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The characteristics of secondary inorganic aerosol including sulfate, nitrate and ammonium (SNA) were investigated during a six-month long heating season in the Harbin-Changchun metropolitan area, i.e., China's only national-level city cluster located in the severe cold climate region. The contribution of SNA to fine particulate matter (PM 2.5 ) tended to decrease with increasing PM 2.5 concentration, opposite to the trend repeatedly observed during winter in Beijing. Heterogeneous sulfate formation was still evident when the daily average temperature was as low as below -10 °C, with the preconditions of high relative humidity (RH; above ∼80%) and high nitrogen dioxide (above ∼60 μg/m 3 ). Both the sulfur oxidation ratio (SOR) and nitrogen oxidation ratio (NOR) were enhanced at high RH, reaching ∼0.3. However, the high RH conditions were not commonly seen during the heating season, which should be responsible for the overall lack of linkage between the SNA contribution and PM 2.5 temporal variation., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2020 Elsevier Ltd. All rights reserved.)

Fine particulate matter (PM 2.5 ) pollution in Beijing was investigated based on field observation and air quality modeling. Measurement results showed that when using elemental carbon (EC) as the reference component, concurrent increases were observed in the relative abundances of sulfate, nitrate, organic carbon (OC) and water-soluble organic carbon (WSOC) when RH exceeded ∼65% during winter. The observed increases could not be explained by variations of primary biomass burning emissions, instead they likely pointed to heterogeneous chemistry and presumably indicated that formation of secondary inorganic and organic aerosols might be related during winter haze events in Beijing. Large gaps were found in winter when comparing the observational and modeling results. In summer, RH exhibited little influence on the observed sulfate/EC, OC/EC or WSOC/EC, and the observed and modeled results were in general comparable for the concentrations of sulfate, EC and OC. This study suggests that distinct yet poorly-understood atmospheric chemistry may be at play in China's winter haze events, and it could be a substantial challenge to properly incorporate the related mechanisms into air quality models., (Copyright © 2019 Elsevier Ltd. All rights reserved.)