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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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Blockchain Applications for Nuclear Safeguards

This chapter discusses the benefits and challenges of using distributed ledger technology (DLT) for international nuclear safeguards purposes. The chap-ter introduces the international safeguards system and the role of the Inter-national Atomic Energy Agency. The chapter describes the evolution of the safeguards system, the IAEA’s core functions and the technical objectives it seeks to achieve. The chapter explains the benefits and drawbacks of deploying DLT for safeguards and presents potential use cases where the technology could be deployed. It ends with a description of the international com-munity’s current perspectives on deployment.

DLT, blockchain technology, international safeguar↗

Coupling between DNA replication, segregation, and the onset of constriction in Escherichia coli

Escherichia coli cell cycle features two critical cell-cycle checkpoints: initiation of replication and the onset of constriction. While the initiation of DNA replication has been extensively studied, it is less clear what triggers the onset of constriction and when exactly it occurs during the cell cycle. Here, using high-throughput fluorescence microscopy in microfluidic devices, we determine the timing for the onset of constriction relative to the replication cycle in different growth rates. Our single-cell data and modeling indicate that the initiation of constriction is coupled to replication-related processes in slow growth conditions. Furthermore, our data suggest that this coupling involves the mid-cell chromosome blocking the onset of constriction via some form of nucleoid occlusion occurring independently of SlmA and the Ter linkage proteins. This work highlights the coupling between replication and division cycles and brings up a new nucleoid mediated control mechanism in E. coli.

59 BASIC BIOLOGICAL SCIENCES↗

Microbubble dynamics and heat transfer in boiling droplets

Dissipating large heat fluxes from a surface is critically important in numerous industrial and natural applications. Boiling based spray cooling and surface texturing are two of the most promising methods being investigated to address this problem. Although our understanding on these topics has significantly improved over past decades, critical gaps remain in the knowledgebase stymieing the realization of their full potential. As an example, while bubble growth in pool boiling have been investigated in detail, comparatively little is known about how the bubbles evolve inside boiling drops. In the present work, we have investigated for the first time, the microbubble dynamics inside water droplets boiling on superhydrophilic textured substrates using high-speed X-ray phase contrast imaging (XRPCI). Our observations show that the transient bubble density variation follows similar characteristics irrespective of the texture spacing at a given surface temperature. For an example microstructure, we found that the number of discrete bubbles on the surface decreases as temperature is increased although their growth rate increases. Here, we observe that bubble growth is highly non-uniform during the lifetime of a drop on the surface. Initially, bubbles grow under diffusion-limited regime, but at later times they grow as ~t 1.45 due to combined effects of coalescence and evaporation. In some conditions, we found that bubbles shrink dramatically af- ter the initial growth spurt presumably due to severe quenching of the surface, and migration of bubbles on the surface. Using the bubble sizes, for the first time we analyzed the heat flux removed by a single bubble and also by all the bubbles at a given time. We find that the highest dissipation through latent- heat component (~600 W/cm 2 ) occurs just in the beginning and thereafter it decreases. We expect that our findings and the analysis would guide further work on the topic and will aid in the overarching goal of engineering surfaces that are more efficient in boiling heat transfer.

42 ENGINEERING↗

Gas generation and intramolecular isotope study in laboratory pyrolysis of the Springfield coal from the Illinois Basin

