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Low clouds play a key role in the Earth-atmosphere energy balance and influence agricultural production and solar-power generation. Smoke aloft has been found to enhance marine stratocumulus through aerosol-cloud interactions, but its role in regions with strong human activities and complex monsoon circulation remains unclear. Here we show that biomass burning aerosols aloft strongly increase the low cloud coverage over both land and ocean in subtropical southeastern Asia. The degree of this enhancement and its spatial extent are comparable to that in the Southeast Atlantic, even though the total biomass burning emissions in Southeast Asia are only one-fifth of those in Southern Africa. We find that a synergetic effect of aerosol-cloud-boundary layer interaction with the monsoon is the main reason for the strong semi-direct effect and enhanced low cloud formation in southeastern Asia. Biomass burning emissions have been shown to influence clouds in the Atlantic, but its influence in other regions is not well known. Here, the authors show that biomass burning aerosols increase the low-cloud cover over subtropical southeastern Asia by a similar magnitude than over the Atlantic.

Non-methane volatile organic compounds (NMVOCs) are important ozone and secondary organic aerosol precursors and play important roles in tropospheric chemistry. In this work, we estimated the total and speciated NMVOC emissions from China's anthropogenic sources during 1990–2017 by using a bottom-up emission inventory framework and investigated the main drivers behind the trends. We found that anthropogenic NMVOC emissions in China have been increasing continuously since 1990 due to the dramatic growth in activity rates and absence of effective control measures. We estimated that anthropogenic NMVOC emissions in China increased from 9.76 Tg in 1990 to 28.5 Tg in 2017, mainly driven by the persistent growth from the industry sector and solvent use. Meanwhile, emissions from the residential and transportation sectors declined after 2005, partly offsetting the total emission increase. During 1990–2017, mass-based emissions of alkanes, alkenes, alkynes, aromatics, oxygenated volatile organic compounds (OVOCs) and other species increased by 274 %, 88 %, 4 %, 387 %, 91 % and 231 %, respectively. Following the growth in total NMVOC emissions, the corresponding ozone formation potential (OFP) increased from 38.2 Tg of O3 in 1990 to 99.7 Tg of O3 in 2017. We estimated that aromatics accounted for the largest share (43 %) of the total OFP, followed by alkenes (37 %) and OVOCs (10 %). Growth in China's NMVOC emissions was mainly driven by the transportation sector before 2000, while industry and solvent use dominated the emission growth during 2000–2010. Since 2010, although emissions from the industry sector and solvent use kept growing, strict control measures on transportation and fuel transition in residential stoves have successfully slowed down the increasing trend, especially after the implementation of China's clean air action since 2013. However, compared to large emission decreases in other major air pollutants in China (e.g., SO2, NOx and primary PM) during 2013–2017, the relatively flat trend in NMVOC emissions and OFP revealed the absence of effective control measures, which might have contributed to the increase in ozone during the same period. Given their high contributions to emissions and OFP, tailored control measures for solvent use and industrial sources should be developed, and multi-pollutant control strategies should be designed to mitigate both PM2.5 and ozone pollution simultaneously.

China’s strategy to concurrently address climate change and air pollution mitigation is hindered by a lack of comprehensive information on source contributions to health damage and carbon emissions. Here we show notable discrepancies between source contributions to CO 2 emissions and fine particulate matter (PM 2.5 )-related mortality by using adjoint emission sensitivity modeling to attribute premature mortality in 2017 to 53 sector and fuel/process combinations with high spatial resolution. Our findings reveal that monetized PM 2.5 health damage exceeds climate impacts in over half of the analyzed subsectors. In addition to coal-fired energy generators and industrial boilers, the combined health and climate costs from energy-intensive processes, diesel-powered vehicles, domestic coal combustion, and agricultural activities exceed 100 billion US dollars, with health-related costs predominating. This research highlights the critical need to integrate the social costs of health damage with climate impacts to develop more balanced mitigation strategies toward these dual goals, particularly during fuel transition and industrial structure upgrading. Comprehensive modeling analysis reveals significant differences in the source contribution of PM 2.5 -related mortality and CO 2 emissions in China, highlighting the need for a balanced approach to synergistic control.

