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Corrigendum to “The Emissions Model Intercomparison Project (Emissions-MIP): quantifying model sensitivity to emission characteristics” published in Atmos. Chem. Phys., 23, 14779–14799, 2023

Anthropogenic emissions of aerosols and precursor compounds are known to significantly affect the energy balance of the Earth–atmosphere system, alter the formation of clouds and precipitation, and have a substantial impact on human health and the environment. Global models are an essential tool for examining the impacts of these emissions. In this study, we examine the sensitivity of model results to the assumed height of SO 2 injection, seasonality of SO 2 and black carbon (BC) particulate emissions, and the assumed fraction of SO 2 emissions that is injected into the atmosphere as particulate phase sulfate (SO 4 ) in 11 climate and chemistry models, including both chemical transport models and the atmospheric component of Earth system models. We find large variation in atmospheric lifetime across models for SO 2 , SO 4 , and BC, with a particularly large relative variation for SO 2 , which indicates that fundamental aspects of atmospheric sulfur chemistry remain uncertain. Of the perturbations examined in this study, the assumed height of SO 2 injection had the largest overall impacts, particularly on global mean net radiative flux (maximum difference of -0.35?W?m-2), SO2 lifetime over Northern Hemisphere land (maximum difference of 0.8?d), surface SO 2 concentration (up to 59?% decrease), and surface sulfate concentration (up to 23?% increase). Emitting SO 2 at height consistently increased SO 2 and SO 4 column burdens and shortwave cooling, with varying magnitudes, but had inconsistent effects across models on the sign of the change in implied cloud forcing. The assumed SO 4 emission fraction also had a significant impact on net radiative flux and surface sulfate concentration. Because these properties are not standardized across models this is a source of inter-model diversity typically neglected in model intercomparisons. These results imply a need to ensure that anthropogenic emission injection height and SO 4 emission fraction are accurately and consistently represented in global models.

Ahsan, Hamza [Pacific Northwest National Laborator↗

Temporally decoherent and spatially coherent vibrations in metal halide perovskites

The long carrier lifetime and defect tolerance in metal halide perovskites (MHPs) are major contributors to the superb performance of MHP optoelectronic devices. Large polarons were reported to be responsible for the long carrier lifetime. Yet microscopic mechanisms of the large polaron formation, including the so-called phonon melting, are still under debate. In this study, time-of-flight inelastic neutron scattering experiments and first-principles density-functional theory calculations were employed to investigate the lattice vibrations (or phonon dynamics) in methylammonium lead iodide, a prototypical example of MHPs. Our findings are that optical phonons lose temporal coherence gradually with increasing temperature which vanishes at the orthorhombic-to-tetragonal structural phase transition. Surprisingly, however, we found that the spatial coherence is still retained throughout the decoherence process. We argue that the temporally decoherent and spatially coherent vibrations contribute to the formation of large polarons in this metal halide perovskite.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Ultrafast Dynamics of Molecules on Surfaces Studied with Time-Resolved XUV Photoelectron Spectroscopy (Final Report)

In this project we set out to make technical advances in time-resolved photoemission from surfaces and study molecule-surface charge transfer processes. Combining a novel light source developed at Stony Brook with a new type of time-of-flight photoemission electron microscope (TOF k-mic) developed in Mainz, Germany, we achieved the former goal. Our light source, based on cavity-enhanced high harmonic generation at 61 MHz repetition rate, enables ultrafast time-resolved photoemission experiments to be conducted with orders of magnitude higher photocurrents than otherwise possible. Critically, this provides the high dynamic range necessary to study perturbatively excited samples, such that one can study the intrinsic dynamics of electrons and holes as they would occur in a device. Combining our light source with the TOF k-mic, we’ve achieved an overall improvement in data rate of time- and angle-resolved photoemission (tr-ARPES) of approximately four orders of magnitude over the previous state-of-the-art using kHz-repetition rate sources and conventional hemispherical electron analyzers. This new instrument is now being used in experiments on 2D materials and organic semiconductors.