Position-specific (PS) isotopes of propane have been proposed as a potential geochemical tool to decipher various geological processes (e.g., thermal cracking, biodegradation, H exchange) in natural reservoirs. The limited studies have been conducted on the PS isotopes of propane from the pyrolysis gases from marine shales, and natural gases sourced from lacustrine and marine kerogens, but little is known on gases produced from the humic kerogen. Here, this study investigated the PS δ 13 C of propane in the closed-system pyrolysis of the Springfield coal, Illinois Basin, Indiana, at 310 to 470 °C (Easy %Ro: 0.76 to 3.07). The C kinetic isotope effect (KIE) of CH 4 produced in both this study and previous low-temperature pyrolysis of the same coal indicates the cleavage of C—O bonds is the main generation pathway at the early kerogen cracking stage, followed by the breakdown of alkyl groups. At the wet-gas cracking stage, C 3 H 8 production from thermally stable compounds has a significant influence on the bulk and position-specific C KIE in the pyrolysis of marine Woodford kerogen and Springfield coal. According to the PS δ 13 C of propane, the central site is likely more enriched in 13 C and the δ 13 C of the terminal site is relatively heterogeneous within the propyl group attached to different functional groups of the gas-prone kerogen. Our findings based on the pyrolysis experiments and natural gas samples indicate thermal cracking and biodegradation appear to alter the δ 13 C cen values more significantly than the δ 13 C ter values of propane. The larger magnitude of ΔC c-t in the kMC simulations (Peterson et al., 2018) compared with those from the marine shale and coal possibly implies the non-random distributions of 13 C of propane precursors in the kerogens. As a new dimension of intramolecular isotopic information of propane, the PS δ 13 C values can contribute to fingerprinting the gas origins and identifying the various geological processes (e.g., kerogen cracking, wet-gas cracking, microbial activities) in sedimentary basins.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A new measurement of amine steric hindrance – N exposure

Here, a new measurement of steric hindrance effect of amines, N exposure, is proposed. N exposure outperforms traditional parameters as it is independent of group-specific parame-ters and accounts for the spatial arrangements of pendant groups. Such a measurement can facilitate the screening of sterically hindered amines for carbon capture with improved CO 2 loading capacities. Along with this study, a script is provided to quantify the N exposure for other amine molecules of interest.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Tip-Enhanced Raman Scattering on Both Sides of the Schrödinger Equation

We report historically, molecular spectroscopists have focused their attention to the right-hand side of the Schrödinger equation. Our major goal had and still has to do with determining a (bio)molecular system’s Hamiltonian operator. From a theoretical spectroscopist’s perspective, this entails varying the parameters of a model Hamiltonian until the predicted observables agree with their experimental analogues. In this context, less emphasis has been put on the left-hand side of the equation, where the interplay between a system and its immediate local environment is described. The latter is particularly meaningful and informative in modern applications of optical microscopy and spectroscopy that take advantage of surface plasmons to enhance molecular scattering cross-sections and to increase the attainable spatial resolution that is classically limited by diffraction. Indeed, the manipulation of light near the apex of a metallic nanotip has enabled single molecule detection, identification, and imaging. The distinct advantages of the so-called tip-enhanced optical nanospectroscopy/nanoimaging approaches are self-evident: ultrahigh spatial resolution (nanometer or better) and ultimate sensitivity (down to yoctomolar) are both attainable, all while retaining the ability to chemically fingerprint one molecule at a time (e.g., through Raman scattering). An equally interesting aspect of the same approach stems from using the properties of a single molecule to characterize the local environment in which it resides. This concept of single molecule spectroscopy on the left-hand side of the Schrödinger equation is certainly not novel and has been discussed in pioneering single molecule studies that ultimately led to a Nobel prize in chemistry. That said, local environment mapping through ultrasensitive optical spectroscopy acquires a unique flavor when executed using tip-enhanced Raman scattering (TERS). This is the subject of this Account.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Surface Enhanced Raman Scattering Selectivity in Proteins Arises from Electron Capture and Resonant Enhancement of Radical Species

