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At least 343 records · Page 19

Volatility Basis Set Distributions and Viscosity of Organic Aerosol Mixtures: Insights from Chemical Characterization Using Temperature-Programmed Desorption–Direct Analysis in Real-Time High-Resolution Mass Spectrometry

Quantitative assessment of gas-particle partitioning of individual components within complex atmospheric organic aerosols (OA) mixtures is critical for predicting and comprehending the formation and evolution of OA particles in the atmosphere. This investigation leverages previously documented data obtained through a temperature programmed desorption - direct analysis in real time – high resolution mass spectrometry (TPD-DART-HRMS) platform. This methodology facilitates the bottom-up construction of volatility basis set (VBS) distributions for constituents found in three biogenic secondary organic aerosol (SOA) mixtures produced through the ozonolysis of a-pinene, limonene, and ocimene. The apparent enthalpies (ΔH*, kJ mol -1 ) and saturated vapor mass concentrations (C T *, µg∙m -3 ) of individual SOA components, determined as a function of temperature (T, K), facilitated an assessment of changes in VBS distributions and gas-particle partitioning with respect to T and atmospheric total organic mass loadings (tOM, µg∙m -3 ). Further, the VBS distributions reveal distinct differences in volatilities among monomers, dimers, and trimers, enabling their categorization into separate volatility bins. At the ambient temperature of T = 298 K, only monomers efficiently partition between gas and particle phases across a broad range of atmospherically relevant total organic mass loadings (tOM) values of 1–100 µg∙m -3 . Partitioning of dimers and trimers becomes notable only at T > 360 K and T > 420 K, respectively. The viscosity of SOA mixtures is assessed using a bottom-up calculation approach, incorporating the input of elemental formulas, ΔH*, C T *, and particle-phase mass fractions of the SOA components. Through this approach, we are able to accurately estimate the variations in SOA viscosity that result from the evaporation of its components. These variations are, in turn, influenced by atmospherically relevant changes in tOM and T. Comparison of the calculated SOA viscosity and diffusivity values with literature reported experimental results shows close agreement, thereby validating the employed calculation approach. These findings underscore the significant potential for TPD-DART-HRMS measurements in enabling the untargeted analysis of organic molecules within OA mixtures. This approach facilitates quantitative assessment of their gas-particle partitioning and allows for the estimation of their viscosity and condensed-phase diffusion, thereby contributing valuable insights to atmospheric models.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Defect characterization and charge transport measurements in high-resolution Ni/n-4H-SiC Schottky barrier radiation detectors fabricated on 250 μ m epitaxial layers

Advances in the growth processes of 4H-SiC epitaxial layers have led to the continued expansion of epilayer thickness, allowing for the detection of more penetrative radioactive particles. In this work, we report the fabrication and characterization of high-resolution Schottky barrier radiation detectors on 250 μm thick n-type 4H-SiC epitaxial layers, the highest reported thickness to date. Several 8 × 8 mm 2 detectors were fabricated from a diced 100 mm diameter 4H-SiC epitaxial wafer grown on a conductive 4H-SiC substrate with a mean micropipe density of 0.11 cm -2 From the Mott–Schottky plots, the effective doping concentration was found to be in the range (0.95–1.85) × 10 14 cm -3 , implying that full depletion could be achieved at ~5.7 kV (0.5 MV/cm at the interface). The current-voltage characteristics demonstrated consistently low leakage current densities of 1–3 nA/cm 2 at a reverse bias of -800 V. This resulted in the pulse-height spectra generated using a 241Am alpha source (5486 keV) manifesting an energy resolution of less than 0.5% full width at half maximum (FWHM) for all the detectors at -200 V. The charge collection efficiencies (CCEs) were measured to be 98–99% with no discernable correlation to the energy resolution. A drift-diffusion model fit to the variation of CCE as a function of bias voltage, revealed a minority carrier diffusion length of ~10 μm. Deep level transient spectroscopy measurements on the best resolution detector revealed that the excellent performance was the result of having ultralow concentrations of the order of 1011 cm-3 lifetime limiting defects—Z 1/2 and EH 6/7 .

