scholarly journals Size-resolved chemical composition, effective density, and optical properties of biomass burning particles

2016 ◽  
Author(s):  
Jinghao Zhai ◽  
Xiaohui Lu ◽  
Ling Li ◽  
Qi Zhang ◽  
Ci Zhang ◽  
...  

Abstract. Biomass burning aerosol has important impact on the global radiative budget. A better understanding of the mixing state and chemical composition of biomass burning particles relative to their optical properties is the goal of a number of current studies. In this work, effective density, chemical composition, and optical properties of rice straw burning particles in the size range of 50–400 nm were measured using a suite of comprehensive methods. A Differential Mobility Analyzer (DMA)-Aerosol Particle Mass analyzer (APM)-Condensation Particle Counter (CPC) system offered detailed information on the effective density as well as mixing state of size-resolved particles. The effective density and chemical composition of individual particles were characterized with a DMA in-line with a Single Particle Aerosol Mass Spectrometer (SPAMS), simultaneously. The multiple modes observed in the size-resolved particle effective density distribution indicated size-dependent external mixing of black carbon (BC), organic carbon (OC) and potassium salts in particles. Particles of 50 nm had the smallest effective density (1.16 g/cm3), due to a relative large proportion of aggregate BC. The average effective densities of 100–400 nm particles ranged from 1.35–1.51 g/cm3 with OC and inorganic salts as dominant components. Both density distribution and single-particle mass spectrometry showed more complex mixing states in larger particles. Upon heating, the separation of the effective density distribution modes testified the existence of less volatile BC or soot and potassium salts. Size-resolved optical properties of biomass burning particles were measured by the Cavity Attenuated Phase Shift spectroscopy (CAPS, λ = 450 & 530 nm). The single scattering albedo (SSA) showed the lowest value for 50 nm particles (0.741 ± 0.007 & 0.889 ± 0.006) because of larger proportion of BC content. Brown carbon played an important role for the SSA of 100–400 nm particles. The Ångström absorption exponent (AAE) values for all particles were above 1.6, indicating the significant presence of brown carbon. Though freshly emitted, the light absorption enhancement (Eabs) was observed for particles larger than 200 nm. Concurrent measurements in our work provide a basis for discussing the physicochemical properties of biomass burning aerosol and its effects on global climate and atmospheric environment.

2017 ◽  
Vol 17 (12) ◽  
pp. 7481-7493 ◽  
Author(s):  
Jinghao Zhai ◽  
Xiaohui Lu ◽  
Ling Li ◽  
Qi Zhang ◽  
Ci Zhang ◽  
...  

Abstract. Biomass burning aerosol has an important impact on the global radiative budget. A better understanding of the correlations between the mixing states of biomass burning particles and their optical properties is the goal of a number of current studies. In this work, the effective density, chemical composition, and optical properties of rice straw burning particles in the size range of 50–400 nm were measured using a suite of online methods. We found that the major components of particles produced by burning rice straw included black carbon (BC), organic carbon (OC), and potassium salts, but the mixing states of particles were strongly size dependent. Particles of 50 nm had the smallest effective density (1.16 g cm−3) due to a relatively large proportion of aggregate BC. The average effective densities of 100–400 nm particles ranged from 1.35 to 1.51 g cm−3 with OC and inorganic salts as dominant components. Both density distribution and single-particle mass spectrometry showed more complex mixing states in larger particles. Upon heating, the separation of the effective density distribution modes confirmed the external mixing state of less-volatile BC or soot and potassium salts. The size-resolved optical properties of biomass burning particles were investigated at two wavelengths (λ =  450 and 530 nm). The single-scattering albedo (SSA) showed the lowest value for 50 nm particles (0.741 ± 0.007 and 0.889 ± 0.006) because of the larger proportion of BC content. Brown carbon played an important role for the SSA of 100–400 nm particles. The Ångström absorption exponent (AAE) values for all particles were above 1.6, indicating the significant presence of brown carbon in all sizes. Concurrent measurements in our work provide a basis for discussing the physicochemical properties of biomass burning aerosol and its effects on the global climate and atmospheric environment.