Plasmon-enhanced Raman scattering is a powerful approach to detecting and characterizing proteins in live and dynamic biological systems. However, the selective detection/enhancement of specific residues as well as spectral diffusion and fluctuations have complicated the interpretation of enhanced Raman spectra and images of biological matter. In this paper, we therefore demonstrate that the amino acid tryptophan (Trp) can capture an electron from an excited plasmon, which generates a radical anion that is resonantly enhanced: a visible excited electronic state slides into resonance upon charging. This surface enhanced resonance Raman scattering (SERRS) mechanism explains the persistence of Trp signatures in the SERS and TERS spectra of proteins. Evidence for this picture includes the observation of visible resonances in the UV-Vis extinction spectrum, changes in the ground state vibrational spectrum, and plasmon-resonance dependent behavior. DFT calculations support the experimental observations. The behavior observed from the free Trp molecule is shown to explain the SERS spectrum of the Trp-cage protein. In effect, resonant Raman scattering from radicals formed through plasmonic excitation represents an under-investigated mechanism that may be exploited for chemical sensing applications. This work was supported by the National Institutes of Health Award R01-GM109988. The authors thank Hannah Shafaat for helpful discussions and providing an azurin sample for comparison. The authors also thank Joel Harris for providing constructive comments on our manuscript.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Underlying Mechanisms of Hot Carrier-Driven Reactivity on Bimetallic Nanostructures

Bimetallic nanostructures exhibit unique catalytic activity and selectivity that is not evident for their monometallic analogs. Such nanostructures contain plasmonic metals, such as gold or silver, that afford highly efficient harvesting of electromagnetic radiation and its conversion into hot carriers. These highly energetic species are transferred to the catalytic metal sub-component of the bimetallic nanostructure, where a large spectrum of chemical reactions may be catalyzed. The strength of the electric field and the interplay between catalytic and plasmonic metals at the nanoscale are thus critically important for the catalytic activity of bimetallic nanostructures. In this study, we investigate the relationship between the catalytic activity and local electric fields sustained on the surface of gold-palladium (Au@PdNPs) and gold-platinum (Au@PtNPs) nanoplates using tip-enhanced Raman spectroscopy (TERS). We image the spatially varying magnitudes of rectified (DC) local electric fields on the surface of these nanostructures and compare them to fields sustained on the surface of monometallic nanoplates. We find substantially larger electric field magnitudes on Au@PdNPs and Au@PtNPs as compared to their monometallic analogs. These findings suggest that catalytic efficiency of bimetallic nanostructures may be mediated and potentially tuned through precise control of electric fields sustained on their surfaces.

Li, Zhandong↗

Nanophotonics for Chemical Imaging and Spectroscopy

The manipulation of light and light-matter interactions on the nanoscale is enabled by the unique optical properties of plasmonic metal nanostructures and nanoparticles. Indeed, engineered hybrid molecular-plasmonic nanostructures have enabled single molecule detection and identification via surface-enhanced Raman scattering (SERS). Further, the same effect is at the core of visualizing single molecules with sub-nanometer spatial resolution via tip-enhanced Raman scattering (TERS). More generally, modern applications of plasmon-enhanced spectroscopy and microscopy fueled advances in fields as diverse as quantum and semiconductor materials, heterogeneous catalysis, and the health sciences, to name a few. All these exciting developments and many more are touched in this virtual special issue (VSI) on nanophotonics. From ultra-precise chemical imaging measurements performed in a scanning tunneling microscope chamber to single molecule spectroscopic measurements performed at solid-air and solid-liquid interfaces, this VSI includes contributions from active practitioners that are all striving to better-understand increasingly complex interfaces encountered in the biological, materials, and chemical sciences.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

The Prevalence of Anions at Plasmonic Nanojunctions: A Closer Look at P-Nitrothiophenol

We revisit the reductive coupling of p-nitrothiophenol (NTP) to form dimercaptoazobenzene (DMAB), herein monitored through gap-mode tip-enhanced Raman spectroscopy (TERS) and nano-imaging. We employ a plasmonic Au probe (100 nm diameter at its apex) illuminated with a 633 nm laser source (50 ?W/?m2 at the sample position) to image a NTP-coated faceted silver nanoparticle (~70 nm diameter). A detailed analysis of the recorded spectra reveals that anionic NTP species contribute to the recorded spectral images, in addition to the more thoroughly described DMAB product. Notably, the signatures of the anions are more pronounced than those of the DMAB product under our present experimental conditions. Our results thus demonstrate that anions and their spectral signatures must be considered in the analysis of plasmon-enhanced spectra and images.

