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At least 559 records · Page 31

Carrier and Phonon Dynamics in Multilayer WSe 2 Captured by Extreme Ultraviolet Transient Absorption Spectroscopy

Carrier and phonon dynamics in a multilayer WSe2 film are captured by extreme ultraviolet (XUV) transient absorption (TA) spectroscopy at the W N 6,7 , W O 2,3 , and Se M 4,5 edges (30–60 eV). After the broadband optical pump pulse, the XUV probe directly reports on occupations of optically excited holes and phonon-induced band renormalizations. Here, when compared with density functional theory calculations, XUV transient absorption due to holes is identified below the W O 3 edge whereas signals at the Se M 4,5 edges are dominated by phonon dynamics. Therein, 0.4 ps hole relaxation time, 1.5 ps carrier recombination time, and 1.7 ps phonon heating time are extracted. The acquisition of hole and phonon-induced signals in a single experiment can facilitate the investigation of the correlations between electron and phonon dynamics. Furthermore, the simultaneous observation of signals from different elements can be further extended to explore photochemical processes in multilayers and alloys, thereby providing key information for their applications in electronics, photocatalysts, and spintronics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Diagrammatic analysis of the density operator for nonlinear optical calculations Pulsed and CW responses

In the present paper a diagrammatic analysis of the density operator for the evaluation of nonlinear optical quantities is considered. The present approach extends earlier diagrammatic analysis by treating the time evolution of both the wave function and its complex conjugate. Time-ordered graphs result, each of which corresponds to a term in the density matrix. Examples involving the third-order susceptibility are discussed for both monochromatic and pulse excitation. In particular coherent rotational transient birefringence is discussed. The diagrams provide a convenient means by which nonlinear optical processes can be precisely defined and the susceptibility readily evaluated.

Yee, T. K.↗

The Illumination of Thunderclouds by Lightning: 4. Volumetric Thunderstorm Imagery

Optical instruments such as the Geostationary Lightning Mapper (GLM) detect lightning based on transient changes in cloud illumination. The horizontal location of lightning is determined from the coordinates of the pixels on the imaging array illuminated during the flash. However, the vertical position of the lightning pulses (approximated by GLM “groups”) below the cloud top cannot be routinely measured from a single space-based instrument. In our prior work, we have developed a machine learning algorithm that can infer optical source altitude for a given pulse based on how the optical energy is distributed across the group footprint and the local Advanced Baseline Imager Cloud-Top Height (CTH). In this fourth part of our thundercloud illumination study, we leverage these source altitudes to generate volumetric GLM imagery of a Colombia thunderstorm. We find that 3D versions of the current GLM meteorological imagery products (that describe thunderstorm kinematics) and thundercloud imagery products (that depict how the flashes appear from space) provide additional insights into lightning activity in the thunderstorm that are lost in the vertical integration used to generate the current 2D GLM gridded products. This new volumetric imaging capability provides a more comprehensive picture of where lightning occurs in the storm, how its physical characteristics vary across three-dimensional space, and how its optical emissions interact with surrounding the cloud medium.

54 ENVIRONMENTAL SCIENCES↗

Neutrino Target-of-Opportunity Observations with Space-based and Suborbital Optical Cherenkov Detectors

Cosmic-ray accelerators capable of reaching ultra-high energies are expected to also produce very high energy neutrinos via hadronic interactions within the source or its surrounding environment. Many of the candidate astrophysical source classes are either transient in nature or exhibit flaring activity. Using the Earth as a neutrino converter, suborbital and space-based optical Cherenkov detectors, such as POEMMA and EUSO-SPB2, will be able to detect upward-moving extensive air showers induced by decaying tau-leptons generated from cosmic tau neutrinos with energies ∼ 10 PeV and above. Both EUSO-SPB2 and POEMMA will be able to quickly repoint, enabling rapid response to astrophysical transient events. We calculate the transient sensitivity and sky coverage for both EUSO-SPB2 and POEMMA, accounting for constraints imposed by the Sun and the Moon on the observation time. We also calculate both detectors’ neutrino horizons for a variety of modeled astrophysical neutrino fluences. We find that both EUSO-SPB2 and POEMMA will achieve transient sensitivities at the level of modeled neutrino fluences for nearby sources. We conclude with a discussion of the prospects of each mission detecting at least one transient event for various modeled astrophysical neutrino sources.

