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At least 847 records · Page 47

The Role of Kinetic Processes in Magnetospheric Dynamics

The question of whether the micro scale controls the macro scale or vice-versa remains one of the most challenging problems in plasmas. A particular topic of interest within this context is collisionless magnetic reconnection, where both points of views are espoused by different groups of researchers. This presentation will focus on this topic. We will begin by analyzing the global properties of magnetic reconnection. Following that, we discuss properties of electron diffusion region dynamics both for guide field and antiparallel reconnection, and how they can be scaled to different inflow conditions. As a next step, we will study typical temporal variations of the microscopic dynamics with the objective of understanding the potential for secular changes to the macroscopic system. The research will be based on a combination of analytical theory and numerical modeling.

Hesse, Michael↗

Comparison of Energetic Electron Fluxes Measured by GPS and THEMIS Spacecraft in the Inner Magnetosphere

Key elements of space weather models are energetic electron fluxes in the inner magnetosphere and the outer radiation belt. Flux depletion is driven by various loss processes: scattering into atmosphere, magnetopause shadowing. Flux enhancement is driven by various acceleration processes: local wave-particle interactions, radial transport, plasma sheet injections. Many of these processes operate on ~ hour timescales. Such mesoscale flux variations are not well traced by equatorial spacecraft with much longer orbits. Energetic electron detectors onboard the Global Positioning System (GPS) constellation provide a unique opportunity for probing such ~ hour-scale flux variations. Measurements from up to 23 identically instrumented GPS satellites cover a wide energy and L-shell range with a subhour time resolution. However, their orbits are inclined and thus all measurements at L-shell >4.3 are off-equatorial. Here, in this report, we present a comparison of equatorial THEMIS and nonequatorial GPS measurements of omnidirectional ≤600 keV electron fluxes. Such a comparison allows us to derive coefficients for using off-equatorial GPS fluxes to infer the equatorial values. These coefficients depend on particle energy and L-shell. We demonstrate a new data set derived from GPS measurements and discuss how it can be used to investigate mesoscale dynamics of energetic electron fluxes in the inner magnetosphere.

79 ASTRONOMY AND ASTROPHYSICS↗

High strain rate nanoindentation testing: Recent advancements, challenges and opportunities

Recent advancements in electronics have renewed the interest in high strain rate nanoindentation testing, resulting in the development of new high strain rate nanoindentation test equipment and test methodologies. Here, in this work, the current state-of-the-art in high strain rate nanoindentation testing is critically reviewed, with focus on three key aspects - the testing equipment's dynamic mechanical and electronic response, test methodology, and post-processing of raw data to obtain hardness and strain rate. The challenges in instrument hardware design and post-test data analysis are discussed, along with optimal strain rate window for accurate high strain rate measurements. Specific focus will be on instrumented high strain rate testing using self-similar indenters at strain rates in excess of 100 s -1 , wherein load and depth of penetration into the sample are both measured or applied.

36 MATERIALS SCIENCE↗

Magnetic probe diagnostics of nonlinear standing waves and bulk ohmic electron power absorption in capacitive discharges

It is recognized that standing wave effects appearing in large-area, very-high-frequency capacitively coupled plasma (CCP) reactors cause center-high plasma non-uniformity. Using a high-frequency magnetic probe, we present a direct experimental diagnostic of the nonlinear standing waves and bulk ohmic electron power absorption dynamics in low pressure CCP discharges for different driving frequencies of 13.56, 30, and 60 MHz. The design, principle, calibration, and validation of the probe are described in detail. Spatial structures of the harmonics of the magnetic field, determined by the magnetic probe, were used to calculate the distributions of the harmonic current and the corresponding ohmic electron power deposition, providing insights into the behavior of nonlinear harmonics. At a low driving frequency, i.e. 13.56 MHz, no remarkable nonlinear standing waves were identified and the bulk ohmic electron power absorption was observed to be negligible. Here, the harmonic magnetic field/current was found to increase dramatically with the driving frequency, due to decreased sheath reactance and more remarkable nonlinear standing waves at a higher driving frequency, leading to the enhancements of the ohmic heating and the plasma density in the bulk, specifically at the electrode center. At a high driving frequency, i.e. 60 MHz, the high-order harmonic current density and the corresponding ohmic electron power absorption exhibited a similar node structure, with the main peak on axis, and one or more minor peaks between the electrode center and the edge, contributing to the center-high profile of the plasma density.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Observation of parallel intersystem crossing and charge transfer-state dynamics in [Fe(bpy) 3 ] 2+ from ultrafast 2D electronic spectroscopy

