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Aerosol particles play crucial roles in both climate dynamics and human health. However, there remains a significant gap in our understanding of aerosol composition and evolution, particularly regarding secondary organic aerosols (SOA), and their interaction with clouds in high-altitude background areas in China. Here we conducted real-time measurements of submicron aerosols (PM1) using aerosol mass spectrometers at a forested mountain site (1128 m a.s.l.) in southeastern China in November 2022. Our results revealed that organic aerosol (OA) constituted a substantial portion of PM1 (41.1 %), with the OA being primarily of secondary origin, as evidenced by a high oxygen-to-carbon (O/C) ratio (0.85–0.96). Positive matrix factorization resolved two distinct SOA factors: less oxidized oxygenated OA (LO-OOA) and more oxidized OOA (MO-OOA). Interestingly, MO-OOA was scavenged efficiently during cloud events, while cloud evaporation contributed significantly to LO-OOA. The ratio of OA/ΔCO increased with a decrease in the O/C ratio, suggesting that OA remaining in cloud droplets generally maintained a moderate oxidation state. Furthermore, our results indicated a higher contribution of organic nitrates to total nitrate during cloudy periods (27 %) compared to evaporative periods (3 %). Notably, a substantial contribution of nitrate in PM1 (20.9 %) was observed, particularly during high PM periods, implying that nitrate formed in polluted areas interacted with clouds and significantly impacted the regional background site. Overall, our study underscores the importance of understanding the dynamics of secondary organic aerosols and the impacts of cloud processing in regional mountainous areas in southeastern China. [ABSTRACT FROM AUTHOR]

Emission controls have substantially brought down aerosol pollution in China; however, aerosol mass reductions have slowed down in recent years in the Pearl River Delta (PRD) region, where secondary organic aerosol (SOA) formation poses a major challenge for air quality improvement. In this study, we characterized the roles of SOA in haze formation in urban Guangzhou in the PRD using year-long aerosol mass spectrometer measurements for the first time and discussed possible pathways of SOA formations. On average, organic aerosols (OA) contribute dominantly (50 %) to nonrefractory submicron aerosol mass (NR-PM 1). The average mass concentration of SOA (including by less- and more-oxidized OA, LOOA and MOOA) contributed most to NR-PM 1 , reaching about 1.7 times that of primary organic aerosols (POA, including hydrocarbon-like and cooking-related OA) and accounting for 32 % of NR-PM 1 , even more than sulfate (22 %) and nitrate (16 %). Seasonal variations of NR-PM 1 revealed that haze-formation mechanisms differed much among distinct seasons. Sulfate mattered more than nitrate in fall, while nitrate was more important than sulfate in spring and winter, with SOA contributing significantly to haze formations in all the seasons. Daytime SOA formation was weak in winter under low oxidant levels and air relative humidity, whereas prominent daytime SOA formation was observed in fall, spring and summer almost on a daily basis, suggesting important roles of photochemistry in SOA formations. Further analysis showed that the coordination of gas-phase photochemistry and subsequent aqueous-phase reactions likely played significant roles in quick daytime SOA formations. Obvious nighttime SOA formations were also frequently observed in spring, fall and winter, and it was found that daytime and nighttime SOA formations together had resulted in the highest SOA concentrations in these seasons and contributed substantially to severe haze formations. Simultaneous increases in nitrate with SOA after sunset suggested the important roles of NO 3 radical chemistry in nighttime SOA formations, and this was further confirmed by a continuous increase in the NO + / NO 2+ fragment ratio that related to measured particulate nitrate after sunset. The findings of this study have promoted our understanding of haze pollution characteristics of the PRD and laid down future directions for investigations of SOA-formation mechanisms in urban areas of southern China that share similar emission sources and meteorological conditions. [ABSTRACT FROM AUTHOR]

