Conspectus
Exchange of reactive trace gases over the biosphere
is a key source
of reactive organic carbon to the atmosphere and thus influences the
formation of both ozone (O3) and secondary organic aerosol
(SOA). Both O3 and aerosol particles are short-lived climate
forcers and impact the radiative balance of the planet, and their
sources and sinks are chemically complex. However, the biosphere also
acts as a deposition sink for organic and inorganic compounds, including
O3, aerosols, and their precursors. Wet and dry deposition
provides a key lever on the lifetime of trace gases and particles
in the atmosphere and thus on their potential to influence the radiative
balance of the planet. The fluxes of reactive trace gases and particles
are part of an atmospheric biogeochemical cycle that includes feedbacks
through drought and other climate components.
Recent advances
in measurement techniques have enabled new field
observations of trace gas and particle fluxes. Our method development
has focused on the leaf, branch, and forest level, although satellite
measurements coupled to modeling also provide promising new approaches
to constraining trace gas fluxes. Leaf chamber measurements of volatile
organic compound (VOC) emissions highlight leaf-to-leaf and plant-to-plant
variability in both photosynthesis and emissions of individual VOCs,
in addition to differences in emissions across different isomers of
monoterpenes. Isomers obviously have different chemical properties
(e.g., reaction rates with OH radicals, SOA yield) and thus hold different
potentials as precursors for short-lived climate forcers.
The
biosphere acts as both sources and sinks of the oxidation products
of monoterpenes and other biogenic VOCs. Developments in chemical
ionization mass spectrometry have recently enabled measurements of
volatile organic acids, which demonstrate a strong temperature-dependent
ecosystem source, as well as a source from in-canopy chemistry. In-canopy
chemistry also influences particle fluxes, although deposition should
dominate their net exchange. Our field observations of chemically
resolved particle fluxes demonstrate the simultaneous, competing processes
driving forest exchange. To separate out these competing processes,
we use black carbon as an inert tracer for particle deposition. Our
recent measurements demonstrate the importance of wet deposition in
controlling particle lifetime in the atmosphere. Overall, new measurement
techniques have enabled both field and laboratory observations to
improve our understanding of biosphere–atmosphere interactions
and their influence on climate processes.