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At least 1,387 records · Page 77

Tellurene Photodetector with High Gain and Wide Bandwidth

Two-dimensional (2D) semiconductors have been extensively explored as a new class of materials with great potential. In particular, black phosphorus (BP) has been considered to be a strong candidate for applications such as high-performance infrared photodetectors. However, the scalability of BP thin film is still a challenge, and its poor stability in the air has hampered the progress of the commercialization of BP devices. Herein, we report the use of hydrothermal-synthesized and air-stable 2D tellurene nanoflakes for broadband and ultrasensitive photodetection. The tellurene nanoflakes show high hole mobilities up to 458 cm 2 /V·s at ambient conditions, and the tellurene photodetector presents peak extrinsic responsivity of 383 A/W, 19.2 mA/W, and 18.9 mA/W at 520 nm, 1.55 μm, and 3.39 μm light wavelength, respectively. Because of the photogating effect, high gains up to 1.9 × 10 3 and 3.15 × 10 4 are obtained at 520 nm and 3.39 μm wavelength, respectively. At the communication wavelength of 1.55 μm, the tellurene photodetector exhibits an exceptionally high anisotropic behavior, and a large bandwidth of 37 MHz is obtained. The photodetection performance at different wavelength is further supported by the corresponding quantum molecular dynamics (QMD) simulations. Our approach has demonstrated the air-stable tellurene photodetectors that fully cover the short-wave infrared band with ultrafast photoresponse.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Advances in Colloidal InP-Based Quantum Dots for Photocatalytic Hydrogen Evolution

Photocatalytic materials for hydrogen generation are typically categorized into UV-absorbing metal oxides and visible-range semiconductors such as chalcogenides or perovskites, which often incorporate toxic elements. To address environmental concerns of the latter group, indium phosphide (InP)-based quantum dots (QDs) have recently emerged as a less toxic alternative. These nanocrystals (NCs) benefit from a broadband and tunable absorption spectrum, which is well matched for solar photochemistry, and offer suitable electronic characteristics to drive photoinduced charge separation. This perspective provides a comprehensive summary of the recent advancements in developing InP-based NCs with a focus on photocatalytic hydrogen production. We discuss synthetic strategies that enhance the catalytic activity of these materials and highlight key challenges that must be addressed to enhance their performance. Finally, we explore future research directions aimed at improving photocatalytic efficiency and integrating InP-based QDs into practical solar-to-fuel conversion systems.

Hydrogen↗

Carrier-Envelope Phase Control in Terahertz Pulse Generation Using InAs Ribbon Metasurfaces

Generation of broadband terahertz (THz) pulses with variable polarization and carrier-envelope phase can enable the tailoring of THz beam wavefronts for advanced applications in THz imaging and spectroscopy and for strong THz field optics. While metasurfaces composed of deeply subwavelength THz emitters have recently been demonstrated to define the polarization and spatial profile of the generated THz fields, precise phase control or synthesis of THz pulse waveforms remains a challenging problem. Here, we propose and demonstrate metasurfaces composed of indium arsenide (InAs) nanoscale ribbon arrays capable of generating THz pulses with variable carrier-envelope phase. We show that different THz generation mechanisms, each contributing distinct phases, can be activated in the ribbons, enabling carrier-envelope phase control spanning a range of π over a wide band of frequencies (∼1–3 THz). This is achieved solely through the ribbon array geometry using linearly polarized optical excitation of the ribbons. The arrays enable precise control of the THz phase and amplitude, opening the door to advanced structured THz wavefront synthesis using ultrathin dielectric metasurfaces.

carrier-envelope phase↗

Terahertz Spectroscopy of Gas Mixtures with Dual Quantum Cascade Laser Frequency Combs

Terahertz laser frequency combs based on quantum cascade lasers provide coherent, broadband, electrically pumped, THz radiation sources for use in future spectroscopic applications. In this work, we explore the feasibility of such lasers in a dual-comb spectroscopy configuration for the detection of multiple molecular samples in the gas phase. The lasers span approximately 180 GHz of optical bandwidth, centered at 3.4 THz, with submilliwatt total optical power. One of the main advantages of dual-comb spectroscopy is its high speed, which opens up the possibility for direct observations of chemical reaction dynamics in the terahertz spectral region. As a proof-of-concept, we recorded continuously evolving spectra from gas mixtures with 1 ms temporal resolution.