2010 ◽  
Vol 67 (8) ◽  
pp. 2451-2468 ◽  
Author(s):  
Kerri A. Pratt ◽  
Andrew J. Heymsfield ◽  
Cynthia H. Twohy ◽  
Shane M. Murphy ◽  
Paul J. DeMott ◽  
...  

Abstract During the Ice in Clouds Experiment–Layer Clouds (ICE-L), aged biomass-burning particles were identified within two orographic wave cloud regions over Wyoming using single-particle mass spectrometry and electron microscopy. Using a suite of instrumentation, particle chemistry was characterized in tandem with cloud microphysics. The aged biomass-burning particles comprised ∼30%–40% by number of the 0.1–1.0-μm clear-air particles and were composed of potassium, organic carbon, elemental carbon, and sulfate. Aerosol mass spectrometry measurements suggested these cloud-processed particles were predominantly sulfate by mass. The first cloud region sampled was characterized by primarily homogeneously nucleated ice particles formed at temperatures near −40°C. The second cloud period was characterized by high cloud droplet concentrations (∼150–300 cm−3) and lower heterogeneously nucleated ice concentrations (7–18 L−1) at cloud temperatures of −24° to −25°C. As expected for the observed particle chemistry and dynamics of the observed wave clouds, few significant differences were observed between the clear-air particles and cloud residues. However, suggestive of a possible heterogeneous nucleation mechanism within the first cloud region, ice residues showed enrichments in the number fractions of soot and mass fractions of black carbon, measured by a single-particle mass spectrometer and a single-particle soot photometer, respectively. In addition, enrichment of biomass-burning particles internally mixed with oxalic acid in both the homogeneously nucleated ice and cloud droplets compared to clear air suggests either preferential activation as cloud condensation nuclei or aqueous phase cloud processing.


2019 ◽  
Author(s):  
Cyrielle Denjean ◽  
Thierry Bourrianne ◽  
Frederic Burnet ◽  
Marc Mallet ◽  
Nicolas Maury ◽  
...  

Abstract. Southern West Africa (SWA) is an African pollution hotspot but a relatively poorly sampled region of the world. We present an overview of in-situ aerosol optical measurements collected over SWA in June and July 2016 as part as the DACCIWA (Dynamics–Aerosol–Chemistry–Clouds Interactions in West Africa) airborne campaign. The aircraft sampled a wide range of air masses, including anthropogenic pollution plumes emitted from the coastal cities, long-range transported biomass burning plumes from Central and Southern Africa and dust plumes from the Sahara and Sahel region, as well as mixtures of these plumes. The specific objective of this work is to characterize the regional variability of the vertical distribution of aerosol particles and their spectral optical properties (single scattering albedo: SSA, asymmetry parameter, extinction mass efficiency, scattering Ångström exponent and absorption Ångström exponent: AAE). First findings indicate that aerosol optical properties in the planetary boundary layer were dominated by a widespread and persistent biomass burning loading from the Southern Hemisphere. Despite a strong increase of aerosol number concentration in air masses downwind of urban conglomerations, spectral SSA were comparable to the background and showed signatures of the absorption characteristics of biomass burning aerosols. In the free troposphere, moderately to strongly absorbing aerosol layers, dominated by either dust or biomass burning particles, occurred occasionally. In aerosol layers dominated by mineral dust particles, SSA varied from 0.81 to 0.92 at 550 nm depending on the variable proportion of anthropogenic pollution particles externally mixed with the dust. Biomass burning aerosol particles were significantly more light absorbing than those previously measured in other areas (e.g. Amazonia, North America) with SSA ranging from 0.71 to 0.77 at 550 nm. The variability of SSA was mainly controlled by variations in aerosol composition rather than in aerosol size distribution. Correspondingly, values of AAE ranged from 0.9 to 1.1, suggesting that lens-coated black carbon particles were the dominant absorber in the visible range for these biomass burning aerosols. Comparison with literature shows a consistent picture of increasing absorption enhancement of biomass burning aerosol from emission to remote location and underscores that the evolution of SSA occurred a long time after emission. The results presented here build a fundamental basis of knowledge about the aerosol optical properties observed over SWA during the monsoon season and can be used in climate modelling studies and satellite retrievals. In particular and regarding the very high absorbing properties of biomass burning aerosols over SWA, our findings suggest that considering the effect of internal mixing on absorption properties of black carbon particles in climate models should help better assessing the direct and semi-direct radiative effects of biomass burning particles.


