Contrasting sources and processes of particulate species in haze days with low and high relative humidity in wintertime Beijing

Although there are many studies of particulate matter (PM) pollution in Beijing, the sources and processes of secondary PM species during haze periods remain unclear. Limited studies have investigated the PM formation in highly polluted environments under low- and high-relative-humidity (RH) conditions. Herein, we present a systematic comparison of species in submicron particles (PM1) in wintertime Beijing (29 December 2014 to 28 February 2015) for clean periods and pollution periods under low- and high-RH conditions. PM1 species were measured with an aerosol chemical species monitor (ACSM) and an Aethalometer. Sources and processes for organic aerosol (OA) were resolved by positive matrix factorization (PMF) with a multilinear engine 2 (ME-2). The comparisons for clean, low-RH pollution and high-RH pollution periods are made from three different aspects, namely (a) mass concentration, (b) mass fraction and (c) growth rate in diurnal profiles. OA is the dominant component of PM1, with an average mass concentration of 56.7 mu g m(-3) (46 %) during high-RH pollution and 67.7 mu g m(-3) (54 %) during low-RH pollution periods. Sulfate had higher concentration and mass fraction during high-RH pollution periods, while nitrate had higher concentration and mass fraction during low-RH pollution periods. The diurnal variations of nitrate and oxygenated organic aerosol (OOA) showed a daytime increase in their concentrations during all three types of periods. Nitrate had similar growth rates during low-RH (0.40 mu g m(-3) h(-1)) and high-RH (0.55 mu g m(-3) h(-1)) pollution periods. OOA had a higher growth rate during low- RH pollution periods (1.0 mu g m(-3) h(-1)) than during high-RH pollution periods (0.40 mu g m(-3) h(-1)). In contrast, sulfate had a decreasing trend during low-RH pollution periods, while it increased significantly with a growth rate of 0.81 mu g m(-3) h(-1) during high-RH pollution periods. These distinctions in mass concentrations, mass fractions and daytime growth rates may be explained by the difference in the formation processes affected by meteorological conditions. In particular, photochemical oxidation and aqueous-phase processes may both produce sulfate and nitrate. The relative importance of the two pathways, however, differs under different meteorological conditions. Additional OOA formation under high-RH (> 70 %) conditions suggests aqueous-related formation pathways. This study provides a general picture of the haze formation in Beiji