74 ATOMIC AND MOLECULAR PHYSICS↗

Time-of-flight detection of terahertz phonon-polariton

A polariton is a fundamental quasiparticle that arises from strong light-matter interaction and as such has attracted wide scientific and practical interest. When light is strongly coupled to the crystal lattice, it gives rise to phonon-polaritons (PPs), which have been proven useful in the dynamical manipulation of quantum materials and the advancement of terahertz technologies. Yet, current detection and characterization methods of polaritons are still limited. Traditional techniques such as Raman or transient grating either rely on fine-tuning of external parameters or complex phase extraction techniques. To overcome these inherent limitations, we propose and demonstrate a technique based on a time-of-flight measurement of PPs. We resonantly launch broadband PPs with intense terahertz fields and measure the time-of-flight of each spectral component with time-resolved second harmonic generation. The time-of-flight information, combined with the PP attenuation, enables us to resolve the real and imaginary parts of the PP dispersion relation. We demonstrate this technique in the van der Waals magnets NiI 2 and MnPS 3 and reveal a hidden magnon-phonon interaction. We believe that this approach will unlock new opportunities for studying polaritons across diverse material systems and enhance our understanding of strong light-matter interaction.

condensed-matter physics↗

Multiple Environmental Influences on the Lightning of Cold-Based Continental Cumulonimbus Clouds. Part I: Description and Validation of Model

In this two-part paper, influences from environmental factors on lightning in a convective storm are assessed with a model. In Part I, an electrical component is described and applied in the Aerosol–Cloud model (AC). AC treats many types of secondary (e.g., breakup in ice–ice collisions, raindrop-freezing fragmentation, rime splintering) and primary (heterogeneous, homogeneous freezing) ice initiation. AC represents lightning flashes with a statistical treatment of branching from a fractal law constrained by video imagery. The storm simulated is from the Severe Thunderstorm Electrification and Precipitation Study (STEPS; 19/20 June 2000). The simulation was validated microphysically [e.g., ice/droplet concentrations and mean sizes, liquid water content (LWC), reflectivity, surface precipitation] and dynamically (e.g., ascent) in our 2017 paper. Predicted ice concentrations (~10 L -1 ) agreed—to within a factor of about 2—with aircraft data at flight levels (-10° to -15°C). Here, electrical statistics of the same simulation are compared with observations. Flash rates (to within a factor of 2), triggering altitudes and polarity of flashes, and electric fields, all agree with the coincident STEPS observations. The “normal” tripole of charge structure observed during an electrical balloon sounding is reproduced by AC. It is related to reversal of polarity of noninductive charging in ice–ice collisions seen in laboratory experiments when temperature or LWC are varied. Positively charged graupel and negatively charged snow at most midlevels, charged away from the fastest updrafts, is predicted to cause the normal tripole. Total charge separated in the simulated storm is dominated by collisions involving secondary ice from fragmentation in graupel–snow collisions.

54 ENVIRONMENTAL SCIENCES↗

Topography and functional traits shape the distribution of key shrub plant functional types in low-Arctic tundra

The expansion of shrubs in the Arctic tundra fundamentally modifies land-atmosphere interactions. However, it remains unclear how shrub distribution and expansion differ across key species due to challenges with discriminating tundra plant species at regional scales. Here, we combined multi-scale, multi-platform remote sensing and in situ trait measurements to elucidate the distribution patterns and primary controls of two representative deciduous-tall-shrub (DTS) genera, Alnus and Salix, in low-Arctic tundra. We show that topographic features were a key control on DTSs, creating heterogeneous, but predictable distributions of Alnus and Salix fractional cover (fCover). Alnus was more tolerant of elevation and slope and was found on hilly uplands (slope >10°) within a specific elevational band (200–400 m above sea level [MSL]). In contrast, Salix occurred at lower elevations (50–300 m MSL) on gentler slopes (3-10°) and required adequate soil moisture associated with its profligate water use. We also show that niche differentiation between Alnus and Salix changed with patch size, where larger patches were more specialized in resource requirements than individual plants of Alnus and Salix. To understand what constrains the growth of DTSs at locations with low fCover, we developed environmental limiting factor models, which showed that topography limits the upper bound of Alnus and Salix fCover in 69.2% and 48.7% of the landscape, respectively. These findings highlight a critical need to better understand and represent topography-controlled processes and functional traits in regulating shrub distribution, as well as a need for more detailed species classification to predict shrubification in the Arctic.

