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At least 631 records · Page 35

Photodriven Ammonia Synthesis from Manganese Nitrides: Photophysics and Mechanistic Investigations

Ammonia synthesis from N,N,O,O-supported manganese(V) nitrides and 9,10-dihydroacridine using proton-coupled electron transfer and visible light irradiation in the absence of precious metal photocatalysts is described. While the reactivity of the nitride correlated with increased absorption of blue light, excited-state lifetimes determined by transient absorption were on the order of picoseconds. Furthermore, this eliminated excited-state manganese nitrides as responsible for bimolecular N–H bond formation. Spectroscopic measurements on the hydrogen source, dihydroacridine, demonstrated that photooxidation of 9,10-dihydroacridine was necessary for productive ammonia synthesis. Transient absorption and pulse radiolysis data for dihydroacridine provided evidence for the presence of intermediates with weak E–H bonds, including the dihydroacridinium radical cation and both isomers of the monohydroacridine radical, but notably these intermediates were unreactive toward hydrogen atom transfer and net N–H bond formation. Additional optimization of the reaction conditions using higher photon flux resulted in higher rates of the ammonia production from the manganese(V) nitrides due to increased activation of the dihydroacridine.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

The Illumination of Thunderclouds by Lightning: 2. The Effect of GLM Instrument Threshold on Detection and Clustering

Abstract Lightning is measured from space using optical instruments that detect transient changes in the illumination of the cloud top. How much of the flash (if any) is recorded by the instrument depends on the instrument detection threshold. NOAA's Geostationary Lightning Mapper (GLM) employs a dynamic threshold that varies across the imaging array and changes over time. This causes flashes in certain regions and at night to be recorded in greater detail than other flashes, and threshold inconsistencies will impose biases on all levels of GLM data products. In this study, we quantify the impact of the varying GLM threshold on event/group/flash detection, flash clustering, and gridded product generation by imposing artificial thresholds on the event data taken from a thunderstorm with a low instrument threshold (∼0.7 fJ). We find that even modest increases in threshold severely impact event (60% loss by 2 fJ, 90% loss by 10 fJ) and group (25% loss by 2 fJ, 81% loss by 10 fJ) detection by suppressing faint illumination of the cloud top from weak sources and scattering. Flash detection is impacted less by threshold increases (4% loss by 2 fJ), but reductions are still significant at higher thresholds (35% loss by 10 fJ, or 44% if single‐group flashes are removed). Undetected pulses cause individual flashes to be split and severely impact the construction of gridded products. All of these factors complicate the interpretation of GLM data, particularly when trended over time under a changing threshold.

54 ENVIRONMENTAL SCIENCES↗

Studies of laser stimulated photodetachment from nanoparticles for particle charge measurements

Determining nanoparticle charge is more challenging than that for microparticles due to change in the particle size during the synthesis substantial plasma property variations, and difficulties in visualizing individual particles, rendering conventional microparticle charge diagnostics ineffective in dusty plasma. In this work, we utilized laser-stimulated photodetachment (LSPD) to deduce the mean charge of nanoparticles. Nanoparticles were grown in an Ar/C 2 H 2 mixture using a capacitively coupled RF discharge and the LSPD induced changes in the electron current monitored by a cylindrical Langmuir probe. LSPD signals were obtained and analyzed across different dust growth phases. The prolonged decay of electron current pulses was attributed to the presence of residual negative ions, caused by the effective electrostatic trapping of these ions and the potential post—LSPD re-formation of new ones. The particle charge was estimated by combining the laser-stimulated photodetachment signal from the probe with the dust density obtained from laser-light extinction using the measured nanoparticle size distribution. For a nanoparticles size range of approximately 100–250 nm and mean diameter of $d$ p ∼154.37 nm, the effective mean charge was estimated to be $\langle$$Q$$\rangle$ d $≈$ 37 elementary charge units. The measured charge values are lower than those predicted by orbital motion limited theory, which may be attributed to significant electron depletion in the nanodusty plasma. LSPD results in Ar/C 2 H 2 nano-dusty plasma confirm the applicability of this method for estimating individual nanoparticle charges. However, it has also been demonstrated that electron detachment from residual background negative ions can influence the detachment current decay and must be carefully considered.

