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NASA NTRS1980

High resolution measurements of galactic cosmic-ray neon, magnesium, and silicon isotopes

High-resolution measurements of the abundances of individual isotopes of neon, magnesium and silicon in galactic cosmic rays are reported. The Caltech Heavy Isotope Spectrometer Telescope on board the ISEE 3 spacecraft was used to obtain measurements in the range 30 to 180 MeV/n at an rms mass resolution of 0.20 amu. Results indicate excesses of Ne-22 as well as Mg-25 and Mg-26 in galactic cosmic rays with respect to their solar system abundances. Calculations of the effects of interstellar propagation and solar modulation on cosmic-ray isotope abundances also imply an Mg-25 + Mg-26 cosmic ray source fraction significantly greater than the solar system fraction, and it is suggested that the cosmic ray source material and solar system material were synthesized under different conditions.

Mewaldt, R. A.↗

DOE OSTI2023

Measurement of the Higgs boson mass in the H → ZZ*→ 4ℓ decay channel using 139 fb –1 of s = 13 TeV pp collisions recorded by the ATLAS detector at the LHC

The mass of the Higgs boson is measured in the H→ZZ * →4ℓ decay channel. The analysis uses proton–proton collision data from the Large Hadron Collider at a centre-of-mass energy of 13 TeV recorded by the ATLAS detector between 2015 and 2018, corresponding to an integrated luminosity of 139 fb –1 . The measured value of the Higgs boson mass is 124.99 ± 0.18(stat.) ± 0.04(syst.) GeV. In final states with muons, this measurement benefits from an improved momentum-scale calibration relative to that adopted in previous publications. The measurement also employs an analytic model that takes into account the invariant-mass resolution of the four-lepton system on a per-event basis and the output of a deep neural network discriminating signal from background events. This measurement is combined with the corresponding measurement using 7 and 8 TeV pp collision data, resulting in a Higgs boson mass of 124.94 ± 0.17(stat.) ± 0.03(syst.) GeV.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

NASA NTRS2012

Enabling the Next Generation of Spaceborne Quadrupole Mass Spectrometers

The quadrupole mass spectrometer (QMS) has over 30 years of spaceflight heritage in making important neutral gas and low energy ion observations. Given their geometrical constraints, these instruments are currently operated at the extreme limit of their capabilities. However, a technique called higher order auxiliary excitation provides a set of novel, robust, electronics-based solutions for improving the performance of these sensors. By driving the quadrupole rods with an additional frequency nearly twice that of the normal RF operating frequency, substantially increased abundance sensitivity, maximum attainable mass resolution, and peak stability can be achieved through operation of voltage scan lines through the center of formed upper stability islands. Such improvements are modeled using numerical simulations of ion trajectories in a quadrupole field with and without applied higher order auxiliary excitation. When compared to a traditional QMS with a mass range up to 500Da, sensors can be designed with the same precision electronics to have expected mass ranges beyond 1500Da with a power increase of less than twice that of its heritage implementations.

Gershman, D. J.↗

DOE OSTI2020

ESI-FTICR-MS Analysis of Organic Matter during Incubations with Nitrogen Addition, Teller Road Site, Seward Peninsula, Alaska

This dataset contains the results of the molecular characterization of water-extractable organic matter collected during soil microcosm incubations of tundra soil. The microcosms contained soil collected in April 2017 from the NGEE Arctic Teller Road Site at mile marker 27 (TL_MM27) near Intensive Site 9 (“Toeslope”) and Intensive Site 5 (“Plateau”). The incubations were conducted under an atmosphere of N2 at 8°C for 55 days, with or without addition of ammonium chloride (NH4Cl). Soils were extracted with deionized water and extracted using Bond Elut PPL cartridges prior to analysis. Molecular characterization was performed using electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry (ESI- FTICR-MS). Two data files are provided with this dataset. The first is the summary, by soil type and treatment, of the mass spectrometry results for formulas (as a % of the total) containing C, H, and O only, and with N, S, and other elements. These formulas were then grouped into nine biochemical classes of compounds based on O:C and H:C ratios. The second file provides soil sample characteristics and the processed high-resolution mass spectrometry results by soil type and treatment.The Next-Generation Ecosystem Experiments: Arctic (NGEE Arctic), was a 10-year research effort (2012-2022) to reduce uncertainty in Earth System Models by developing a predictive understanding of carbon-rich Arctic ecosystems and feedbacks to climate. NGEE Arctic was supported by the Department of Energy’s Office of Biological and Environmental Research.The NGEE Arctic project had two field research sites: 1) located within the Arctic polygonal tundra coastal region on the Barrow Environmental Observatory (BEO) and the North Slope near Utqiagvik (Barrow), Alaska and 2) multiple areas on the discontinuous permafrost region of the Seward Peninsula north of Nome, Alaska.Through observations, experiments, and synthesis with existing datasets, NGEE Arctic provided an enhanced knowledge base for multi-scale modeling and contributed to improved process representation at global pan-Arctic scales within the Department of Energy’s Earth system Model (the Energy Exascale Earth System Model, or E3SM), and specifically within the E3SM Land Model component (ELM).