alder↗

Rapid evolution of aerosol particles and their optical properties downwind of wildfires in the western US

Abstract. During the first phase of the Biomass Burn Operational Project (BBOP) field campaign, conducted in the Pacific Northwest, the DOE G-1 aircraft was used to follow the time evolution of wildfire smoke from near the point of emission to locations 2–3.5 h downwind. In nine flights we made repeated transects of wildfire plumes at varying downwind distances and could thereby follow the plume's time evolution. On average there was little change in dilution-normalized aerosol mass concentration as a function of downwind distance. This consistency hides a dynamic system in which primary aerosol particles are evaporating and secondary ones condensing. Organic aerosol is oxidized as a result. On all transects more than 90 % of aerosol is organic. In freshly emitted smoke aerosol, NH4+ is approximately equivalent to NO3. After 2 h of daytime aging, NH4+ increased and is approximately equivalent to the sum of Cl, SO42, and NO3. Particle size increased with downwind distance, causing particles to be more efficient scatters. Averaged over nine flights, mass scattering efficiency (MSE) increased in ∼ 2 h by 56 % and doubled in one flight. Mechanisms for redistributing mass from small to large particles are discussed. Coagulation is effective at moving aerosol from the Aitken to accumulation modes but yields only a minor increase in MSE. As absorption remained nearly constant with age, the time evolution of single scatter albedo was controlled by age-dependent scattering. Near-fire aerosol had a single scatter albedo (SSA) of 0.8–0.9. After 1 to 2 h of aging SSAs were typically 0.9 and greater. Assuming global-average surface and atmospheric conditions, the observed age dependence in SSA would change the direct radiative effect of a wildfire plume from near zero near the fire to a cooling effect downwind.

54 ENVIRONMENTAL SCIENCES↗

Profile observations of the Arctic atmospheric boundary layer with the BELUGA tethered balloon during MOSAiC

During the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition, the Balloon-bornE moduLar Utility for profilinG the lower Atmosphere (BELUGA) was deployed from an ice floe drifting in the Fram Strait from 29 June to 27 July 2020. The BELUGA observations aimed to characterize the cloudy Arctic atmospheric boundary layer above the sea ice using a modular setup of five instrument packages. The in situ measurements included atmospheric thermodynamic and dynamic state parameters (air temperature, humidity, pressure, and three-dimensional wind), broadband solar and terrestrial irradiance, aerosol particle microphysical properties, and cloud particle images. In total, 66 profile observations were collected during 33 balloon flights from the surface to maximum altitudes of 0.3 to 1.5 km. The profiles feature a high vertical resolution of 0.01 m to 1 m, including measurements below, inside, and above frequently occurring low-level clouds. This publication describes the balloon operations, instruments, and the obtained data set. We invite the scientific community for joint analysis and model application of the freely available data on PANGAEA.

54 ENVIRONMENTAL SCIENCES↗

Chemical imaging of individual stratospheric particles sampled over North America

The increasing size, severity, and frequency of wildfires have led to dramatic increases in particulate matter concentrations in the troposphere. Severe wildfires can generate intense convective systems capable of transporting large quantities of biomass burning organic aerosols (BBOA) to the upper troposphere and lower stratosphere (UTLS). Chemically complex organic matter and light-absorbing carbonaceous material is introduced into stratospheric regions that were historically isolated from direct surface emissions. In this study, stratospheric particles were sampled over North America during the Dynamics and Chemistry of the Summer Stratosphere (DCOTSS) campaign, an aircraft-based research project designed to characterize convective perturbation in the UTLS. Particle samples collected from six research flights during summer 2022 were analyzed using Computer-Controlled Scanning Electron Microscopy and Scanning Transmission X-ray Microscopy to investigate particle size distributions, morphology, chemical composition, and mixing state of stratospheric particles along transects across the continental United States and adjacent Pacific Ocean airspace. Analysis revealed that all sampled particles contained detectable levels of carbon, with most exhibiting organic volume fractions of 0.37 ± 0.20. Notably, about 5% of the particles also contained soot inclusions, which indicates the presence of refractory black carbon transported to stratospheric altitudes and provides direct evidence of wildfire-derived black carbon reaching the UTLS. Typical particle morphology exhibits organic shells over soot and inorganic cores and suggests secondary processing and aging of BBOA during transport to and within the UTLS. These findings provide compelling evidence that wildfire emissions play a critical role in affecting the long-term composition and radiative properties of stratospheric particles.

