Photochemically produced ozone in the emission from large‐scale tropical vegetation fires

Delany, A. C.; Haagensen, P.; Walters, Stacy; Wartburg, A. F.; Crutzen, Paul J.

doi:10.1029/jd090id01p02425

Cited by 126 publications

(53 citation statements)

References 15 publications

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“…According to Piazena (1996), UV-A irradiation at 10 km height can be 70-150 % higher than at ground level depending on solar elevation. Coupled with the high levels of O 3 found in aged BB plumes (Delany et al, 1985;Andreae et al, 1988;Crutzen and Andreae, 1990;Ziemke et al, 2009; Konovalov et al, 2011;Dupont et al, 2012;Martins et al, 2012;Akagi et al, 2013), uptake of O 3 by BBA compounds can be significant. For example, using a solar elevation angle of ∼ 70 • C, which roughly corresponds to a summer afternoon in the midwestern US, UV-A irradiation at 10 km height is 9.52 × 10 15 photons cm −2 s −1 .…”

Section: Atmospheric Implicationsmentioning

confidence: 99%

“…In the atmosphere, however, BBA particles are exposed to gas phase oxidants such as O 3 , resulting in multiphase chemical reactions, which can cause chemical and physical modification of the particles, a process known as chemical ageing (Hennigan et al, 2010;Kessler et al, 2010;Hennigan et al, 2011;Knopf et al, 2006Knopf et al, , 2011Shiraiwa et al, 2012). It has been shown that O 3 can be photochemically created in BB plumes, with reported concentration levels as high as 100 ppb (Delany et al, 1985;Andreae et al, 1988;Crutzen and Andreae, 1990;Ziemke et al, 2009;Konovalov et al, 2011;Dupont et al, 2012;Martins et al, 2012;Akagi et al, 2013). Therefore, heterogeneous oxidation reactions inside a BB plume can cause chemical modification of particles and biomolecular marker species, potentially having subsequent effects on source apportionment (Robinson et al, 2006b;Lin et al, 2010).…”

Section: Introductionmentioning

confidence: 99%

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Photosensitised heterogeneous oxidation kinetics of biomass burning aerosol surrogates by ozone using an irradiated rectangular channel flow reactor

Forrester

Knopf

2013

Atmos. Chem. Phys.

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Abstract. Heterogeneous reaction kinetics involving organic aerosol and atmospheric oxidants such as ozone can be enhanced under visible or UV irradiation in the presence of a photosensitiser, with subsequent implications for the climate, cloud radiative properties, air quality, and source appointment. In this study we report the steady-state reactive uptake coefficient, γ, of O3 by levoglucosan and 5-nitroguaiacol acting as surrogates for biomass burning aerosol particles, with and without the presence of Pahokee peat acting as a photosensitiser. The reactive uptake has been determined in the dark and as a function of visible and UV-A irradiation and ozone concentration. In addition, γ was determined for 1 : 1, 1 : 10, and 1 : 100 by mass mixtures of Pahokee peat and 5-nitroguaiacol, and for a 10 : 1 : 3 mixture of levoglucosan, Pahokee peat, and 5-nitroguaiacol. We developed a novel irradiated rectangular channel flow reactor (I-RCFR) that was operated under low pressures of about 2–4 hPa, and allowed for uniform irradiation of the organic substrates. The I-RCFR was coupled to a chemical ionisation mass spectrometer and has been successfully validated by measuring the kinetics between various organic species and oxidants. γ of O3 and levoglucosan in the dark and under visible and UV-A irradiation was determined to be in the range of (2–11) × 10−6 and did not change in the presence of Pahokee peat. The determined γ of O3 and 5-nitroguaiacol in the dark was 5.7 × 10−6 and was only enhanced under UV-A irradiation, yielding a value of 3.6 × 10−5. γ of the 1 : 1 Pahokee peat/5-nitroguaiacol substrate was enhanced under visible and UV-A irradiation to 2.4 × 10−5 and 2.8 × 10−5, respectively. Decreasing the amount of Pahokee peat in the 5-nitroguaiacol/Pahokee peat substrate resulted in lower values of γ under visible irradiation, however, γ was consistent under UV-A irradiation regardless of the amount of Pahokee peat. The 10 : 1 : 3 mixture by mass of levoglucosan, Pahokee peat, and 5-nitroguaiacol, under both visible and UV-A irradiation yielded γ values of 2.8 × 10−5 and 1.4 × 10−5, respectively. γ was determined as a function of photon flux for O3 with the 1 : 1 Pahokee peat/5-nitroguaiacol substrate, yielding a linear relationship under both visible and UV-A irradiation. γ of O3 with the 1 : 1 Pahokee peat/5-nitroguaiacol substrate was determined as a function of ozone concentration and exhibited an inverse dependence of γ on ozone concentration, commonly interpreted as a Langmuir–Hinshelwood mechanism. The reactive uptake data have been represented by a Langmuir-type isotherm. From the O3 uptake data under visible irradiation, the following fit parameters have been derived: ks = (5.5 ± 2.7) × 10−19 cm2 s−1 molecule−1 and KO3 = (2.3 ± 2.0) × 10−12 cm3 molecule−1; and under UV-A irradiation: ks = (8.1 ± 2.0) × 10−19 cm2 s−1 molecule−1 and KO3 = (1.7 ± 0.7) × 10−12 cm3 molecule−1. The oxidative power, or the product of γ and [O3], was determined for O3 with the 1 : 1 Pahokee peat/5-nitroguaiacol substrate and was in the range of (1.2–26) × 106 molecule cm−3. Atmospheric particle lifetimes were estimated for a 0.4 μm 5-nitroguaiacol particle as a function of visible and UV-A irradiation and ozone concentration.