Tonia M Venters↗

Controlling Ligand Excimer Formation with Dipole Changes in Emissive Rare-Earth/Phosphonic Acid Complexes

The interactions between substituted arylvinyl phosphonic acid (AVPA) ligands within a Eu-AVPA complex are shown to influence the outcomes of excited state evolution after photoexcitation. Compared with unfunctionalized AVPAs, pairs of ligands functionalized with CF 3 in the para position preassociate in the ground state of complexes with Eu 3+ according to calculated geometry optimizations. The CF 3 -substituted AVPA complexes show evidence of red-shifted optical absorption and undergo more efficient excimer formation, as revealed by transient absorption spectroscopy. We rationalize this behavior through simulations of excited-state geometry optimizations that reveal evolution toward interligand phenyl-phenyl planarity for specific excited states. Emission from complexed Eu 3+ after energy transfer from the ligand is found to be weaker with CF 3 substitution, which we hypothesize is due to intracomplex, interligand aggregates with excimer-promoting geometries. These observations point to the need to consider ground-state geometries as well as dynamic excited-state processes to understand the flow of energy in rare earth coordination complexes.

09 BIOMASS FUELS↗

Non-equilibrium entropy production and information dissipation in a non-Markovian quantum dot

This study measures trajectory-level entropy production and information dissipation in a driven, non-Markovian quantum dot using time-resolved optical dynamics and machine-learning-based analysis. Although not a 2D-material system, it is relevant because it demonstrates quantitative extraction of nonequilibrium dynamics from nanoscale optical fluctuations, which is conceptually connected to the proposed studies of transient charge and spin dynamics at interfaces.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Investigation of laser dynamics, modulation and control by means of intra-cavity time varying perturbation

Work continued on a number of projects aimed at the generation of tunable visible, infrared, and ultraviolet light; and on the control of this light by means of novel mode-locking and modulation techniques. Progress is summarized for the following projects: (1) the transient modelocking of the Nd:YAG laser and application of short optical pulses; (2) studies of the sodium-xenon excimer laser; (3) development of techniques for vacuum ultraviolet holography; and (4) studies of multiple photon pumped xenon and argon excimer lasers.

Harris, S. E.↗

Improved LEEM ranges over four decades

Low-energy electron magnetometer is suitable for terrestrial and aerial applications. Electron beam strikes tantalum collector plates in device, amplifying current and converting it to frequency. Current difference increases with beam deflection, providing measure of local field strength. LEEM operation requires no liquid helium unlike superconducting quantum interference device. LEEM sensitivity compares favorably with that of optical absorption magnetometers, and microsecond response range makes analyzing fast magnetic transients and signatures possible.

Singh, J. J.↗

The Outbursts and Orbit of the Accreting Pulsar GS 1843-02=2S 1845-024

We present observations of a series of 10 transient outbursts of pulsed hard x-ray flux from the 10.6 mHz accreting pulsar GS 1843-02 using the Burst and Transient Source Experiment (BATSE) on the Compton Observatory. These outbursts occurred regularly every 242 days, coincident with the ephemeris of the periodic transient GRO J1849-03 (Zhang et al. 1996)), which has recently been identified with the the SAS 3 source 2S 1845-024 (Soffitta et al. 1998). Our pulsed detection provides the first clear identification of GS 1843-02 with 2S 1845-024. We present a pulse timing analysis which shows that the 2S 1845-024 outbursts occur near the periastron passage of a highly eccentric (e = 0.88 q 0.01) 242.18 +/- 0.01 day period binary orbit about a high mass (M(sub opt) > 7 solar mass companion. The orbit and transient outburst pattern suggest a Be star/X-ray pulsar system, however the optical companion is unknown. Our observations show a long-term spin-up trend, with most of the spin-up occurring during the outbursts. From the measured spin-up rates and inferred mass accretion rates we conclude that an accretion disk is present during the outbursts.

Finger, Mark H.↗

FORTE Measurements of Global Optical Lightning Waveforms and Implications for Optical Lightning Detection

Lightning processes generate a diverse collection of optical pulses from current traversing the lightning channels. These signals are then broadened spatially and temporally via scattering in the clouds. The resulting waveforms measured from space with instruments like the photodiode detector (PDD) on the Fast On-orbit Recording of Transient Events (FORTE) satellite have a variety of shapes. In this study, we use coincident optical and Radio-Frequency measurements to document the properties of optical PDD waveforms associated with different types of lightning, estimate delays from scattering in the clouds, and comment on how pulse shape impacts optical lightning detection. We find that the attributes of optical pulses recorded by the PDD are consistent with prior studies, but vary globally and with event amplitude. The most powerful lightning tends to be single-peaked with faster rise times (median: ~100 µs) and shorter effective widths (median: ~400 µs) than normal lightning. Particularly dim events, meanwhile, include cases of broad optical waveforms with sustained optical emission throughout the PDD record, which the pixelated FORTE Lightning Location System (LLS) instrument has difficulty detecting. We propose that this is due to the optical signal being divided between individual LLS pixels that are each, individually, not bright enough to trigger. We use PDD waveforms and Monte Carlo radiative transfer modeling to demonstrate that increasing the temporal and spatial resolution of a pixelated lightning imager will make it more difficult to detect these broad/dim pulses as their energy becomes divided between additional pixels/integration frames.