Sharpe, Steven [Purdue Univ., West Lafayette, IN (↗

Horizontal Splitter Design For FFA@CEBAF Energy Upgrade: Current Status

Thomas Jefferson National Accelerator Facility (Jefferson Lab) is currently studying the feasibility of an energy upgrade based upon Fixed-Field Alternating Gradient (FFA) permanent magnet technology. The current plan is to replace the highest-energy recirculation arcs with FFA arcs, increasing the total number of beam recirculations, thus the energy. In order to accommodate multiple passes in the FFA arcs, horizontal splitters are being designed to control the beam parameters entering the FFA arcs, as well as the time of flight and R_56. In the current design, six passes will recirculate through the FFA arcs, necessitating the design of six independent beamlines to control the optics and beam dynamics matching into the arcs. These beamlines must fit into the current CEBAF tunnel, while allowing for personnel and equipment access. They must also be flexible enough to accommodate the beam under realistic operational conditions and fluctuations. The constraints on the system are highly restrictive, complicating the design. This document will describe the current state of the design, and indicate the work remaining for a complete conceptual design.

Benesch, Jay↗

Understanding Growth Dynamics and Yield Prediction of Sorghum Using High Temporal Resolution UAV Imagery Time Series and Machine Learning

Unmanned aerial vehicles (UAV) carrying multispectral cameras are increasingly being used for high-throughput phenotyping (HTP) of above-ground traits of crops to study genetic diversity, resource use efficiency and responses to abiotic or biotic stresses. There is significant unexplored potential for repeated data collection through a field season to reveal information on the rates of growth and provide predictions of the final yield. Generating such information early in the season would create opportunities for more efficient in-depth phenotyping and germplasm selection. This study tested the use of high-resolution time-series imagery (5 or 10 sampling dates) to understand the relationships between growth dynamics, temporal resolution and end-of-season above-ground biomass (AGB) in 869 diverse accessions of highly productive (mean AGB = 23.4 Mg/Ha), photoperiod sensitive sorghum. Canopy surface height (CSM), ground cover (GC), and five common spectral indices were considered as features of the crop phenotype. Spline curve fitting was used to integrate data from single flights into continuous time courses. Random Forest was used to predict end-of-season AGB from aerial imagery, and to identify the most informative variables driving predictions. Improved prediction of end-of-season AGB (RMSE reduction of 0.24 Mg/Ha) was achieved earlier in the growing season (10 to 20 days) by leveraging early- and mid-season measurement of the rate of change of geometric and spectral features. Early in the season, dynamic traits describing the rates of change of CSM and GC predicted end-of-season AGB best. Late in the season, CSM on a given date was the most influential predictor of end-of-season AGB. The power to predict end-of-season AGB was greatest at 50 days after planting, accounting for 63% of variance across this very diverse germplasm collection with modest error (RMSE 1.8 Mg/ha). End-of-season AGB could be predicted equally well when spline fitting was performed on data collected from five flights versus 10 flights over the growing season. This demonstrates a more valuable and efficient approach to using UAVs for HTP, while also proposing strategies to add further value.

54 ENVIRONMENTAL SCIENCES↗

Measuring Transverse Displacements Using Unmanned Aerial Systems Laser Doppler Vibrometer (UAS-LDV): Development and Field Validation

Measurement of bridge displacements is important for ensuring the safe operation of railway bridges. Traditionally, contact sensors such as Linear Variable Displacement Transducers (LVDT) and accelerometers have been used to measure the displacement of the railway bridges. However, these sensors need significant effort in installation and maintenance. Therefore, railroad management agencies are interested in new means to measure bridge displacements. This research focuses on mounting Laser Doppler Vibrometer (LDV) on an Unmanned Aerial System (UAS) to enable contact-free transverse dynamic displacement of railroad bridges. Researchers conducted three field tests by flying the Unmanned Aerial Systems Laser Doppler Vibrometer (UAS-LDV) 1.5 m away from the ground and measured the displacement of a moving target at various distances. The accuracy of the UAS-LDV measurements was compared to the Linear Variable Differential Transducer (LVDT) measurements. The results of the three field tests showed that the proposed system could measure non-contact, reference-free dynamic displacement with an average peak and root mean square (RMS) error for the three experiments of 10% and 8% compared to LVDT, respectively. Such errors are acceptable for field measurements in railroads, as the interest prior to bridge monitoring implementation of a new approach is to demonstrate similar success for different flights, as reported in the three results. This study also identified barriers for industrial adoption of this technology and proposed operational development practices for both technical and cost-effective implementation.

