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Rainer Volkamer Simulation Chamber Experiments of Relevance to Atmospheric Chemistry FUNDING: NATIONAL SCIENCE FOUNDATION Simulation chambers are tools to study the chemical kinetics and products of chemical reactions in absence of the convoluted complexity of field observations, which arises from multiple emission sources, atmospheric transport and chemical transformations. Understanding the reaction mechanism and kinetics of chemical reactions is needed to represent atmospheric chemistry in numerical models. Our group has more than 15 years of experience in developing simulation chambers, and in 2011 we carried out simulation-chamber experiments using facilities at the Paul Scherrer Institute (PSI), in Switzerland, and at the University of Manchester (UoM), United Kingdom. Traditional models represent secondary organic aerosol (SOA) formation based on the gas-phase oxidation of a limited set of organic precursor molecules. However, these models tend to underestimate the degree of oxygenation of actual SOA, indicating missing processes. One SOA source increasingly recognized as important—yet currently not well understood—is glyoxal (CHOCHO), the smallest alpha-dicarbonyl. Unlike traditional SOA precursors, glyoxal forms SOA by partitioning to the aqueous phase (Ervens and Volkamer, 2010). At PSI, we have studied Henry’s Law constants for glyoxal uptake to laboratory-generated aerosols containing sulfate. These studies combined University of Colorado 56 CIRES Annual Report 2011 CU LED-CE-DOAS setup at the PSI simulation chamber. Light Emitting Diode Cavity Enhanced Differential Optical Absorption Spectroscopy (CU LED-CE-DOAS, Sinreich et al., 2010) measurements of gas-phase glyoxal with online High Resolution Time-of-Flight Aerosol Mass Spectrometry (HR-Tof-AMS) and time-resolved High-Performance Liquid Chromatography Electrospray Ionization Tandem Mass Spectrometry (HPLC ESI MS/ MS) particle-phase measurements. We characterize for the first time the time-resolved evolution of glyoxal partitioning; relate molecular-specific measurements to AMS mass spectra; and investigated the effects of visible light on the reversibility of glyoxal uptake to ammonium sulfate (AS) and mixed AS/fulvic acid seed aerosols under relativehumidity (RH) conditions ranging from 50 percent to 85 percent RH. Another set of simulation-chamber experiments further investigated recent field evidence that glyoxal is present in elevated concentrations in the marine boundary layer over the tropical Pacific Ocean more than 3,000 km from any land (Thalman and Volkamer, 2010). At UoM, the source for glyoxal was investigated by means of simulationchamber and flow-tube studies that used two custommade CU LED-CE-DOAS, designed and assembled in Boulder, Colo., to probe whether glyoxal is released as the result of the exposure of atmospheric oxidants (O3, OH) to organics within sea-spray aerosols, and on a bulk surface proxy ocean.
John Wahr Applications of Time-Variable Gravity Measurements from GRACE FUNDING: NASA, JET PROPULSION LABORATORY The GRACE (Gravity Recovery and Climate Experiment) satellite mission, launched by NASA and the German Space Agency in March 2002, is providing global maps of the Earth’s gravity field to astonishing accuracy every month. Because the Earth’s gravity field is caused by its mass distribution, time-variations in gravity as determined from GRACE data can be used to estimate monthto-month changes in the Earth’s mass distribution. GRACE can recover mass variability at scales of about 250–300 km and larger. We have been using these data to look at a number of geophysical signals, particularly those that involve the storage of water (including snow and ice) on continents and in the polar ice sheets. As one example, because of its large effective footprint and its sensitivity to mass, GRACE offers the best available method for measuring the total mass balance of the polar ice sheets. Figure 1 shows monthly GRACE results (black line; the orange line is a smoothed version) for the mass variability summed over the entire Greenland ice sheet, between April 2002 and March 2011. The trend of the best-fitting straight line is about 220 gigatons/yr of ice-mass loss, which corresponds to enough water each year to cover all of Colorado to a depth of almost 1 meter. There is a notable downward curvature to the results, indicating that the mass-loss rate was increasing during this time period. But hiding behind this reasonably simple single time series is a mass-loss signal of considerable spatial and temporal complexity. Figure 2, for example, shows how the mass-loss rate was distributed across Greenland for four two-year timespans, as determined from the GRACE solutions. It shows the mass loss began in earnest in about 2005, in southeast Greenland. That region tended to stabilize in 2007, while at the same time significant mass loss appeared in the northwest. During the last couple of years, the mass-loss pattern reverted to something closer to the 2005–2007 pattern. The main source of these dramatic mass-loss rates is increased velocities of outlet glaciers. The GRACE results indicate how volatile those velocities have been and suggest that the dynamics controlling those velocities will be difficult to sort out. Figure 1: Monthly GRACE results (black line; the orange line is a smoothed version) for the mass variability summed over the entire Greenland ice sheet, between April 2002 and March 2011. Figure 2: How the mass-loss rate was distributed across Greenland for four two-year timespans, as determined from the GRACE solutions. CIRES Annual Report 2011 57