Phase transitions of nanoparticles are of fundamental importance in atmospheric sciences, but current understanding is insufficient to explain observations at the nano-scale. In particular, discrepancies exist between observations and model predictions of deliquescence and efflorescence transitions and the hygroscopic growth of salt nanoparticles. Here we show that these discrepancies can be resolved by consideration of particle size effects with consistent thermodynamic data. We present a new method for the determination of water and solute activities and interfacial energies in highly supersaturated aqueous solution droplets (Differential Köhler Analysis). Our analysis reveals that particle size can strongly alter the characteristic concentration of phase separation in mixed systems, resembling the influence of temperature. Owing to similar effects, atmospheric secondary organic aerosol particles at room temperature are expected to be always liquid at diameters below ~20 nm. We thus propose and demonstrate that particle size should be included as an additional dimension in the equilibrium phase diagram of aerosol nanoparticles. Although phase transitions are fundamental for understanding aerosol particles, current models are insufficient to explain observations at the nanoscale. Here, the authors present a method for investigating droplets, suggesting particle size is a key determinant in the phase diagram of nanoparticles.

The MIX inventory is developed for the years 2008 and 2010 to support the Model Inter-Comparison Study for Asia (MICS-Asia) and the Task Force on Hemispheric Transport of Air Pollution (TF HTAP) by a mosaic of up-to-date regional emission inventories. Emissions are estimated for all major anthropogenic sources in 29 countries and regions in Asia. We conducted detailed comparisons of different regional emission inventories and incorporated the best available ones for each region into the mosaic inventory at a uniform spatial and temporal resolution. Emissions are aggregated to five anthropogenic sectors: power, industry, residential, transportation, and agriculture. We estimate the total Asian emissions of 10 species in 2010 as follows: 51.3 Tg SO2, 52.1 Tg NOx, 336.6 Tg CO, 67.0 Tg NMVOC (non-methane volatile organic compounds), 28.8 Tg NH3, 31.7 Tg PM10, 22.7 Tg PM2.5, 3.5 Tg BC, 8.3 Tg OC, and 17.3 Pg CO2. Emissions from China and India dominate the emissions of Asia for most of the species. We also estimated Asian emissions in 2006 using the same methodology of MIX. The relative change rates of Asian emissions for the period of 2006–2010 are estimated as follows: −8.1 % for SO2, +19.2 % for NOx, +3.9 % for CO, +15.5 % for NMVOC, +1.7 % for NH3, −3.4 % for PM10, −1.6 % for PM2.5, +5.5 % for BC, +1.8 % for OC, and +19.9 % for CO2. Model-ready speciated NMVOC emissions for SAPRC-99 and CB05 mechanisms were developed following a profile-assignment approach. Monthly gridded emissions at a spatial resolution of 0.25°  ×  0.25° are developed and can be accessed from http://www.meicmodel.org/dataset-mix.

Nitrous acid (HONO) is a precursor of the hydroxyl radical (OH), a key oxidant in the degradation of most air pollutants. Field measurements indicate a large unknown source of HONO during the day time. Release of nitrous acid (HONO) from soil has been suggested as a major source of atmospheric HONO. We hypothesize that nitrite produced by biological nitrate reduction in oxygen-limited microzones in wet soils is a source of such HONO. Indeed, we found that various contrasting soil samples emitted HONO at high water-holding capacity (75–140%), demonstrating this to be a widespread phenomenon. Supplemental nitrate stimulated HONO emissions, whereas ethanol (70% v/v) treatment to minimize microbial activities reduced HONO emissions by 80%, suggesting that nitrate-dependent biotic processes are the sources of HONO. High-throughput Illumina sequencing of 16S rRNA as well as functional gene transcripts associated with nitrate and nitrite reduction indicated that HONO emissions from soil samples were associated with nitrate reduction activities of diverse Proteobacteria . Incubation of pure cultures of bacterial nitrate reducers and gene-expression analyses, as well as the analyses of mutant strains deficient in nitrite reductases, showed positive correlations of HONO emissions with the capability of microbes to reduce nitrate to nitrite. Thus, we suggest biological nitrate reduction in oxygen-limited microzones as a hitherto unknown source of atmospheric HONO, affecting biogeochemical nitrogen cycling, atmospheric chemistry, and global modeling.

With improving PM 2.5 air quality, the tropospheric ozone (O 3 ) has become the top issue of China’s air pollution control. Here, we combine comprehensive observational data analysis with models to unveil the contributions of different processes and precursors to the change of O 3 during COVID-19 lockdown in the Yangtze River Delta (YRD), one of the most urbanized megacity regions of eastern China. Despite a 44 to 47% reduction in volatile organic compounds (VOCs) and nitrogen oxides (NO x ) emissions, maximum daily 8-h average (MDA8) ozone concentrations increase from 28 ppbv in pre-lockdown to 43 ppbv in lockdown period. We reproduce this transition with the WRF-Chem model, which shows that ~80% of the increase in MDA8 is due to meteorological factors (seasonal variation and radiation), and ~20% is due to emission reduction. We find that daytime photochemistry does not lead to an increase but rather a decrease of daytime O 3 production during the lockdown. However, the reduced O 3 production is overwhelmed by the weakened nitric oxide (NO) titration resulting in a net increase of O 3 concentration. Although the emission reduction increases O 3 concentration, it leads to a decrease in the O x (O 3  + NO 2 ) concentration, suggesting reduced atmospheric oxidation capacity on a regional scale. The dominant effect of NO titration demonstrates the importance of prioritizing VOCs reduction, especially from solvent usage and the petrochemical industry with high emission ratios of VOCs/NO x.