42 ENGINEERING↗

Inference of the neutron down-scatter ratio using neutron time-of-flight data for DT-layered implosions on the OMEGA laser

First analysis of the neutron time of flight (nTOF) data is presented to infer the areal density using the neutron down-scatter ratio (DSR) for OMEGA deuterium–tritium (DT)-layered (cryogenic) implosions. The required very-high-dynamic range (nTOF) signal is constructed using an nTOF detector [Forrest et al., Rev. Sci. Ins. 83, 10D919 (2012)] with multiple time-gated photomultiplier tubes. The nTOF data are analyzed using a forward-fit technique to account for the detector responses and infer the DSR and areal density for DT-layered implosions. The areal densities inferred using this analysis are found to be in agreement with the areal densities measured using the magnetic recoil spectrometer detector that is located in a similar line-of-sight. This work establishes the feasibility of the DSR measurement using nTOF data on OMEGA and provides an additional areal-density measurement that will benefit the assessment of the implosion performance and 3D reconstruction of the imploded core.

47 OTHER INSTRUMENTATION↗

Time of Flight Secondary Ion Mass Spectrometry for Characterization of Pt-Coated Porous Transport Layers in PEM Water Electrolyzers

Titanium-based porous transport layers (PTLs) and iridium-based catalyst layers (CLs) are two main components of proton exchange membrane water electrolyzers (PEMWEs). PTLs are typically coated with platinum to minimize interfacial losses and to support long-term operation. Optimizing coatings and the PTL-CL interface requires comprehensive characterization. This study establishes time-of-flight secondary ion mass spectrometry (ToF-SIMS) as a valuable technique for PTL characterization, addressing capabilities and limitations related to PTL morphology. A methodology was developed that uses a Cs + sputter beam for dynamic depth profiling, with data collected in both positive-ion (MCs + ) and negative-ion modes to generate depth profiles, 2D ion maps, and 3D ion reconstructions. ToF-SIMS detected relative differences in platinum-layer thickness between samples; these trends were validated by cross-sectional scanning transmission electron microscope (STEM) measurements and flat-titanium substrate controls. Interfacial oxide layers are identified in both ion modes, with enhanced oxide sensitivity in negative mode. The technique’s high sensitivity enables detection of nanometer-scale coatings and trace impurities within the bulk PTL structure. These results provide a methodological framework for analyzing Pt-coated PTLs, with the potential to extend to other components in PEMWEs and other electrolyzer systems.

36 MATERIALS SCIENCE↗

Balancing Impedance and Controllability in Response Reconstruction with $\mathrm{TS-IMMAT}$

In a prior work the authors proposed a variant on the Impedance Matched Multi-Axis Test (IMMAT) in which a fixture is defined, called the Transmission Simulator (TS), and the desired environment is matched at a set of sensors on the TS. If the motion of the TS is matched then the response of the rest of the component will also match, provided that the attached component has the same dynamics as it did when the environment was measured. Hence, one would like the TS to be flexible so that it reproduces the boundary conditions that the component of interest experiences during flight, but the more flexible the TS, the more shakers might be needed to control its response. This work presents a derivation that gives expressions for these two potential error sources in TS-IMMAT. Then, various case studies are presented, both on simulated and real hardware, to understand the importance of each error term in practical testing. The theory explains the phenomena that were observed when using measurements from a component that flew on a sounding rocket. The environmental response was measured and then various fixtures were attached, each comprising more of the next assembly, or the hardware to which the component was attached in flight. MIMO testing was repeated with each fixture and the results were compared to seek to understand the role of the impedance match in this type of testing. Here the results show that the number of modes that are active in the transmission simulator is also very important, and so the best solution balances these two considerations. An improved method of simulating the MIMO test is then proposed, so simulations can be used to predict what fixture, or transmission simulator, will give the best results in a TS-IMMAT test.