dust particle charge↗

A CUPID Li2100MoO4 scintillating bolometer tested in the CROSS underground facility

A scintillating bolometer based on a large cubic Li$_{2}$$^{100}$MoO$_4$ crystal (45 mm side) and a Ge wafer (scintillation detector) has been operated in the CROSS cryogenic facility at the Canfranc underground laboratory in Spain. The dual-readout detector is a prototype of the technology that will be used in the next-generation $0\nu2\beta$ experiment CUPID. The measurements were performed at 18 and 12 mK temperature in a pulse tube dilution refrigerator. This setup utilizes the same technology as the CUORE cryostat that will host CUPID and so represents an accurate estimation of the expected performance. The Li$_{2}$$^{100}$MoO$_4$ bolometer shows a high energy resolution of 6 keV FWHM at the 2615 keV $\gamma$ line. The detection of scintillation light for each event triggered by the Li$_{2}$$^{100}$MoO$_4$ bolometer allowed for a full separation ($\sim$8$\sigma$) between $\gamma$($\beta$) and $\alpha$ events above 2 MeV. The Li$_{2}$$^{100}$MoO$_4$ crystal also shows a high internal radiopurity with $^{228}$Th and $^{226}$Ra activities of less than 3 and 8 $\mu$Bq/kg, respectively. Taking also into account the advantage of a more compact and massive detector array, which can be made of cubic-shaped crystals (compared to the cylindrical ones), this test demonstrates the great potential of cubic Li$_{2}$$^{100}$MoO$_4$ scintillating bolometers for high-sensitivity searches for the $^{100}$Mo $0\nu2\beta$ decay in CROSS and CUPID projects.

47 OTHER INSTRUMENTATION↗

Exploring Fabrication of Ultra-low Absorption, Multilayer, Hafnium High Reflectors

Ultra-low absorption, high damage threshold coatings are critical for the advancement of the high power CW laser technologies, and in most cases, are a limiting factor for the output power. Since high power CW laser systems enable extremely high power irradiances, when the light is incident on an HR mirror, part of the energy is absorbed and converted into heat, which can have many detrimental side effects. The worst-case scenarios are optical distortion and laser-induced damage. These optics must operate reliably with irradiances of 100's kW/cm 2 to MW/cm 2 . The highest pulsed laser damage threshold high reflectors are consistently fabricated with hafnia material. However, hafnia is not the material of choice for high power CW laser systems because of very high absorption and scatter properties, factors of >100x higher than tantala-silica, due to its poly crystalline nature. This study focuses on CW laser use applications, where the coatings’ laser damage resistance is largely limited by the inherent absorption of the coating materials. The goal is to study the feasibility of utilizing a “composite” hafnium-silica and a “doped” hafnia-silica target materials to prohibit crystallization. The results from the study were extremely successful. Hafnia high reflectors coatings generated from this study exhibited one micron absorption values of approximately 1 ppm, which are the lowest reported values to date.

36 MATERIALS SCIENCE↗

Polysiloxane Scintillators for Efficient Neutron and Gamma-Ray Pulse Shape Discrimination

Plastic scintillators based on thermoplastics, such as polystyrene and poly(vinyl toluene) (PVT), are capable of neutron and γ radiation detection via pulse shape discrimination (PSD) when overdoped with select fluorescent molecules. This class of plastic scintillator has been extensively studied but is limited to applications suitable for thermoplastics. For applications requiring flexibility, scintillators composed of elastomers, such as polysiloxanes, offer an alternative to PVT scintillators. Polysiloxane scintillators are inherently flexible and have a short processing time on the order of 3 h in air and equivalent or better detection capability at reduced doping concentration (<5 wt %). This work presents polysiloxane-based scintillators, containing only 1–5 wt % of 2,5 diphenyl-oxazole (PPO) or 9,9-dimethyl-2-phenyl-9H-fluorene (PhF) as primary dopants and 9,9-dimethyl-2,7-distyryl-9H-fluorene (SFS) as a wavelength shifter. A 5 wt % PPO polysiloxane sample had improved neutron and gamma ray PSD and comparable light yield than EJ-299-33 tested under the same conditions, i.e., figure of merit (FoM) of 1.33 ± 0.03 at 450 keV ee and light yield of 94% relative to EJ-299-33. The 5 wt % PhF-polysiloxane sample had a higher light yield, 144% of EJ-299-33 but lower FoM under the same conditions (FoM of 1.09 ± 0.03). Furthermore, this work highlights the potential of polysiloxanes as a matrix for PSD capable plastic scintillators.