Hydroxyl radicals (OH) are a key species in atmospheric photochemistry. In the lower atmosphere, up to ~30% of the primary OH radical production is attributed to the photolysis of nitrous acid (HONO), and field observations suggest a large missing source of HONO. We show that soil nitrite can release HONO and explain the reported strength and diurnal variation of the missing source. Fertilized soils with low pH appear to be particularly strong sources of HONO and OH. Thus, agricultural activities and land-use changes may strongly influence the oxidizing capacity of the atmosphere. Because of the widespread occurrence of nitrite-producing microbes, the release of HONO from soil may also be important in natural environments, including forests and boreal regions.

Biomass burning (BB) aerosols can influence regional and global climate through interactions with radiation, clouds, and precipitation. Here, we investigate the impact of BB aerosols on the energy balance and hydrological cycle over the Amazon Basin during the dry season. We performed simulations with a fully coupled meteorology–chemistry model, the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem), for a range of different BB emission scenarios to explore and characterize nonlinear effects and individual contributions from aerosol–radiation interactions (ARIs) and aerosol–cloud interactions (ACIs). The ARIs of BB aerosols tend to suppress low-level liquid clouds by local warming and increased evaporation and to facilitate the formation of high-level ice clouds by enhancing updrafts and condensation at high altitudes. In contrast, the ACIs of BB aerosol particles tend to enhance the formation and lifetime of low-level liquid clouds by providing more cloud condensation nuclei (CCN) and to suppress the formation of high-level ice clouds by reducing updrafts and condensable water vapor at high altitudes (>8 km). For scenarios representing the lower and upper limits of BB emission estimates for recent years (2002–2016), we obtained total regional BB aerosol radiative forcings of −0.2 and 1.5 W m−2, respectively, showing that the influence of BB aerosols on the regional energy balance can range from modest cooling to strong warming. We find that ACIs dominate at low BB emission rates and low aerosol optical depth (AOD), leading to an increased cloud liquid water path (LWP) and negative radiative forcing, whereas ARIs dominate at high BB emission rates and high AOD, leading to a reduction of LWP and positive radiative forcing. In all scenarios, BB aerosols led to a decrease in the frequency of occurrence and rate of precipitation, caused primarily by ACI effects at low aerosol loading and by ARI effects at high aerosol loading. The dependence of precipitation reduction on BB aerosol loading is greater in a strong convective regime than under weakly convective conditions. Overall, our results show that ACIs tend to saturate at high aerosol loading, whereas the strength of ARIs continues to increase and plays a more important role in highly polluted episodes and regions. This should hold not only for BB aerosols over the Amazon, but also for other light-absorbing aerosols such as fossil fuel combustion aerosols in industrialized and densely populated areas. The importance of ARIs at high aerosol loading highlights the need for accurately characterizing aerosol optical properties in the investigation of aerosol effects on clouds, precipitation, and climate.

In recent years, severe haze events often occurred in China, causing serious environmental problems. The mechanisms responsible for the haze formation, however, are still not well understood, hindering the forecast and mitigation of haze pollution. Our study of the 2012–13 winter haze events in Beijing shows that atmospheric water vapour plays a critical role in enhancing the heavy haze events. Under weak solar radiation and stagnant moist meteorological conditions in winter, air pollutants and water vapour accumulate in a shallow planetary boundary layer (PBL). A positive feedback cycle is triggered resulting in the formation of heavy haze: (1) the dispersal of water vapour is constrained by the shallow PBL, leading to an increase in relative humidity (RH); (2) the high RH induces an increase of aerosol particle size by enhanced hygroscopic growth and multiphase reactions to increase particle size and mass, which results in (3) further dimming and decrease of PBL height, and thus further depressing of aerosol and water vapour in a very shallow PBL. This positive feedback constitutes a self-amplification mechanism in which water vapour leads to a trapping and massive increase of particulate matter in the near-surface air to which people are exposed with severe health hazards.