scholarly journals Atmospheric tar balls: aged primary droplets from biomass burning?

2014 ◽  
Vol 14 (13) ◽  
pp. 6669-6675 ◽  
Author(s):  
A. Tóth ◽  
A. Hoffer ◽  
I. Nyirő-Kósa ◽  
M. Pósfai ◽  
A. Gelencsér

Abstract. Atmospheric tar balls are particles of special morphology and composition that are fairly abundant in the plumes of biomass smoke. These particles form a specific subset of brown carbon (BrC) which has been shown to play a significant role in atmospheric shortwave absorption and, by extension, climate forcing. Here we suggest that tar balls are produced by the direct emission of liquid tar droplets followed by heat transformation upon biomass burning. For the first time in atmospheric chemistry we generated tar-ball particles from liquid tar obtained previously by dry distillation of wood in an all-glass apparatus in the laboratory with the total exclusion of flame processes. The particles were perfectly spherical with a mean optical diameter of 300 nm, refractory, externally mixed, and homogeneous in the contrast of the transmission electron microscopy (TEM) images. They lacked any graphene-like microstructure and exhibited a mean carbon-to-oxygen ratio of 10. All of the observed characteristics of laboratory-generated particles were very similar to those reported for atmospheric tar-ball particles in the literature, strongly supporting our hypothesis regarding the formation mechanism of atmospheric tar-ball particles.

2013 ◽  
Vol 13 (12) ◽  
pp. 33089-33104 ◽  
Author(s):  
A. Tóth ◽  
A. Hoffer ◽  
I. Nyirő-Kósa ◽  
M. Pósfai ◽  
A. Gelencsér

Abstract. Atmospheric tar balls are particles of special morphology and composition that are abundant in the plumes of biomass smoke. These particles form a specific subset of brown carbon (BrC) which has been shown to play a significant role in atmospheric shortwave absorption and thus climate forcing. Formerly tar balls were hypothesized to be formed in secondary processes in the atmosphere from lignin pyrolysis products. Based on their typical size distributions, morphology, chemical characteristics and other features we now suggest that tar balls are initially produced by the emission of primary tar droplets upon biomass burning. To verify our hypothesis tar balls were produced under laboratory conditions with the total exclusion of flame processes. An all-glass apparatus was designed and tar ball particles were generated from liquid tar obtained previously by dry distillation of wood. The size range, morphology and the chemical composition of the laboratory-generated tar ball particles were similar to those observed in biomass smoke plumes or elsewhere in the atmosphere. Based on our results and the chemical and physical characteristics of tar we suggest that tar balls can be formed by the chemical transformation of emitted primary tar droplets.


2018 ◽  
Vol 115 (49) ◽  
pp. 12413-12418 ◽  
Author(s):  
Melinda R. Nicewonger ◽  
Murat Aydin ◽  
Michael J. Prather ◽  
Eric S. Saltzman

Biomass burning drives changes in greenhouse gases, climate-forcing aerosols, and global atmospheric chemistry. There is controversy about the magnitude and timing of changes in biomass burning emissions on millennial time scales from preindustrial to present and about the relative importance of climate change and human activities as the underlying cause. Biomass burning is one of two notable sources of ethane in the preindustrial atmosphere. Here, we present ice core ethane measurements from Antarctica and Greenland that contain information about changes in biomass burning emissions since 1000 CE (Common Era). The biomass burning emissions of ethane during the Medieval Period (1000–1500 CE) were higher than present day and declined sharply to a minimum during the cooler Little Ice Age (1600–1800 CE). Assuming that preindustrial atmospheric reactivity and transport were the same as in the modern atmosphere, we estimate that biomass burning emissions decreased by 30 to 45% from the Medieval Period to the Little Ice Age. The timing and magnitude of this decline in biomass burning emissions is consistent with that inferred from ice core methane stable carbon isotope ratios but inconsistent with histories based on sedimentary charcoal and ice core carbon monoxide measurements. This study demonstrates that biomass burning emissions have exceeded modern levels in the past and may be highly sensitive to changes in climate.


2021 ◽  
Author(s):  
Delia Segato ◽  
Maria Del Carmen Villoslada Hidalgo ◽  
Ross Edwards ◽  
Elena Barbaro ◽  
Paul Vallelonga ◽  
...  

Abstract. Biomass burning influences global atmospheric chemistry by releasing greenhouse gases and climate-forcing aerosols. There is controversy about the magnitude and timing of Holocene changes in biomass burning emissions from millennial to centennial time scales and, in particular, on the possible impact of ancient civilizations. Here we present a 5 kyr record of fire activity proxies levoglucosan, black carbon and ammonium measured in the RECAP ice core, drilled in the coastal East Greenland and therefore affected by processes occurring in the High North Atlantic Region. Levoglucosan and ammonium fluxes show high levels from 5 to 4.5 kyr followed by an abrupt decline, possibly due to monotonic decline in Northern Hemisphere summer insolation. Levoglucosan and black carbon show an abrupt decline at 1.1 kyr BP (before 2000 AD), suggesting a decline in wildfire regime in the Icelandic territory due to the extensive land clearing caused by Viking colonizers. A minimum is reached at 0.5 kyr BP for all fire proxies, after which levoglucosan and ammonium fluxes increase again, in particular over the last 200 years. We find that the fire regime reconstructed from RECAP fluxes seems mainly related to climatic changes, however over the last millennium human activities might have had a substantial influence controlling the occurrence of fire.