42 ENGINEERING↗

Reaching 90% Photoluminescence Quantum Yield in One-Dimensional Metal Halide C 4 N 2 H 14 PbBr 4 by Pressure-Suppressed Nonradiative Loss

Low-dimensional perovskite-related metal halides have emerged as a new class of light-emitting materials with tunable broadband emission from self-trapped excitons (STEs). Although various types of low-dimensional structures have been developed, fundamental understating of the structure–property relationships for this class of materials is still very limited, and further improvement of their optical properties remains greatly important. Here, we report a significant pressure-induced photoluminescence (PL) enhancement in a one-dimensional hybrid metal halide C 4 N 2 H 14 PbBr 4 , and the underlying mechanisms are investigated using in situ experimental characterization and first-principles calculations. Under a gigapascal pressure scale, the PL quantum yields (PLQYs) were quantitatively determined to show a dramatic increase from the initial value of 20% at ambient conditions to over 90% at 2.8 GPa. With in situ characterization of photophysical properties and theoretical analysis, we found that the PLQY enhancement was mainly attributed to the greatly suppressed nonradiative decay. Pressure can effectively tune the energy level of self-trapped states and increase the exciton binding energy, which leads to a larger Stokes shift. The resulting highly localized excitons with stronger binding reduce the probability for carrier scattering, to result in the significantly suppressed nonradiative decay. Overall, our findings clearly show that the characteristics of STEs in low-dimensional metal halides can be well-tuned by external pressure, and enhanced optical properties can be achieved.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Watching Excited State Dynamics with Optical and X-ray Probes: The Excited State Dynamics of Aquocobalamin and Hydroxocobalamin

Femtosecond time-resolved X-ray absorption (XANES) at the Co K-edge, X-ray emission (XES) in the Co Kβ and valence-to-core regions, and broadband UV–vis transient absorption are combined to probe the femtosecond to picosecond sequential atomic and electronic dynamics following photoexcitation of two vitamin B12 compounds, hydroxocobalamin and aquocobalamin. Polarized XANES difference spectra allow identification of sequential structural evolution involving first the equatorial and then the axial ligands, with the latter showing rapid coherent bond elongation to the outer turning point of the excited state potential followed by recoil to a relaxed excited state structure. Time-resolved XES, especially in the valence-to-core region, along with polarized optical transient absorption suggests that the recoil results in the formation of a metal-centered excited state with a lifetime of 2–5 ps. In conclusion, this combination of methods provides a uniquely powerful tool to probe the electronic and structural dynamics of photoactive transition-metal complexes and will be applicable to a wide variety of systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Real-Time Elemental and Isotopic Measurements of Molten Salt Systems through Laser-Induced Breakdown Spectroscopy

Molten salt reactors are an emerging advanced nuclear reactor concept in which the fuel is dissolved into the working fluid in the form of a high-temperature molten salt. The complex, mobile, and corrosive nature of this fluid presents a fundamental challenge for analytical measurements. Tracking species throughout the reactor is important for ensuring proper operation. This article presents laser-induced breakdown spectroscopy (LIBS) used to monitor the elemental composition of a molten salt and corresponding hydrogen isotopic shifts in real-time. A NaNO 3 –KNO 3 eutectic salt was saturated with protium and deuterium gases, then the effluent aerosol stream formed using an argon sparging vessel was monitored with LIBS. This modular LIBS system permitted several spectrometers to be used simultaneously to capture high-resolution isotopic shifts and provide broadband elemental coverage. Further, the results exhibit how LIBS can be used to understand salt–gas chemical and physical interactions such as diffusion. Furthermore, LIBS’ broad elemental coverage can provide greater insight into the chemical reactions within the salt vessel such as the formation of water vapor by monitoring hydrogen and oxygen signatures simultaneously. Ultimately, this study demonstrates the analytical possibilities of LIBS for real-time monitoring of isotopes and elemental composition in molten salt systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Acoustic Energy Release During the Laboratory Seismic Cycle: Insights on Laboratory Earthquake Precursors and Prediction

