Log normal-like concentration distributions are ubiquitously observed in the environment. However, the mechanistic origins are not well understood. In this paper, we show that first order exponential ...kinetics onsets log-normal concentration distributions, under certain assumptions. Given the ubiquity of exponential kinetics, e.g., source and sink processes, this model suggests an explanation for the frequent observation in the environment, and elsewhere. We compare this model to other mechanisms affecting concentration distributions, e.g., source mixing. Finally, we discuss possible implications for data analysis and modelling, e.g., log-normal rates and fluxes.
Estimating the relative contributions from multiple potential sources of a specific component in a mixed environmental matrix is a general challenge in diverse fields such as atmospheric, ...environmental and earth sciences. Perhaps the most common strategy for tackling such problems is by setting up a system of linear equations for the fractional influence of different sources. Even though an algebraic solution of this approach is possible for the common situation with N
+
1 sources and N source markers, such methodology introduces a bias, since it is implicitly assumed that the calculated fractions and the corresponding uncertainties are independent of the variability of the source distributions. Here, a random sampling (RS) strategy for accounting for such statistical bias is examined by investigating rationally designed synthetic data sets. This random sampling methodology is found to be robust and accurate with respect to reproducibility and predictability. This method is also compared to a numerical integration solution for a two-source situation where source variability also is included. A general observation from this examination is that the variability of the source profiles not only affects the calculated precision but also the mean/median source contributions.
► Source variability is an important issue for source apportionment. ► A random sampling technique is used to introduce such variability. ► This technique is examined using synthetic data sets. ► It is found to be both robust and accurate. ► The variability influences both mean source contributions and uncertainties.
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 Δ(14)C/δ(13)C 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 burial of terrestrial organic carbon (terrOC) in marine sediments contributes to the regulation of atmospheric CO
on geological timescales and may mitigate positive feedback to present-day ...climate warming. However, the fate of terrOC in marine settings is debated, with uncertainties regarding its degradation during transport. Here, we employ compound-specific radiocarbon analyses of terrestrial biomarkers to determine cross-shelf transport times. For the World's largest marginal sea, the East Siberian Arctic shelf, transport requires 3600 ± 300 years for the 600 km from the Lena River to the Laptev Sea shelf edge. TerrOC was reduced by ~85% during transit resulting in a degradation rate constant of 2.4 ± 0.6 kyr
. Hence, terrOC degradation during cross-shelf transport constitutes a carbon source to the atmosphere over millennial time. For the contemporary carbon cycle on the other hand, slow terrOC degradation brings considerable attenuation of the decadal-centennial permafrost carbon-climate feedback caused by global warming.
Thick haze plagued northeastern China in January 2013, strongly affecting both regional climate and human respiratory health. Here, we present dual carbon isotope constrained (Δ14C and δ13C) source ...apportionment for combustion-derived black carbon aerosol (BC) for three key hotspot regions (megacities): North China Plain (NCP, Beijing), the Yangtze River Delta (YRD, Shanghai), and the Pearl River Delta (PRD, Guangzhou) for January 2013. BC, here quantified as elemental carbon (EC), is one of the most health-detrimental components of PM2.5 and a strong climate warming agent. The results show that these severe haze events were equally affected (∼30%) by biomass combustion in all three regions, whereas the sources of the dominant fossil fuel component was dramatically different between north and south. In the NCP region, coal combustion accounted for 66% (46–74%, 95% C.I.) of the EC, whereas, in the YRD and PRD regions, liquid fossil fuel combustion (e.g., traffic) stood for 46% (18–66%) and 58% (38–68%), respectively. Taken together, these findings suggest the need for a regionally-specific description of BC sources in climate models and regionally-tailored mitigation to combat severe air pollution events in East Asia.