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Section: Atmospheric Implicationsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Photosensitised heterogeneous oxidation kinetics of biomass burning aerosol surrogates by ozone using an irradiated rectangular channel flow reactor

Forrester

Knopf

2013

Atmos. Chem. Phys.

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“…In contrast, areas with the highest convective cloud activity showed the highest production of these species. As it is typical for high ozone concentrations to form in evolving smoke plumes (Delany et al, 1985;Hobbs et al, 1996), there can be adequate oxidation potential in the environment for secondary processes to occur.…”

Section: Particle Evolution Processesmentioning

confidence: 99%

A review of biomass burning emissions part II: intensive physical properties of biomass burning particles

Reid¹,

et al. 2005

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Abstract. The last decade has seen tremendous advances in atmospheric aerosol particle research that is often performed in the context of climate and global change science. Biomass burning, one of the largest sources of accumulation mode particles globally, has been closely studied for its radiative, geochemical, and dynamic impacts. These studies have taken many forms including laboratory burns, in situ experiments, remote sensing, and modeling. While the differing perspectives of these studies have ultimately improved our qualitative understanding of biomass-burning issues, the varied nature of the work make inter-comparisons and resolutions of some specific issues difficult. In short, the literature base has become a milieu of small pieces of the biomass-burning puzzle. This manuscript, the second part of four, examines the properties of biomass-burning particle emissions. Here we review and discuss the literature concerning the measurement of smoke particle size, chemistry, thermodynamic properties, and emission factors. Where appropriate, critiques of measurement techniques are presented. We show that very large differences in measured particle properties have appeared in the literature, in particular with regards to particle carbon budgets. We investigate emissions uncertainties using scale analyses, which shows that while emission factors for grass and brush are relatively well known, very large uncertainties still exist in emission factors of boreal, temperate and some tropical forests. Based on an uncertainty analysis of the community data set of biomass burning measurements, we present simplified models for particle size and emission factors. We close this review paper with a discussion of the community experimental data, point to lapses in the data set, and prioritize future research topics.

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“…Numerous investigations of the atmospheric impact of tropical fires have given clear evidence that elevated levels of ozone over South America and Africa are due to the excessive burning of forests and savannah, the rain forest otherwise acting as an important net sink for ozone (e.g., Delany et al, 1985;Browell et al, 1988;Gregory et al, 1988;Crutzen and Andreae, 1990;Richardson et al, 1991;Kirchhoff and Marinho, 1994;Kirchhoff, 1996;Kirchhoff et al, 1996). A retrieval of satellite measurements has given evidence of substantial ozone export to the tropical oceanic regions (Fishman et al, 1986;Fishman and Larsen, 1987), a strong burden to the otherwise clean troposphere in the Southern Hemisphere during certain periods of the year.…”

Section: Introductionmentioning

confidence: 99%

Stratospheric ozone in boreal fire plumes – the 2013 smoke season over central Europe

et al. 2015

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Abstract. In July 2013 very strong boreal fire plumes were observed at the northern rim of the Alps by lidar and ceilometer measurements of aerosol, ozone and water vapour for about 3 weeks. In addition, some of the lower-tropospheric components of these layers were analysed at the Global Atmosphere Watch laboratory at the Schneefernerhaus highaltitude research station (2650 m a.s.l., located a few hundred metres south-west of the Zugspitze summit). The high amount of particles confirms our hypothesis that fires in the Arctic regions of North America lead to much stronger signatures in the central European atmosphere than the multitude of fires in the USA. This has been ascribed to the prevailing anticyclonic advection pattern during favourable periods and subsidence, in contrast to warm-conveyor-belt export, rainout and dilution frequently found for lower latitudes. A high number of the pronounced aerosol structures were positively correlated with elevated ozone. Chemical ozone formation in boreal fire plumes is known to be rather limited. Indeed, these air masses could be attributed to stratospheric air intrusions descending from remote high-latitude regions, obviously picking up the aerosol on their way across Canada. In one case, subsidence from the stratosphere over Siberia over as many as 15-20 days without increase in humidity was observed although a significant amount of Canadian smoke was trapped. These coherent air streams lead to rather straight and rapid transport of the particles to Europe.

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Photochemically produced ozone in the emission from large‐scale tropical vegetation fires

Cited by 126 publications

References 15 publications

Photosensitised heterogeneous oxidation kinetics of biomass burning aerosol surrogates by ozone using an irradiated rectangular channel flow reactor

Photosensitised heterogeneous oxidation kinetics of biomass burning aerosol surrogates by ozone using an irradiated rectangular channel flow reactor

A review of biomass burning emissions part II: intensive physical properties of biomass burning particles

Stratospheric ozone in boreal fire plumes – the 2013 smoke season over central Europe

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