scholarly journals Black and brown carbon over central Amazonia: Long-term aerosol measurements at the ATTO site

2017 ◽  
Author(s):  
Jorge Saturno ◽  
Bruna A. Holanda ◽  
Christopher Pöhlker ◽  
Florian Ditas ◽  
Qiaoqiao Wang ◽  
...  
Keyword(s):  
El Niño ◽  
Light Absorption ◽  
Rain Forest ◽  
El Nino ◽  
Aerosol Particles ◽  
Wavelength Dependence ◽  
Brown Carbon ◽  
Amazon Rain Forest ◽  
Central Amazonia ◽  
Measurement Period

Abstract. The Amazon rain forest is considered a very sensitive ecosystem that could be significantly affected by a changing climate. It is still one of the few places on Earth where the atmosphere in the continent approaches near-pristine conditions for some periods of the year. The Amazon Tall Tower Observatory (ATTO) has been built in central Amazonia to monitor the atmospheric and forest ecosystem conditions. The atmospheric conditions at the ATTO site oscillate between biogenic and biomass burning (BB) dominated states. By using a comprehensive ground-based aerosol measurement setup, we studied the physical and chemical properties of aerosol particles at the ATTO site. This paper presents results from 2012 to 2017, with special focus on light absorbing aerosol particles. The aerosol absorption wavelength dependence (expressed as the absorption Ångström exponent, åabs) was usually below 1.0 and increased during the presence of smoke transported from fires in the southern and eastern regions of the Amazon or advected from savanna fires in Africa. In this study, the brown carbon (BrC) contribution to light absorption at 370 nm was obtained by calculating the theoretical wavelength dependence of åabs (WDA). Our calculations resulted in BrC contributions of 17–29 % (25th and 75th percentiles) to total light absorption at 370 nm (σap 370) during the measurement period (2012–2017). The BrC contribution increased up to 27–47 % during fire events occurring under the influence of El Niño, between September and November 2015. An extended time series of ATTO and ZF2 (another Amazon rain forest sampling site) data showed enhanced light scattering and absorption coefficients during El Niño periods in 2009 and 2015. Long-range transport (LRT) aerosol particles that reached the central Amazon Basin from Africa or from southern Amazon exhibited a wide range of black carbon (BC) to carbon monoxide (CO) enhancement ratios (ERBC) (between 4 and 15 ng m−3 ppb−1) reflecting the variability of fuels, combustion phase, and removal processes in the atmosphere. Higher ERBC were measured during the dry season when we observed values up to 15 ng m−3 ppb−1, which were related to the lowest single scattering albedo (ω0) measured during the studied period, (0.86–0.93). A parameterization of åabs as a function of the BC to OA mass ratio was investigated and was found applicable to tropical forest emissions but further investigation is required, especially by segregating fuel types. Additionally, important enhancements of the BC mass absorption cross‑section (αabs) were found over the measurement period. This enhancement could be linked to heavy coating of the BC aerosol particles. In the future, the BC mixing state should be systematically investigated by using different instrumental approaches.

scholarly journals Black and brown carbon over central Amazonia: long-term aerosol measurements at the ATTO site

2018 ◽  
Vol 18 (17) ◽  
pp. 12817-12843 ◽  
Author(s):  
Jorge Saturno ◽  
Bruna A. Holanda ◽  
Christopher Pöhlker ◽  
Florian Ditas ◽  
Qiaoqiao Wang ◽  
...  
Keyword(s):  
Optical Properties ◽  
El Niño ◽  
El Nino ◽  
Dry Season ◽  
Wet Season ◽  
Aerosol Optical Properties ◽  
Brown Carbon ◽  
Central Amazonia ◽  
Physical And Chemical ◽  
Aerosol Properties