Abstract Machine learning can predict the timing and magnitude of laboratory earthquakes using statistics of acoustic emissions. The evolution of acoustic energy is critical for lab earthquake prediction; however, the connections between acoustic energy and fault zone processes leading to failure are poorly understood. Here, we document in detail the temporal evolution of acoustic energy during the laboratory seismic cycle. We report on friction experiments for a range of shearing velocities, normal stresses, and granular particle sizes. Acoustic emission data are recorded continuously throughout shear using broadband piezo‐ceramic sensors. The coseismic acoustic energy release scales directly with stress drop and is consistent with concepts of frictional contact mechanics and time‐dependent fault healing. Experiments conducted with larger grains (10.5 μm) show that the temporal evolution of acoustic energy scales directly with fault slip rate. In particular, the acoustic energy is low when the fault is locked and increases to a maximum during coseismic failure. Data from traditional slide‐hold‐slide friction tests confirm that acoustic energy release is closely linked to fault slip rate. Furthermore, variations in the true contact area of fault zone particles play a key role in the generation of acoustic energy. Our data show that acoustic radiation is related primarily to breaking/sliding of frictional contact junctions, which suggests that machine learning‐based laboratory earthquake prediction derives from frictional weakening processes that begin very early in the seismic cycle and well before macroscopic failure.

58 GEOSCIENCES↗

Fine-Scale Variability of Observed and Simulated Surface Albedo Over the Southern Great Plains

Surface albedo can be highly variable in both space and time. The Department of Energy’s Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems (HI-SCALE) field study provides a unique opportunity to characterize the variability over the Southern Great Plains of the United States using integrated tower, aircraft, and satellite observations of the surface albedo and Normalized Difference Vegetation Index (NDVI). The primary advantage of the aircraft and satellite observations is the ability to examine the spatial distribution of surface albedo and NDVI over a large area, while the tower measurements have the ability to examine both diurnal and day-to-day variability at a single location. In general, consistency was found between both the broadband (BB) albedo and NDVI measured from the surface, air and space. There was a small increase from 0.186 to 0.194 in the aircraft BB surface albedo between May and September (about 4% change), while the MODIS black-sky BB surface albedo increased from 0.151 to 0.166 over the same period (about 10% change) while the standard deviations in the aircraft and MODIS BB albedo were similar. The largest seasonal differences in both the aircraft BB albedo and NDVI were found for areas with winter wheat or forest, while areas with pasture or grasses showed a smaller seasonal diversity. The Weather Research and Forecasting (WRF) model was used to simulate the BB surface albedo. In comparison with the aircraft and satellite observations, the WRF-simulated BB surface albedo had no seasonal change and a much narrower distribution.

Berg, Larry K.↗

Infrasound and Gravity Waves Over the Andes Observed by a Pressure Sensor on Board a Stratospheric Balloon

The study of infrasound (acoustic) and gravity waves sources and propagation in the atmosphere of a planet gives us precious insight on atmosphere dynamics, climate, and even internal structure. The implementation of modern pressure sensors with high rate sampling on stratospheric balloons is improving their study. In our work we analyzed the data from the National Aeronautics and Space Administration Ultra Long Duration Balloon mission (16 May to 30 June 2016). Here, we focus on the balloon's transit of the Andes Mountains. We detected gravity waves that are associated to troposphere convective activity and mountain waves. An increase of the horizontal wavelengths from 50 to 70 km with increasing distance to the mountains is favoring the presence of mountain waves. We also report on the detection of infrasounds generated by the mountains in the 0.01–0.1 Hz range with a pressure amplitude increase by a factor 2 relative background signal. Besides, we characterized the decrease of microbaroms power when the balloon was flying away from the ocean coast. These observations suggest, in a way similar to microseisms for seismometers, that microbaroms are the main background noise sources recorded in the stratosphere even far from the ocean sources. Finally, we observed a broadband signal above the Andes, between 0.45 and 2 Hz, probably associated with a thunderstorm. The diversity of geophysical phenomena captured in less than a day of observation stresses the interest of high rate pressure sensors on board long-duration balloon missions.

54 ENVIRONMENTAL SCIENCES↗

Lightning Interferometry Uncertainty, Beam Steering Interferometry, and Evidence of Lightning Being Ignited by a Cosmic Ray Shower

Abstract We present an uncertainty analysis on correlation‐based time delay estimate, the basis for broadband lightning interferometry. A normal interferometry would yield much higher uncertainties than the theoretically predicted lower bound due to finite correlation window lengths. However, if the signals are aligned in time, the uncertainties approach the lower bound and can be used to indicate the interferometric uncertainties. Based on this, we introduce a beam steering interferometry technique. It first estimates a direction centroid for the lightning sources with a normal interferometry and computes the time delays among the signals. It then shifts the raw data with the time delays to align the signals roughly in time and reprocess the aligned signals. It finally pushes the reprocessed results to their correct positions, based on the time delays estimated in the first step. We apply this technique on a fast positive breakdown (FPB) process that started a normal intracloud lightning. The FPB process is shown to have a much more complex structure and development than a normal interferometry would provide. More importantly, from both interferometric and polarization analyses, the FPB appears to be ignited by a cosmic ray shower (CRS). We estimate the radio frequency strength and frequency content related to a presumed CRS in a thunderstorm electric field and find that they are in agreement with the observations. We examine the electric field effect of the CRS front and find that it could raise the field above the threshold for positive breakdown and is capable of igniting the FPB (and the lightning).

