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Results for “Charge distributions”

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 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Ion-Pair Reorganization Regulates Reactivity in Photoredox Catalysts

Cyclometalated and polypyridyl complexes of d6 metals are promising photoredox catalysts, using light to drive reactions with high kinetic or thermodynamic barriers via the generation of reactive radical intermediates. However, while tuning of their redox potentials, absorption energy, excited-state lifetime and quantum yield are well-known criteria for modifying activity, other factors could be important. Here we show that dynamic ion-pair reorganization controls the reactivity of a photoredox catalyst, [Ir[dF(CF3)ppy]2(dtbpy)]X. Time-resolved dielectric-loss experiments show how counter-ion identity influences excited-state charge distribution, evincing large differences in both the ground- and excited-state dipole moment depending on whether X is a small associating anion (PF6-) that forms a contact-ion pair versus a large one that either dissociates or forms a solvent-separated pair (BArF4-). These differences correlate with the reactivity of the photocatalyst toward both reductive and oxidative electron transfer, amounting to a 4-fold change in selectivity toward oxidation versus reduction. These results suggest that ion pairing could be an underappreciated factor that modulates reactivity in ionic photoredox catalysts.

catalysis↗
DOE OSTI2024

Tailoring Ion Transport in Li 3‐3y Ho 1+y Cl 6‐x Br x via Transition‐Metal Free Structural Planes and Charge Carrier Distribution

Abstract Localized atomistic disorder in halide‐based solid electrolytes (SEs) can be leveraged to boost Li + mobility. In this study, Li + transport in structurally modified Li 3 HoCl 6 , via Br − introduction and Li + deficiency, is explored. The optimized Li 3‐3 y Ho 1+ y Cl 6‐ x Br x achieves an ionic conductivity of 3.8 mS cm −1 at 25 °C, the highest reported for holmium halide materials. 6,7 Li nuclear magnetic resonance and relaxometry investigations unveil enhanced ion dynamics with bromination, attaining a Li + motional rate neighboring 116 MHz. X‐ray diffraction analyses reveal mixed‐anion‐induced phase transitions with disproportionate octahedral expansions and distortions, creating Ho‐free planes with favorable energetics for Li + migration. Bond valence site energy analysis highlights preferred Li + transport pathways, particularly in structural planes devoid of Ho 3+ blocking effects. Molecular dynamics simulations corroborate enhanced Li + diffusion with Br − introduction into Li 3 HoCl 6 . Li‐Ho electrostatic repulsions in the (001) plane presumably drive Li + diffusion into the Ho‐free (002) layer, enabling rapid intraplanar Li + motion and exchange between the 2d and 4h sites. Li 3‐3 y Ho 1+ y Cl 6‐ x Br x also demonstrates good battery cycling stability. These findings offer valuable insights into the intricate correlations between structure and ion transport and will help guide the design of high‐performance fast ion conductors for all‐solid‐state batteries.

Chemistry↗
DOE OSTI2022

Femtosecond X-ray Spectroscopy Directly Quantifies Transient Excited-State Mixed Valency

Quantifying charge delocalization associated with short-lived photoexcited states of molecular complexes in solution remains experimentally challenging, requiring local element specific femtosecond experimental probes of time-evolving electron transfer. In this study, we quantify the evolving valence hole charge distribution in the photoexcited charge transfer state of a prototypical mixed valence bimetallic iron–ruthenium complex, [(CN) 5 Fe II CNRu III (NH 3 ) 5 ]-, in water by combining femtosecond X-ray spectroscopy measurements with time-dependent density functional theory calculations of the excited-state dynamics. We estimate the valence hole charge that accumulated at the Fe atom to be 0.6 ± 0.2, resulting from excited-state metal-to-metal charge transfer, on an ~ 60 fs time scale. Our combined experimental and computational approach provides a spectroscopic ruler for quantifying excited-state valency in solvated complexes.

