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.

The dual carbon isotope signatures and optical properties of carbonaceous aerosols have been investigated simultaneously for the first time in the South Asian outflow during an intensive campaign at the Maldives Climate Observatory on Hanimaadhoo (MCOH) (February and March 2012). As one component of the Cloud Aerosol Radiative Forcing Dynamics Experiment, this paper reports on the sources and the atmospheric processing of elemental carbon (EC) and water‐soluble organic carbon (WSOC) as examined by a dual carbon isotope approach. The radiocarbon (Δ¹⁴C) data show that WSOC has a significantly higher biomass/biogenic contribution (86 ± 5%) compared to EC (59 ± 4%). The more ¹³C‐enriched signature of MCOH‐WSOC (−20.8 ± 0.7‰) compared to MCOH‐EC (−25.8 ± 0.3‰) and megacity Delhi WSOC (−24.1 ± 0.9‰) suggests that WSOC is significantly more affected by aging during long‐range transport than EC. The δ¹³C‐Δ¹⁴C signal suggests that the wintertime WSOC intercepted over the Indian Ocean largely represents aged primary biomass burning aerosols. Since light‐absorbing organic carbon aerosols (Brown Carbon (BrC)) have recently been identified as potential contributors to positive radiative forcing, optical properties of WSOC were also investigated. The mass absorption cross section of WSOC (MAC₃₆₅) was 0.5 ± 0.2 m² g⁻¹ which is lower than what has been observed at near‐source sites, indicating a net decrease of WSOC light‐absorption character during long‐range transport. Near‐surface WSOC at MCOH accounted for ~1% of the total direct solar absorbance relative to EC, which is lower than the BrC absorption inferred from solar spectral observations of ambient aerosols, suggesting that a significant portion of BrC might be included in the water‐insoluble portion of organic aerosols.

Organic aerosol (OA) constitutes a substantial fraction of fine particles and affects both human health and climate. It is becoming clear that OA absorbs light substantially (hence termed Brown Carbon, BrC), adding uncertainties to global aerosol radiative forcing estimations. The few current radiative-transfer and chemical-transport models that include BrC primarily consider sources from biogenic and biomass combustion. However, radiocarbon fingerprinting here clearly indicates that light-absorbing organic carbon in winter Beijing, the capital of China, is mainly due to fossil sources, which contribute the largest part to organic carbon (OC, 67 ± 3%) and its sub-constituents (water-soluble OC, WSOC: 54 ± 4%, and water-insoluble OC, WIOC: 73 ± 3%). The dual-isotope (Δ¹⁴C/δ¹³C) signatures, organic molecular tracers and Beijing-tailored emission inventory identify that this fossil source is primarily from coal combustion activities in winter, especially from the residential sector. Source testing on Chinese residential coal combustion provides direct evidence that intensive coal combustion could contribute to increased light-absorptivity of ambient BrC in Beijing winter. Coal combustion is an important source to BrC in regions such as northern China, especially during the winter season. Future modeling of OA radiative forcing should consider the importance of both biomass and fossil sources.