Fossil and non-fossil source contributions to atmospheric carbonaceous aerosols during extreme spring grassland fires in Eastern Europe

In early spring the Baltic region is frequently affected by high-pollution events due to biomass burning in that area. Here we present a comprehensive study to investigate the impact of biomass/grass burning (BB) on the evolution and composition of aerosol in Preila, Lithuania, during springtime open fires. Non-refractory submicron particulate matter (NR-PM1) was measured by an Aerodyne aerosol chemical speciation monitor (ACSM) and a source apportionment with the multilinear engine (ME-2) running the positive matrix factorization (PMF) model was applied to the organic aerosol fraction to investigate the impact of biomass/grass burning. Satellite observations over regions of biomass burning activity supported the results and identification of air mass transport to the area of investigation. Sharp increases in biomass burning tracers, such as levoglucosan up to 683 ngm-3 and black carbon (BC) up to 17 μgm-3 were observed during this period. A further separation between fossil and non-fossil primary and secondary contributions was obtained by coupling ACSM PMF results and radiocarbon (14C) measurements of the elemental (EC) and organic (OC) carbon fractions. Non-fossil organic carbon (OCnf/ was the dominant fraction of PM1, with the primary (POCnf/ and secondary (SOCnf/ fractions contributing 26–44% and 13–23% to the total carbon (TC), respectively. 5–8% of the TC had a primary fossil origin (POCf/, whereas the contribution of fossil secondary organic carbon (SOCf/ was 4–13 %. Nonfossil EC (ECnf/ and fossil EC (ECf/ ranged from 13–24 and 7–13 %, respectively. Isotope ratios of stable carbon and nitrogen isotopes were used to distinguish aerosol particles associated with solid and liquid fossil fuel burning.

Fossil and Nonfossil Sources of Organic and Elemental Carbon Aerosols in the Outflow from Northeast China

Source quantification of carbonaceous aerosols in the Chinese outflow regions still remains uncertain despite their high mass concentrations. Here, we unambiguously quantified fossil and nonfossil contributions to elemental carbon (EC) and organic carbon (OC) of total suspended particles (TSP) from a regional receptor site in the outflow of Northeast China using radiocarbon measurement. OC and EC concentrations were lower in summer, representing mainly marine air, than in other seasons, when air masses mostly traveled over continental regions in Mongolia and northeast China. The annual-mean contribution from fossil-fuel combustion to EC was 76 ± 11% (0.1−1.3 μg m−3). The remaining 24 ± 11% (0.03−0.42 μg m−3) was attributed to biomass burning, with slightly higher contribution in the cold period (∼31%) compared to the warm period (∼21%) because of enhanced emissions from regional biomass combustion sources in China. OC was generally dominated by nonfossil sources, with an annual average of 66 ± 11% (0.5−2.8 μg m−3), approximately half of which was apportioned to primary biomass burning sources (34 ± 6%). In winter, OC almost equally originated from primary OC (POC) emissions and secondary OC (SOC) formation from fossil fuel and biomass-burning sources. In contrast, summertime OC was dominated by primary biogenic emissions as well as secondary production from biogenic and biomass-burning sources, but fossil-derived SOC was the smallest contributor. Distinction of POC and SOC was performed using primary POC-to-EC emission ratios separated for fossil and nonfossil emissions.

Fossil versus contemporary sources of fine elemental and organic carbonaceous particulate matter during the DAURE campaign in Northeast Spain

