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.

To estimate the emissions of anthropogenic semivolatile organic compounds (SOCs) from East Asia and to identify unique SOC molecular markers in Asian air masses, high-volume air samples were collected on the island of Okinawa, Japan between 22 March and 2 May 2004. Contributions from different source regions (China, Japan, the Koreas, Russia, and ocean/local) were estimated by use of source region impact factors (SRIFs). Elevated concentrations of hexachlorobenzene (HCB), hexachlorcyclohexanes (HCHs), dichlorodiphenyltrichloroethanes (DDTs), and particulate-phase polycyclic aromatic hydrocarbons (PAHs) were attributed to air masses from China. A large proportion of the variation in the current-use pesticides, gas-phase PAHs, and polychlorinated biphenyl (PCB) concentrations was explained by meteorology. Chlordanes showed a technical mixture profile and similar concentrations regardless of source region. alpha/gamma HCH and trans/cis chlordane ratios did not vary significantly with different source regions and had regional averages of 2.5 +/- 1.0 and 1.2 +/- 0.3, respectively. Particulate-phase PAH concentrations were significantly correlated (p value < 0.05) with other incomplete combustion byproduct concentrations, including elemental mercury (Hg0), CO, NOx, black carbon, submicrometer aerosols, and SO2. By use of measured PAH, CO, and black carbon concentrations and estimated CO and black carbon emission inventories, the emission of six carcinogenic particulate-phase PAHs was estimated to be 1518-4179 metric tons/year for Asia and 778-1728 metric tons/year for China, respectively. These results confirm that East Asian outflow contains significant emissions of carcinogenic particulate-phase PAHs.

[1] East Asia, including China, is the largest source of anthropogenic black carbon (BC). In estimating the BC emissions from this region, it is advantageous to use BC mass concentrations measured at remote locations on the ocean appropriately distant from the large sources because of spatially uniform distributions through mixing during transport. We made continuous measurements of the BC mass concentration with an accuracy of about 10% at Cape Hedo on Okinawa Island, Japan, in the East China Sea, from

[1] Aerosol chemical composition and gaseous species were measured at Cape Hedo, Okinawa, Japan (CHO), during the ABC/EAREX project period in March 2005, using high-time-resolution instruments including an Aerodyne quadrupole aerosol mass spectrometer (Q-AMS), a tapered element oscillating microbalance (TEOM), and gas monitors in order to investigate the transport and subsequent chemical transformation of aerosol in the east Asian region. Sulfate was the dominant species in fine aerosol mode and the average concentration of ammonium, sulfate and organics was 1.25, 6.37 and 2.16 mg m À3 , respectively. The sulfate concentration observed at CHO in 2005 was about 1.5-2 times higher than that in 1994. For the majority of high-sulfate observations, the air mass was transported from the central east Chinese region (between Shanghai and the Shandong Peninsula). Sulfate transport was intermittent and strongly correlated with the passage of synoptic-scale high-/low-pressure systems. Chemical components and their concentration showed significant change on 17-18 March, which is accounted for by the change in air mass origin and the synoptic-scale weather system. In addition, it is suggested that the difference of air quality at the air mass origin reflects the chemical composition at CHO. The high sulfate concentration required heterogeneous conversion of SO 2 to sulfate at a rate of 2.0% h À1 . A pronounced signal at m/z = 44 confirmed that organic compounds were oxidized.