Abstract. The Amazon rainforest is a sensitive ecosystem experiencing the combined pressures of progressing deforestation and climate change. Its atmospheric conditions oscillate between biogenic and biomass burning (BB) dominated states. The Amazon further represents one of the few remaining continental places where the atmosphere approaches pristine conditions during occasional wet season episodes. The Amazon Tall Tower Observatory (ATTO) has been established in central Amazonia to investigate the complex interactions between the rainforest ecosystem and the atmosphere. Physical and chemical aerosol properties have been analyzed continuously since 2012. This paper provides an in-depth analysis of the aerosol's optical properties at ATTO based on data from 2012 to 2017. The following key results have been obtained. The aerosol scattering and absorption coefficients at 637 nm, σsp,637 and σap,637, show a pronounced seasonality with lowest values in the clean wet season (mean ± SD: σsp,637=7.5±9.3 M m−1; σap,637=0.68±0.91 M m−1) and highest values in the BB-polluted dry season (σsp,637=33±25 M m−1; σap,637=4.0±2.2 M m−1). The single scattering albedo at 637 nm, ω0, is lowest during the dry season (ω0=0.87±0.03) and highest during the wet season (ω0=0.93±0.04). The retrieved BC mass absorption cross sections, αabs, are substantially higher than values widely used in the literature (i.e., 6.6 m2 g−1 at 637 nm wavelength), likely related to thick organic or inorganic coatings on the BC cores. Wet season values of αabs=11.4±1.2 m2 g−1 (637 nm) and dry season values of αabs=12.3±1.3 m2 g−1 (637 nm) were obtained. The BB aerosol during the dry season is a mixture of rather fresh smoke from local fires, somewhat aged smoke from regional fires, and strongly aged smoke from African fires. The African influence appears to be substantial, with its maximum from August to October. The interplay of African vs. South American BB emissions determines the aerosol optical properties (e.g., the fractions of black vs. brown carbon, BC vs. BrC). By analyzing the diel cycles, it was found that particles from elevated aerosol-rich layers are mixed down to the canopy level in the early morning and particle number concentrations decrease towards the end of the day. Brown carbon absorption at 370 nm, σap,BrC,370, was found to decrease earlier in the day, likely due to photo-oxidative processes. BC-to-CO enhancement ratios, ERBC, reflect the variability of burnt fuels, combustion phases, and atmospheric removal processes. A wide range of ERBC between 4 and 15 ng m−3 ppb−1 was observed with higher values during the dry season, corresponding to the lowest ω0 levels (0.86–0.93). The influence of the 2009/2010 and 2015/2016 El Niño periods and the associated increased fire activity on aerosol optical properties was analyzed by means of 9-year σsp and σap time series (combination of ATTO and ZF2 data). Significant El Niño-related enhancements were observed: in the dry season, σsp,637 increased from 24±18 to 48±33 M m−1 and σap, 637 from 3.8±2.8 to 5.3±2.5 M m−1. The absorption Ångström exponent, åabs, representing the aerosol absorption wavelength dependence, was mostly <1.0 with episodic increases upon smoke advection. A parameterization of åabs as a function of the BC-to-OA mass ratio for Amazonian aerosol ambient measurements is presented. The brown carbon (BrC) contribution to σap at 370 nm was obtained by calculating the theoretical BC åabs, resulting in BrC contributions of 17 %–29 % (25th and 75th percentiles) to σap 370 for the entire measurement period. The BrC contribution increased to 27 %–47 % during fire events under El Niño-related drought conditions from September to November 2015. The results presented here may serve as a basis to understand Amazonian atmospheric aerosols in terms of their interactions with solar radiation and the physical and chemical-aging processes that they undergo during transport. Additionally, the analyzed aerosol properties during the last two El Niño periods in 2009/2010 and 2015/2016 offer insights that could help to assess the climate change-related potential for forest-dieback feedbacks under warmer and drier conditions.

scholarly journals Production of particulate brown carbon during atmospheric aging of residential wood-burning emissions

2018 ◽  
Vol 18 (24) ◽  
pp. 17843-17861 ◽  
Author(s):  
Nivedita K. Kumar ◽  
Joel C. Corbin ◽  
Emily A. Bruns ◽  
Dario Massabó ◽  
Jay G. Slowik ◽  
...  
Keyword(s):  
Black Carbon ◽  
Light Absorption ◽  
Wavelength Dependence ◽  
Organic Aerosol ◽  
Geometric Standard Deviation ◽  
Wood Combustion ◽  
Brown Carbon ◽  
Atmospheric Aging ◽  
Aerosol Absorption ◽  
Uv Visible

Abstract. We investigate the optical properties of light-absorbing organic carbon (brown carbon) from domestic wood combustion as a function of simulated atmospheric aging. At shorter wavelengths (370–470 nm), light absorption by brown carbon from primary organic aerosol (POA) and secondary organic aerosol (SOA) formed during aging was around 10 % and 20 %, respectively, of the total aerosol absorption (brown carbon plus black carbon). The mass absorption cross section (MAC) determined for black carbon (BC, 13.7 m2 g−1 at 370 nm, with geometric standard deviation GSD =1.1) was consistent with that recommended by Bond et al. (2006). The corresponding MAC of POA (5.5 m2 g−1; GSD =1.2) was higher than that of SOA (2.4 m2 g−1; GSD =1.3) at 370 nm. However, SOA presents a substantial mass fraction, with a measured average SOA ∕ POA mass ratio after aging of ∼5 and therefore contributes significantly to the overall light absorption, highlighting the importance of wood-combustion SOA as a source of atmospheric brown carbon. The wavelength dependence of POA and SOA light absorption between 370 and 660 nm is well described with absorption Ångström exponents of 4.6 and 5.6, respectively. UV-visible absorbance measurements of water and methanol-extracted OA were also performed, showing that the majority of the light-absorbing OA is water insoluble even after aging.

scholarly journals Attribution of aerosol light absorption to black carbon, brown carbon, and dust in China – interpretations of atmospheric measurements during EAST-AIRE