2020 ◽  
Vol 237 ◽  
pp. 08016
Author(s):  
Christina-Anna Papanikolaou ◽  
Elina Giannakaki ◽  
Alex Papayannis ◽  
Maria Tombrou ◽  
Maria Mylonaki ◽  
...  

A long-lasting biomass burning event affected Europe from 27 August to 3 September 2018. The biomass burning aerosol layers were observed with ground- and space-based lidars in heights ranged between 2-7 km (a.s.l.). The mean backscatter coefficient for the ground-based stations ranged between 0.29 and 1.51 Mm-1sr-1, while the CALIPSO retrieved values ranged between 0.43 and 1.83 Mm-1sr-1. Moreover, the mean Ångström exponent (AEb) values, relevant to backscatter, ranged from 0.83 to 1.04 for the aforementioned lidar stations. At the same time, the mean AEb values obtained from CALIPSO ranged between 0.17 and 1.89. The mean particle depolarization ratio ranged between 0.037 and 0.080.


2017 ◽  
Author(s):  
Guohua Zhang ◽  
Qinhao Lin ◽  
Long Peng ◽  
Yuxiang Yang ◽  
Yuzhen Fu ◽  
...  

Abstract. While ground-based works suggest the significance of in-cloud production (or aqueous formation) to oxalate, direct evidence is rare. With the in situ measurements performed at a remote mountain site (1690 m a.s.l.) in southern China, we first reported the size-resolved mixing state of oxalate in the cloud droplet residual (cloud RES), the cloud interstitial (cloud INT), and ambient (cloud-free) particles by single particle mass spectrometry. The results support the growing evidence that in-cloud aqueous reactions promote the formation of oxalate, with ~ 15 % of the cloud RES and cloud INT particles containing oxalate, in contrast to only ~ 5 % of the cloud-free particles. Furthermore, individual particle analysis provides unique insight into the formation and evolution of oxalate during in-cloud processing. Oxalate was predominantly (> 70 % in number) internally mixed with the aged biomass burning particles, highlighting the impact of biomass burning on the formation of oxalate. In contrast, oxalate was underrepresented in aged elemental carbon particles, although they represented the largest fraction of the detected particles. It can be interpreted by the individual particle mixing state that the aged biomass burning particles contained an abundance of organic components serving as precursors for oxalate. Through the analysis of the relationship between oxalate and organic acid ions (−45[HCO2]−, −59[CH3CO2]−, −71[C2H3CO2]−, −73[C2HO3]−), the results show that in-cloud aqueous reaction dramatically improved the conversion of organic acids to oxalate. The abundance of glyoxylate associated with the aged biomass burning particles is the controlling factor for the in-cloud production of oxalate. Since only limited information on oxalate is available in the free troposphere, the results also provide an important reference for future understanding of the abundance, evolution and climate impacts of oxalate.


2017 ◽  
Vol 17 (22) ◽  
pp. 13891-13901 ◽  
Author(s):  
Guohua Zhang ◽  
Qinhao Lin ◽  
Long Peng ◽  
Yuxiang Yang ◽  
Yuzhen Fu ◽  
...  

