Analysis of cloud condensation nuclei composition and growth kinetics using a pumped counterflow virtual impactor and aerosol mass spectrometer

摘要

We present a new method of determining the size and composition of CCN-active aerosol particles. Method utility is illustrated through a series of ambient measurements. A continuous-flow thermal-gradient diffusion chamber (TGDC), pumped counterflow virtual impactor (PCVI), and Aerodyne time-of-flight mass spectrometer (AMS) are operated in series. Ambient particles are sampled into the TGDC, where a constant supersaturation is maintained, and CCN-active particles grow to approx 2.5 +- 0.5 (mu)m. The output flow from the TGDC is directed into the PCVI, where a counterflow of dry N_(2) gas opposes the particle-laden flow, creating a region of zero axial velocity. This stagnation plane can only be traversed by particles with sufficient momentum, which depends on their size. Particles that have activated in the TGDC cross the stagnation plane and are entrained in the PCVI output flow, while the unactivated particles are diverted to a pump. Because the input gas is replaced by the counterflow gas with better than 99 percent efficiency at the stagnation plane, the output flow consists almost entirely of dry N_(2) and water evaporates from the activated particles. In this way, the system yields an ensemble of CCN-active particles whose chemical composition and size are analyzed using the AMS. Measurements of urban aerosol in downtown Toronto identified an external mixture of CCN-active particles consisting almost entirely of ammonium nitrate and ammonium sulfate, with CCN-inactive particles of the same size consisting of a mixture of ammonium nitrate, ammonium sulfate, and organics. We also discuss results from the first field deployment of the TGDC-PCVI-AMS system, conducted from mid-May to mid-June 2007 in Egbert, Ontario, a semirural site approx 80 km north of Toronto influenced both by clean air masses from the north and emissions from the city. Organic-dominated particles sampled during a major biogenic event exhibited higher CCN activity and/or faster growth kinetics than urban outflow from Toronto, despite the latter having a higher inorganic content and higher O:C ratio. During both events, particles were largely internally mixed.