Combustion-derived black carbon (BC) aerosols accelerate glacier melting in the Himalayas and in Tibet (the Third Pole (TP)), thereby limiting the sustainable freshwater supplies for billions of people. However, the sources of BC reaching the TP remain uncertain, hindering both process understanding and efficient mitigation. Here we present the source-diagnostic Δ¹⁴C/δ¹³C compositions of BC isolated from aerosol and snowpit samples in the TP. For the Himalayas, we found equal contributions from fossil fuel (46±11%) and biomass (54±11%) combustion, consistent with BC source fingerprints from the Indo-Gangetic Plain, whereas BC in the remote northern TP predominantly derives from fossil fuel combustion (66±16%), consistent with Chinese sources. The fossil fuel contributions to BC in the snowpits of the inner TP are lower (30±10%), implying contributions from internal Tibetan sources (for example, yak dung combustion). Constraints on BC sources facilitate improved modelling of climatic patterns, hydrological effects and provide guidance for effective mitigation actions.

To quantitatively evaluate the effect of carbonaceous aerosols on the south edge of the Tibetan Plateau, aerosol samples were collected weekly from August 2009 to July 2010 at Qomolangma (Mt. Everest) Station for Atmospheric and Environmental Observation and Research (QOMS, 28.36° N, 86.95° E, 4276 m a.s.l.). The average concentrations of organic carbon (OC), elemental carbon (EC) and water-soluble organic carbon were 1.43, 0.25 and 0.77 μg m⁻³, respectively. The concentration levels of OC and EC at QOMS are comparable to those at high-elevation sites on the southern slopes of the Himalayas (Langtang and Nepal Climate Observatory at Pyramid, or NCO-P), but 3 to 6 times lower than those at Manora Peak, India, and Godavari, Nepal. Sulfate was the most abundant anion species followed by nitrate, accounting for 25 and 12% of total ionic mass, respectively. Ca²⁺ was the most abundant cation species (annual average of 0.88 μg m⁻³). The dust loading, represented by Ca²⁺ concentration, was relatively constant throughout the year. OC, EC and other ionic species (NH₄⁺, K⁺, NO₃⁻ and SO₄²⁻) exhibited a pronounced peak in the pre-monsoon period and a minimum in the monsoon season, being similar to the seasonal trends of aerosol composition reported previously from the southern slope of the Himalayas, such as Langtang and NCO-P. The strong correlation of OC and EC in QOMS aerosols with K⁺ and levoglucosan indicates that they mainly originated from biomass burning. The fire spots observed by MODIS and backward air-mass trajectories further demonstrate that in pre-monsoon season, agricultural and forest fires in northern India and Nepal were most likely sources of carbonaceous aerosol at QOMS. Moreover, the CALIOP observations confirmed that air-pollution plumes crossed the Himalayas during this period. The highly coherent variation of daily aerosol optical depth (500 nm) between QOMS and NCO-P indicates that both slopes of the Himalayas share a common atmospheric environment regime. In addition to large-scale atmospheric circulation, the unique mountain/valley breeze system can also have an important effect on air-pollutant transport.

Brown carbon (BrC) has recently emerged as an important light-absorbing aerosol. This study provides interannual and seasonal variations in light absorption properties, chemical composition, and sources of water-soluble BrC (WS-BrC) based on PM₁₀ samples collected in Godavari, Nepal, from April 2012 to May 2014. The mass absorption efficiency of WS-BrC at 365 nm (MAE₃₆₅) shows a clear seasonal variability, with the highest MAE₃₆₅ of 1.05 ± 0.21 m² g^–1 in premonsoon season and the lowest in monsoon season (0.59 ± 0.16 m² g^–1). The higher MAE₃₆₅ values in nonmonsoon seasons are associated with fresh biomass burning emissions. This is further substantiated by a strong correlation (r = 0.79, P < 0.01) between Abs₃₆₅ (light absorption coefficient at 365 nm) and levoglucosan. We found, using fluorescence techniques, that humic-like and protein-like substances are the main chromophores in WS-BrC and responsible for 80.2 ± 4.1% and 19.8 ± 4.1% of the total fluorescence intensity, respectively. BrC contributes to 8.78 ± 3.74% of total light absorption over the 300–700 nm wavelength range. Considering the dominant contribution of biomass burning to BrC over Godavari, this study suggests that reduction in biomass burning emission may be a practical method for climate change mitigation in South Asia.