We present results from the international field campaign DAURE (Detn. of the sources of atm. Aerosols in Urban and Rural Environments in the Western Mediterranean), with the objective of apportioning the sources of fine carbonaceous aerosols. Submicron fine particulate matter (PM1) samples were collected during Feb.-March 2009 and July 2009 at an urban background site in Barcelona (BCN) and at a forested regional background site in Montseny (MSY). We present radiocarbon (14C) anal. for elemental and org. carbon (EC and OC) and source apportionment for these data. We combine the results with those from component anal. of aerosol mass spectrometer (AMS) measurements, and compare to levoglucosan-based ests. of biomass burning OC, source apportionment of filter data with inorg. compn. + EC + OC, submicron bulk potassium (K) concns., and gaseous acetonitrile concns. At BCN, 87 % and 91 % of the EC on av., in winter and summer, resp., had a fossil origin, whereas at MSY these fractions were 66 % and 79 %. The contribution of fossil sources to org. carbon (OC) at BCN was 40 % and 48 %, in winter and summer, resp., and 31 % and 25 % at MSY. The combination of results obtained using the 14C technique, AMS data, and the correlations between fossil OC and fossil EC imply that the fossil OC at Barcelona is ∼47 % primary whereas at MSY the fossil OC is mainly secondary (∼85 %). Day-to-day variation in total carbonaceous aerosol loading and the relative contributions of different sources predominantly depended on the meteorol. transport conditions. The estd. biogenic secondary OC at MSY only increased by ∼40 % compared to the order-of-magnitude increase obsd. for biogenic volatile org. compds. (VOCs) between winter and summer, which highlights the uncertainties in the estn. of that component. Biomass burning contributions estd. using the 14C technique ranged from similar to slightly higher than when estd. using other techniques, and the different estns. were highly or moderately correlated. Differences can be explained by the contribution of secondary org. matter (not included in the primary biomass burning source ests.), and/or by an over-estn. of the biomass burning OC contribution by the 14C technique if the estd. biomass burning EC/OC ratio used for the calcns. is too high for this region. Acetonitrile concns. correlate well with the biomass burning EC detd. by 14C. K is a noisy tracer for biomass burning. [on SciFinder(R)]

Sources and contributions of wood smoke during winter in London: assessing local and regional influences

Determining the contribution of wood smoke to air pollution in large cities such as London is becoming increasingly important due to the changing nature of domestic heating in urban areas. During winter, biomass burning emissions have been identified as a major cause of exceedances of European air quality limits. The aim of this work was to quantify the contribution of biomass burning in London to concentrations of PM2:5 and determine whether local emissions or regional contributions were the main source of biomass smoke. To achieve this, a number of biomass burning chemical tracers were analysed at a site within central London and two sites in surrounding rural areas. Concentrations of levoglucosan, elemental carbon (EC), organic carbon (OC) and K+ were generally well correlated across the three sites. At all the sites, biomass burning was found to be a source of OC and EC, with the largest contribution of EC from traffic emissions, while for OC the dominant fraction included contributions from secondary organic aerosols, primary biogenic and cooking sources. Source apportionment of the EC and OC was found to give reasonable estimation of the total carbon from non-fossil and fossil fuel sources based upon comparison with estimates derived from 14C analysis. Aethalometer-derived black carbon data were also apportioned into the contributions frombiomass burning and traffic and showed trends similar to those observed for EC. Mean wood smoke mass at the sites was estimated to range from 0.78 to 1.0 μgm-3 during the campaign in January–February 2012. Measurements on a 160m tower in London suggested a similar ratio of brown to black carbon (reflecting wood burning and traffic respectively) in regional and London air. Peaks in the levoglucosan and K+ concentrations were observed to coincide with low ambient temperature, consistent with domestic heating as a major contributing local source in London. Overall, the source of biomass smoke in London was concluded to be a background regional source overlaid by contributions from local domestic burning emissions. This could have implications when considering future emission control strategies during winter and may be the focus of future work in order to better determine the contributing local sources.