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Aemulus $\nu$: precise predictions for matter and biased tracer power spectra in the presence of neutrinos

Here we present the Aemulusν simulations: a suite of 150 (1.05 h -1 Gpc) 3 N-body simulations with a mass resolution of 3.51 × 10 10 Ω cb /0.3 h -1 M ⊙ in a wνCDM cosmological parameter space. The simulations have been explicitly designed to span a broad range in σ8 to facilitate investigations of tension between large scale structure and cosmic microwave background cosmological probes. Neutrinos are treated as a second particle species to ensure accuracy to 0.5 eV, the maximum neutrino mass that we have simulated. By employing Zel'dovich control variates, we increase the effective volume of our simulations by factors of 10-10 5 depending on the statistic in question. As a first application of these simulations, we build new hybrid effective field theory and matter power spectrum surrogate models, demonstrating that they achieve ≤ 1% accuracy for k ≤ 1 hMpc -1 and 0 ≤ z ≤ 3, and ≤ 2% accuracy for k ≤ 4 hMpc -1 for the matter power spectrum. We publicly release the trained surrogate models, and estimates of the surrogate model errors in the hope that they will be broadly applicable to a range of cosmological analyses for many years to come.

79 ASTRONOMY AND ASTROPHYSICS↗

NASA NTRS1997

Cosmic Ray-Air Shower Measurement from Space

A feasibility study has been initiated to observe from space the highest energy cosmic rays above 1021 eV. A satellite observatory concept, the Maximum-energy Auger (Air)-Shower Satellite (MASS), is recently renamed as the Orbital Wide-angle Collector (OWL) by taking its unique feature of using a very wide field-of-view (FOV) optics. A huge array of imaging devices (about 10(exp 6) pixels) is required to detect and record fluorescent light profiles of cosmic ray cascades in the atmosphere. The FOV of MASS could extend to as large as about 60 in. diameter, which views (500 - 1000 km) of earth's surface and more than 300 - 1000 cosmic ray events per year could be observed above 1020 eV. From far above the atmosphere, the MASS/OWL satellite should be capable of observing events at all angles including near horizontal tracks, and would have considerable aperture for high energy photon and neutrino observation. With a large aperture and the spatial and temporal resolution, MASS could determine the energy spectrum, the mass composition, and arrival anisotropy of cosmic rays from 1020 eV to 1022 eV; a region hitherto not explored by ground-based detectors such as the Fly's Eye and air-shower arrays. MASS/OWL's ability to identify cosmic neutrinos and gamma rays may help providing evidence for the theory which attributes the above cut-off cosmic ray flux to the decay of topological defects. Very wide FOV optics system of MASS/OWL with a large array of imaging devices is applicable to observe other atmospheric phenomena including upper atmospheric lightning. The wide FOV MASS optics being developed can also improve ground-based gamma-ray observatories by allowing simultaneous observation of many gamma ray sources located at different constellations.

Takahashi, Yoshiyuki↗

DOE OSTI2021

Rapid Automated Annotation and Analysis of N-Glycan Mass Spectrometry Imaging Data Sets Using NGlycDB in METASPACE