Shao, Xuan‐Min↗

Using Ambient Noise Seismic Interferometry and Local and Teleseismic Earthquakes to Determine Crustal Thickness and Moho Structure of the Northwestern Gulf of Mexico Margin

Abstract The northwestern part of the Gulf of Mexico has undergone two episodes of continental rifting and collision and produced structural artifacts that are now buried under many kilometers of sediments, complicating investigations of the region. The deep sedimentary package precludes outcrops and points to a need for the application of seismic techniques, but low rates of seismicity in the region and sparse seismic monitoring limit the utility of traditional seismic methods. We therefore use diverse data to perform two‐dimensional seismic tomography across the dry land portion of the margin. Data are gleaned from teleseismic and regional earthquakes, postcritical SsPmp arrivals, and direct P wave energy identified with seismic interferometry that were recorded by a broadband, three‐component array and partially overlapping short‐period, vertical‐component array. The Pn and postcritical SsPmp phase help constrain the Moho discontinuity, which a previous receiver function study suggested was absent beneath the seaward portion of this transect. A high‐velocity body is observed in the crust at the same location as the Houston Magnetic Anomaly, possibly marking rocks from the Alleghenian continental assembly. The crust thins from NW to SE, indicating that extension occurred mostly to the south of the Ouachita orogeny. Our model indicates that the margin's sediment package reaches a maximum thickness of ~15 km at the coast and becomes unresolvably thin near the Llano Uplift.

58 GEOSCIENCES↗

Regional Moment Tensor Inversion Using Rotational Observations

There are benefits from the addition of rotational motions to translational displacements for moment tensor (MT) inversions. The rotational radiation pattern is orthogonal to the shear radiation pattern, thus incorporating rotations is equivalent to gaining another observation point on the focal sphere. We demonstrated this by simulating curl and displacement wavefields for a regional distance station. Thus, one 6-C station (3-Component translational + 3-Component rotational) gathers the same information on radiation pattern as two 3-C stations at 90° azimuth from one another along the focal plane axis, which is sometimes difficult to obtain when restricted to surface sensors. We added rotational Green's functions to a regional MT inversion scheme (long-period, time-domain, and linear inversion) by computing spatial gradients from f-κ reflectivity synthetics. For rotational data, we used Array Derived Rotations (ADR) from Piñon Flats Observatory Array and Golay array deployed during IRIS Community Wavefield Demonstration Experiment. The hope is to ultimately use compact and field deployable broadband rotational seismometers instead of ADRs. Rotational motions were predicted from well-constrained deviatoric MT solutions of nine earthquakes recorded by the arrays and other seismic networks. Additionally, we formed three station sparse datasets with (3-C and 6-C) and without rotational ground motions (3-C only) for eight earthquakes testing the benefits of including rotational waveforms in MT inversions when they are equally weighted with translational waveforms. Adding rotational motions improved the double-couple components and reduced compensated-linear-vector-dipole and isotropic components in full-MT solutions using sparse datasets with poor coverage.

58 GEOSCIENCES↗

Radio Frequency Characteristics of Volcanic Lightning and Vent Discharges

In this study, we analyze the pulse width and spectral content of vent discharges and volcanic lightning flashes. We made measurements of electrical activity with a broadband very high frequency antenna (20–80 MHz) during an explosive eruption of Sakurajima volcano on November 8, 2019. The individual impulses that comprise vent discharges and volcanic lightning were analyzed to determine the fundamental width of the impulses and the rate of fall-off of their energy spectral density. The results show that vent discharges are more similar to volcanic lightning than they are different. Here, the mean pulse width for both vent discharges and volcanic lightning was 50 ns. Both types of electrical activity had similar spectral content; the average slope of the amplitude spectra was –3.4 for both. Further, examination of the pulse width and spectral slope distributions showed that while the distributions of volcanic lightning and vent discharges are statistically distinct from each other, the distribution of vent discharges is a subset of the distribution of volcanic lightning.