2021 ◽  
Author(s):  
Antonio G. Bruno ◽  
Jeremy J. Harrison ◽  
David P. Moore ◽  
Martyn P. Chipperfield ◽  
Richard J. Pope

<p>Hydrogen cyanide (HCN) is one of the most abundant cyanides present in the global atmosphere, and is a tracer of biomass burning, especially for peatland fires. The HCN lifetime is 2–5 months in the troposphere but several years in the stratosphere. Understanding the physical and chemical mechanisms of HCN variability is important due to its non-negligible role in the nitrogen cycle. The main source of tropospheric HCN is biomass burning with minor contributions from industry and transport. The main loss mechanism of atmospheric HCN is the reaction with the hydroxyl radical (OH). Ocean uptake is also important, while in the stratosphere oxidation by reaction with O(<sup>1</sup>D) needs to be considered.</p><p>HCN variability can be investigated using chemical model simulations, such as three-dimensional (3-D) chemical transport models (CTMs). Here we use an adapted version of the TOMCAT 3-D CTM at a 1.2°x1.2° spatial resolution from the surface to ~60 km for 12 idealised HCN tracers which quantify the main loss mechanisms of HCN, including ocean uptake, atmospheric oxidation reactions and their combinations. The TOMCAT output of the HCN distribution in the period 2004-2020 has been compared with HCN profiles measured by the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) over an altitude grid from 6 to 42 km. HCN model data have also been compared with ground-based measurements of HCN columns from NDACC FTIR stations and with in-situ volume mixing ratios (VMRs) from NOAA ground-based measurement sites.</p><p>The model outputs for the HCN tracer with full treatment of the loss processes generally agree well with ACE-FTS measurements, as long as we use recent laboratory values for the atmospheric loss reactions. Diagnosis of the individual loss terms shows that decay of the HCN profile in the upper stratosphere is due mainly to the O(<sup>1</sup>D) sink. In order to test the magnitude of the tropospheric OH sink and the magnitude of the ocean sink, we also show the comparisons of the model tracers with surface-based observations. The implications of our results for understanding HCN and its variability are then discussed.</p>


2010 ◽  
Vol 10 (5) ◽  
pp. 2335-2351 ◽  
Author(s):  
D. Chang ◽  
Y. Song

Abstract. Biomass burning in tropical Asia emits large amounts of trace gases and particulate matter into the atmosphere, which has significant implications for atmospheric chemistry and climatic change. In this study, emissions from open biomass burning over tropical Asia were evaluated during seven fire years from 2000 to 2006 (1 March 2000–31 February 2007). The size of the burned areas was estimated from newly published 1-km L3JRC and 500-m MODIS burned area products (MCD45A1). Available fuel loads and emission factors were assigned to each vegetation type in a GlobCover characterisation map, and fuel moisture content was taken into account when calculating combustion factors. Over the whole period, both burned areas and fire emissions showed clear spatial and seasonal variations. The size of the L3JRC burned areas ranged from 36 031 km2 in fire year 2005 to 52 303 km2 in 2001, and the MCD45A1 burned areas ranged from 54 790 km2 in fire year 2001 to 148 967 km2 in 2004. Comparisons of L3JRC and MCD45A1 burned areas using ground-based measurements and other satellite data were made in several major burning regions, and the results suggest that MCD45A1 generally performed better than L3JRC, although with a certain degree of underestimation in forest areas. The average annual L3JRC-based emissions were 123 (102–152), 12 (9–15), 1.0 (0.7–1.3), 1.9 (1.4–2.6), 0.11 (0.09–0.12), 0.89 (0.63–1.21), 0.043 (0.036–0.053), 0.021 (0.021–0.023), 0.41 (0.34–0.52), 3.4 (2.6–4.3), and 3.6 (2.8–4.7) Tg yr−1 for CO2, CO, CH4, NMHCs, NOx, NH3, SO2, BC, OC, PM2.5, and PM10, respectively, whereas MCD45A1-based emissions were 122 (108–144), 9.3 (7.7–11.7), 0.63 (0.46–0.86), 1.1 (0.8–1.6), 0.11 (0.10–0.13), 0.54 (0.38–0.76), 0.043 (0.038–0.051), 0.033 (0.032–0.037), 0.39 (0.34–0.47), 3.0 (2.6–3.7), and 3.3 (2.8–4.0) Tg yr−1. Forest burning was identified as the major source of the fire emissions due to its high carbon density. Although agricultural burning was the second highest contributor, it is possible that some crop residue combustion was missed by satellite observations. This possibility is supported by comparisons with previously published data, and this result may be due to the small size of the field crop residue burning. Fire emissions were mainly concentrated in Indonesia, India, Myanmar, and Cambodia. Furthermore, the peak in the size of the burned area was generally found in the early fire season, whereas the maximum fire emissions often occurred in the late fire season.