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

High-Resolution Momentum Imaging—From Stern’s Molecular Beam Method to the COLTRIMS Reaction Microscope [Book Chapter]

Multi-particle momentum imaging experiments are now capable of providing detailed information on the properties and the dynamics of quantum systems in Atomic, Molecular and Photon (AMO) physics. Historically, Otto Stern can be considered the pioneer of high-resolution momentum measurements of particles moving in a vacuum and he was the first to obtain sub-atomic unit (a.u.) momentum resolution (Schmidt-Böcking et al. in The precision limits in a single-event quantum measurement of electron momentum and position, these proceedings). A major contribution to modern experimental atomic and molecular physics was his so-called molecular beam method, which Stern developed and employed in his experiments. With this method he discovered several fundamental properties of atoms, molecules and nuclei. As corresponding particle detection techniques were lacking during his time, he was only able to observe the averaged footprints of large particle ensembles. Today it is routinely possible to measure the momenta of single particles, because of the tremendous progress in single particle detection and data acquisition electronics. A “state-of-the-art” COLTRIMS reaction microscope can measure, for example, the momenta of several particles ejected in the same quantum process in coincidence with sub-a.u. momentum resolution. Such setups can be used to visualize the dynamics of quantum reactions and image the entangled motion of electrons inside atoms and molecules. This review will briefly summarize Stern’s work and then present in longer detail the historic steps of the development of the COLTRIMS reaction microscope. Furthermore, some benchmark results are shown which initially paved the way for a broad acceptance of the COLTRIMS approach. Finally, a small selection of milestone work is presented which has been performed during the last two decades.

Jahnke, T.↗

High-resolution national mapping of natural gas composition substantially updates methane leakage impacts

Methane is emitted from oil and gas operations alongside heavier hydrocarbons and non-hydrocarbon gases, shaping emissions management decision-making, including air quality impacts. Yet, most assessments assume fixed gas composition, overlooking significant spatial and temporal variations. Here, we generate a high-resolution, data-driven map of natural gas composition across the United States, reconstructing methane, heavier hydrocarbons, and non-hydrocarbon species using spatio-temporal interpolation and oil-and-gas production patterns. Our approach is able to reduce composition prediction errors by 39% in terms of Mean Absolute Error (MAE) compared to standard techniques and reveals that methane loss rates have been underestimated by more than 50% in some regions. Beyond methane, we uncover substantial variability in co-emitted gases, exposing blind spots in current emissions inventories and emissions management frameworks. Our work enables more accurate emissions assessments, guides targeted measurement strategies, and informs emissions management decision-making. It also provides a general framework for prediction in environmental applications that integrate sparse measurements with auxiliary variables.

03 NATURAL GAS↗

High Resolution Aerosol Jet Printed Components with Electrodeposition-Enhanced Conductance

Aerosol Jet Printing (AJP) is one technique of additive manufacturing used in the printing of electronics components. AJP enables the patterning of features at the ~10 μm–100 μm scale based on hardware and print parameters. Additionally, optimization of print conditions enables the printing of high-resolution features with linewidths approaching 10 μm. The aerosol jet printing of electronic parts can be limited by the conductivities which are achievable by Ag nanoparticle inks (typically 15%–25% of bulk Ag). For certain electronics applications, the increased conductivity produces unacceptable loses during operation and methods are needed to increase the conductance of the devices without sacrificing resolution. Here, we report on the AJP of inductor spirals conductor traces of linewidth 50 μm separated by 55 μm gaps. The conductivity of these features is enhanced by electrodeposition of Cu onto the Ag, resulting in a decrease in resistance of 35–45x. Impedance measurements demonstrate that the addition of Cu by electrodeposition to a 27-turn spiral inductor resulted in an inductance of 3.6 μH. Finally, we demonstrate the use of a lift-off process to produce free-standing, flexible, conductive films using AJP.