Wang, Chih-Feng↗

Synthesis of Cp* Terphenylamido U(III) Iodide Complexes with a Substitutable Iodide Position to Generate Terminal U(III)–(κ 3 -BH 4 ) Complexes

Reaction of Cp*UI 2 (THF) 3 (Cp* = pentamethylcyclopentadienide; THF = tetrahydrofuran) with Na R3 TerNH ( R3 Ter = 2,6(2,4,6-R 3 C 6 H 2 ) 2 C 6 H 3 ; R = Me, Et, iPr) gave the U(III) monoiodide complexes Cp*( R3 TerNH)UI (R = Me, 1-Me; R = Et, 2-Et; R = iPr, 3-iPr). These complexes contain a functionalizable iodide position which reacts favorably with NaBH4 to give the κ 3 -borohydride complexes Cp*( R3 TerNH)U(H 3 BH) (R = Me, 4-Me; R = Et, 5-Et; R = iPr, 6-iPr). All compounds were experimentally characterized by SC-XRD, 1 H and 11 B NMR spectroscopy as well as UV–vis–NIR and FTIR analyses. DFT calculations corroborate the experimental findings, confirming the 5f 3 U(III) configuration across the entire series and revealing an increased U 5f orbital contribution in the borohydride derivatives. All compounds exhibit small but non-negligible U(III)–(η 6 -arene) δ-back-bonding interactions arising from the unpaired 5f electrons. Calculated steric parameters show progressively greater shielding of the U(III) center with increasing bulk of the terphenyl substituents from Me to iPr.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Author Correction: Genome-guided isolation of the hyperthermophilic aerobe Fervidibacter sacchari reveals conserved polysaccharide metabolism in the Armatimonadota

