Observational Evidence of Large Contribution from Primary Sources for Carbon Monoxide in the South Asian Outflow.

South Asian air is among the most polluted in the world, causing premature death of millions and asserting a strong perturbation of the regional climate. A central component is carbon monoxide (CO), which is a key modulator of the oxidizing capacity of the atmosphere and a potent indirect greenhouse gas. While CO concentrations are declining elsewhere, South Asia exhibits an increasing trend for unresolved reasons. In this paper, we use dual-isotope (δ13C and δ18O) fingerprinting of CO intercepted in the South Asian outflow to constrain the relative contributions from primary and secondary CO sources. Results show that combustion-derived primary sources dominate the wintertime continental CO fingerprint (fprimary ∼ 79 ± 4%), significantly higher than the global estimate (fprimary ∼ 55 ± 5%). Satellite-based inventory estimates match isotope-constrained fprimary-CO, suggesting observational convergence in source characterization and a prospect for model-observation reconciliation. This "ground-truthing" emphasizes the pressing need to mitigate incomplete combustion activities for climate/air quality benefits in South Asia.

Source Quantification of South Asian Black Carbon Aerosols with Isotopes and Modeling.

Black carbon (BC) aerosols perturb climate and impoverish air quality/human health-affecting ∼1.5 billion people in South Asia. However, the lack of source-diagnostic observations of BC is hindering the evaluation of uncertain bottom-up emission inventories (EIs) and thereby also models/policies. Here, we present dual-isotope-based (Δ14C/δ13C) fingerprinting of wintertime BC at two receptor sites of the continental outflow. Our results show a remarkable similarity in contributions of biomass and fossil combustion, both from the site capturing the highly populated highly polluted Indo-Gangetic Plain footprint (IGP; Δ14C-fbiomass = 50 ± 3%) and the second site in the N. Indian Ocean representing a wider South Asian footprint (52 ± 6%). Yet, both sites reflect distinct δ13C-fingerprints, indicating a distinguishable contribution of C4-biomass burning from peninsular India (PI). Tailored-model-predicted season-averaged BC concentrations (700 ± 440 ng m-3) match observations (740 ± 250 ng m-3), however, unveiling a systematically increasing model-observation bias (+19% to -53%) through winter. Inclusion of BC from open burning alone does not reconcile predictions (fbiomass = 44 ± 8%) with observations. Direct source-segregated comparison reveals regional offsets in anthropogenic emission fluxes in EIs, overestimated fossil-BC in the IGP, and underestimated biomass-BC in PI, which contributes to the model-observation bias. This ground-truthing pinpoints uncertainties in BC emission sources, which benefit both climate/air-quality modeling and mitigation policies in South Asia.

Leakage of old carbon dioxide from a major river system in the Canadian Arctic.

The Canadian Arctic is warming at an unprecedented rate. Warming-induced permafrost thaw can lead to mobilization of aged carbon from stores in soils and rocks. Tracking the carbon pools supplied to surrounding river networks provides insight on pathways and processes of greenhouse gas release. Here, we investigated the dual-carbon isotopic characteristics of the dissolved inorganic carbon (DIC) pool in the main stem and tributaries of the Mackenzie River system. The radiocarbon (14C) activity of DIC shows export of "old" carbon (2,380 ± 1,040 14C years BP on average) occurred during summer in sampling years. The stable isotope composition of river DIC implicates degassing of aged carbon as CO2 from riverine tributaries during transport to the delta; however, information on potential drivers and fluxes are still lacking. Accounting for stable isotope fractionation during CO2 loss, we show that a large proportion of this aged carbon (60 ± 10%) may have been sourced from biospheric organic carbon oxidation, with other inputs from carbonate weathering pathways and atmospheric exchange. The findings highlight hydrologically connected waters as viable pathways for mobilization of aged carbon pools from Arctic permafrost soils.

Sulfur-isotope anomalies recorded in Antarctic ice cores as a potential proxy for tracing past ozone layer depletion events.

Changes in the cosmic-ray background of the Earth can impact the ozone layer. High-energy cosmic events [e.g. supernova (SN)] or rapid changes in the Earth's magnetic field [e.g. geomagnetic Excursion (GE)] can lead to a cascade of cosmic rays. Ensuing chemical reactions can then cause thinning/destruction of the ozone layer-leading to enhanced penetration of harmful ultraviolet (UV) radiation toward the Earth's surface. However, observational evidence for such UV "windows" is still lacking. Here, we conduct a pilot study and investigate this notion during two well-known events: the multiple SN event (≈10 kBP) and the Laschamp GE event (≈41 kBP). We hypothesize that ice-core-Δ33S records-originally used as volcanic fingerprints-can reveal UV-induced background-tropospheric-photochemical imprints during such events. Indeed, we find nonvolcanic S-isotopic anomalies (Δ33S ≠ 0‰) in background Antarctic ice-core sulfate during GE/SN periods, thereby confirming our hypothesis. This suggests that ice-core-Δ33S records can serve as a proxy for past ozone-layer-depletion events.

Photochemical degradation affects the light absorption of water-soluble brown carbon in the South Asian outflow.

Light-absorbing organic aerosols, known as brown carbon (BrC), counteract the overall cooling effect of aerosols on Earth's climate. The spatial and temporal dynamics of their light-absorbing properties are poorly constrained and unaccounted for in climate models, because of limited ambient observations. We combine carbon isotope forensics (δ13C) with measurements of light absorption in a conceptual aging model to constrain the loss of light absorptivity (i.e., bleaching) of water-soluble BrC (WS-BrC) aerosols in one of the world's largest BrC emission regions-South Asia. On this regional scale, we find that atmospheric photochemical oxidation reduces the light absorption of WS-BrC by ~84% during transport over 6000 km in the Indo-Gangetic Plain, with an ambient first-order bleaching rate of 0.20 ± 0.05 day-1 during over-ocean transit across Bay of Bengal to an Indian Ocean receptor site. This study facilitates dynamic parameterization of WS-BrC absorption properties, thereby constraining BrC climate impact over South Asia.