Transition metal-based charge-transfer complexes represent a broad class of inorganic compounds with diverse photochemical applications. Charge-transfer complexes based on earth-abundant elements have been of increasing interest, particularly the canonical [Fe(bpy) 3 ] 2+ . Photoexcitation into the singlet metal–ligand charge transfer ( 1 MLCT) state is followed by relaxation first to the ligand-field manifold and then to the ground state. While these dynamics have been well-studied, processes within the MLCT manifold that facilitate and/or compete with relaxation have been more elusive. We applied ultrafast two-dimensional electronic spectroscopy (2DES) to disentangle the dynamics immediately following MLCT excitation of this compound. First, dynamics ascribed to relaxation out of the initially formed 1 MLCT state was found to correlate with the inertial response time of the solvent. Second, the additional dimension of the 2D spectra revealed a peak consistent with a ~20 fs 1 MLCT → 3 MLCT intersystem crossing process. These two observations indicate that the complex simultaneously undergoes intersystem crossing and direct conversion to ligand-field state(s). Resolution of these parallel pathways in this prototypical earth-abundant complex highlights the ability of 2DES to deconvolve the otherwise obscured excited-state dynamics of charge-transfer complexes.

2-dimensional electronic spectroscopy↗

Ultrafast Nanoimaging of Spin-Mediated Shear Waves in an Acoustic Cavity

Strong spin–lattice coupling in van der Waals (vdW) magnets shows potential for innovative magneto-mechanical applications. Here, nanoscale and picosecond imaging by ultrafast electron microscopy reveal heterogeneous spin-mediated coherent acoustic phonon dynamics in a thin-film cavity of the vdW antiferromagnet FePS3. The harmonics of the interlayer shear acoustic modes are observed, in which the even and odd harmonics exhibit distinct nanoscopic dynamics. Corroborated by acoustic wave simulation, the role of defects in forming even harmonics is elucidated. Above the Néel temperature (T N ), the interlayer shear acoustic harmonics are suppressed, while the in-plane traveling wave is predominantly excited. The dominant acoustic dynamics shifts from the out-of-plane shear to the in-plane traveling wave across T N , demonstrating that magnetic properties can influence phonon scattering pathways. In conclusion, the spatiotemporally resolved structural characterization provides valuable nanoscopic insights for interlayer-shear-mode-based acoustic cavities, opening up possibilities for magneto-mechanical applications of vdW magnets.

36 MATERIALS SCIENCE↗

Transient Second-Order Nonlinear Media: Breaking the Spatial Symmetry in the Time Domain via Hot-Electron Transfer

Second-order optical effects are essential to the active control of light and the generation of new spectral components. The inversion symmetry, however, prevents achieving a bulk $χ^{(2)}$ response, limiting the portfolio of the second-order nonlinear materials. Here, we demonstrate subpicosecond conversion of a statically passive dielectric to a transient second-order nonlinear medium upon the ultrafast transfer of hot electrons. Induced by an optical switching signal, the amorphous dielectric with vanishing intrinsic $χ^{(2)}$ develops dynamically tunable second-order nonlinear responses. By taking the second-harmonic generation as an example, we show that breaking the inversion symmetry through hot-electron dynamics can be leveraged to address the critical need for all-optical control of second-order nonlinearities in nanophotonics. We report our approach can be generically adopted in a variety of material and device platforms, offering a new class of complex nonlinear media with promising potentials for all-optical information processing.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Upconversion of Infrared Light by Graphitic Microparticles Due to Photoinduced Structural Modification