36 MATERIALS SCIENCE↗

Argon broad ion beam sectioning and high resolution scanning electron microscopy imaging of hydrated alite

Highlights: • The native fibrous outer and dense inner C-S-H structure are preserved by using low energy argon broad ion beam sectioning. • Possible artefacts of the preparation and imaging of hydrated alite are shown and discussed. • An approach for a semi automated pore analysis of the obtained high resolution images is demonstrated. Scanning electron microscopy (SEM) imaging is able to visualize micro- to nano-structures of cement and concrete. A prerequisite is that the sample preparation preserves the native structure of the specimen. In this study, argon broad ion beam (BIB) sectioning is compared to state-of-the-art sample preparation (resin embedding, polishing) for hydrated alite. Additionally, it is investigated if during BIB, sample cooling is beneficial to avoid deterioration of cement hydrates. The aim is to quantitatively measure pore size distributions in hardened alite pastes. Therefore, not only optimized sample preparation but also optimized imaging conditions are investigated. Finally, it is demonstrated that by image analysis pores down to a diameter of 5 nm in hydrated alite pastes can be quantitatively analysed.

36 MATERIALS SCIENCE↗

The National Climate Data Base (NCDB): A Bias-Corrected High-Resolution Climate Dataset

Assessing renewable energy resources under future climate scenarios has been highlighted in recent years to analyze and understand potential impacts of future change in renewable generation on the power sector. Solar energy is well-known as the most plentiful among various renewable resources and usually converted to electricity using photovoltaics (PV) technologies, and the global deployment of PV technology has increased rapidly in recent decades. In this study, we develop a statistical technique to downscale the future projection of solar irradiance for PV energy-related applications. A set of Regional Climate Model (RCM)-based projections obtained from the North American Coordinated Regional Climate Downscaling Experiment (NA-CORDEX) are used as inputs to statistical methods to generate high-resolution global horizontal irradiance (GHI) over the contiguous United States (CONUS). The main steps of the statistical downscaling method include (1) regridding RCM output (0.22 degree and daily resolutions) to handle the modeled-observed data sets on a common grid, (2) correcting bias of RCM GHI using satellite-derived observation, and (3) implementing temporal and spatial downscaling to generate GHI at 8-km and hourly resolution. Basically, complex physical processes and interactions between solar radiation and various atmospheric constituents lead solar irradiance to be highly variable and uncertain. Underrepresentation of clouds from the RCM parameterizations is the main source of error and uncertainty in modeling solar irradiance. Thus, we adapt and use the high-quality satellite-derived data from the National Solar Radiation Database (NSRDB) to analyze the bias and error of RCM GHI as well as estimate the statistical parameters for spatial and temporal downscaling. This presentation will summarize the comprehensive analysis conducted to produce and assess the results under two climate scenarios (RCP4.5 and RCP8.5). We will also present a detailed validation demonstrating the strengths of the proposed downscaling method and future extension of this research.

climate data↗

Tethered balloon system and High-Resolution Mass Spectrometry Reveal Increased Organonitrates Aloft Compared to the Ground Level

Atmospheric particles play critical roles in climate. However, significant knowledge gaps remain regarding the vertically resolved organic molecular-level composition of atmospheric particles due to aloft sampling challenges. To address this, we use a tethered balloon system at the Southern Great Plains Observatory and high-resolution mass spectrometry to, respectively, collect and characterize organic molecular formulas (MF) in the ground level and aloft (up to 750 m) samples. We show that organic MF uniquely detected aloft were dominated by organonitrates (139 MF; 54% of all uniquely detected aloft MF). Organonitrates that were uniquely detected aloft featured elevated O/C ratios (0.73 ± 0.23) compared to aloft organonitrates that were commonly observed at the ground level (0.63 ± 0.22). Unique aloft organic molecular composition was positively associated with increased cloud coverage, increased aloft relative humidity (~40% increase compared to ground level), and decreased vertical wind variance. Furthermore, 29% of extremely low volatility organic compounds in the aloft sample were truly unique to the aloft sample compared to the ground level, emphasizing potential oligomer formation at higher altitudes. Overall, this study highlights the importance of considering vertically resolved organic molecular composition (particularly for organonitrates) and hypothesizes that aqueous phase transformations and vertical wind variance may be key variables affecting the molecular composition of aloft organic aerosol.