42 ENGINEERING↗

Experimental results from the characterization of a 32-channels mixed-signal processor for the GAPS experiment

This work describes the experimental results obtained from the characterization of a 32-channels readout ASIC that is the core of a module composed by 4 Lithium-drifted Silicon, Si(Li), detectors. The module is the building block of a tracker in an upcoming balloon experiment. The activity is carried out within the General AntiParticle Spectrometer (GAPS) international collaboration, whose objective is the indirect detection of dark matter through the detection of antiparticles present in cosmic rays at low energies. The balloon flight is foreseen in 2024 from the McMurdo station in Antarctica. The ASIC is designed in a 180 nm CMOS technology and has 32 low-noise analog readout channels featuring a dynamic compression of the signal, an 11-bit SAR ADC, and a digital back-end section responsible for channel setting and for sending digital information to the data acquisition system of the tracker. This work has a twofold goal: it intends on the one hand to verify the performance of the circuit, on the other to select at least 300 good samples to be used for the assembly of the GAPS Si(Li) tracker.

Riceputi, Elisa↗

Time-of-flight vs time-of-arrival in neutron spectroscopic measurements for high energy density plasmas

The neutron time-of-flight (nToF) diagnostic technique has a lengthy history in Inertial Confinement Fusion (ICF) and High Energy Density (HED) Science experiments. Its initial utility resulted from the simple relationship between the full width half maximum of the fusion peak signal in a distant detector and the burn averaged conditions of an ideal plasma producing the flux [Lehner and Pohl, Z. Phys. 207, 83–104 (1967)]. More recent precision measurements [Gatu-Johnson et al., Phys. Rev. E 94(8), 021202 (2016)] and theoretical studies [Munro, Nucl. Fusion 56, 035001 (2016)] have shown the spectrum to be more subtle and complicated, driving the desire for an absolute calibration of the spectrum to disambiguate plasma dynamics from the conditions producing thermonuclear reactions. In experiments where the neutron production history is not well measured, but the neutron signal is preceded by a concomitant flux of photons, the spectrum can be in situ calibrated using a set of collinear detectors to obtain a true “time-of-flight” measurement. This article presents the motivation and overview of this technique along with estimates of the experimental precision needed to make useful measurements in existing and future nToF systems such as the pulsed power Z-machine located in Albuquerque, NM, at Sandia National Laboratories.

Fusion experiments↗

Stratus and Stratocumulus Cloud Microphysics and Drizzle Relationships With CCN Modality

High resolution extended-range cloud condensation nuclei (CCN) spectral comparisons with cloud microphysics and drizzle of the Physics of Stratocumulus Tops (POST) field experiment confirmed results in the Marine Stratus/Stratocumulus Experiment (MASE). Both of these stratus cloud projects demonstrated that bimodal CCN spectra typically caused by cloud processing were associated with clouds that exhibited higher concentrations of smaller droplets with narrower distributions and less drizzle than clouds associated with unimodal CCN spectra. Resulting brighter clouds and increased cloudiness could enhance both indirect aerosol effects (IAE). These stratus findings are opposite of analogous measurements in two cumulus cloud projects, which showed bimodal CCN associated with fewer larger droplets more broadly distributed and with more drizzle than clouds associated with unimodal CCN. Resulting reduced cumulus brightness and cloudiness could reduce both IAE. Physics of Stratocumulus Tops (POST) flights in air masses with higher CCN concentrations, N CCN , showed more extremes of the stratus characteristics. However, POST flights with lower N CCN showed opposite droplet characteristics similar to the cumulus clouds, yet still showed less drizzle in clouds associated with bimodal CCN, but not as much less as the flights with higher N CCN . Since all MASE clouds were in polluted air masses, while the two cumulus projects were in clean air masses we deduce from these four projects that both the dynamic stratus/cumulus differences (vertical wind) and N CCN are responsible for the microphysics and drizzle differences among these projects. This is because the clean POST characteristics are a hybrid between MASE/POST high N CCN and the two cumulus projects.

bimodality↗