Correction to: Nature Communicationshttps://doi.org/10.1038/s41467-024-53784-3, published online 4 November 2024 In the version of this article initially published, Table 1 did not include the properties of the taxa being proposed or refer directly to another location in the main manuscript describing the properties. As such, the original manuscript did not comply with Rule 27 (2)(c) of the ICNP. Also, Table 1 listed the order Fervidibacterales as the nomenclatural type for the class Fervidibacteria, which violates latest emended version of Rule 15 stating that the nomenclatural type for a class must be a genus. Below we provide a modification of Table 1 containing protologues with these errors corrected. We have also changed the order of the taxa in the table to meet the most common ordering. (Table presented.) Taxon names proposed under the ICNP Proposed taxon Etymology Description Genus Fervidibacter Fer.vi.di.bac’ter. L. masc. adj. fervidus, hot, steaming; N.L. masc. n. bacter, a rod; N.L. masc. n. Fervidibacter, a hot rod Thermophilic or hyperthermophilic inhabitants of freshwater thermal environments. All members are likely polysaccharide-degrading chemoheterotrophs with numerous carbohydrate-active enzymes encoded in their genomes. Aerobic, with high-affinity and/or low-affinity terminal oxidases present in the genomes. The oxidative pentose phosphate pathway and the tricarboxylic acid cycle are complete in genomes belonging to the genus. Gram-stain-negative and diderm cell envelope structure. Ovoid- to rod-shaped morphology. Spores are not formed. The genus is a distinct phylogenetic lineage in the family Fervidibacteraceae, the order Fervidibacterales, and the class Fervidibacteria in the phylum Armatimonadota. The type species is Fervidibacter sacchariT. Species Fervidibacter sacchari sac’cha.ri. N.L. gen. n. sacchari, of sugar Hyperthermophilic, microaerophilic, facultatively anaerobic, and grows chemoheterotrophically on monosaccharides and polysaccharides. Cells are ovoid- to rod-shaped, Gram-stain negative, and are 0.9–1.3 µm in width and 1.6–3.6 µm in length. Grows between 65 and 87.5 °C and an optimum temperature of 80 °C, and a pH range of 6.5–8.6 with an optimum pH of 7.5. Grows at an optimum O2 concentration of 5–10%. Grows on D-arabinose, D-galactose, D-glucose, D-rhamnose, D-ribose, D-xylose, chondroitin sulfate, colloidal chitin, galactan, gellan gum, guar gum, karaya gum, locust bean gum, xantham gum, xyloglucan, β-glucan, glycogen, starch, AFEX-pretreated corn stover, miscanthus, sugarcane bagasse, acetate and casamino acids. Grows weakly on xyloglucan under fermentation conditions. The major fatty acids (>10%) are C16:0, C18:0 and/or cyclo-C17:0, and iso-C16:0. The major respiratory quinones (>10%) are MK-8 and MK-9. The isolate and genomes of the species have been recovered from geothermal springs in the Great Basin, Nevada, USA. GC content of genomes range between 51–52%. Subunits for both the high-affinity and low-affinity terminal oxidases are encoded in the genomes. Genomes also encode a Group 3d [NiFe] hydrogenase, which produces hydrogen as an electron sink for NAD+ regeneration. The type strain PD1T (= JCM 39283T = DSM 113467T) was isolated from Great Boiling Spring in Nevada, USA. Family Fervidibacteraceae Fer.vi.di.bac.te.ra’ce.ae. N.L. masc. n. Fervidibacter type genus of the family; L. suff. -aceae ending to denote a family; N.L. fem. pl. n. Fervidibacteraceae the family of the genus Fervidibacter Thermophilic or hyperthermophilic inhabitants of freshwater thermal environments. All members are likely polysaccharide-degrading chemoheterotrophs with numerous carbohydrate-active enzymes encoded in their genomes. Aerobic, with high-affinity and/or low-affinity terminal oxidases present in the genomes. The oxidative pentose phosphate pathway and the tricarboxylic acid cycle are complete in genomes belonging to the family. The family is a distinct phylogenetic lineage in the order Fervidibacterales and the class Fervidibacteria in the phylum Armatimonadota. The type genus is Fervidibacter. Order Fervidibacterales Fer.vi.di.bac.te.ra’les. N.L. masc. n. Fervidibacter type genus of the order; L. suff. -ales ending to denote an order; N.L. fem. pl. n. Fervidibacterales the order of the genus Fervidibacter Thermophilic or hyperthermophilic inhabitants of freshwater thermal environments. All members are likely polysaccharide-degrading chemoheterotrophs with numerous carbohydrate-active enzymes encoded in their genomes. Aerobic or strictly anaerobic. Phylogenomic placement of this lineage within the Fervidibacteria and relative evolutionary divergence supports delineation of this lineage as an order within the class Fervidibacteria and phylum Armatimonadota. The type genus is Fervidibacter. Class Fervidibacteria Fer.vi.di.bac.te’ri.a. N.L. masc. n. Fervidibacter type genus of the type order of the class; L. suff. -ia ending to denote a class; N.L. neut. pl. n. Fervidibacteria the class of the order Fervidibacterales Thermophilic or hyperthermophilic inhabitants of freshwater thermal environments. All members are likely polysaccharide-degrading chemoheterotrophs with numerous carbohydrate-active enzymes encoded in their genomes. Aerobic or strictly anaerobic. Phylogenomic placement of this lineage within the Armatimonadota and relative evolutionary divergence supports delineation of this lineage as a class within the Armatimonadota. The type genus is Fervidibacter. The error has not been corrected in the PDF or HTML versions of the Article.