54 ENVIRONMENTAL SCIENCES↗

Dynamic Earthquake Triggering in Southern California in High Resolution: Intensity, Time Decay, and Regional Variability

Abstract Earthquake triggering by seismic waves has been recognized as a phenomenon for nearly 30 years. However, our ability to study dynamic triggering has been limited by our ability to capture the triggering stresses accurately and record the resultant earthquakes. Here we use full waveforms from a dense seismic network and a modern, high‐resolution seismic catalog to measure triggering in Southern California from 2008 to 2017 based on interevent time ratios. We find that the fractional seismicity rate change, which we term triggering intensity or triggerability, as a function of peak strain change for the period of ∼20 s due to distant earthquakes is monotonically increasing and compatible with earlier measurements made with a disjoint data set from 1984 to 2008. A triggering strain of 1 microstrain is equivalent to the local productivity generated by an M 1.8 earthquakes. This result implies that a prediction of seismicity rate changes can be made based on recorded ground shaking using the same formalism as currently used for aftershock prediction. For a teleseismic event, this small level of triggering occurs throughout the region and thus aggregates to a regional effect. We find that the triggering rate decays after the triggerer follows an Omori‐Utsu law, but at a much slower rate than a typical aftershock sequence. The slow decay rate suggests that an ancillary process such as creep or fluid flow must be part of dynamic triggering. The prevalence of triggering in areas of creep or fluid involvement reinforces this inference. A triggering cascade of secondary earthquakes is insufficient to explain the data.

Miyazawa, Masatoshi↗

Enhancing Lithium-Ion Battery Aging Simulations: Coupling a High-Resolution, 3D, Grain-Scale Electromechanical Model to a Single-Particle Model

One of the main goals in modeling lithium-ion batteries is to improve/predict longevity and resilience of new chemistries. Unfortunately, this requires simulation of thousands of charge/discharge cycles, which can be rather time consuming depending on the fidelity of the simulation. The purpose of this talk is to discuss a new modeling framework that couples a high-resolution, continuous damage model (CDM) to a single particle model (SPM) resulting in a good combination of speed and fidelity. In previous work, a 3D, continuum-level chemo-mechanical model was developed to investigate cracking within a single cathode particle comprised of hundreds to thousands of randomly oriented grains. The CDM predicted that particle fracture is primarily due to non-ideal grain interactions with slight dependence on high-rate charge demands. Essentially, when neighboring grains were misaligned, they expanded different rates relative to one another leading to high stresses and ultimately the formation of intraparticle cracks. The model predicted that small particles with large grains develop significantly less damage than larger particles with small grains. Finally, the model predicted most of the chemo-mechanical damage accumulates in the first charge after formation. This chemo-mechanical "damage saturation" effect indicated that initial particle fracture occurs within the first few cycles, while long-term cathode degradation is not solely chemo-mechanically induced. This led to a need for simulating fatigue-like mechanism that degrade the battery over longer time scales. In order to reach the time scales, need to resolve fatigue-like degradation, the CDM needs to be complemented by a faster model. Therefore, recent efforts have been focused on using results from the CDM to inform parameters within the SPM. These parameters are homogenization factors that are associated with diffusion, particle radius, and/or exchange current density. By coupling the CDM to the SPM, the aging simulation is broken up into two domains: short-term and long-term degradation. The short-term degradation occurs over a single cycle and is handled by the CDM due of its high fidelity, but relatively expensive computational cost. Such mechanism include break-in crack caused by mismatches in grain orientation. The long-term degradation occurs over tens of cycles and is handled by the SPM due it's computational efficiency. Most of the fatigue-like mechanism fall into this category. The eventual goal of this modeling framework is to upscale to a psudo-2D model allowing for full electrode simulation, which are informed by high-fidelity grain-scale simulations.

electrochemistry↗

Constructing a High‐Resolution Aftershock Catalog for the 2017 Mw 8.2 Tehuantepec Earthquake Sequence Using a Machine Learning–Based Workflow

The 8 September 2017 Mw 8.2 Tehuantepec earthquake was the largest instrumentally recorded normal‐faulting earthquake in Mexico. The mainshock occurred offshore within the Tehuantepec seismic gap, generating >30,000 aftershocks in the following year. We applied an open‐source, machine learning (ML)–assisted workflow to construct a high‐resolution aftershock catalog using data from temporary and permanent seismic networks in southern Mexico. The workflow integrates PhaseNet for phase detection; GaMMA for phase association; and VELEST, HypoInverse, and HypoDD for velocity modeling and relocation. We processed seven months of continuous waveform data from 29 broadband stations, including a temporary rapid‐response deployment that improved station coverage of the offshore rupture zone. To evaluate performance, we compared our results against analyst‐reviewed picks and event locations from the Servicio Sismológico Nacional catalog. The resulting catalog contains 11,374 relocated earthquakes and represents the most comprehensive published dataset for this sequence, incorporating the first full use of the temporary network. Relocated hypocenters show improved depth control and align well with the Slab2.0 subduction geometry, revealing clearer separation between offshore slab events and onshore crustal seismicity. This study demonstrates that combining ML‐based detection with established methods provides a scalable and reproducible approach for constructing high‐quality earthquake catalogs in tectonically complex environments and offers practical guidance for adapting similar workflows to other earthquake sequences.