Imaging N-glycan spatial distribution in tissues using mass spectrometry imaging (MSI) is emerging as a promising tool in biological and clinical applications. However, there is currently no high throughput tool for visualization and molecular annotation of N-glycans in MSI data, which significantly slows down data processing and hampers the applicability of this approach. In this work, we present how METASPACE, an open-source cloud engine for molecular annotation of MSI data, can be used to automatically annotate, visualize, analyze, and interpret high-resolution mass spectrometry-based spatial N-glycomics data. METASPACE is an emerging tool in spatial metabolomics, but the lack of compatible glycan databases has limited its application for comprehensive N-glycan annotations from MSI datasets. We created NGlycDB, a public database of N-glycans, by adapting available glycan databases. We demonstrate the applicability of NGlycDB in METASPACE by analyzing MALDI-MSI data from formalin-fixed paraffin-embedded (FFPE) human kidney and mouse lung tissue sections. We added NGlycDB to METASPACE for public use, thus facilitating applications of MSI in glycobiology.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2019

An X-Ray Spectroscopic Search For Dark Matter And Unidentified Line Signatures In The Perseus Cluster With Hitomi

The reported detection of a 3.5 keV emission signal in the Perseus cluster core by Bulbulet al. (2014, ApJ, 789, 13) was ruled out at high confidence in analysis conducted by Aharonian et al. (2017, ApJ, 837, L15) of X-ray spectra at 5 eV energy resolution obtained with the Hitomi observatory Soft X-ray Spectrometer (SXS). Using the same data, we search the full 2–12 keV SXS energy band for previously unidentified emission and absorption features. No significant unidentified line emission or absorption is found. Line flux upper limits (1σper resolution element) vary with photon energy and assumed intrinsic width, decreasing from∼100 at 2 keV to<10 photons cm−2s−1sr−1over most of the 5–10 keV energy range for a Gaussian line with Doppler broadening of 640 kms−1. Limits for narrower and broader lines have a similar energy dependence and are systematically smaller and larger, respectively. These line flux limits are used to constrain the decay rate of hypothetical dark matter candidates. For the sterile neutrino decay rate, we place new constraints over the mass range of 4–24 keV with mass resolution better than any previous X-ray analysis. Additionally, the accuracy of relevant thermal spectral models and atomic data are evaluated. The Perseus cluster spectra may be described by a composite of multi-temperature thermal and active galactic nuclei (AGN) power-law continua. Superposed on these, a few line emission signals possibly originating from unmodeled atomic processes (including SiXIV and FeXXV)are marginally detected and tabulated. Comparisons with previous X-ray upper limits and future prospects for dark matter searches using high-energy resolution spectroscopy are discussed.

Takayuki Tamura↗

DOE OSTI2025

An In Situ , Automated High-Explosives Aging Method Utilizing Two-Dimensional Gas Chromatography–Mass Spectrometry

Understanding chemical changes that occur in high explosives as they age is of great importance to the safe employment and storage of these compounds. Traditional methods of aging high explosives even under accelerated aging conditions are time intensive with durations on the order of months to years. The nature of traditional aging analyses reduces each sample to a snapshot data point often separated widely in time, requiring many assumptions as to how the degradation products develop. Further complicating matters, several analytical techniques are typically employed for each sample analysis in order to ascertain an entire picture of the decomposition pathways. To address these shortcomings with existing methods, a new method of accelerated aging of high explosives utilizing comprehensive two-dimensional gas chromatography coupled to high-resolution mass spectrometry (GC × GC-HRMS) was developed using 2,4,6,8,10,12-hexanitro-2,4,6,8,10,12-hexaazaisowurtzitane (CL-20) as a model compound for method development. This in situ automated method reduces the time scale of aging to a matter of hours using the inlet of the GC × GC as the aging vessel. GC × GC in combination with HRMS allowed for the collection of both evolved gases and other decomposition products produced during the entire aging process in real time with HRMS providing far greater certainty in identification of explosives aging products. Additionally, this method allowed for a higher throughput of samples with greatly simplified sample preparation. Chemometric analysis of the GC × GC-HRMS data set via the alteration analysis (ALA) enabled discovery of statistically significant chemical changes providing insight into the variation of decomposition pathways with varying aging temperatures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2012

Negative Ion Chemistry in the Coma of Comet 1P/Halley

Negative ions (anions) were identified in the coma of comet 1P/Halley from in-situ measurements performed by the Giotto spacecraft in 1986. These anions were detected with masses in the range 7-110 amu, but with insufficient mass resolution to permit unambiguous identification. We present details of a new chemical-hydrodynamic model for the coma of comet Halley that includes - for the first time - atomic and molecular anions, in addition to a comprehensive hydrocarbon chemistry. Anion number densities arc calculated as a function of radius in the coma, and compared with the Giotto results. Important anion production mechanisms arc found to include radiative electron attachment, polar photodissociation, dissociative electron attachment, and proton transfer. The polyyne anions C4H(-) and C6H(-) arc found to be likely candidates to explain the Giotto anion mass spectrum in the range 49-73 amu. Thc CN(-) anion probably makes a significant contribution to the mass spectrum at 26 amu. Larger carbon-chain anions such as C8H(1) can explain the peak near 100 amu provided there is a source of large carbon-chain-bearing molecules from the cometary nucleus.