Recent reports of upconversion and white light emission from graphitic particles warrant an explanation of the physics behind the process. A model is offered, wherein the upconversion is facilitated by photoinduced electronic structure modification allowing for multiphoton processes. As per the prediction of the model, it is experimentally shown that graphite upconverts infrared light centered around 1.31 μm (0.95 eV) to broadband white light centered around 0.85 μm (1.46 eV). The results suggest that upconversion from shortwave infrared (≈3 μm, 0.45 eV) to visible region may be possible. The experiments show that the population dynamics of the electronic states involved in this upconversion process occur in the timescale of milliseconds.

Sharma, Rohin↗

Disentangling the effects of non-adiabatic interactions upon ion self-diffusion within warm dense hydrogen

Warm dense matter is a material state in the region of parameter space connecting condensed matter to classical plasma physics. In this intermediate regime, we investigate the significance of non-adiabatic electron-ion interactions upon ion dynamics. To disentangle non-adiabatic from adiabatic electron-ion interactions, we compare the ion self-diffusion coefficient from the non-adiabatic electron force field computational model with an adiabatic, classical molecular dynamics simulation. A classical pair potential developed through a force-matching algorithm ensures the only difference between the models is due to the electronic inertia. Here, we implement this new method to characterize non-adiabatic effects on the self-diffusion of warm dense hydrogen over a wide range of temperatures and densities. Ultimately we show that the impact of non-adiabatic effects is negligible for equilibrium ion dynamics in warm dense hydrogen.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Interfacial electron transfer of perylenes: Influence of the anchor binding mode

Interfacial electron transfer (IET) through saturated single-linker and dual-linker groups from a perylene chromophore into nanostructured TiO2 films was studied by ultrafast spectroscopy. Perylene chromophores with one and two propanoic acid linker groups in the peri and ortho positions were investigated. In comparison to previously studied perylenes bound via unsaturated acrylic acid linkers, the chromophores with saturated linkers showed bi-exponential IET dynamics. Two distinct transfer times were observed that indicate the presence of two concurrent binding modes. A comparison between ortho- and peri-substituted sensitizers resulted in slower IET dynamics and weaker electronic coupling for ortho substitution. Finally, IET from sensitizers with saturated linker groups is neither promoted nor hindered by a second linker group. This indicates that only one of the two linkers binds covalently to the surface. This study reveals the importance of the anchor-binding mode and design considerations of the linker for regulating IET.

Chemistry↗

Ghost-imaging-enhanced noninvasive spectral characterization of stochastic x-ray free-electron-laser pulses

Abstract High-intensity ultrashort X-ray free-electron laser (XFEL) pulses are revolutionizing the study of fundamental nonlinear x-ray matter interactions and coupled electronic and nuclear dynamics. To fully exploit the potential of this powerful tool for advanced x-ray spectroscopies, a noninvasive spectral characterization of incident stochastic XFEL pulses with high resolution is a key requirement. Here we present a methodology that combines high-acceptance angle-resolved photoelectron time-of-flight spectroscopy and ghost imaging to enhance the quality of spectral characterization of x-ray free-electron laser pulses. Implementation of this noninvasive high-resolution x-ray diagnostic can greatly benefit the ultrafast x-ray spectroscopy community by functioning as a transparent beamsplitter for applications such as transient absorption spectroscopy in averaging mode as well as covariance-based x-ray nonlinear spectroscopies in single-shot mode where the shot-to-shot fluctuations inherent to a self-amplified spontaneous emission (SASE) XFEL pulse are a powerful asset.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

First Flight of the Gamma-Ray Imager Polarimeter for Solar Flares (GRIPS) Instrument