Garcia, Marc [The University of Texas at El Paso, ↗

Comprehensive defect evaluation of advanced nuclear fuels using high-resolution acoustic signals and optimized sensor separation

Graphite pebble composite structures based on TRistructural-ISOtropic (TRISO) particles are being developed as core nuclear fuels in advanced power reactors, promising safe operation at increased temperatures. Ensuring the structural integrity of these nuclear fuels requires comprehensive and accurate non-destructive evaluation (NDE) techniques to characterize defects and damage in the pebbles. However, traditional acoustic evaluation methods face limitations in defect characterization due to the highly attenuative, and geometrically and compositionally complex nature of these structures. This study proposes an improved acoustic NDE technique for accurate detection and classification of anticipated relevant defects and damage in graphite pebbles using high-resolution acoustic signals and optimized transmit-receive sensor networks. The proposed approach utilizes a triangular three-sensor network as the base unit, comprising three transmit-receive sensors. The sensor separation distance, as well as acoustic excitation center frequency, pulse-width, and bandwidth are optimized to enhance spatial resolution and improve signal-to-noise ratio, enabling effective characterization of the smallest size and widest range of defects in pebbles. Furthermore, the use of the triangular sensor configuration instead of a more conventional transmit-receive sensor pair expands the inspection region from a one-dimensional linear path to a two-dimensional area, increasing spatial coverage. To mitigate challenges associated with processing of complex acoustic signals arising from high-frequency, high-bandwidth excitation in these structures, a machine-learning-based signal processing algorithm is integrated with the sensor network. In the machine-learning-based algorithm, multi-domain features are extracted from the acoustic signals to capture intricate signal characteristics, significantly improving defect identification and classification compared to traditional approaches. The proposed acoustic NDE technique offers considerable promise for practical and reliable defect/damage diagnostics of advanced nuclear pebble fuels.

42 ENGINEERING↗

Advancing conventional High-Resolution Electron Microscopy

Due to the exceptional performance of most modern commercial transmission electron microscopes, the achievement of phase-contrast imaging resolution in the sub-2Å range is today a routine exercise, provided the samples are compliant. Nonetheless, there remains room for improvement, and the purpose of this manuscript is to highlight procedures that might be employed by the practicing microscopist for advancing conventional high resolution electron microscopy.

440800* -- Miscellaneous Instrumentation-- (1990-)↗

Determining g A / g V with High-Resolution Spectral Measurements Using a LiInSe 2 Bolometer

Neutrinoless double beta decay (0νββ) processes sample a wide range of intermediate forbidden nuclear transitions, which may be impacted by quenching of the axial vector coupling constant (g A /g V ), the uncertainty of which plays a pivotal role in determining the sensitivity reach of 0νββ experiments. Here we present measurements performed on a high-resolution LiInSe 2 bolometer in a “source = detector” configuration to measure the spectral shape of the fourfold forbidden β decay of 115 In . The value of g A /g V is determined by comparing the spectral shape of theoretical predictions to the experimental β spectrum taking into account various simulated background components as well as a variety of detector effects. We find evidence of quenching of g A /g V at >5 σ with a model-dependent quenching factor of 0.655 ± 0.002 as compared to the free-nucleon value for the interacting shell model. We also measured the 115 In half-life to be [5.18 ± 0.06(stat) $^{+0.005}_{- 0.015}$(sys)] x 10 14 yr within the interacting shell model framework. This Letter demonstrates the power of the bolometeric technique to perform precision nuclear physics single-β decay measurements, which along with improved nuclear modeling can help reduce the uncertainties in the calculation of several decay nuclear matrix elements including those used in 0νββ sensitivity calculations.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

