Abstract
The Two Column Aerosol Project (TCAP) investigated uncertainties in the aerosol direct effect in the northern hemisphere mid-latitudes. The University of Colorado 2D-MAX-DOAS and LED-CE-DOAS instruments were collocated with DOE’s Atmospheric Radiation Measurement (ARM) Mobile Facility (AMF) and Mobile Aerosol Observing System (MAOS) during the TCAP-1 campaign at Cape Cod, MA (1 July to 13 August 2012). We have performed atmospheric radiation closure studies to evaluate the use of a novel parameter, i.e., the Raman Scattering Probability (RSP). We have performed first measurements of RSP almucantar scans, and measure RSP in spectra of scattered solar photons at 350nm and 430nm. Radiative Transfer Modelling of RSP demonstrate that the RSP measurement is maximally sensitive to infer even extremely low aerosol optical depth (AOD < 0.01) reliably by DOAS at low solar relative azimuth angles. We further assess the role of elevated aerosol layers on near surface observations of oxygen collision complexes, O 2-O2. Elevated aerosol layers modify the near surface absorption of O2-O2 and RSP. The combination of RSP and O2-O2 holds largely unexplored potential to better constrain elevated aerosol layers and measure column aerosol optical properties such as aerosol effective radius, extinction, aerosol phase functions and refractive indices. The TCAPmore » deployment also provides a time series of reactive trace gas vertical profiles, i.e., nitrogen dioxide (NO2) and glyoxal (C2H2O2), which are measured simultaneously with the aerosol optical properties by DOAS. NO2 is an important precursor for ozone (O3) that modifies oxidative capacity. Glyoxal modifies oxidative capacity and is a source for brown carbon by forming secondary organic aerosol (SOA) via multiphase reactions in aerosol and cloud water. We have performed field measurements of these gases during TCAP, and conducted laboratory experiments to quantify for the first time the Setschenow salting constant, KS, of glyoxal in sulfate aerosols. Knowledge about KS is prerequisite to predict how increasing sulfate concentrations since pre-industrial times have modified the formation of SOA from biogenic gases in atmospheric models.« less
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