2011 - Cooperative Institute for Research in Environmental Sciences ...
2011 - Cooperative Institute for Research in Environmental Sciences ...
2011 - Cooperative Institute for Research in Environmental Sciences ...
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Complete analysis of the three completed HIAPER<br />
(High-Altitude Instrumented Airborne Plat<strong>for</strong>m <strong>for</strong> <strong>Environmental</strong><br />
<strong>Research</strong>) Pole-to-Pole Observations (HIPPO)<br />
deployments was presented at the American Geophysical<br />
Union Fall Meet<strong>in</strong>g <strong>in</strong> 2010. The results suggest that these<br />
measurements can be used to provide a s<strong>in</strong>gle “typical remote”<br />
black carbon (BC) mass distribution <strong>for</strong> comparison<br />
to global models. Additionally, even <strong>in</strong> very different remote<br />
air masses, the estimated impact on BC absorption of<br />
shortwave solar radiation by dry coat<strong>in</strong>gs on BC cores was<br />
found to be fairly uni<strong>for</strong>m, and to lie <strong>in</strong> good agreement<br />
with previous lower-stratospheric results. In the exceptionally<br />
clean Southern Hemisphere, measurements made<br />
<strong>in</strong> the third HIPPO deployment revealed two populations<br />
of BC-conta<strong>in</strong><strong>in</strong>g aerosol dist<strong>in</strong>guished by the amount of<br />
dry coat<strong>in</strong>gs associated with the BC cores. This observation<br />
may provide a strong constra<strong>in</strong>t on the absolute and<br />
relative ag<strong>in</strong>g of BC-conta<strong>in</strong><strong>in</strong>g aerosol and its transport<br />
timescales <strong>in</strong> global models.<br />
At present a manuscript present<strong>in</strong>g these analyses and<br />
results is <strong>in</strong> preparation <strong>for</strong> publication <strong>in</strong> Geophysical<br />
<strong>Research</strong> Letters.<br />
J. P. SCHWARZ<br />
The NSF/NCAR GV research aircraft used <strong>for</strong> the HIPPO mission with a<br />
backdrop of the mounta<strong>in</strong>s of American Samoa.<br />
Milestone 2. Exam<strong>in</strong>e organosulfate molecules <strong>in</strong> atmospheric<br />
aerosols. Impact: Organosulfate molecules<br />
can be <strong>for</strong>med when reaction products of isoprene and<br />
other biogenic organic products encounter acidic sulfate<br />
particles. Laboratory calibrations and a review of more<br />
than 10 years of field data will allow an assessment of the<br />
importance of these compounds <strong>in</strong> many atmospheric<br />
situations, <strong>in</strong>clud<strong>in</strong>g the Amazon boundary layer and the<br />
free troposphere over the United States.<br />
Organosulfate compounds have recently been identified<br />
with<strong>in</strong> aerosol particles <strong>in</strong> laboratory smog chamber studies.<br />
Organosulfate compounds <strong>for</strong>m when isoprene oxidation<br />
products react with acidic sulfate aerosol particles.<br />
Gas-phase isoprene emitted from broadleaf vegetation<br />
constitutes an enormous flux of organic material <strong>in</strong>to the<br />
atmosphere, and convert<strong>in</strong>g a small fraction of this emitted<br />
mass to condensed phase species would add dramatically<br />
to atmospheric aerosol load<strong>in</strong>gs. Isoprene-derived<br />
organosulfates have not been previously observed <strong>in</strong> the<br />
real atmosphere.<br />
For this project, organosulfate compounds were detected<br />
<strong>in</strong> free tropospheric aerosol by an airborne s<strong>in</strong>gle particle<br />
mass spectrometer <strong>in</strong>strument. Laboratory calibrations<br />
enabled estimations of organosulfate aerosol mass load<strong>in</strong>gs<br />
<strong>for</strong> a variety of atmospheric regions <strong>in</strong>clud<strong>in</strong>g the<br />
Arctic, cont<strong>in</strong>ental midlatitudes and the tropics. Organo-<br />
sulfate load<strong>in</strong>gs were highest <strong>in</strong> tropical and midlatitude<br />
air masses situated downw<strong>in</strong>d of strong isoprene sources<br />
such as the Amazon and the southeastern U.S., where<br />
isoprene-derived organosulfates contributed from 1-20%<br />
of total aerosol mass regionally. This research provides<br />
new evidence on how urban and <strong>in</strong>dustrial emissions of<br />
sulfur compounds comb<strong>in</strong>e with typical biogenic emissions<br />
to generate substantial aerosol mass on regional and<br />
global scales. These results were published <strong>in</strong> the Proceed<strong>in</strong>gs<br />
of the National Academy of Science and presented at the<br />
American Association <strong>for</strong> Aerosol <strong>Research</strong> and American<br />
Geophysical Union annual meet<strong>in</strong>gs.<br />
Milestone 3. Use data from the 2010 CalNex Air Quality<br />
Study to <strong>in</strong>vestigate secondary organic aerosol (SOA) <strong>for</strong>mation<br />
<strong>in</strong> the urban Los Angeles area. Impact: This CIRES<br />
research will enable us to quantify the anthropogenic<br />
source of SOA to the atmosphere, which is currently not<br />
well understood. By comb<strong>in</strong><strong>in</strong>g the results from multiple<br />
measurements, we will <strong>in</strong>vestigate how the budget of<br />
organic carbon <strong>in</strong> the gas and aerosol phases changes as a<br />
function of the degree of photochemical process<strong>in</strong>g. The<br />
results will be used to estimate the global source of SOA<br />
derived from anthropogenic volatile organic compounds<br />
and other urban precursors.<br />
Work has started on the analysis of gas- and aerosolphase<br />
organic carbon species obta<strong>in</strong>ed dur<strong>in</strong>g the Cal-<br />
Nex (<strong>Research</strong> at the Nexus of Air Quality and Climate<br />
Change) field study <strong>in</strong> 2010, with a special focus on the<br />
production of secondary organic aerosol (SOA). Initial<br />
analyses focused on the emissions characterization of<br />
volatile organic compounds, the chemical <strong>for</strong>mation<br />
of glyoxal and other reaction <strong>in</strong>termediates and on the<br />
weekend-weekday effect <strong>in</strong> the production of SOA. First<br />
results were presented at the CalNex workshop <strong>in</strong> Sacramento,<br />
Calif., <strong>in</strong> May <strong>2011</strong>. A detailed analysis of glyoxal<br />
measurements made at the ground site <strong>in</strong> Pasadena, Calif.,<br />
was per<strong>for</strong>med with the help of box-model calculations,<br />
and the manuscript is currently under review. This study<br />
found that the production of several reaction <strong>in</strong>termedi-<br />
CIRES Annual Report <strong>2011</strong> 131