Abstract. While ground-based works suggest the significance of in-cloud production (or aqueous formation) to oxalate, direct evidence is rare. With the in situ measurements performed at a remote mountain site (1690 m above sea level) in southern China, we first reported the size-resolved mixing state of oxalate in the cloud droplet residual (cloud RES), the cloud interstitial (cloud INT), and ambient (cloud-free) particles by single particle mass spectrometry. The results support the growing evidence that in-cloud aqueous reactions promote the formation of oxalate, with  ∼  15 % of the cloud RES and cloud INT particles containing oxalate in contrast to only  ∼  5 % of the cloud-free particles. Furthermore, individual particle analysis provides unique insight into the formation of oxalate during in-cloud processing. Oxalate was predominantly (> 70 % in number) internally mixed with the aged biomass-burning particles, highlighting the impact of biomass burning on the formation of oxalate. In contrast, oxalate was underrepresented in aged elemental carbon particles, although they represented the largest fraction of the detected particles. It can be interpreted by the individual particle mixing state that the aged biomass-burning particles contained an abundance of organic components serving as precursors for oxalate. Through the analysis of the relationship between oxalate and organic acids (−45[HCO2]−, −59[CH3CO2]−, −71[C2H3CO2]−, −73[C2HO3]−), the results show that in-cloud aqueous reactions dramatically improved the conversion of organic acids to oxalate. The abundance of glyoxylate associated with the aged biomass-burning particles is a controlling factor for the in-cloud production of oxalate. Since only limited information on oxalate is available in the free troposphere, the results also provide an important reference for future understanding of the abundance, evolution, and climate impacts of oxalate.


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.


2012 ◽  
Vol 12 (4) ◽  
pp. 1681-1700 ◽  
Author(s):  
R. M. Healy ◽  
J. Sciare ◽  
L. Poulain ◽  
K. Kamili ◽  
M. Merkel ◽  
...  

Abstract. An Aerosol Time-Of-Flight Mass Spectrometer (ATOFMS) was deployed to investigate the size-resolved chemical composition of single particles at an urban background site in Paris, France, as part of the MEGAPOLI winter campaign in January/February 2010. ATOFMS particle counts were scaled to match coincident Twin Differential Mobility Particle Sizer (TDMPS) data in order to generate hourly size-resolved mass concentrations for the single particle classes observed. The total scaled ATOFMS particle mass concentration in the size range 150–1067 nm was found to agree very well with the sum of concurrent High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and Multi-Angle Absorption Photometer (MAAP) mass concentration measurements of organic carbon (OC), inorganic ions and black carbon (BC) (R2 = 0.91). Clustering analysis of the ATOFMS single particle mass spectra allowed the separation of elemental carbon (EC) particles into four classes: (i) EC attributed to biomass burning (ECbiomass), (ii) EC attributed to traffic (ECtraffic), (iii) EC internally mixed with OC and ammonium sulfate (ECOCSOx), and (iv) EC internally mixed with OC and ammonium nitrate (ECOCNOx). Average hourly mass concentrations for EC-containing particles detected by the ATOFMS were found to agree reasonably well with semi-continuous quantitative thermal/optical EC and optical BC measurements (r2 = 0.61 and 0.65–0.68 respectively, n = 552). The EC particle mass assigned to fossil fuel and biomass burning sources also agreed reasonably well with BC mass fractions assigned to the same sources using seven-wavelength aethalometer data (r2 = 0.60 and 0.48, respectively, n = 568). Agreement between the ATOFMS and other instrumentation improved noticeably when a period influenced by significantly aged, internally mixed EC particles was removed from the intercomparison. 88% and 12% of EC particle mass was apportioned to fossil fuel and biomass burning respectively using the ATOFMS data compared with 85% and 15% respectively for BC estimated from the aethalometer model. On average, the mass size distribution for EC particles is bimodal; the smaller mode is attributed to locally emitted, mostly externally mixed EC particles, while the larger mode is dominated by aged, internally mixed ECOCNOx particles associated with continental transport events. Periods of continental influence were identified using the Lagrangian Particle Dispersion Model (LPDM) "FLEXPART". A consistent minimum between the two EC mass size modes was observed at approximately 400 nm for the measurement period. EC particles below this size are attributed to local emissions using chemical mixing state information and contribute 79% of the scaled ATOFMS EC particle mass, while particles above this size are attributed to continental transport events and contribute 21% of the EC particle mass. These results clearly demonstrate the potential benefit of monitoring size-resolved mass concentrations for the separation of local and continental EC emissions. Knowledge of the relative input of these emissions is essential for assessing the effectiveness of local abatement strategies.


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