The Gamma-Ray Imager/Polarimeter for Solar ares (GRIPS) instrument is a balloon-borne telescope designed to study solar-flare particle acceleration and transport. We describe GRIPS's first Antarctic long-duration flight in January 2016 and report preliminary calibration and science results. Electron and ion dynamics, particle abundances and the ambient plasma conditions in solar flares can be understood by examining hard X-ray (HXR) and gamma-ray emission (20 keV to 10 MeV). Enhanced imaging, spectroscopy and polarimetry of flare emissions in this energy range are needed to study particle acceleration and transport questions. The GRIPS instrument is specifically designed to answer questions including: What causes the spatial separation between energetic electrons producing hard X-rays and energetic ions producing gamma-ray lines? How anisotropic are the relativistic electrons, and why can they dominate in the corona? How do the compositions of accelerated and ambient material vary with space and time, and why? GRIPS's key technological improvements over the current solar state of the art at HXR/gamma-ray energies, the Reuven Ramaty High Energy Solar Spectroscopic Imager (RHESSI), include 3D position-sensitive germanium detectors (3D-GeDs) and a single-grid modulation collimator, the multi-pitch rotating modulator (MPRM). The 3D-GeDs have spectral FWHM resolution of a few hundred keV and spatial resolution less than 1cu mm. For photons that Compton scatter, usually greater or equal to 150 keV, the energy deposition sites can be tracked, providing polarization measurements as well as enhanced background reduction through Compton imaging. Each of GRIPS's detectors has 298 electrode strips read out with ASIC/FPGA electronics. In GRIPS's energy range, indirect imaging methods provide higher resolution than focusing optics or Compton imaging techniques. The MPRM grid-imaging system has a single-grid design which provides twice the throughput of a bi-grid imaging system like RHESSI. The grid is composed of 2.5 cm deep tungsten-copper slats, and quasi-continuous FWHM angular coverage from 12.5-162 arcsecs are achieved by varying the slit pitch between 1-13 mm. This angular resolution is capable of imaging the separate magnetic loop footpoint emissions in a variety of are sizes. In comparison, RHESSI's 35-arcsec resolution at similar energies makes the footpoints resolvable in only the largest ares.

Duncan, Nicole↗

Frequency Control and Disturbance Containment Using Grid-Forming Embedded Storage Networks

The paper presents a distributed approach for operating a network of inverter-based energy storage resources embedded in a bulk power system. Departing from their traditional role of steady-state reserves, the storage assets in the network are utilized as frequency-responsive resources shaping system dynamics. The power electronics converter systems interfacing the storage resources are equipped with local controllers designed to respond under transient disturbances. To this end, a safety-constrained distributed control strategy is explored. The paper compares the performance of converter-interfaced grid-forming and grid-following storage networks for fast frequency control and disturbance containment/localization. Sensitivity studies are performed to study the impact of storage size, steady-state dispatch, and controller design on dynamic performance. The findings are presented through case studies with results from the IEEE test systems.

Chatterjee, Kaustav (ORCID:0000000153273860)↗

Role of effective mass and long-range interactions in the band-gap renormalization of photoexcited semiconductors

Understanding how to control changes in the electronic structure and related dynamical renormalizations by external driving fields is the key for understanding ultrafast spectroscopy and applications in electronics. Here, we focus on the band gap's modulation by external electric fields and uncover the effect of band dispersion on the gap renormalization. We employ the Green's function formalism using the real-time Dyson expansion to account for dynamical correlations induced by photodoping. The many-body formalism captures the dynamics of systems with long-range interactions, carrier mobility, and variable electron and hole effective mass. We also demonstrate that mean-field simulations based on the Hartree-Fock Hamiltonian, which lacks dynamical correlations, yields a qualitatively incorrect picture of band-gap renormalization. We find the trend that increasing effective mass, thus decreasing mobility, leads to as much as a 6% enhancement in band-gap renormalization. Further, the renormalization is strongly dependent on the degree of photodoping. As the screening induced by free electrons and holes effectively reduces any long-range and interband interactions for highly excited systems, we show that there is a specific turnover point with a minimal band gap. Here, we further demonstrate that the optical gap renormalization follows the same trend though its magnitude is altered by the Moss-Burstein effect.