54 ENVIRONMENTAL SCIENCES↗

Limitations of cetane number to predict transient combustion phenomena in high-pressure fuel sprays

Fundamental understanding of in-cylinder processes in diesel engines is important to screen emerging biofuels and advanced combustion modes that can reduce greenhouse gas emissions and regulated pollutants including soot. In this study, the role of fuel properties on spray development and combustion is investigated by systematically isolating chemical and thermophysical effects. Three different fuels are considered, two with similar chemical properties and two with similar thermophysical properties with one fuel common to both groups. Experiments are performed in a constant-pressure flow chamber de-signed to provide stable test conditions and facilitate acquisition of at least 150 injections in quick succession for each fuel under reacting conditions at high-pressure, high-temperature ambient conditions using a modified conventional diesel engine injector. Further, high speed optical diagnostics including rainbow schlieren deflectometry, OH* chemiluminescence, and a two-color pyrometry system are employed to simultaneously image the transient spray and reacting jets. Image analysis is performed to determine liquid length, vapor penetration length, timing and location of first stage and main ignition events, lift-off location, total soot mass, and more. Results show that fuels with similar chemical properties or cetane number (CN) exhibit similar delay times for first stage and main ignition events as may be expected, but very different liquid length, first stage and main ignition locations, lift-off length, apparent turbulent flame speed, and soot formation. As such, the ability to characterize candidate biofuels with CN or other parameters derived from simple flame configurations is called into question. In this study, thermo-physical properties controlling the liquid length are identified as the main contributing factor for the observed differences.

33 ADVANCED PROPULSION SYSTEMS↗

Stimulated Emission from Below the Bandgap in Giant Quantum Shells

Colloidal semiconductor nanocrystals (NCs) have emerged as promising candidates for developing solution-processable optical gain media, with potential applications in integrated photonic circuits and lasers. However, the deployment of NCs in these technologies has been hindered by nonradiative Auger recombination of multiexciton states, which shortens the optical gain lifetime and reduces its spectral range. Here, we demonstrate that these limitations can be overcome by using giant colloidal quantum shells (g-QSs), comprising a quantum-confined CdSe shell grown over a large (~14 nm) CdS bulk core. Such bulk-nanoscale architecture minimizes exciton–exciton interactions, leading to suppressed Auger recombination and one of the broadest gain bandwidths reported for colloidal nanomaterials, spanning energies both above and, remarkably, below the bandgap. Ultrafast transient absorption and photoluminescence measurements demonstrate that the high-energy portion of optical gain arises from states containing more than 15 excitons per particle while the unusual sub-bandgap gain behaviour results from an Auger-assisted radiative recombination, a mechanism that has traditionally been viewed as a loss pathway. Altogether, these results reveal a unique gain regime associated with bulk-nanocrystal hybrid systems, which offers a promising path toward solution-processable light sources.

Absorption↗

Coherent helicity-dependent spin-phonon oscillations in the ferromagnetic van der Waals crystal CrI3

Abstract The discovery of two-dimensional systems hosting intrinsic magnetic order represents a seminal addition to the rich landscape of van der Waals materials. CrI 3 is an archetypal example, where the interdependence of structure and magnetism, along with strong light-matter interactions, provides a new platform to explore the optical control of magnetic and vibrational degrees of freedom at the nanoscale. However, the nature of magneto-structural coupling on its intrinsic ultrafast timescale remains a crucial open question. Here, we probe magnetic and vibrational dynamics in bulk CrI 3 using ultrafast optical spectroscopy, revealing spin-flip scattering-driven demagnetization and strong transient exchange-mediated interactions between lattice vibrations and spin oscillations. The latter yields a coherent spin-coupled phonon mode that is highly sensitive to the driving pulse’s helicity in the magnetically ordered phase. Our results elucidate the nature of ultrafast spin-lattice coupling in CrI 3 and highlight its potential for applications requiring high-speed control of magnetism at the nanoscale.

