We report the evolution of the mixing state of black carbon (BC) particles in urban plumes measured by an airborne single particle soot photometer. The aircraft observations were conducted over the ocean near the coast of Japan in March 2004. The number fiaction of coated BC particles with a core diameter of 180 mn increased from 0.35 to 0.63 within 12 hours (h), namely 2.3% h-1, after being emitted from the Nagoya urban area in Japan. BC particles with a core diameter of 250 nm increased at the slower rate of 1.0% h-1. The increase in coated BC particles was associated with increases in non-sea salt sulfate and water-soluble organic carbon by a factor of approximately two, indicating that these compounds contributed to the coating on the BC particles. These results give direct evidence that BC particles become internally mixed on a time scale of 12 h in urban plumes. Copyright 2007 by the American Geophysical Union.

Ground-based measurements of aerosols and trace gases were conducted at an urban site in Tokyo (Komaba) and a site 50 km to the north (Kisai) during July-August 2004. An Aerodyne aerosol mass spectrometer (AMS) was deployed at each measurement site to investigate the chemical evolution of submicron organic aerosol (OA) in polluted air. The mass concentrations of OA at the Kisai site were systematically higher than those at the Komaba site and were correlated with ozone under southerly conditions. The rate of increase of OA at the Kisai site is investigated using the photochemical age derived from the ratio of alkyl nitrates to their parent hydrocarbons. The OA concentrations in processed air (age of 8-16 h) were 4-5 times larger than those in fresh emissions (age ∼ 0), suggesting that the OA concentrations can be significantly enhanced within ∼0.5 days under conditions of high photochemical activity. Copyright 2006 by the American Geophysical Union.

Online measurements of water-soluble organic carbon (WSOC) aerosols were made using a particle-into-liquid sampler (PILS) combined with a total organic carbon (TOC) analyzer at a rural site in the Pearl River Delta region, China, in July 2006. A macroporous nonionic (DAX-8) resin was used to quantify hydrophilic and hydrophobic WSOC, which are defined as the fractions of WSOC that penetrated through and retained on the DAX-8 column, respectively. Laboratory calibrations showed that hydrophilic WSOC (WSOCHPI) included low-molecular aliphatic dicarboxylic acids and carbonyls, saccharides, and amines, while hydrophobic WSOC (WSOCHPO) included longer-chain aliphatic dicarboxylic acids and carbonyls, aromatic acids, phenols, organic nitrates, cyclic acids, and fulvic acids. On average, total WSOC (TWSOC) accounted for 60% of OC, and WSOCHPO accounted for 60% of TWSOC. Both WSOC HIP and WSOCHPO increased with photochemical aging determined from the NOx/NOy ratio. In particular, the average WSOCHPO mass was found to increase by a factor of five within a timescale of ∼10 hours, which was substantially larger than that of WSOCHPI (by a factor of 2-3). The total increase in OC mass with photochemical aging was associated with the large increase in WSOCHPO mass. These results, combined with the laboratory calibrations, suggest that significant amounts of hydrophobic organic compounds (likely containing large carbon numbers) were produced by photochemical processing. By contrast, water-insoluble OC (WIOC) mass did not exhibit significant changes with photochemical aging, suggesting that chemical transformation of WIOC to WSOC was not a dominant process for the production of WSOC during the study period. Copyright 2009 by the American Geophysical Union.

Ground-based measurements of aerosol and trace gases were conducted at a rural site in Beijing in the summer of 2006 as a part of the Campaigns of Air Quality Research in Beijing and Surrounding Region 2006 (CAREBeijing 2006). The size-resolved chemical composition of submicron aerosol was measured using an Aerodyne quadrupole aerosol mass spectrometer (AMS). The data obtained from 15 August to 10 September 2006 are presented. Meteorological analysis shows that the measurement period can be characterized as a cycle of low wind speed periods over the course of a few days (stagnant periods) followed by rapid advection of clean air from the north/northwest mostly due to passage of a midlatitude cyclone. Mass concentrations of total measured aerosol with diameters less than 1 μm. (total. PM1), which is defined as the sum of elemental carbon and nonrefractory components measured by the AMS, were highly variable, ranging from. ∼2 to ∼100 μm-3, Large variability of the PM1 composition and drastic changes in the sulfate (SO 2-4) size distribution were observed to be associated with the cycle of stagnant periods and advection of clean air, indicating that both chemical and physical properties of aerosols were significantly altered on a time scale of a few days. We have found the dominance of organic aerosol at lower total PM1 mass loadings and that of SO2-4 at higher mass loadings, which may have important implications for the PM control strategy in Beijing. Possible factors affecting the evolution of the mass concentration and size distribution of SO2-4 are discussed. Copyright 2009 by the American Geophysical Union.

An analysis of diabatic heating and moistening processes from 12 to 36 h lead time forecasts from 12 Global Circulation Models are presented as part of the “Vertical structure and physical processes of the Madden-Julian Oscillation (MJO)” project. A lead time of 12–36 h is chosen to constrain the large-scale dynamics and thermodynamics to be close to observations while avoiding being too close to the initial spin-up of the models as they adjust to being driven from the Years of Tropical Convection (YOTC) analysis. A comparison of the vertical velocity and rainfall with the observations and YOTC analysis suggests that the phases of convection associated with the MJO are constrained in most models at this lead time although the rainfall in the suppressed phase is typically overestimated. Although the large-scale dynamics is reasonably constrained, moistening and heating profiles have large intermodel spread. In particular, there are large spreads in convective heating and moistening at midlevels during the transition to active convection. Radiative heating and cloud parameters have the largest relative spread across models at upper levels during the active phase. A detailed analysis of time step behavior shows that some models show strong intermittency in rainfall and differences in the precipitation and dynamics relationship between models. The wealth of model outputs archived during this project is a very valuable resource for model developers beyond the study of the MJO. In addition, the findings of this study can inform the design of process model experiments, and inform the priorities for field experiments and future observing systems.