High-Resolution Photoelectron Spectroscopy of NO3 – Vibrationally Excited Along Its ν3 Mode

The nitrate (NO3) radical has long been the subject of both experimental and theoretical studies due to its complex electronic structure resulting from vibronic interactions between its X̃2A2' and B̃2E' states. In particular, the definite assignment of the fundamental of its degenerate stretching vibration (ν3) is still under debate. Here, we report high-resolution photoelectron spectra of vibrationally pre-excited NO3- using the recently developed IR-cryo-SEVI technique. The anions are excited through infrared (IR) excitation near 1350 cm-1, accessing the ν3 and 2ν3(e') vibrational levels with band centers at 1350.5 and ∼2700 cm-1, respectively. The IR-cryo-SEVI spectrum for 2ν3 pre-excitation shows clear evidence for an intense 321 transition. From the position of this feature (30031 cm-1), the electron affinity of NO3 also determined in this work (31680 cm-1), and the IR excitation energy, we obtain a fundamental frequency of 1051 cm-1 for the ν3 fundamental of the NO3 radical. This assignment and other features in the IR-cryo-SEVI spectra are supported by spectral simulations based on a vibronic Köppel-Domcke-Cederbaum Hamiltonian. The simulations also show that nearly all features in the IR-cryo-SEVI spectra arise because of pseudo-Jahn-Teller coupling between the X̃ and B̃ states of NO3. The results and analysis presented here settle a long-standing controversy regarding the ν3 frequency of NO3.

Anions↗

Scaling High-Resolution Soil Organic Matter Composition to Improve Predictions of Potential Soil Respiration Across the Continental United States

Despite the importance of microbial soil organic matter (SOM) respiration in regulating the flux of carbon between soils and the atmosphere, soil carbon cycling models remain primarily based on climate and soil properties, leading to large uncertainty in predictions. To address this knowledge gap, we analyzed high-resolution water-extractable SOM profiles from soil cores collected across the United States by the 1,000 Soils Pilot of the Molecular Observation Network. Our innovation lies in using machine learning to distill thousands of SOM formula into tractable units; and it enables integrating data from molecular measurements into soil respiration models. In surface soils, SOM chemistry provided better estimates of potential soil respiration than soil physicochemistry, and using them combined yielded the best prediction. Overall, we identify specific subsets of organic molecules that may improve predictions of global soil respiration and create a strong basis for developing new representations in process-based models.

54 ENVIRONMENTAL SCIENCES↗

High Resolution Study of 40 Ca to Constrain Potassium Nucleosynthesis in NGC 2419

The globular cluster NGC 2419 was the first to exhibit a Mg-K anticorrelation, linked to hydrogen burning at temperatures between 80-260 MK. However, the key K-destroying reaction, 39 K(p,γ) 40 Ca, has a large rate uncertainty in this range. We significantly constrain this rate with a high resolution 39 K( 3 He,d) 40 Ca study. We resolve the $E$$^{c.m.}_{r}$ = 154 keV resonance in 39 K+p for the first time, increasing the previous rate by up to a factor 13 and reducing its 1σ width by up to a factor of 42. As a result, reaction network calculations for NGC 2419 suggest that this could lower temperatures needed to reproduce the Mg-K anticorrelation.

39 ≤ A ≤ 58↗

OReole-FM: successes and challenges toward billion-parameter foundation models for high-resolution satellite imagery

While the pretraining of Foundation Models (FMs) for remote sensing (RS) imagery is on the rise, models remain restricted to a few hundred million parameters. Scaling models to billions of parameters has been shown to yield unprecedented benefits including emergent abilities, but requires data scaling and computing resources typically not available outside industry R&D labs. In this work, we pair high-performance computing resources including Frontier supercomputer, America's first exascale system, and high-resolution optical RS data to pretrain billion-scale FMs. Our study assesses performance of different pretrained variants of vision Transformers across image classification, semantic segmentation and object detection benchmarks, which highlight the importance of data scaling for effective model scaling. Moreover, we discuss construction of a novel TIU pretraining dataset, model initialization, with data and pretrained models intended for public release. By discussing technical challenges and details often lacking in the related literature, this work is intended to offer best practices to the geospatial community toward efficient training and benchmarking of larger FMs.

Ambrozio Dias, Philipe↗