An ice-core based history of Siberian forest fires since AD 1250

Forest fires play a key role in the global carbon cycle and thus, can affect regional and global climate. Although fires in extended areas of Russian boreal forests have a considerable influence on atmospheric greenhouse gas and soot concentrations, estimates of their impact on climate are hampered by a lack of data on the history of forest fires. Especially regions with strong continental climate are of high importance due to an intensified development of wildfires. In this study we reconstruct the fire history of Southern Siberia during the past 750 years using ice-core based nitrate, potassium, and charcoal concentration records from Belukha glacier in the continental Siberian Altai. A period of exceptionally high forest-fire activity was observed between AD 1600 and 1680, following an extremely dry period AD 1540-1600. Ice-core pollen data suggest distinct forest diebacks and the expansion of steppe in response to dry climatic conditions. Coherence with a paleoenvironmental record from the 200 km distant Siberian lake Teletskoye shows that the vegetational shift AD 1540-1680, the increase in fire activity AD 1600-1680, and the subsequent recovery of forests AD 1700 were of regional significance. Dead biomass accumulation in response to drought and high temperatures around AD 1600 probably triggered maximum forest-fire activity AD 1600-1680. The extreme dry period in the 16th century was also observed at other sites in Central Asia and is possibly associated with a persistent positive mode of the Pacific Decadal Oscillation (PDO). No significant increase in biomass burning occurred in the Altai region during the last 300 years, despite strongly increasing temperatures and human activities. Our results imply that precipitation changes controlled fire-regime and vegetation shifts in the Altai region during the past 750 years. We conclude that high sensitivity of ecosystems to occasional decadal-scale drought events may trigger unprecedented environmental reorganizations under global-warming conditions.

The Carrington event not observed in most ice core nitrate records

The Carrington Event of 1859 is considered to be among the largest space weather events of the last 150 years. We show that only one out of 14 well-resolved ice core records from Greenland and Antarctica has a nitrate spike dated to 1859. No sharp spikes are observed in the Antarctic cores studied here. In Greenland numerous spikes are observed in the 40 years surrounding 1859, but where other chemistry was measured, all large spikes have the unequivocal signal, including co-located spikes in ammonium, formate, black carbon and vanillic acid, of biomass burning plumes. It seems certain that most spikes in an earlier core, including that claimed for 1859, are also due to biomass burning plumes, and not to solar energetic particle (SEP) events. We conclude that an event as large as the Carrington Event did not leave an observable, widespread imprint in nitrate in polar ice. Nitrate spikes cannot be used to derive the statistics of SEPs.

Current and future variations of nutrient depositions and influences on tree growth

Current nutrient deposition shows episodic variations which likely may impact the local nutrient cycle at the RBSF. Comparing analyses of deposition data during present-day atmospheric circulation and phases of high biomass burning in the Amazon, characteristic relationships between remote emissions and local deposition are determined. By using projections drawn from the special report on emission scenarios (SRES) in combination with a trajectory modeling tool, future nutrient deposition conditions of the mountain ecosystem are assessed. Observations of relations between climatic variables, current time series of nutrient deposition, and tree growth point to an impact of the remote fertilization effect of atmospheric matters, emitted primarily by human activities like biomass burning and agricultural and industrial sources. The increasing emissions in the future may have adverse effects on the ecosystem in the long run.

Fossil and Non-Fossil Sources of Different Carbonaceous Fractions in Fine and Coarse Particles by Radiocarbon Measurement

Radiocarbon offers a unique possibility for unambiguous source apportionment of carbonaceous particles due to a direct distinction of non-fossil and fossil carbon. In this work, particulate matter of different size fractions was collected at 4 sites in Switzerland to examine whether fine and coarse carbonaceous particles exhibit different fossil and contemporary sources. Elemental carbon (EC) and organic carbon (OC) as well as water-soluble OC (WSOC) and water-insoluble OC (WINSOC) were separated and determined for subsequent 14C measurement. In general, both fossil and non-fossil fractions in OC and EC were found more abundant in the fine than in the coarse mode. However, a substantial fraction (~20 ± 5%) of fossil EC was found in coarse particles, which could be attributed to traffic-induced non-exhaust emissions. The contribution of biomass burning to coarse-mode EC in winter was relatively high, which is likely associated to the coating of EC with organic and/or inorganic substances emitted from intensive wood burning. Further, fossil OC (i.e. from vehicle emissions) was found to be smaller than non-fossil OC due to the presence of primary biogenic OC and/or growing in size of wood-burning OC particles during aging processes. 14C content in WSOC indicated that the second organic carbon rather stems from non-fossil precursors for all samples. Interestingly, both fossil and non-fossil WINSOC concentrations were found to be higher in fine particles than in coarse particles in winter, which is likely due to primary wood burning emissions and/or secondary formation of WINSOC.