Cordiner, M. A.↗

NASA NTRS1979

Cosmic ray isotope abundances from chromium to nickel

IRIS, a telescope consisting of a large-area precision Cerenkov detector, scintillators, spark chambers, and a passive stack of Lexan polycarbonate track detectors, was exposed to the primary cosmic radiation for 6.6 sq m sr hr in a balloon flight in 1976. This measurement has yielded the isotopic composition of the iron-group elements Cr, Mn, Fe, and Ni with an average mass resolution of 0.65 amu for the energies 320-500 MeV per amu at the detector. This experiment places the most severe constraints to date on deviation from solar-system composition of the source of the cosmic radiation. Upper limits of 10 percent are placed on the ratios Fe-54/Fe-56 and Fe-58/Fe-56, which are inconsistent with large departures from solar system source composition reported by other workers. The isotopic measurements of Fe and Ni preclude the possibility that these cosmic rays were produced in a single e-process zone. The mean mass of Mn is less than 55, indicating the presence of electron-capture species produced by spallation.

Tarle, G.↗

DOE OSTI2021

Measurement report: Molecular composition, optical properties, and radiative effects of water-soluble organic carbon in snowpack samples from northern Xinjiang, China

Abstract. Water-soluble organic carbon (WSOC) in the cryosphere has an important impact on the biogeochemistry cycling and snow–ice surface energy balance through changes in the surface albedo. This work reports on the chemical characterization of WSOC in 28 representative snowpack samples collected across a regional area of northern Xinjiang, northwestern China. We employed multimodal analytical chemistry techniques to investigate both bulk and molecular-level composition of WSOC and its optical properties, informing the follow-up radiative forcing (RF) modeling estimates. Based on the geographic differences and proximity of emission sources, the snowpack collection sites were grouped as urban/industrial (U), rural/remote (R), and soil-influenced (S) sites, for which average WSOC total mass loadings were measured as 1968 ± 953 ng g−1 (U), 885 ± 328 ng g−1 (R), and 2082 ± 1438 ng g−1 (S), respectively. The S sites showed the higher mass absorption coefficients at 365 nm (MAC365) of 0.94 ± 0.31 m2 g−1 compared to those of U and R sites (0.39 ± 0.11 m2 g−1 and 0.38 ± 0.12 m2 g−1, respectively). Bulk composition of WSOC in the snowpack samples and its basic source apportionment was inferred from the excitation–emission matrices and the parallel factor analysis featuring relative contributions of one protein-like (PRLIS) and two humic-like (HULIS-1 and HULIS-2) components with ratios specific to each of the S, U, and R sites. Additionally, a sample from site 120 showed unique pollutant concentrations and spectroscopic features remarkably different from all other U, R, and S samples. Molecular-level characterization of WSOC using high-resolution mass spectrometry (HRMS) provided further insights into chemical differences among four types of samples (U, R, S, and 120). Specifically, many reduced-sulfur-containing species with high degrees of unsaturation and aromaticity were uniquely identified in U samples, suggesting an anthropogenic source. Aliphatic/protein-like species showed the highest contribution in R samples, indicating their biogenic origin. The WSOC components from S samples showed high oxygenation and saturation levels. A few unique CHON and CHONS compounds with high unsaturation degree and molecular weight were detected in the 120 sample, which might be anthraquinone derivatives from plant debris. Modeling of the WSOC-induced RF values showed warming effects of 0.04 to 0.59 W m−2 among different groups of sites, which contribute up to 16 % of that caused by black carbon (BC), demonstrating the important influences of WSOC on the snow energy budget.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1975

High resolution Cerenkov and range detectors for balloon-borne cosmic-ray experiment

A combination of an active Cerenkov detector and passive range detectors is proposed for the high resolution measurement of isotopic composition in the neighborhood of iron in the galactic cosmic rays. A large area (4,300 sq cm) Cerenkov counter and passive range detectors were tested. Tests with heavy ions (2.1 GeV/amu C-12, 289 MeV/amu Ar-40, and 594 MeV/amu Ne-20) revealed the spatial uniformity of response of the Cerenkov counter to be better than 1% peak-to-peak. Light collection efficiency is independent of projectile energy and incidence angle to within at least 0.5%. Passive Lexan track recorders to measure range in the presence of the nuclear interaction background which results from stopping particles through 0.9 interaction lengths of matter were also tested. It was found that nuclear interactions produce an effective range straggling distribution only approximately 75% wider than that expected from range straggling alone. The combination of these tested techniques makes possible high mass resolution in the neighborhood of iron.