The Campaign on Atmospheric Aerosol Research network of China (CARE-China) is a long-term project for the study of the spatio-temporal distributions of physical aerosol characteristics as well as the chemical components and optical properties of aerosols over China. This study presents the first long-term data sets from this project, including 3 years of observations of online PM_2.5 mass concentrations (2012–2014) and 1 year of observations of PM_2.5 compositions (2012–2013) from the CARE-China network. The average PM_2.5 concentration at 20 urban sites is 73.2 µg m⁻³ (16.8–126.9 µg m⁻³), which was 3 times higher than the average value from the 12 background sites (11.2–46.5 µg m⁻³). The PM_2.5 concentrations are generally higher in east-central China than in the other parts of the country due to their relatively large particulate matter (PM) emissions and the unfavourable meteorological conditions for pollution dispersion. A distinct seasonal variability in PM_2.5 is observed, with highs in the winter and lows during the summer at urban sites. Inconsistent seasonal trends were observed at the background sites. Bimodal and unimodal diurnal variation patterns were identified at both urban and background sites. The chemical compositions of PM_2.5 were analysed at six paired urban and background sites located within the most polluted urban agglomerations – North China Plain (NCP), Yangtze River delta (YRD), Pearl River delta (PRD), North-east China region (NECR), South-west China region (SWCR) – and the cleanest region of China – the Tibetan Autonomous Region (TAR). The major PM_2.5 constituents across all the urban sites are organic matter (OM, 26.0 %), SO₄²⁻ (17.7 %), mineral dust (11.8 %), NO₃⁻ (9.8 %), NH₄⁺ (6.6 %), elemental carbon (EC) (6.0 %), Cl⁻ (1.2 %) at 45 % RH and unaccounted matter (20.7 %). Similar chemical compositions of PM_2.5 were observed at background sites but were associated with higher fractions of OM (33.2 %) and lower fractions of NO₃⁻ (8.6 %) and EC (4.1 %). Significant variations of the chemical species were observed among the sites. At the urban sites, the OM ranged from 12.6 µg m⁻³ (Lhasa) to 23.3 µg m⁻³ (Shenyang), the SO₄²⁻ ranged from 0.8 µg m⁻³ (Lhasa) to 19.7 µg m⁻³ (Chongqing), the NO₃⁻ ranged from 0.5 µg m⁻³ (Lhasa) to 11.9 µg m⁻³ (Shanghai) and the EC ranged from 1.4 µg m⁻³ (Lhasa) to 7.1 µg m⁻³ (Guangzhou). The PM_2.5 chemical species at the background sites exhibited larger spatial heterogeneities than those at urban sites, suggesting different contributions from regional anthropogenic or natural emissions and from long-range transport to background areas. Notable seasonal variations of PM_2.5-polluted days were observed, especially for the megacities in east-central China, resulting in frequent heavy pollution episodes occurring during the winter. The evolution of the PM_2.5 chemical compositions on polluted days was consistent for the urban and nearby background sites, where the sum of sulfate, nitrate and ammonia typically constituted much higher fractions (31–57 %) of PM_2.5 mass, suggesting fine-particle pollution in the most polluted areas of China assumes a regional tendency, and the importance of addressing the emission reduction of secondary aerosol precursors including SO₂ and NO_x. Furthermore, distinct differences in the evolution of [NO₃⁻]∕[SO₄²⁻] ratio and OC∕EC ratio on polluted days imply that mobile sources and stationary (coal combustion) sources are likely more important in Guangzhou and Shenyang, respectively, whereas in Beijing it is mobile emission and residential sources. As for Chongqing, the higher oxidation capacity than the other three cities suggested it should pay more attention to the emission reduction of secondary aerosol precursors. This analysis reveals the spatial and seasonal variabilities of the urban and background aerosol concentrations on a national scale and provides insights into their sources, processes and lifetimes.