Long-term perspective on wildfires in the western USA

Understanding the causes and consequences of wildfires in forests of the western United States requires integrated information about fire, climate changes, and human activity on multiple temporal scales. We use sedimentary charcoal accumulation rates to construct long-term variations in fire during the past 3,000 y in the American West and compare this record to independent fire-history data from historical records and fire scars. There has been a slight decline in burning over the past 3,000 y, with the lowest levels attained during the 20th century and during the Little Ice Age (LIA, ca. 1400-1700 CE Common Era]). Prominent peaks in forest fires occurred during the Medieval Climate Anomaly (ca. 950-1250 CE) and during the 1800s. Analysis of climate reconstructions beginning from 500 CE and population data show that temperature and drought predict changes in biomass burning up to the late 1800s CE. Since the late 1800s, human activities and the ecological effects of recent high fire activity caused a large, abrupt decline in burning similar to the LIA fire decline. Consequently, there is now a forest ``fire deficit'' in the western United States attributable to the combined effects of human activities, ecological, and climate changes. Large fires in the late 20th and 21st century fires have begun to address the fire deficit, but it is continuing to grow.

High secondary aerosol contribution to particulate pollution during haze events in China

Rapid industrialization and urbanization in developing countries has led to an increase in air pollution, along a similar trajectory to that previously experienced by the developed nations. In China, particulate pollution is a serious environmental problem that is influencing air quality, regional and global climates, and human health. In response to the extremely severe and persistent haze pollution experienced by about 800 million people during the first quarter of 2013 (refs 4, 5), the Chinese State Council announced its aim to reduce concentrations of PM2.5 (particulate matter with an aerodynamic diameter less than 2.5micrometres) by up to 25 per cent relative to 2012 levels by 2017 (ref. 6). Such efforts however require elucidation of the factors governing the abundance and composition of PM2.5, which remain poorly constrained in China. Here we combine a comprehensive set of novel and state-of-the-art offline analytical approaches and statistical techniques to investigate the chemical nature and sources of particulate matter at urban locations in Beijing, Shanghai, Guangzhou and Xi'an during January 2013. We find that the severe haze pollution event was driven to a large extent by secondary aerosol formation, which contributed 30-77 per cent and 44-71 per cent (average for all four cities) of PM2.5 and of organic aerosol, respectively. On average, the contribution of secondary organic aerosol (SOA) and secondary inorganic aerosol (SIA) are found to be of similar importance (SOA/SIA ratios range from 0.6 to 1.4). Our results suggest that, in addition to mitigating primary particulate emissions, reducing the emissions of secondary aerosol precursors from, for example, fossil fuel combustion and biomass burning is likely to be important for controlling China's PM2.5 levels and for reducing the environmental, economic and health impacts resulting from particulate pollution.

Combining charcoal sediment and molecular markers to infer a Holocene fire history in the Maya Lowlands of Petén, Guatemala

Vegetation changes in the Maya Lowlands during the Holocene are a result of changing climate conditions, solely anthropogenic activities, or interactions of both factors. As a consequence, it is difficult to assess how tropical ecosystems will cope with projected changes in precipitation and land-use intensification over the next decades. We investigated the role offire during the Holocene by combining macroscopic charcoal and the molecular fire proxies levoglucosan, mannosan and galactosan. Combining these two different fire proxies allows a more robust understanding of the complex history of fire re- gimes at different spatial scales during the Holocene. In order to infer changes in past biomass burning, we analysed a lake sediment core from Lake Peten Itza, Guatemala, and compared our results with millennial-scale vegetation and climate change available in the area. We detected three periods of high fire activity during the Holocene: 9500 e 6000 cal yr BP, 3700 cal yr BP and 2700 cal yr BP. We attribute the first maximum mostly to climate conditions and the last maximum to human activities. The rapid change between burned vegetation types at the 3700 cal yr BP fire maximum may result from human activity.