36 MATERIALS SCIENCE↗

Nanoscale reshaping of resonant dielectric microstructures by light-driven explosions

Femtosecond-laser-assisted material restructuring employs extreme optical intensities to localize the ablation regions. To overcome the minimum feature size limit set by the wave nature of photons, there is a need for new approaches to tailored material processing at the nanoscale. Here, we report the formation of deeply-subwavelength features in silicon, enabled by localized laser-induced phase explosions in prefabricated silicon resonators. Using short trains of mid-infrared laser pulses, we demonstrate the controllable formation of high aspect ratio (>10:1) nanotrenches as narrow as ~ $λ / 80$. The trench geometry is shown to be scalable with wavelength, and controlled by multiple parameters of the laser pulse train, such as the intensity and polarization of each laser pulse and their total number. Particle-in-cell simulations reveal localized heating of silicon beyond its boiling point and suggest its subsequent phase explosion on the nanoscale commensurate with the experimental data. The observed femtosecond-laser assisted nanostructuring of engineered microstructures (FLANEM) expands the nanofabrication toolbox and opens exciting opportunities for high-throughput optical methods of nanoscale structuring of solid materials.

42 ENGINEERING↗

Electro-optic characterization of synthesized infrared-visible light fields

The measurement and control of light field oscillations enable the study of ultrafast phenomena on sub-cycle time scales. Electro-optic sampling (EOS) is a powerful field characterization approach, in terms of both sensitivity and dynamic range, but it has not reached beyond infrared frequencies. Here, we show the synthesis of a sub-cycle infrared-visible pulse and subsequent complete electric field characterization using EOS. The sampled bandwidth spans from 700 nm to 2700 nm (428 to 110 THz). Tailored electric-field waveforms are generated with a two-channel field synthesizer in the infrared-visible range, with a full-width at half-maximum duration as short as 3.8 fs at a central wavelength of 1.7 µm (176 THz). EOS detection of the complete bandwidth of these waveforms extends it into the visible spectral range. To demonstrate the power of our approach, we use the sub-cycle transients to inject carriers in a thin quartz sample for nonlinear photoconductive field sampling with sub-femtosecond resolution.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Strong-field Driven Sub-cycle Band Structure Modulation and Dephasing Control

In this work, we present measurements of ultrafast electric-field observables in magnesium oxide using a non-resonant nonlinear optical interaction. Using field observables, we show that strong laser fields modulate the band structure on sub-cycle timescales, thereby altering the material’s nonlinear optical response. We perform time-dependent perturbation theory calculations using a field-dependent dispersion relation and semiconductor Bloch equation calculations, both of which agree with experimental observations. Furthermore, we extract pulse decay times from the real-time signal electric field envelope and show sub-cycle control of dephasing times. Our work offers a new perspective on strong-field-driven electron dynamics in solids through electric-field observables. The demonstrated attosecond modulation of the nonlinear response could have important implications for quantum light generation and quantum spectroscopy using nonlinear optical processes.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

The Illumination of Thunderclouds by Lightning: 1. The Extent and Altitude of Optical Lightning Sources

