Wildfire smoke, consisting primarily of organic aerosols, has profound impacts on air quality, climate and human health. Wildfire organic aerosol evolves over long-time photochemical oxidation due to the formation and ageing of secondary organic aerosol, which substantially changes its magnitude and properties. However, there are large uncertainties in the long-time ageing of wildfire organic aerosol because of the distinct ageing behaviours of the complex organic emissions. Here we developed an oxidation model that simulates the ageing of wildfire organic emissions in the full volatility range on a precursor level and integrated insights from single-species ageing and wildfire emissions ageing experiments and field plume observations to constrain the long-time ageing of wildfire organic aerosol. The model captured the enhancement of organic aerosol mass (2–8 times) and oxygen-to-carbon ratio (1–4 times) in the wildfire ageing experiments. It also reconciled a long-standing discrepancy between field and laboratory observations of the magnitude of secondary organic aerosol formation. The model indicated large emissions-driven variations in precursor contributions to secondary organic aerosol, which further evolve with long-time ageing. The estimated global wildfire secondary organic aerosol production (139 ± 34 Tg per year) was much higher than previous studies omitting or under-constraining long-time ageing.

Limited research has been conducted on the contributions of local and nonlocal emission sources to ambient fine particulate matter (PM2.5) and ozone (O3) and their associated mortality. In this study, we estimated the total mortality resulting from long-term PM2.5 and O3 exposures in California in 2012 using multiple concentration response functions (CRFs) and attributed the estimated mortality to different emission groups. The point estimates of PM2.5-associated mortality in California ranged from 12,700 to 26,700, of which 53% were attributable to in-state anthropogenic emissions. Based on new epidemiological evidence, we estimated that O3 could be associated with up to 13,700 deaths from diseases of both the respiratory and cardiovascular systems in California. In addition, 75% of the ambient O3 in California was due to distant emissions outside the western United States, leading to 92% of the O3-associated mortality. Overall, distant emissions lead to greater mortality burdens of air pollution in California than local anthropogenic emissions.

The multi‐spectral satellite sensors such as MODIS have a large swath, high spatial resolution, and well onboard calibration, enabling aerosol retrievals with daily global coverage. Despite numerous available bands, MODIS aerosol algorithms over land typically only utilize measurements from 2 to 3 spectral wavelengths to retrieve Aerosol Optical Depth (AOD) based on prescribed aerosol models. To make full use of multi‐spectral measurements and prior information, we developed an aerosol algorithm based on physics‐informed deep learning (PDL) approach. With physical constraint from radiative transfer simulation, PDL can construct model functions between the whole spectral measurements and each retrieved aerosol parameter separately. AERONET validations in eastern China show that MODIS PDL algorithm can accurately retrieve AOD and fine AOD (R = 0.936) at 1 km resolution and has reliable performance in coarse AOD as well as notable sensitivity to aerosol absorption. The flexible and efficient PDL method provides a generalized algorithm for common multi‐spectral satellite measurements.

This study analyzed the aerosol optical properties derived by SKYRAD.pack versions 5.0 and 4.2 (referred to as V5.0 and V4.2) using the radiometer measurements over Qionghai and Yucheng in China, two new sites of the sky radiometer network (SKYNET). As V5.0 uses an a priori size distribution function (SDF) of a bimodal log-normal function, the volume size distribution retrieved by V5.0 presented bimodal patterns with a 0.1–0.2 µm fine particle mode and a 3.0–6.0 µm coarse particle mode both over Qionghai and Yucheng. The differences in the volume size distributions between the two versions were very large for the coarse mode with a radius of over 5 µm. The single scattering albedos (SSAs) by V5.0 correlated with SSAs by V4.2 with R=0.88, 0.87, 0.90, 0.88, and 0.92 at wavelengths of 400, 500, 670, 870, and 1020 nm over Qionghai, respectively. The correlation coefficients were around 0.95, 0.95, 0.96, 0.94, and 0.91 at the five channels in Yucheng. An error of ±5 % for the solid view angle (SVA) introduced about ±2 % differences in retrieved SSA values both by V4.2 and V5.0. An error of ±50 % for ground surface albedo (A_g) caused about 1 % averaged differences in retrieved SSA values by the two versions. With the atmospheric pressure (PRS) increased by 1 %, 2 %, 3 %, and 4 %, the averaged changes in SSAs did not exceed 0.8 % both by V4.2 and V5.0. The SSA differences at 500 nm between the two versions decreased, while aerosol optical depths (AODs) increased over both sites. The seasonal variability of the aerosol properties over Qionghai and Yucheng was investigated based on SKYRAD.pack V5.0. The seasonal averaged AOD over Qionghai had higher values in spring, winter, and autumn and lower values in summer. The AOD averages were commonly higher in summer and spring than in winter and autumn in Yucheng. The lowest seasonal averaged SSAs were both observed in winter at the two sites. The fraction of the fine aerosol particles was much smaller in summer than in other seasons over Qionghai; the volume fraction of the coarse-mode particle in Yucheng had much larger values compared to the fine-mode particle in all seasons. The validation results provide valuable references for continued improvement of the retrieval algorithms of SKYNET and other aerosol observational networks.

The reductions in aerosols often exacerbate climate warming. It remains unclear how to effectively alleviate PM _2.5 pollution while minimizing the penalty on climate warming. Here we identify the clean air measures in China that are associated with low aerosol climate penalty efficiency (ACPE), which is defined as aerosol radiative forcing per unit PM _2.5 concentration reduction. The measures in transportation, residential combustion, and open burning sectors generally caused lower ACPE [0.07, 0.24, and 0.10 (W m ⁻² )/(μg m ⁻³ )] than those from other sectors [0.34–0.46 (W m ⁻² )/(μg m ⁻³ )]. This is ascribed to relatively small decreases in cloud concentration nuclei per unit PM _2.5 reduction in these sectors, which is further attributed to either relatively low aerosol hygroscopicity or relatively small decrease in aerosol number. Most measures in the former three sectors have low ACPE of <0.15 [(W m ⁻² )/(μg m ⁻³ )] and thus may be prioritized for synergistically controlling PM _2.5 pollution and climate warming.

Achieving carbon neutrality and improving air quality are pivotal sustainability strategies for the Global South countries. However, their global climate impacts over a realistic timescale remain unclear. Here we evaluate the climate impacts of China’s carbon neutrality and Beautiful China policies using a fully coupled Earth system model and updated future anthropogenic emission scenarios. We find that, for an unexpectedly long time through ~2070, China’s air pollutant reductions can cause a large global surface warming (0.12 ± 0.09 K for 2050–2070) that almost offsets the cooling from concurrent CO₂ emission reduction (0.16 ± 0.05 K for 2050–2070), compared to a business-as-usual scenario. This warming is mainly attributed to reduced SO₂ and organic matter emissions. Moreover, combined air pollutants and CO₂ declines create a striking hemispheric temperature change contrast, because of the stronger aerosol-induced heating in the Northern Hemisphere. Considering that most future air pollutant reductions represent synergistic effects of carbon neutrality policies, the associated inevitable warming effect over decades highlights the importance of exploring more aggressive policies including early carbon neutrality, methane reductions, and negative carbon emissions.