Evaluating Organic Aerosol Sources and Evolution with
a Combined Molecular Composition and Volatility Framework Using the
Filter Inlet for Gases and Aerosols (FIGAERO)
Posted on 2020-07-10 - 15:05
ConspectusThe complex array of sources and transformations
of organic carbonaceous
material that comprises an important fraction of atmospheric fine
particle mass, known as organic aerosol, has presented a long running
challenge for accurate predictions of its abundance, distribution,
and sensitivity to anthropogenic activities. Uncertainties about changes
in atmospheric aerosol particle sources and abundance over time translate
to uncertainties in their impact on Earth’s climate and their
response to changes in air quality policy. One limitation in our understanding
of organic aerosol has been a lack of comprehensive measurements of
its molecular composition and volatility, which can elucidate sources
and processes affecting its abundance. Herein we describe advances
in the development and application of the Filter Inlet for Gases and
Aerosols (FIGAERO) coupled to field-deployable High-Resolution Time-of-Flight
Chemical Ionization Mass Spectrometers (HRToF-CIMS). The FIGAERO HRToFCIMS
combination broadly probes gas and particulate OA molecular composition
by using programmed thermal desorption of particles collected on a
Teflon filter with subsequent detection and speciation of desorbed
vapors using inherently quantitative selected-ion chemical ionization.
The thermal desorption provides a means to obtain quantitative insights
into the volatility of particle components and thus the physicochemical
nature of the organic material that will govern its evolution in the
atmosphere.In this Account, we discuss the design and operation
of the FIGAERO,
when coupled to the HRToF-CIMS, for quantitative characterization
of the molecular-level composition and effective volatility of organic
aerosol in the laboratory and field. We provide example insights gleaned
from its deployment, which improve our understanding of organic aerosol
sources and evolution. Specifically, we connect thermal desorption
profiles to the effective equilibrium saturation vapor concentration
and enthalpy of vaporization of detected components. We also show
how application of the FIGAERO HRToF-CIMS to environmental simulation
chamber experiments and the field provide new insights and constraints
on the chemical mechanisms governing secondary organic aerosol formation
and dynamic evolution. We discuss the associated challenges of thermal
decomposition during desorption and calibration of both the volatility
axis and signal. We also illustrate how the FIGAERO HRToF-CIMS can
provide additional insights into organic aerosol through isothermal
evaporation experiments as well as for detection of ultrafine particulate
composition. We conclude with a description of future opportunities
and needs for its ability to further organic aerosol science.
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Thornton, Joel A.; Mohr, Claudia; Schobesberger, Siegfried; D’Ambro, Emma L.; Lee, Ben H.; Lopez-Hilfiker, Felipe D. (2020). Evaluating Organic Aerosol Sources and Evolution with
a Combined Molecular Composition and Volatility Framework Using the
Filter Inlet for Gases and Aerosols (FIGAERO). ACS Publications. Collection. https://doi.org/10.1021/acs.accounts.0c00259
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AUTHORS (6)
JT
Joel A. Thornton
CM
Claudia Mohr
SS
Siegfried Schobesberger
ED
Emma L. D’Ambro
BL
Ben H. Lee
FL
Felipe D. Lopez-Hilfiker
KEYWORDS
desorptionvolatilityevolutionOAsimulation chamber experimentsOrganic Aerosol SourcesFIGAERO HRToFCIMS combinationaerosol particle sourcesFIGAERO HRToF-CIMSair quality policyfield-deployable High-Resolution Ti...abundanceselected-ion chemical ionizationinsightequilibrium saturation vapor concen...Filter Inlet