Organic aerosol (OA) particles affect climate forcing and human health, but their sources and evolution remain poorly characterized. We present a unifying model framework describing the atmospheric evolution of OA that is constrained by high-time-resolution measurements of its composition, volatility, and oxidation state. OA and OA precursor gases evolve by becoming increasingly oxidized, less volatile, and more hygroscopic, leading to the formation of oxygenated organic aerosol (OOA), with concentrations comparable to those of sulfate aerosol throughout the Northern Hemisphere. Our model framework captures the dynamic aging behavior observed in both the atmosphere and laboratory: It can serve as a basis for improving parameterizations in regional and global models.

Organic aerosol (OA) data acquired by the Aerosol Mass Spectrometer (AMS) in 37 field campaigns were deconvolved into hydrocarbon‐like OA (HOA) and several types of oxygenated OA (OOA) components. HOA has been linked to primary combustion emissions (mainly from fossil fuel) and other primary sources such as meat cooking. OOA is ubiquitous in various atmospheric environments, on average accounting for 64%, 83% and 95% of the total OA in urban, urban downwind, and rural/remote sites, respectively. A case study analysis of a rural site shows that the OOA concentration is much greater than the advected HOA, indicating that HOA oxidation is not an important source of OOA, and that OOA increases are mainly due to SOA. Most global models lack an explicit representation of SOA which may lead to significant biases in the magnitude, spatial and temporal distributions of OA, and in aerosol hygroscopic properties.

Poor air quality is globally the largest environmental health risk. Epidemiological studies have uncovered clear relationships of gaseous pollutants and particulate matter (PM) with adverse health outcomes, including mortality by cardiovascular and respiratory diseases. Studies of health impacts by aerosols are highly multidisciplinary with a broad range of scales in space and time. We assess recent advances and future challenges regarding aerosol effects on health from molecular to global scales through epidemiological studies, field measurements, health-related properties of PM, and multiphase interactions of oxidants and PM upon respiratory deposition. Global modeling combined with epidemiological exposure-response functions indicates that ambient air pollution causes more than four million premature deaths per year. Epidemiological studies usually refer to PM mass concentrations, but some health effects may relate to specific constituents such as bioaerosols, polycyclic aromatic compounds, and transition metals. Various analytical techniques and cellular and molecular assays are applied to assess the redox activity of PM and the formation of reactive oxygen species. Multiphase chemical interactions of lung antioxidants with atmospheric pollutants are crucial to the mechanistic and molecular understanding of oxidative stress upon respiratory deposition. The role of distinct PM components in health impacts and mortality needs to be clarified by integrated research on various spatiotemporal scales for better evaluation and mitigation of aerosol effects on public health in the Anthropocene.

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[1] The radiative impact of the mixing state of black carbon (BC) aerosol is investigated in Asian outflow. The mixing state and size distribution of BC aerosol were measured with a ground-based single-particle soot photometer at a remote island (Fukue) in Japan in spring 2007. The mass concentration of BC in Asian continental air masses reached 0.5 mg m À3 , with a mass median diameter of 200-220 nm. The median value of the shell/core diameter ratio increased to $1.6 in Asian continental and maritime air masses with a core diameter of 200 nm, while in free tropospheric and Japanese air masses it was 1.3-1.4. On the basis of theoretical calculations using the size distribution and mixing state of BC aerosol, scattering and absorption properties of PM 1 aerosols were calculated under both dry and ambient conditions, considering the hygroscopic growth of aerosols. It was estimated that internal mixing enhanced the BC absorption by a factor of 1.5-1.6 compared to external mixing. The calculated absorption coefficient was 2-3 times higher in Asian continental air masses than in clean air. Coatings reduced the single-scattering albedo (SSA) of PM 1 aerosol by 0.01-0.02, which indicates the importance of the mixing state of BC aerosol in evaluating its radiative influence. The SSA was sensitive to changes in air mass type, with a value of $0.98 in Asian continental air masses and $0.95 in Japanese and free tropospheric air masses under ambient conditions.