitation in CuInSe 2 Nanocrystals with Organic or Inorganic Surface Passivation

CuInSe 2 nanocrystals offer promise for optoelectronics including thin-film photovoltaics and printed electronics. Additive manufacturing methods such as photonic curing controllably sinter particles into quasi-continuous films and offer improved device performance. To gain understanding of nanocrystal response under such processing conditions, we investigate impacts of photoexcitation on colloidal nanocrystal lattices via time-resolved X-ray diffraction. We probe three sizes of particles and two capping ligands (oleylamine and inorganic S 2- ) to evaluate resultant crystal lattice temperature, phase stability, and thermal dissipation. Elevated fluences produce heating and loss of crystallinity, the onset of which exhibits particle size dependence. We find size-dependent recrystallization and cooling lifetimes ranging from 90 to 200 ps with additional slower cooling on the nanosecond time scale. Sulfide-capped nanocrystals show faster recrystallization and cooling compared to oleylamine-capped nanocrystals. Using these lifetimes, we find interfacial thermal conductivities from 3 to 28 MW/(m 2 K), demonstrating that ligand identity strongly influences thermal dissipation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