Nou, Nancy O↗

Molecular imaging of plant-microbe interactions on the Brachypodium seed surface

Plant growth-promoting rhizobacteria (PGPR) play a crucial role in biological control and pathogenic defense on and with-in plant tissues, however the mechanism(s) by which plants associate with PGPR to elicit such beneficial effects needs further study. Here, we present high mass resolution time-of-flight secondary ion mass spectrometry (ToF-SIMS) imaging of Brachypodium distachyon (Brachypodium) seeds with and without exposure to two model PGPR, i.e., Gram-negative Pseudomonas fluorescens SBW25::GFP (P.) and Gram-positive Arthrobacter chlorophenolicus A6::GFP (A.). Delayed image extraction was used to image PGPB-treated seed sections to reveal morphological changes. ToF-SIMS spectral compari-son, principal component analysis (PCA), and two-dimensional (2D) imaging show that the selected PGPR have different effects on the host seed surface, resulting in changes in chemical composition and morphology. Metabolite prod-ucts and biomarkers, such as flavonoids, phenolic com-pounds, fatty acids, and indole-3-acetic acid (IAA), were ob-served on the PGPR-treated seed surfaces. These compounds had different distributions on the Brachypodium seed surface for the two PGPR, indicating that the different bacteria elicited distinct responses from the host. Our results illustrate that ToF-SIMS is an effective tool to study plant-microbe interac-tions and to provide insightful information with submicrome-ter lateral resolution of the chemical distributions associated with morphological features, potentially offering a new way to study the mechanisms underlying beneficial roles of PGPR.

PGPR, Brachypodium distachyon, ToF-SIMS, metabolit↗

High-volume and -adiabat capsule (“HVAC”) ignition: Lowered fuel compression requirements using advanced Hohlraums

Lower-than-expected deuterium–tritium fuel areal densities have been experimentally inferred across a variety of high-convergence, nominally low-adiabat implosion campaigns at the National Ignition Facility (NIF) using cylinder-shaped Hohlraums [Hurricane et al., Phys. Plasmas 26, 052704 (2019)]. A leading candidate explanation is the presence of atomic mix between the fuel and ablator from hydrodynamic instability growth [Clark et al., Phys. Plasmas 26, 050601 (2019)], leading to reduced fuel compressibility and an effectively higher (in-flight) fuel adiabat α. Tolerating a high-α implosion can be obtained with significantly higher capsule absorbed energy Ecap according to the one-dimensional (1-D) ignition-threshold-factor analytic scaling [S. Atzeni and J. Meyer-ter-Vehn, Nucl. Fusion 41, 465 (2001)], ITF∼Ecap·α−1.8. Recent experiments with large Al shells in rugby-shaped Hohlraums have established high laser-capsule coupling efficiencies of ≽ 30% [Ping et al., Nat. Phys. 15, 138 (2019)], enabling a path to Ecap≽ 0.5 MJ at the NIF and increased performance margin M ≡ ITF − 1. The ability to operate at high adiabat with large capsules using nonstandard Hohlraums leads to the predicted onset of a volume-ignition mode, defined as when both the entire fuel is the “hot spot” and inertial confinement is principally provided by the ablator compared with the compressed fuel. Such an ignition mode, normally reserved for high-Z targets, e.g., double shells [Amendt et al., Phys. Plasmas 14, 056312 (2007)], is predicted to lead to lower fuel convergence and less exposure to mix due to the intended high adiabat—but at the expense of ∼3–4 × reduced (1-D) yield compared with conventional central hot-spot ignition designs.

Amendt, Peter (ORCID:0000000174021777)↗

Homogeneous, Micron-Scale High-Energy-Density Matter Generated by Relativistic Laser-Solid Interactions

Short-pulse, laser-solid interactions provide a unique platform for studying complex high-energy-density mat ter. We present the first demonstration of solid density, micron-scale keV plasmas uniformly heated by a high contrast, 400 nm laser at intensities up to 2×10 21 W/cm 2 . High-resolution spectral analysis of X-ray emission reveals uniform heating up to 3.0 keV over 1 µm depths. Particle-in-cell simulations indicate the production of a uniformly heated keV plasma to depths of 2 µm. The significant bulk heating and presence of highly-ionized ions deep within the target are attributed to the few MeV hot electrons that become trapped and undergo refluxing within the target sheath fields. In conclusion, these conditions enable the differentiation of atomic physics models such as ionization potential depression in high energy density environments.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Improving Deep Neural Networks’ Training for Image Classification With Nonlinear Conjugate Gradient-Style Adaptive Momentum