Water‐soluble organic carbon (WSOC) is a major constituent (~ 20–80%) of the total organic carbon aerosol over the Indian subcontinent during the dry winter season. Due to its multiple primary and ...secondary formation pathways, the sources of WSOC are poorly characterized. In this study, we present radiocarbon constraints on the biomass versus fossil sources of WSOC in PM2.5 for the 2010/2011 winter period for the megacity Delhi, situated in the northern part of the heavily polluted Indo‐Gangetic Plain. The fossil fuel contribution to Delhi WSOC (21 ± 4%) is similar to that recently found at two South Asian background sites. In contrast, the stable carbon isotopic composition of Delhi WSOC is less enriched in 13C relative to that at the two receptor sites. Although potentially influenced also by source variability, this indicates that near‐source WSOC is less affected by atmospheric aging. In addition, the light absorptive properties of Delhi WSOC were studied. The mass absorption cross section at 365 nm (MAC365) was 1.1–2.7 m2/g with an Absorption Ångström Exponent ranging between 3.1 and 9.3. Using a simplistic model the relative absorptive forcing of the WSOC compared to elemental carbon in 2010/2011 wintertime Delhi was estimated to range between 3 and 11%. Taken together, this near‐source study shows that WSOC in urban Delhi comes mainly (79%) from biomass burning/biogenic sources. Furthermore, it is less influenced by photochemical aging compared to WSOC at South Asian regional receptor sites and contributes with a relatively small direct absorptive forcing effect.
Key Points
The fossil source contribution to PM2.5 WSOC in New Delhi is 21 ± 4%
WSOC is less enriched in 13C in near‐source aerosols compared to aged aerosols
Delhi PM2.5 WSOC extracts demonstrate small light absorptive properties
Emissions from biomass burning contribute significantly to water-soluble organic carbon (WSOC) and light-absorbing organic carbon (brown carbon). Ambient atmospheric samples were collected at an ...urban site in Beijing during winter and summer, along with source samples from residential crop straw burning. Carbonaceous aerosol species, including organic carbon (OC), elemental carbon (EC), WSOC and multiple saccharides as well as water-soluble potassium (K+) in PM2.5 (fine particulate matter with size less than 2.5 μm) were measured. Chemical signatures of atmospheric aerosols in Beijing during winter and summer days with significant biomass burning influence were identified. Meanwhile, light absorption by WSOC was measured and quantitatively compared to EC at ground level. The results from this study indicated that levoglucosan exhibited consistently high concentrations (209 ± 145 ng m−3) in winter. Ratios of levoglucosan/mannosan (L/M) and levoglucosan/galacosan (L/G) indicated that residential biofuel use is an important source of biomass burning aerosol in winter in Beijing. Light absorption coefficient per unit ambient WSOC mass calculated at 365 nm is approximately 1.54 ± 0.16 m2 g−1 in winter and 0.73 ± 0.15 m2 g−1 in summer. Biomass burning derived WSOC accounted for 23 ± 7% and 16 ± 7% of total WSOC mass, and contributed to 17 ± 4% and 19 ± 5% of total WSOC light absorption in winter and summer, respectively. It is noteworthy that, up to 30% of total WSOC light absorption was attributed to biomass burning in significant biomass-burning-impacted summer day. Near-surface light absorption (over the range 300–400 nm) by WSOC was about ∼40% of that by EC in winter and ∼25% in summer.
•High and relatively stable levoglucosan concentrations were found in Beijing in winter.•Light absorption from biomass burning to WSOC was evaluated in Beijing.•Light absorption (300–400 nm) by WSOC relative to EC was ∼40% (winter) and ∼25% (summer).•Residential biomass burning is non-negligible source to fine PM in Beijing winter.
The radiative absorption enhancement of ambient black carbon (BC), by light-refractive coatings of atmospheric aerosols, constitutes a large uncertainty in estimates of climate forcing. The direct ...measurements of radiative absorption enhancement require the experimentally-removing the coating materials in ambient BC-containing aerosols, which remains a challenge. Here, the absorption enhancement of the BC core by non-absorbing aerosol coatings was quantified using a two-step removal of both inorganic and organic matter coatings of ambient aerosols. The mass absorption cross-section (MAC) of decoated/pure atmospheric BC aerosols of 4.4±0.8m2g−1 was enhanced to 9.6±1.8m2g−1 at 678-nm wavelength for ambiently-coated BC aerosols at a rural Northern China site. The enhancement of MAC (EMAC) rises from 1.4±0.3 in fresh combustion emissions to ~3 for aged ambient China aerosols. The three-week high-intensity campaign observed an average EMAC of 2.25±0.55, and sulfates were primary drivers of the enhanced BC absorption.
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•A method was developed to remove coatings surrounding BC in ambient aerosols.•The MAC of decoated BC of 4.4 was enhanced to 9.6m2g−1 for ambient BC aerosols.•BC radiative forcing in the ambient atmosphere was enhanced by a factor of ~2.•BC absorption enhancement peaked in day time driven by secondary sulfate
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 (Δ
C/δ
C) 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.
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