Approximation methods for many-body systems↗

Giant isotope effect on phonon dispersion and thermal conductivity in methylammonium lead iodide

Lead halide perovskites are strong candidates for high-performance low-cost photovoltaics, light emission, and detection applications. A hot-phonon bottleneck effect significantly extends the cooling time of hot charge carriers, which thermalize through carrier–optic phonon scattering, followed by optic phonon decay to acoustic phonons and finally thermal conduction. To understand these processes, we adjust the lattice dynamics independently of electronics by changing isotopes. We show that doubling the mass of hydrogen in methylammonium lead iodide by replacing protons with deuterons causes a large 20 to 50% softening of the longitudinal acoustic phonons near zone boundaries, reduces thermal conductivity by ~50%, and slows carrier relaxation kinetics. Phonon softening is attributed to anticrossing with the slowed libration modes of the deuterated molecules and the reduced thermal conductivity to lowered phonon velocities. Our results reveal how tuning the organic molecule dynamics enables control of phonons important to thermal conductivity and the hot-phonon bottleneck.

36 MATERIALS SCIENCE↗

Ligand-Structure-Dependent Coherent Vibrational Wavepacket Dynamics in Pyrazolate-Bridged Pt(II) Dimers

Bimetallic transition metal complexes have gained increasing attention because of their versatile functions in solar energy conversion and photonics applications arising from inter-metal electronic coupling. In bimetallic platinum (Pt) complexes, electronic communication between the Pt-centered and ligand-centered moieties have been shown to be critical for defining their excited-state dynamic trajectories undergoing either localized ligand centered (LC)/metal-to-ligand-charge-transfer (MLCT) transitions or delocalized metal-metal-to-ligand-charge-transfer (MMLCT) transitions. The branching of the excited-state intersystem crossing (ISC) trajectories are modulated through structural factors that alter the relative energies of the different states. In this study, we investigated the correlation of the structural factors influencing the excited state trajectories. Using femtosecond broadband transient absorption (fs-BBTA) spectroscopy, ultrafast dynamics in the excited state of two select Pt(II) dimers have been mapped out using their coherent vibrational wavepacket signatures in corresponding transient absorption spectra. To examine how the ligand moieties of the Pt(II) dimers influence excited-state dynamics and the coherent vibrational wavepacket behavior, here we carried out comparative studies on two pyrazolate-bridged Pt(II) dimers of the general formula [Pt( t Bu 2 Pz)(N^C)] 2 ( t Bu 2 Pz = 3,5-di-tert-butylpyrazole); N^C = 7,8-benzoquinoline (bzq, 1) or 1-phenylisoquinoline (piq, 2)). We found that photoexcitation into the low energy absorption bands of 1 and 2 respectively induce the formation of 1 MMLCT states from which ultrafast ISC proceeds, resulting in stimulated emission quenching and decoherence of the vibrational wavepacket motions. The results obtained in this study suggest that both energetics and the structural rigidity of the aromatic cyclometalating ligands in 1 and 2 can significantly influence dynamics along the excited state trajectory characterized by dephasing of the coherent oscillations. The collective results provide direct evidence of how ligand structure alters electronic dynamics along excited state trajectories associated with ISC processes, providing insight into using ligand design to steer photochemical processes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Status of Dynamic Radioisotope Power System Development for NASA Missions

Under the Radioisotope Power Systems Program, NASA and the Department of Energy have been advancing a novel Radioisotope Power System (RPS) based on dynamic energy conversion. This approach will manifest a dynamic RPS (DRPS) option with a conversion efficiency at least three times greater than thermoelectric based RPS. Significant progress has recently been made towards this end. A one-year system design phase has been completed by industry partner Aerojet Rocketdyne which resulted in a 300-We DRPS with convertor-level redundancy. In-house technology development at NASA Glenn Research Center has demonstrated the conversion devices in relevant environments and shown all requirements can be met. Progress has also been made on the control electronics necessary for dynamic energy conversion. Flight-like controllers were recently upgraded and achieved an 11-percentage-point increase in efficiency. Control architectures have been developed to handle the multi-convertor arrangements in the latest DRPS design. A system-level DRPS Testbed is being assembled now that will experimentally demonstrate the DRPS concept being pursued.

Stirling↗