Ahlen, S. P.↗

DOE OSTI2021

Metaproteomics reveals insights into microbial structure, interactions, and dynamic regulation in defined communities as they respond to environmental disturbance

Abstract Background Microbe-microbe interactions between members of the plant rhizosphere are important but remain poorly understood. A more comprehensive understanding of the molecular mechanisms used by microbes to cooperate, compete, and persist has been challenging because of the complexity of natural ecosystems and the limited control over environmental factors. One strategy to address this challenge relies on studying complexity in a progressive manner, by first building a detailed understanding of relatively simple subsets of the community and then achieving high predictive power through combining different building blocks (e.g., hosts, community members) for different environments. Herein, we coupled this reductionist approach with high-resolution mass spectrometry-based metaproteomics to study molecular mechanisms driving community assembly, adaptation, and functionality for a defined community of ten taxonomically diverse bacterial members of Populus deltoides rhizosphere co-cultured either in a complex or defined medium. Results Metaproteomics showed this defined community assembled into distinct microbiomes based on growth media that eventually exhibit composition and functional stability over time. The community grown in two different media showed variation in composition, yet both were dominated by only a few microbial strains. Proteome-wide interrogation provided detailed insights into the functional behavior of each dominant member as they adjust to changing community compositions and environments. The emergence and persistence of select microbes in these communities were driven by specialization in strategies including motility, antibiotic production, altered metabolism, and dormancy. Protein-level interrogation identified post-translational modifications that provided additional insights into regulatory mechanisms influencing microbial adaptation in the changing environments. Conclusions This study provides high-resolution proteome-level insights into our understanding of microbe-microbe interactions and highlights specialized biological processes carried out by specific members of assembled microbiomes to compete and persist in changing environmental conditions. Emergent properties observed in these lower complexity communities can then be re-evaluated as more complex systems are studied and, when a particular property becomes less relevant, higher-order interactions can be identified.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2020

Ultra High Performance Liquid Chromatography with Quadrupole Time-of-Flight Mass Spectrometry and Fisher Ratio Analysis for Discovery-Based Analysis

The ability to discover minute differences between samples or sample classes for ultrahigh performance liquid chromatography coupled to quadrupole time-of-flight mass spectrometry (UHPLC-QTOF) can be a challenging endeavor especially when these differences are not known a priori. Indeed a typical UHPLC-QTOF analysis time of ~15 minutes can generate over 4 gigabytes of information for a single sample. Implementation of chemometrics such as Fisher ratio (F-ratio) analysis will allow the analyst to quickly and precise probe the chemical differences between different samples or sample classes. F-ratio analysis can be used to find sample or sample class distinguishing compounds reducing the 5 gigabytes of information into a simple, yet informative hit list. Moreover through combinatorial rearrangement, it is possible to determine a F-ratio threshold to separate the real and non-real hits. The F-ratio software presented herein is a semi-automated algorithm that processes the raw, exported .csv files from the SCIEX 500R QTOF in as little as 30 seconds. While further research is needed to modify and perfect the software to deal with high resolution mass spectra precise to 0.0001 Daltons, the current software, precise to 0.1 Da, is able to find significant chemical differences despite some of them being at extremely low concentrations nearing the limit of detection.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2025

VIPER’s Mass Spectrometer observing lunar operations (MSolo)