Millennial changes in North American wildfire and soil activity over the last glacial cycle

Climate changes in the North Atlantic region during the last glacial cycle were dominated by the slow waxing and waning of the North American ice sheet as well as by intermittent, millennial-scale Dansgaard–Oeschger climate oscillations. However, prior to the last deglaciation, the responses of North American vegetation and biomass burning to these climate variations are uncertain. Ammonium in Greenland ice cores, a product from North American soil emissions and biomass burning events, can help to fill this gap. Here we use continuous, high-resolution measurements of ammonium concentrations between 110,000 to 10,000 years ago from the Greenland NGRIP and GRIP ice cores to reconstruct North American wildfire activity and soil ammonium emissions. We find that on orbital timescales soil emissions increased under warmer climate conditions when vegetation expanded northwards into previously ice-covered areas. For millennial-scale interstadial warm periods during Marine Isotope Stage 3, the fire recurrence rate increased in parallel to the rapid warmings, whereas soil emissions rose more slowly, reflecting slow ice shrinkage and delayed ecosystem changes. We conclude that sudden warming events had little impact on soil ammonium emissions and ammonium transport to Greenland, but did result in a substantial increase in the frequency of North American wildfires.

Wet deposition of fossil and non-fossil derived particulate carbon: insights from radiocarbon measurement

Radiocarbon (14C) measurements of both organic carbon (OC) and elemental carbon (EC) allow a more detailed source apportionment, leading to a full and unambiguous distinction and quantification of the contributions from non-fossil and fossil sources. A thermal-optical method with a commercial OC/EC analyzer to isolate water-insoluble OC (WIOC) and EC for their subsequent 14C measurement was applied for the first time to filtered precipitation samples collected at a costal site in Portugal and at a continental site in Switzerland. Our results show that WIOC in precipitation is dominated by non-fossil sources such as biogenic and biomass-burning emissions regardless of rain origins and seasons, whereas EC sources are shared by fossil-fuel combustion and biomass burning. In addition, monthly variation of WIOC in Switzerland was characterized by higher abundance in warm than in cold seasons, highlighting the importance of biogenic emissions to particulate carbon in rainwater. Samples with high particulate carbon concentrations in Portugal were found to be associated with increased biogenic input. Despite the importance of non-fossil sources, fossil emissions account for approximately 20% of particulate carbon in wet deposition for our study, which is in line with fossil contribution in bulk rainwater dissolved organic carbon as well as aerosol WIOC and EC estimated by the 14C approach from other studies.

Source apportionment of elemental carbon in Beijing, China: insights from radiocarbon and organic marker measurements

Elemental carbon (EC) or black carbon (BC) in the atmosphere has a strong influence on both climate and human health. In this study, radiocarbon (14C) based source apportionment is used to distinguish between fossil fuel and biomass burning sources of EC isolated from aerosol filter samples collected in Beijing from June 2010 to May 2011. The 14C results demonstrate that EC is consistently dominated by fossil-fuel combustion throughout the whole year with a mean contribution of 79% ± 6% (ranging from 70% to 91%), though EC has a higher mean and peak concentrations in the cold season. The seasonal molecular pattern of hopanes (i.e., a class of organic markers mainly emitted during the combustion of different fossil fuels) indicates that traffic-related emissions are the most important fossil source in the warm period and coal combustion emissions are significantly increased in the cold season. By combining 14C based source apportionment results and picene (i.e., an organic marker for coal emissions) concentrations, relative contributions from coal (mainly from residential bituminous coal) and vehicle to EC in the cold period were estimated as 25 ± 4% and 50 ± 7%, respectively, whereas the coal combustion contribution was negligible or very small in the warm period.

The Interaction Between Forest Fires and Human Activity in Southern Switzerland

The impact of human activities on the fire regime in southern Switzerland was studied using (pre)historical charcoal and pollen data from lake sediments and statistical data from the 20th century. The cultural impact on forest fire was established by correlating charcoal-influx data with pollen percentages of anthropogenic indicators such as Plantago lanceolata, the Cerealia (sum of Avena t., Triticum t. and Hordeum t.) and Secale. During the 20th century, fire frequency was correlated with precipitation, dry and very dry periods and landscape management indicators. The effects of human activity on the fire regime are clearly recognisable since at least the Neolithic period. Using palaeoecological or statistical data, the variations in fire regime originating from anthropogenic actions may be differentiated from those due to climatic changes if they are sufficiently conspicuous.