2018 ◽  
Author(s):  
Lei Liu ◽  
Jian Zhang ◽  
Liang Xu ◽  
Qi Yuan ◽  
Dao Huang ◽  
...  

Abstract. Aerosol-cloud interaction remains a major source of uncertainty in climate forcing estimate. Our knowledge about the aerosol-cloud interaction is particularly weak in heavily polluted conditions. In this study, cloud residual (cloud RES) and cloud interstitial (cloud INT) particles were collected during cloud events under different pollution levels from 22 July to 1 August, 2014 at Mt. Tai (1532 m above sea level) located in the North China Plain (NCP). Transmission electron microscopy (TEM) was used to investigate size, composition, and mixing state of individual cloud RES and INT particles. Our results show that S-rich particles were predominant (78 %) during clean periods (PM2.5 


2007 ◽  
Vol 7 (4) ◽  
pp. 12657-12686 ◽  
Author(s):  
K. Hungershöfer ◽  
K. Zeromskiene ◽  
Y. Iinuma ◽  
G. Helas ◽  
J. Trentmann ◽  
...  

Abstract. A better characterisation of the optical properties of biomass burning aerosol as a function of the burning conditions is required in order to quantify their effects on climate and atmospheric chemistry. Controlled laboratory combustion experiments with different fuel types were carried out at the combustion facility of the Max Planck Institute for Chemistry (Mainz, Germany) as part of the 'Impact of Vegetation Fires on the Composition and Circulation of the Atmosphere' (EFEU) project. Using the measured size distributions as well as mass scattering and absorption efficiencies, Mie calculations provided mean effective refractive indices of 1.60−0.010i and 1.56−0.010i (λ=0.55 μm) for smoke particles emitted from the combustion of savanna grass and an African hardwood (musasa), respectively. The relatively low imaginary parts suggest that the light-absorbing carbon of the investigated fresh biomass burning aerosol is only partly graphitized, resulting in strongly scattering and less absorbing particles. While the observed variability in mass scattering efficiencies was consistent with changes in particle size, the changes in the mass absorption efficiency can only be explained, if the chemical composition of the particles varies with combustion conditions.


2020 ◽  
Author(s):  
Margaret Marvin ◽  
Paul Palmer ◽  
Fei Yao ◽  
Barry Latter ◽  
Richard Siddans ◽  
...  

<p>Mainland and maritime Southeast Asia is home to more than 655 million people, representing nearly 10% of the global population. The dry season in this region is typically associated with intense biomass burning activity, which leads to a significant increase in surface air pollutants that are harmful to human health, including ozone (O<sub>3</sub>) and fine (radii smaller than 2.5 microns) particulate matter (PM<sub>2.5</sub>). Latitude-based differences in dry season timing and land use distinguish two regional biomass burning regimes: (1) agricultural waste burning on the peninsular mainland from February through April and (2) coastal peat burning across the equatorial islands in September and October. The type and amount of material burned determines the chemical composition of emissions and subsequently their impact on regional air quality. Understanding the individual and collective roles of these biomass burning regimes is a crucial step towards developing effective air quality mitigation strategies for Southeast Asia. Here, we use the nested GEOS-Chem atmospheric chemistry transport model (horizontal resolution of 0.25° x 0.3125°) to simulate fire-atmosphere interactions over Southeast Asia during March and September of 2014, when emissions peak from the two regional burning seasons. Based on our analysis of model output, we report how these two distinct biomass burning regimes impact the photochemical environment over Southeast Asia and what the resulting consequences are for surface air quality. We will also present a critical evaluation of our model using ground-based and satellite observations of atmospheric composition across the region.</p>


2004 ◽  
Vol 4 (3) ◽  
pp. 2569-2613
Author(s):  
N. H. Savage ◽  
K. S. Law ◽  
J. A. Pyle ◽  
A. Richter ◽  
H. Nüß ◽  
...  

Abstract. This paper compares column measurements of NO2 made by the GOME instrument on ERS-2 to model results from the TOMCAT global CTM. The overall correlation between the model and observations is good (0.79 for the whole world, and 0.89 for north America) but the modelled columns are too large over polluted areas (gradient of 1.4 for North America and 1.9 for Europe). NO2 columns in the region of outflow from North America into the Atlantic seem too high in winter in the model compared to the GOME results, whereas the modelled columns are too small off the coast of Africa where there appear to be biomass burning plumes in the satellite data. Several hypotheses are presented to explain these discrepancies. Weaknesses in the model treatment of vertical mixing and chemistry appear to be the most likely explanations. It is shown that GOME and other satellite data will be of great value in furthering our understanding of atmospheric chemistry and in targeting and testing future model development and case studies.


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