36 MATERIALS SCIENCE↗

Light-Induced Transient Lattice Dynamics and Metastable Phase Transition in CH 3 NH 3 PbI 3 Nanocrystals

In this study, methylammonium lead iodide (MAPbI 3 ) perovskite nanocrystals (NCs) offer desirable optoelectronic properties with prospective utility in photovoltaics, lasers, and light-emitting diodes (LEDs). Structural rearrange-ments of MAPbI 3 in response to photoexcitation, such as lattice distortions and phase transitions, are of particular interest, as these engender long carrier lifetime and bolster carrier diffusion. Here, we use variable temperature X-ray diffraction (XRD) and synchrotron-based transient X-ray diffraction (TRXRD) to investigate lattice response following ultrafast optical excitation. MAPbI 3 NCs are found to slowly undergo a phase transition from the tetragonal to a pseudocubic phase over the course of 1 ns under 0.02-4.18 mJ/cm 2 fluence photoexcitation, with apparent nonthermal lattice distortions attributed to polaron formation. Lattice recovery exceeds time scales expected for both carrier recombination and thermal dissipation, indicating meta-stability likely due to the proximal phase transition, with symmetry-breaking along equatorial and axial directions. These findings are relevant for fundamental understanding and applications of structure-function properties.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Exosat and IUE observations of SW UMa during superoutburst

IUE and Exosat observations obtained during the March 1986 superoutburst of the SU UMa type dwarf nova SW UMa are presented. The observations show the presence of a hot, extensive, optically thick disk. The UV fluxes show an increase of 1000 over the quiescent values, implying a large increase in mass accretion rate. The Exosat obserations show an increase in the soft X-ray count rate by a factor of 44 over quiescence, while the medium-energy flux remains undetected. The most surprising result is that the softness ratio in superoutburst is similar to the quiescent value of 0.3. No variation at the orbital or spin periods or at the superhump period are evident in the superoutburst X-ray data. A transient variation is observed at 5.1 minutes similar to that observed in the optical a few days after the X-ray observations.

Szkody, Paula↗

Kilonova light-curve interpolation with neural networks

Kilonovae are the electromagnetic transients created by the radioactive decay of freshly synthesized elements in the environment surrounding a neutron star merger. To study the fundamental physics in these complex environments, kilonova modeling requires, in part, the use of radiative transfer simulations. The microphysics involved in these simulations results in high computational cost, prompting the use of emulators for parameter inference applications. Utilizing a training set of 22 248 high-fidelity simulations (composed of 412 unique ejecta parameter combinations evaluated at 54 viewing angles), we use a neural network to efficiently train on existing radiative transfer simulations and predict light curves for new parameters in a fast and computationally efficient manner. Our neural network can generate millions of new light curves in under a minute. We discuss our emulator's degree of off-sample reliability and parameter inference of the AT2017gfo observational data. Finally, we discuss tension introduced by multiband inference in the parameter inference results, particularly with regard to the neural network's recovery of viewing angle. Published by the American Physical Society 2024

79 ASTRONOMY AND ASTROPHYSICS↗

Radiation-Induced Long-Lived Transients and Metal Particle Formation in Solid KCl–MgCl 2 Mixtures

Here, the electron paramagnetic resonance and diffuse reflectance-optical absorption spectra of room-temperature γ-irradiated KCl–MgCl 2 binary solid salt mixtures (98:2 mol % and 2:98 mol %) and the eutectic (68:32 mol %) are reported. Additionally, powder X-ray diffraction of the pristine salts and thermal annealing studies of the irradiated salts were performed to evaluate the radiolysis product stability, annihilation, and association in metallic particles. The main long-lived transient species detected in 98:2 mol % KCl–MgCl 2 salts were perturbed F-centers, that is, trapped electrons (e t – ) in the vicinity of Mg ions (λ max at 561 nm), and the radiolytic reduction of Mg 2+ to Mg + and Mg 0 . Thermal annealing promoted the diffusion of defects to yield polycations (Mg n + ). On the other hand, irradiation of 2:98 mol % KCl/MgCl 2 salts showed the formation of cationic and neutral Mg dimers (Mg 2 + and Mg 2 ) and trimers as well as centers with a rhombic powder pattern apparently consisting of an electron shared between three Mg 2+ nuclei associated with an anion vacancy (ν a + –Mg 3 5+ ). Trapped electrons (e t – ) (F-centers) were not observed in the irradiated eutectic mixture; instead, Mg 2 , Mg 0 , and Cl 3 – were observed. It was observed that the higher temperature for thermal ionization of radiation-reduced Mg species decreased the extent of electron recombination reactions and the disproportionation of Cl 3 – compared to the pure KCl but enhanced the aggregation of Mg into larger metallic microstructures (metallic particles).

36 MATERIALS SCIENCE↗