Momentum is crucial in stochastic gradient-based optimization algorithms for accelerating or improving training deep neural networks (DNNs). In deep learning practice, the momentum is usually weighted by a well-calibrated constant. However, tuning the hyperparameter for momentum can be a significant computational burden. In this article, we propose a novel adaptive momentum for improving DNNs training; this adaptive momentum, with no momentum-related hyperparame- ter required, is motivated by the nonlinear conjugate gradient (NCG) method. Stochastic gradient descent (SGD) with this new adaptive momentum eliminates the need for the momentum hyperparameter calibration, allows using a significantly larger learning rate, accelerates DNN training, and improves the final accuracy and robustness of the trained DNNs. For example, SGD with this adaptive momentum reduces classification errors for training ResNet110 for CIFAR10 and CIFAR100 from 5.25% to 4.64% and 23.75% to 20.03%, respectively. Furthermore, SGD, with the new adaptive momentum, also benefits adversarial training and, hence, improves the adversarial robustness of the trained DNNs.

97 MATHEMATICS AND COMPUTING↗

Low-Level Liquid-Bearing Clouds Contribute to Seasonal Lower Atmosphere Stability and Surface Energy Forcing over a High-Mountain Watershed Environment

Measurements of atmospheric structure and surface energy budgets distributed along a high-altitude moun tain watershed environment near Crested Butte, Colorado, from two separate, but coordinated, field campaigns, Surface Atmosphere Integrated field Laboratory (SAIL) and Study of Precipitation, the Lower Atmosphere, and Surface for Hydrometeorology (SPLASH), are analyzed. This study identifies similarities and differences in how clouds influence the radiative budget over one snow-free summer season (2022) and two snow-covered seasons (2021/22; 2022/23) for this alpine location. A relationship between lower-tropospheric stability stratification and longwave radiative flux from the presence or absence of clouds is identified. When low clouds persisted, often with signatures of supercooled liquid in win ter, the lower troposphere experienced weaker stability, while radiatively clear skies that are less likely to be influenced by liquid droplets were associated with appreciably stronger lower-tropospheric stratification. Corresponding surface turbu lent heat fluxes partitioned differently based upon the cloud–stability stratification regime derived from early morning radiosounding profiles. Combined with the differences in the radiative budget largely resulting from dramatic seasonal dif ferences in surface albedo, the lower atmosphere stratification, surface energy budget, and near-surface thermodynamics are shown to be modified by the effective longwave radiative forcing of clouds. The diurnal evolution of thermodynamics and surface energy components varied depending on the early morning stratification state. Thus, the importance of quies cent versus synoptically active large-scale meteorology is hypothesized as a critical forcing for cloud properties and associ ated surface energy budget variations. The physical relationships between clouds, radiation, and stratification can provide a useful suite of metrics for process understanding and to evaluate numerical models in such an undersampled, highly com plex terrain environment.

54 ENVIRONMENTAL SCIENCES↗

ORBITAL ANGULAR MOMENTUM BEAMS RESEARCH USING A FREE-ELECTRON LASER OSCILLATOR

Orbital angular momentum (OAM) photon beams are excellent tools for non-contact optical manipulation of mat- ter in a broad photon energy range. A free-electron laser (FEL) oscillator is well-suited for studying OAM beams with various features including a wide spectral coverage, wavelength tunability, two-color lasing, polarization control, etc. Here, we report the first experimental demonstration of superposed OAM beams from an oscillator FEL. Lasing at around 458 nm, we have generated superposed OAM beams up to the fourth order as a superposition of two pure OAM modes with opposite helicities. These generated beams have a good beam quality, a high degree of circular polarization, and high power. Using external rf modulation with frequen- cies from 1 to 30 Hz, we also developed a pulsed mode operation of the OAM beams with a highly reproducible temporal structure. FEL operation showcased in this work can be extended to higher photon energies, e.g. using a future x-ray FEL oscillator. The operation of such an OAM FEL also paves the way for the generation of OAM gamma-ray beams via Compton scattering.

Liu, P.↗