The Volatiles Investigating Polar Exploration Rover (VIPER) is a lunar volatiles detection and measurement mission that will land on Mons Mouton near Nobile crater, close to the Moon’s south pole. One of the analytical instruments embedded within the rover is the Mass Spectrometer observing lunar operations (MSolo) instrument. VIPER’s data will ultimately be used to create lunar water resource maps that may enable a sustained presence on the lunar surface. As VIPER navigates several kilometers of terrain, its onboard analytical instrumentation will characterize the presence of volatiles along the traverse path and identify candidate locations for drilling. Upon selection of a drilling site, the rover will position itself and deploy an auguring, percussive drill down to a meter depth. Upon extraction, regolith cuttings captured by the auger are deposited on the surface; an activity that will initiate the release of any volatile gases that are subsequently detected and quantified by MSolo. MSolo is designed to identify low-molecular-weight volatiles (between m/z 1-100) with unit mass resolution. Volatiles of interest include D/H and O18/O16 bearing species, including possible water contained within the lunar regolith. MSolo is a modified, commercial off-the-shelf (COTS) system, meaning the instrument is based on a commercially available unit that has been ruggedized for space applications.

MSolo↗

DOE OSTI2025

OzMALDI: A Gas-Phase, In-Source Ozonolysis Reaction for Efficient Double-Bond Assignment in Mass Spectrometry Imaging with Matrix-Assisted Laser Desorption/Ionization

Lipids make up an important class of biomolecules with diverse structures and varied chemical functions. This diversity is a major challenge in chemical analysis and limits our understanding of biological functions and regulation. A major way lipid isomers differ is by double-bond (db) position, and analyzing db-isomers is especially challenging for mass spectrometry imaging (MSI). Ozonolysis can be used to determine the dbposition and has been paired with MSI before. However, previous techniques require increased analysis time to allow for gas-phase reactions within an ion trap or ion mobility cell or additional sample preparation time to allow for offline ozonation. Here, we introduce a new ozonolysis method inside the matrix-assisted laser desorption-ionization (MALDI) source, termed OzMALDI, that simultaneously produces ozonides from all unsaturated lipids. This allows us to determine db-positions without adding additional reaction time while maintaining the high mass resolution provided by Orbitrap MS. This new technique is especially effective at determining multiple db-positions in lipids containing polyunsaturated fatty acids, which is a limitation of many previous techniques. OzMALDI-MSI was applied to the analysis of rat brain and genetically engineered Camelina and soybean seed samples, demonstrating the utility of this method and uncovering novel biological information.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Novel Application of Machine Learning Techniques for Rapid Source Apportionment of Aerosol Mass Spectrometer Datasets

In this work, we apply machine learning approaches sparse multinomial logistic regression to classify aerosol mass spectrometer (AMS) unit mass resolution (UMR) data followed by an ensemble regression technique for source apportionment of organic aerosols (OA). The classifier was trained on 60 well characterized laboratory and positive matrix factorization (PMF) deconvolved reference spectra to identify eight OA types. These include four laboratory-derived secondary organic aerosol (SOA) spectra, which include isoprene photooxidation SOA, isoprene epoxydiols (IEPOX) SOA, a monoterpene SOA type that includes a-pinene and ß-pinene SOA, and aromatic SOA from oxidation of naphthalene and m-xylene precursors, as well as PMF deconvolved spectra for three primary organic aerosol (POA) types, namely, hydrocarbon-like organic aerosol (HOA), biomass burning organic aerosol (BBOA), and cooking OA (COA), and a more oxidized oxygenated OA type (MO-OOA). A 5-fold cross-validation strategy, repeated 10 times, was used to assess the classifier’s performance. The classifier had high classification accuracy for COA, aromatic SOA, and isoprene SOA spectra but incorrectly classified ~9% by number of MO-OOA spectra as BBOA, 12% of BBOA spectra as HOA (and vice versa), and 18% of IEPOX-SOA spectra as aromatic SOA. Next, an ensemble regression model was trained on an artificially generated dataset consisting of mixtures of different OA types to assess its ability to predict fractional mass abundances from classification probabilities of various OA species obtained from the multinomial logistic regression classifier trained on the reference spectra. Ultimately, the proposed approach was applied for source apportionment of aircraft-based AMS measurements of OA UMR spectra during the HI-SCALE field campaign. On two representative days (May 6th and 18th, 2016), the algorithm determined that ~50-60% of OA by mass was MO-OOA, which represented a highly aged organic aerosol mixture from different sources. On both days, BBOA was determined to contribute less than 10% to OA by mass. However, on May 18th, the aromatic SOA fraction was higher compared to that on May 6th. The proposed approach is capable of rapidly analyzing AMS data in real time, making it suitable for applications where rapid source apportionment of AMS OA spectra is desirable.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