Biomass burning organic aerosol (BBOA) impacts significantly on climate directly through scattering and absorbing solar radiation and indirectly through acting as cloud condensation nuclei. However, fundamental parameters in the simulation of BBOA radiative effects and cloud activities such as size distribution and refractive index remain poorly parameterized in models. In this study, biomass burning events with high combustion efficiency characterized by a high black carbon (BC) to BBOA ratio (0.22 on average) were frequently observed during autumn in the Pearl River Delta region, China. An improved absorption Ångström exponent (AAE) ratio method considering both variations and spectral dependence of black carbon AAE was proposed to differentiate brown carbon (BrC) absorptions from total aerosol absorptions. BBOA size distributions, mass scattering and absorption efficiency were retrieved based on the changes in aerosol number size distribution, scattering coefficients and derived BrC absorptions that occurred with BBOA spikes. Geometric mean diameter of BBOA volume size distribution Dgv depended largely on combustion conditions, ranging from 245 to 505 nm, and a linear relationship between Dgv and ΔBC/ΔBBOA ​​​​​​​ was achieved. The retrieved real part of the BBOA refractive index ranges from 1.47 to 1.64, with evidence showing that its variations might depend largely on combustion efficiency, which is rarely investigated in existing literature but which however requires further comprehensive investigations. Retrieved imaginary parts of BBOA refractive index (mi,BBOA) correlated highly with ΔBC/ΔBBOA (R>0.88) but differ a lot from previous parameterization schemes. The reason behind the inconsistency might be that single formula parameterizations of mi,BBOA over the whole BC/BBOA range were used in previous studies which might deviate substantially for specific BC/BBOA ranges. Thus, a new scheme that parameterizes wavelength-dependent mi,BBOA was presented, which filled the gap for field-based BBOA absorptivity parameterizations of ​​​​​​​BC/BBOA >0.1. These findings have significant implications for simulating BBOA climate effects and suggest that linking both BBOA refractive index and BBOA volume size distributions to BC content might be a feasible and a good choice for climate models. [ABSTRACT FROM AUTHOR]

Water uptake abilities of organic aerosol under sub-saturated conditions play critical roles in direct aerosol radiative effects and atmospheric chemistry; however, field characterizations of the organic aerosol hygroscopicity parameter κOA under sub-saturated conditions remain limited. In this study, a field campaign was conducted to characterize κOA at a relative humidity of 80 % with hourly time resolution for the first time in the Pearl River Delta region of China. Observation results show that, during this campaign, secondary organic aerosol (SOA) dominated total organic aerosol mass (mass fraction > 70 % on average), which provides a unique opportunity to investigate influences of SOA formation on κOA. Results demonstrate that the commonly used organic aerosol oxidation level parameter O/C was weakly correlated with κOA and failed to describe the variations in κOA. However, the variations in κOA were well reproduced by mass fractions of organic aerosol factor resolved based on aerosol mass spectrometer measurements. The more oxygenated organic aerosol (MOOA) factor, exhibiting the highest average O/C (∼ 1) among all organic aerosol factors, was the most important factor driving the increase in κOA and was commonly associated with regional air masses. The less oxygenated organic aerosol (LOOA; average O/C of 0.72) factor revealed strong daytime production, exerting negative effects on κOA. Surprisingly, the aged biomass burning organic aerosol (aBBOA) factor also formed quickly during daytime and shared a similar diurnal pattern with LOOA but had much lower O/C (0.39) and had positive effects on κOA. The correlation coefficient between κOA and mass fractions of aBBOA and MOOA in total organic aerosol mass reached above 0.8. The contrasting effects of LOOA and aBBOA formation on κOA demonstrate that volatile organic compound (VOC) precursors from diverse sources and different SOA formation processes may result in SOA with different chemical composition, functional properties and microphysical structure, consequently exerting distinct influences on κOA and rendering single oxidation level parameters (such as O/C) unable to capture those differences. Aside from that, distinct effects of aBBOA on κOA were observed during different episodes, suggesting that the hygroscopicity of SOA associated with similar sources might also differ much under different emission and atmospheric conditions. Overall, these results highlight that it is imperative to conduct more research on κOA characterization under different meteorological and source conditions and examine its relationship with VOC precursor profiles and formation pathways to formulate a better characterization and develop more appropriate parameterization approaches in chemical and climate models. [ABSTRACT FROM AUTHOR]

Black carbon (BC) is the most important light-absorbing species in the atmosphere and has a strong positive direct radiative forcing. Recent studies found that BC-containing particles may also modify the structure of planetary boundary layer and thus enhance haze pollution, especially in densely populated areas, for instance, in China. It is however difficult to quantify these effects due to their complex mixing state, hygroscopicity and the high spatial variability of concentration. During an intensive field campaign conducted in the North China Plain in a cold season, the mass size distribution and mixing state of BC was measured with a single particle soot photometer (SP2). During a severe haze event, the BC mass concentration exceeded 15 ug m-3. Stemming from the strong aging process under high relative humidity condition, freshly emitted BC particle was observed to turn into internally mixing within a short time scale. To understand the variation of the hygroscopicity of BC during its aging process, the hygroscopic growth factor of BC-containing particles was measured with a combination of a hygroscopic tandem differential mobility analyzer and a SP2. The particle hygroscopic growth factor was found to be correlated with the volume fraction of BC. During haze events, a fraction of the more-hygroscopic mode particles was observed to contain BC cores; while a minor fraction of the hydrophobic mode particles contained no BC. [ABSTRACT FROM AUTHOR]