Abstract Optical space‐based lightning sensors including NOAA's Geostationary Lightning Mapper (GLM) detect lightning though its transient illumination of the surrounding clouds. What space‐based optical lightning sensors measure is influenced by the physical attributes of the light source, the location of the source within the cloud scene, and the spatial variations in cloud composition. We focus on the lightning channels that serve as optical sources for GLM groups and flashes in this first part of our thundercloud illumination study. We match Lightning Mapping Array (LMA) sources with GLM groups and flashes during two thunderstorms to examine channel segments that are active during optical emission. We find that in each storm, the LMA sources matched with GLM groups are small (median: 3 km) compared to GLM pixels (nominal: 8 km), and preferentially come from high altitudes in the cloud (>8–10 km). The detection advantage for high‐altitude sources permits GLM to resolve faint optical pulses near the cloud top that might be missed from lower altitudes. However, the most energetic groups can be detected from all altitudes, and the largest groups largely originate at low altitudes. The relationship between group energy and illuminated area depends on flash development within the cloud medium, and flash development into different cloud regions can be identified by tracking GLM metrics of cloud illumination over time.

58 GEOSCIENCES↗

Comparative analysis of new crystal and plastic scintillators for fast and thermal neutron detection

This paper considers scintillation and physical properties of efficient organic scintillators tested as single crystals and as components of plastics with pulse shape discrimination (PSD). For the first time, single crystals of 9,9-dimethyl-2-phenyl-9H-fluorene (PhF) were grown for studies of the basic scintillation properties of this new compound. Comparison to classical organic crystals, like anthracene, trans-stilbene, and p-terphenyl, and to more recently introduced organic glass showed that the new crystal belongs to a group of the most efficient scintillators, with light output exceeding that of trans-stilbene and PSD comparable to that of p-terphenyl. Furthermore, additional studies were conducted to evaluate scintillation performance and physical properties, like hardness and dye leaching, of plastic scintillators prepared with PhF, organic glass, and liquid diisopropylnaphthalene (DIPN) that were considered as examples for potential replacement of PPO (2,5-diphenyloxazole) in current commercial PSD plastic scintillators. Comparison of the highest performing plastic scintillators prepared with these dyes shows that PhF formulations produced a record light output (LO) increase of 69 % relative to EJ-200. Similar improvements obtained with 6 Li-loaded formulations showed that future development of PSD plastics should not be limited to use of PPO but must involve the search and exploration of new efficient dyes that may lead to discovery of much brighter organic scintillators with improved physical properties required for fast and thermal neutron detection, fast neutron spectroscopy, and antineutrino detection applications.

9,9-dimethyl-2-phenyl-9H-fluorene↗

Nonresonant Raman Control of Ferroelectric Polarization

Important advances is recently made in the search for materials with complex multi-phase landscapes that host photoinduced metastable collective states with exotic functionalities. In almost all cases so far, the desired phases are accessed by exploiting light–matter interactions via the imaginary part of the dielectric function through above-bandgap or resonant mode excitation. Nonresonant Raman excitation of coherent modes is experimentally observed and proposed for dynamic material control, but the resulting atomic excursion is limited to perturbative levels. Here, in this study, this challenge is overcome by employing nonresonant ultrashort pulses with low photon energies well below the bandgap. Using mid-infrared pulses, ferroelectric reversal is induced in lithium niobate, and the large-amplitude mode displacements are characterized through femtosecond stimulated Raman scattering and second harmonic generation. This approach, validated by first-principle calculations, defines a novel method for synthesizing hidden phases with unique functional properties and manipulating complex energy landscapes at reduced energy consumption and ultrafast speeds.

Shi, Jiaojian [Stanford Univ., CA (United States);↗

Driving ultrafast spin and energy modulation in quantum well states via photo-induced electric fields

Abstract The future of modern optoelectronics and spintronic devices relies on our ability to control the spin and charge degrees of freedom at ultrafast timescales. Rashba spin-split quantum well states, 2D states that develop at the surface of strong spin-orbit coupling materials, are ideal given the tunability of their energy and spin states. So far, however, most studies have only demonstrated such control in a static way. In this study, we demonstrate control of the spin and energy degrees of freedom of surface quantum well states on Bi 2 Se 3 at picosecond timescales. By means of a focused laser pulse, we modulate the band-bending, producing picosecond time-varying electric fields at the material’s surface, thereby reversibly modulating the quantum well spectrum and Rashba effect. Moreover, we uncover a dynamic quasi-Fermi level, dependent on the Lifshitz transition of the second quantum well band bottom. These results open a pathway for light-driven spintronic devices with ultrafast switching of electronic phases, and offer the interesting prospect to extend this ultrafast photo-gating technique to a broader host of 2D materials.