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

Pseudorapidity distributions of charged particles as a function of mid- and forward rapidity multiplicities in pp collisions at $\sqrt{s}$ = 5.02, 7 and 13 TeV

The multiplicity dependence of the pseudorapidity density of charged particles in proton–proton (pp) collisions at centre-of-mass energies √s = 5.02, 7 and 13 TeV measured by ALICE is reported. The analysis relies on track segments measured in the midrapidity range (|η| < 1.5). Results are presented for inelastic events having at least one charged particle produced in the pseudorapidity interval |η| < 1. The multiplicity dependence of the pseudorapidity density of charged particles is measured with mid- and forward rapidity multiplicity estimators, the latter being less affected by autocorrelations. A detailed comparison with predictions from the PYTHIA 8 and EPOS LHC event generators is also presented. The results can be used to constrain models for particle production as a function of multiplicity in pp collisions.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
NASA NTRS1979

Secondary emission effects on spacecraft charging: Energy distribution considerations

The conditions under which multiple valued solutions occur by computing the floating potential of an isolated eclipses surface on a geosynchronous orbit spacecraft were examined. Different approximations for the electron spectra during a geomagnetic substorm were used. The result indicates that if the incident electron flux has a Maxwellian energy distribution, the ratio of the secondary emitted current to the incident electron current is independent of the spacecraft potential. In this case a single value solution to the current equation occurs.

Sanders, N. L.↗
NASA NTRS1979

Mapping of electrical potential distribution with charged particle beams

Potentials were measured using a beam of soft X-rays in air at 2 x 10 to the -5 power Torr. Ions were detected by a continuous-dynode electron multiplier after they passed through a retarding field. Ultimate resolution depends upon the diameter of the X-ray beam which was 3 mm. When the fields in the region of interest were such to disperse the ions, only a small fraction were detected and the method of measurement was not very reliable. Yet reasonable data could be collected if the ions traveled in parallel paths toward the detector. Development should concentrate on increasing the aperture of the detector from the pinhole which was used to something measured in centimeters. Also increasing the strength of the source would provide a stronger signal and more reliable data. Measurements were made at an estimated ion current to 10 to the -15 power A from a 10 cm length of the X-ray beam, this current being several orders of magnitude below what would have a perturbing effect on the region to be measured. Consequently, the source strength can be increased and prospects for this method of measurement are good.

Robinson, J. W.↗
NASA NTRS1982

Mapping of electrical potential distributions with charged particle beams

Methods for measuring electrostatic potentials on and near dielectric surfaces charged to several kilovolts are studied. Secondary emission from those charged dielectrics is measured. Candidates for potential measurement include the induced charge, from which potential is calculated; the trajectory endpoints of either high or low energy particles traversing the region near the surface; trajectory impact on the surface; and creating ions at points of interest near the surface. Some of the methods require computer simulations and iterative calculation if potential maps are to be generated. Several approaches are described and compared. A method using a half-cylinder as a test chamber and low-energy probing beams is adapted for the measurement of seconary emission.

Robinson, J. W.↗
DOE OSTI2024

Diamond of infrared equivalences in abelian gauge theories

We demonstrate a tree-level equivalence between four distinct infrared objects in (d+2)-dimensional Abelian gauge theories. These are (i) the large gauge charge Q ϵ where the function ϵ on the sphere parametrizing large gauge transformations is identified with the Goldstone mode θ of spontaneously broken large gauge symmetry; (ii) the soft effective action that captures the dynamics of the soft and Goldstone modes; (iii) the edge mode action with Neumann boundary conditions; and (iv) the Wilson line dressing of a scattering amplitude, including a novel dressing for soft photons, which have local charge distributions despite having vanishing global charge. The promotion of the large gauge parameter to the dynamical Goldstone and the novel dressing of soft gauge particles give rise to intriguing possibilities for the future study of infrared dynamics of gauge theories and gravity.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