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COOPERATIVE INSTITUTE FOR RESEARCH
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2 CIRES Annual Report 2011 From the
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Executive Summary and Research High
Page 8 and 9: which is a learning community and m
Page 10 and 11: and community preparedness and disa
Page 12 and 13: 10 CIRES Annual Report 2011 Year in
Page 14 and 15: Council of Fellows n Waleed Abdalat
Page 16 and 17: Organization The Cooperative Instit
Page 18 and 19: CREATING A DYNAMIC RESEARCH ENVIRON
Page 20 and 21: DAVID OONK/CIRES CIRES Director Kon
Page 22 and 23: CIRES Communications It has long be
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Page 26 and 27: Richard Armstrong The Glaciers and
Page 28 and 29: Roger Bilham Block Bounding Bookshe
Page 30 and 31: John Cassano Polar Climate and Mete
Page 32 and 33: Xinzhao Chu LIDAR Research Campaign
Page 34 and 35: Joost de Gouw Sources and Chemistry
Page 36 and 37: Lang Farmer Development of a Microi
Page 38 and 39: Baylor Fox-Kemper Improving Subgrid
Page 40 and 41: Craig Jones Understanding the Origi
Page 42 and 43: Peter Molnar Tibet and the Asian Mo
Page 44 and 45: David Noone A Modern Approach to Pa
Page 46 and 47: Judith Perlwitz Exploring Mechanism
Page 48 and 49: Balaji Rajagopalan with graduate st
Page 50 and 51: Mark C. Serreze Rapid Arctic Change
Page 52 and 53: Robert Sievers Innovative Vaccine D
Page 54 and 55: Margaret Tolbert Laboratory Studies
Page 56 and 57: Greg Tucker Is Climate Change Etche
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Page 66 and 67: Climate Diagnostics Center The miss
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Page 72 and 73: WESTERN WATER ASSESSMENT n Impacts
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Page 76 and 77: VISITING FELLOWS With partial spons
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Page 86 and 87: Figure 1: Simplified schematic show
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Page 96 and 97: 1. The spatial Figure distribution
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Page 102 and 103: workflows that make use of SPIDR’
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CLIMATESYSTEMVARIABILITY CSV-01 Det
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We greatly expanded the holdings in
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CSD-12EmissionsandAtmosphericCompos
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tolysis) and global warming potenti
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Milestone 4. Analyze balloon-borne
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GMD-05OzoneDepletion FEDERAL LEADS:
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feedbacks, on the SSTs in the model
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Milestone 1. Add additional glacier
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Several climate-monitoring products
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atmospheric removal of methylglyoxa
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Figure 1: Global image of the Radia
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profiling radars with radio acousti
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RP-04 Intercontinental Transport an
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ates can be understood by productio
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Milestone 3. Maintain a constituent
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stakeholders and decision makers as
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Milestone 3. Explore the expanding
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140 CIRES Annual Report 2011 Measur
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Refereed Publications, 2010 Abdalat
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Brunt, KM, HA Fricker, L Padman, TA
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Phys., 10(10), 4795-4807, doi: 10.5
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of Arapaho Glacier, Front Range, Co
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to nutrients in streams and rivers
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Moritz, MA, TJ Moody, MA Krawchuk,
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with a first-guess approach, J. Geo
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stable water isotopes in climate mo
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G Keppel-Aleks, EA Kort, R Macatang
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Non-Refereed Publications, 2010 Ale
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and DZ Friday (2010), Digital eleva
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Refereed Journals in which CIRES Sc
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Honors and Awards, 2010 Abdalati, W
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Conferences, Workshops, Events, Pre
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170 CIRES Annual Report 2011 Append
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Acronyms 20CR Twentieth Century Rea
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ESRL Earth System Research Laborato
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MERRA Modern Era Retrospective-Anal
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SXI Solar X-ray Imager TES Total Em
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2011 - Cooperative Institute for Research in Environmental Sciences ...

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