36 MATERIALS SCIENCE↗

Coupled nuclear–electronic decay dynamics of O2 inner valence excited states revealed by attosecond XUV wave-mixing spectroscopy

Multiple Rydberg series converging to the $O_2^+$ c $^{4}Σ^{-}_{u}$ state, accessed by 20-25 eV extreme ultraviolet (XUV) light, serve as important model systems for the competition between nuclear dissociation and electronic autoionization. The dynamics of the lowest member of these series, the $3sσ_g $ state around 21 eV, has been challenging to study owing to its ultra-short lifetime (<10 fs). Here, we apply transient wave-mixing spectroscopy with an attosecond XUV pulse to investigate the decay dynamics of this electronic state. Lifetimes of 5.8 ± 0.5 fs and 4.5 ± 0.7 fs at 95% confidence intervals are obtained for v = 0 and v = 1 vibrational levels of the 3s Rydberg state, respectively. A theoretical treatment of predissociation and electronic autoionization finds that these lifetimes are dominated by electronic autoionization. The strong dependence of the electronic autoionization rate on the internuclear distance because of two ionic decay channels that cross the 3s Rydberg state results in the different lifetimes of the two vibrational levels. The calculated lifetimes are highly sensitive to the location of the 3s potential with respect to the decay channels; by slight adjustment of the location, values of 6.2 and 5.0 fs are obtained computationally for the v = 0 and v = 1 levels, respectively, in good agreement with experiment. Overall, an intriguing picture of the coupled nuclear-electronic dynamics is revealed by attosecond XUV wave-mixing spectroscopy, indicating that the decay dynamics are not a simple competition between isolated autoionization and predissociation processes.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Techniques for studying materials under extreme states of high energy density compression

The properties of materials under extreme conditions of pressure and density are of key interest to a number of fields, including planetary geophysics, materials science, and inertial confinement fusion. In geophysics, the equations of state of planetary materials, such as hydrogen and iron, under ultrahigh pressure and density provide a better understanding of their formation and interior structure [Celliers et al., “Insulator-metal transition in dense fluid deuterium,” Science 361, 677–682 (2018) and Smith et al., “Equation of state of iron under core conditions of large rocky exoplanets,” Nat. Astron. 2, 591–682 (2018)]. The processes of interest in these fields occur under conditions of high pressure (100 GPa–100 TPa), high temperature (>3000 K), and sometimes at high strain rates (>103 s−1) depending on the process. With the advent of high energy density (HED) facilities, such as the National Ignition Facility (NIF), Linear Coherent Light Source, Omega Laser Facility, and Z, these conditions are reachable and numerous experimental platforms have been developed. To measure compression under ultrahigh pressure, stepped targets are ramp-compressed and the sound velocity, measured by the velocity interferometer system for any reflector diagnostic technique, from which the stress-density of relevant materials is deduced at pulsed power [M. D. Knudson and M. P. Desjarlais, “High-precision shock wave measurements of deuterium: Evaluation of exchange-correlation functionals at the molecular-to-atomic transition,” Phys. Rev. Lett. 118, 035501 (2017)] and laser [Smith et al., “Equation of state of iron under core conditions of large rocky exoplanets,” Nat. Astron. 2, 591–682 (2018)] facilities. To measure strength under high pressure and strain rates, experimenters measure the growth of Rayleigh–Taylor instabilities using face-on radiography [Park et al., “Grain-size-independent plastic flow at ultrahigh pressures and strain rates,” Phys. Rev. Lett. 114, 065502 (2015)]. The crystal structure of materials under high compression is measured by dynamic x-ray diffraction [Rygg et al., “X-ray diffraction at the national ignition facility,” Rev. Sci. Instrum. 91, 043902 (2020) and McBride et al., “Phase transition lowering in dynamically compressed silicon,” Nat. Phys. 15, 89–94 (2019)]. Medium range material temperatures (a few thousand degrees) can be measured by extended x-ray absorption fine structure techniques, Yaakobi et al., “Extended x-ray absorption fine structure measurements of laser-shocked V and Ti and crystal phase transformation in Ti,” Phys. Rev. Lett. 92, 095504 (2004) and Ping et al., “Solid iron compressed up to 560 GPa,” Phys. Rev. Lett. 111, 065501 (2013), whereas more extreme temperatures are measured using x-ray Thomson scattering or pyrometry. This manuscript will review the scientific motivations, experimental techniques, and the regimes that can be probed for the study of materials under extreme HED conditions.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Time Refraction of Spin Waves