58 GEOSCIENCES↗

Nano-FTIR Investigation of the CM Chondrite Allan Hills 83100

Mid-infrared (MIR) spectroscopy has been used with great success to quantitatively determine the mineralogy of geologic samples. It has been employed in a variety of contexts from determining bulk composition of powdered samples to spectroscopic imaging of rock thin sections via micro-Fourier transform infrared (micro-FTIR) imaging spectroscopy. Recent advances allow for IR measurements at the nanoscale. Near field nanoscale infrared imaging and spectroscopy with a broadband source (nano-FTIR) enable understanding of the spatial relationships between compositionally distinct materials within a sample. This will be of particular use when analyzing returned samples from Bennu and Ryugu, which are thought to be compositionally like CI or CM1/2 carbonaceous chondrites. Returned samples will likely contain olivine/pyroxene chondrules that have been transformed into hydrous phyllosilicates, sulfides, carbonates, and other alteration phases. The use of near-field infrared techniques to probe the boundaries between once pristine chondrules and alteration phases at the nanoscale is a novel approach to furthering our understanding of the compositional evolution of carbonaceous asteroids and the processes that drive their evolution. Here we report the results of nano-FTIR spectroscopy and imaging measurements performed on the carbonaceous chondrite Allan Hills (ALH) 83100 (CM1/2). We show with nanoscale resolution that spatially resolved Fe-Mg variations exist within the phyllosilicates around a chondrule rim. We also present effects of crystal orientation on the nano-FTIR spectra to account for the spectral differences between the meteorite and mineral spectra.

58 GEOSCIENCES↗

Sensitivity of the Arctic Sea Ice Cover to the Summer Surface Scattering Layer

Here, the ‘surface scattering layer’ (SSL) is the highly-scattering, coarse-grained ice layer that forms on the surface of melting, drained sea ice during spring and summer. Ice of sufficient thickness with an SSL has an observed persistent broadband albedo of ~0.65, resulting in a strong influence on the regional solar partitioning. Experiments during the MOSAiC expedition showed that the SSL re-forms in approximately one day following manual removal. Coincident spectral albedo measurements provide insight into the SSL evolution, where albedo increased on sunny days with higher solar insolation. Comparison with experiments in radiative transfer and global climate models show that the sea ice albedo is greatly impacted by the SSL thickness. The presence of SSL is a significant component of the ice-albedo feedback, with an albedo impact of the same order as melt ponds. Changes in SSL and implications for Arctic sea ice within a warming climate are uncertain.

54 ENVIRONMENTAL SCIENCES↗

Rapid Refreezing of a Marginal Ice Zone Across a Seafloor Distributed Acoustic Sensor

Abstract Seismic instruments such as broadband seismometers and distributed acoustic sensors (DAS) have a demonstrated potential for wide‐scale and continuous in situ monitoring of near‐surface environmental and anthropogenic processes. DAS is attractive for development as a multi‐geophysical observatory due to the prevalence of existing fiber infrastructure in regions with environmental, cultural, or strategic significance. Here we present results from a multi‐seasonal acquisition of DAS data on a seafloor cable in the Beaufort Sea, Alaska. During a November 2021 data collect we captured the rapid transition of ambient noise characteristics from an “ice‐free” state to an “ice‐bound” state. A sea ice formation front was plainly visible on the DAS record and was observed to propagate 20 km seaward over a period of 8 hr. Satellite‐based instrumentation were unable to record this event due to cloud cover, low light conditions, and orbital frequency.

Baker, Michael G.↗

Midwinter Dry Spells Amplify Post‐Fire Snowpack Decline

Abstract Increasing wildfire and declining snowpacks in mountain regions threaten water availability. We combine satellite‐based fire detections with snow seasonality classifications to examine fire activity in California's seasonal and ephemeral snow zones. We find a nearly tenfold increase in fire activity during 2020–2021 versus 2001–2019. Accumulation season broadband snow albedo declined 25%–71% at two burned sites (2021 and 2022) according to in‐situ data relative to un‐burned conditions, with greater declines associated with increased burn severity. By enhancing snowpack susceptibility to melt, both decreased snow albedo and canopy drove midwinter melt during a multi‐week dry spell in 2022. Despite similar meteorological conditions in December–February 2013 and 2022–linked to persistent high pressure weather regimes–minimal melt occurred in 2013. Post‐fire snowpack differences are confirmed with satellite measurements. With growing geographical overlap between wildfire and snow, our findings suggest California's snowpack is increasingly vulnerable to the compounding effects of dry spells and wildfire.

54 ENVIRONMENTAL SCIENCES↗