Here, we present an experimental study of time refraction of spin waves (SWs) propagating in microscopic waveguides under the influence of time-varying magnetic fields. Using space- and time-resolved Brillouin light scattering microscopy, we demonstrate that the broken translational symmetry along the time coordinate results in a loss of energy conservation for SWs and thus allows for a broadband and controllable shift of the SW frequency. With an integrated design of SW waveguide and microscopic current line for the generation of strong, nanosecond-long, magnetic field pulses, a conversion efficiency up to 39% of the carrier SW frequency is achieved, significantly larger compared to photonic systems. Given the strength of the magnetic field pulses and its strong impact on the SW dispersion relation, the effect of time refraction can be quantified on a length scale comparable to the SW wavelength. Furthermore, we utilize time refraction to excite SW bursts with pulse durations in the nanosecond range and a frequency shift depending on the pulse polarity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Ultrafast Dynamics of Intrinsic Anomalous Hall Effect in the Topological Antiferromagnet Mn 3 Sn

Here, we investigate ultrafast dynamics of the anomalous Hall effect (AHE) in the topological antiferromagnet Mn 3 ⁢Sn with sub-100 fs time resolution. Optical pulse excitations largely elevate the electron temperature up to 700 K, and terahertz probe pulses clearly resolve ultrafast suppression of the AHE before demagnetization. The result is well reproduced by microscopic calculation of the intrinsic Berry-curvature mechanism while the extrinsic contribution is clearly excluded. Our work opens a new avenue for the study of nonequilibrium AHE to identify the microscopic origin by drastic control of the electron temperature by light.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Measuring Local Turbulence Along the Optical Path: Multi-Beam Optical Seeing Sensor

Deflection of light along the optical path is a major source of image degradation for ground-based telescopes. Methods have been developed to measure upper atmospheric seeing based on models of the turbulence in the atmosphere, but due to boundary conditions, transmission within telescope enclosures is more complex. The Multi-beam Optical Seeing Sensor (MOSS) directly measures the component of the image quality degradation from inhomogeneity of the index of refraction within the telescope dome. MOSS outputs four near-parallel beams of light that travel along the optical path and are imaged by the telescope’s detector, landing like starlight on the telescope’s focal plane. By using a strobed light source, we can ‘freeze’ the instantaneous index variations transverse to the optical path. This system captures both ‘dome’ and ‘mirror’ seeing. Through plotting the standard deviation of differential motion between pairs of beams, MOSS enables characterization of the length scale of turbulence within the dome. The temporal coherence of temperature gradients can be probed with different pulse lengths, and the spatial coherence by comparing pairs at different separations across the aperture of the telescope. Optical path turbulence measurements, alongside other telemetry metrics, will guide thermal and airflow management to optimize image quality. A MOSS prototype was installed in the 1.2[Formula: see text]m Auxiliary Telescope (AuxTel) at the Vera C. Rubin Observatory in Chile, and preliminary data constrain the optical path turbulence with a lower bound of 1.4 arcsec. The optical path turbulence varied throughout the night of observing.

Astronomical seeing↗