2009 ◽  
Vol 9 (6) ◽  
pp. 2035-2050 ◽  
Author(s):  
M. Yang ◽  
S. G. Howell ◽  
J. Zhuang ◽  
B. J. Huebert
Keyword(s):  
Optical Properties ◽  
Black Carbon ◽  
Light Absorption ◽  
Northern China ◽  
Wavelength Dependence ◽  
Atmospheric Measurements ◽  
Brown Carbon ◽  
Mass Distributions ◽  
Limit Value ◽  
Light Absorbers

Abstract. Black carbon, brown carbon, and mineral dust are three of the most important light absorbing aerosols. Their optical properties differ greatly and are distinctive functions of the wavelength of light. Most optical instruments that quantify light absorption, however, are unable to distinguish one type of absorbing aerosol from another. It is thus instructive to separate total absorption from these different light absorbers to gain a better understanding of the optical characteristics of each aerosol type. During the EAST-AIRE (East Asian Study of Tropospheric Aerosols: an International Regional Experiment) campaign near Beijing, we measured light scattering using a nephelometer, and light absorption using an aethalometer and a particulate soot absorption photometer. We also measured the total mass concentrations of carbonaceous (elemental and organic carbon) and inorganic particulates, as well as aerosol number and mass distributions. We were able to identify periods during the campaign that were dominated by dust, biomass burning, fresh (industrial) chimney plumes, other coal burning pollution, and relatively clean (background) air for Northern China. Each of these air masses possessed distinct intensive optical properties, including the single scatter albedo and Ångstrom exponents. Based on the wavelength-dependence and particle size distribution, we apportioned total light absorption to black carbon, brown carbon, and dust; their mass absorption efficiencies at 550 nm were estimated to be 9.5, 0.5 (a lower limit value), and 0.03 m2/g, respectively. While agreeing with the common consensus that black carbon is the most important light absorber in the mid-visible, we demonstrated that brown carbon and dust could also cause significant absorption, especially at shorter wavelengths.

scholarly journals Aerosol number fluxes over the Amazon rain forest during the wet season

2009 ◽  
Vol 9 (24) ◽  
pp. 9381-9400 ◽  
Author(s):  
L. Ahlm ◽  
E. D. Nilsson ◽  
R. Krejci ◽  
E. M. M&amp;aring;rtensson ◽  
M. Vogt ◽  
...  
Keyword(s):  
Rain Forest ◽  
Large Scale ◽  
Friction Velocity ◽  
Aerosol Particles ◽  
Deposition Flux ◽  
Wet Season ◽  
Transfer Velocity ◽  
Aerosol Emission ◽  
Amazon Rain Forest ◽  
Particle Fluxes

Abstract. Number fluxes of particles with diameter larger than 10 nm were measured with the eddy covariance method over the Amazon rain forest during the wet season as part of the LBA (The Large Scale Biosphere Atmosphere Experiment in Amazonia) campaign 2008. The primary goal was to investigate whether sources or sinks dominate the aerosol number flux in the tropical rain forest-atmosphere system. During the measurement campaign, from 12 March to 18 May, 60% of the particle fluxes pointed downward, which is a similar fraction to what has been observed over boreal forests. The net deposition flux prevailed even in the absolute cleanest atmospheric conditions during the campaign and therefore cannot be explained only by deposition of anthropogenic particles. The particle transfer velocity vt increased with increasing friction velocity and the relation is described by the equation vt = 2.4×10−3×u* where u* is the friction velocity. Upward particle fluxes often appeared in the morning hours and seem to a large extent to be an effect of entrainment fluxes into a growing mixed layer rather than primary aerosol emission. In general, the number source of primary aerosol particles within the footprint area of the measurements was small, possibly because the measured particle number fluxes reflect mostly particles less than approximately 200 nm. This is an indication that the contribution of primary biogenic aerosol particles to the aerosol population in the Amazon boundary layer may be low in terms of number concentrations. However, the possibility of horizontal variations in primary aerosol emission over the Amazon rain forest cannot be ruled out.

scholarly journals African volcanic emissions influencing atmospheric aerosol particles over the Amazon rain forest

2017 ◽  
Author(s):  
Jorge Saturno ◽  
Florian Ditas ◽  
Marloes Penning de Vries ◽  
Bruna A. Holanda ◽  
Mira L. Pöhlker ◽  
...  
Keyword(s):  
Rain Forest ◽  
Amazon Basin ◽  
Dimethyl Sulfide ◽  
Aerosol Particles ◽  
Amazon Region ◽  
Volcanic Emissions ◽  
Airborne Measurements ◽  
Amazon Rain Forest ◽  
Sulfur Emissions

Abstract. Long-range transport (LRT) plays an important role in the Amazon rain forest by bringing in different primary and secondary aerosol particles from distant sources. The atmospheric oxidation of dimethyl sulfide (DMS), emitted from marine plankton, is considered an important sulfate source over the Amazon rain forest, with a lesser contribution from terrestrial soil and vegetation sulfur emissions. Volcanic sulfur emissions from Africa could be a source of particulate sulfate to the Amazonian atmosphere upon transatlantic transport but no observations have been published. By using satellite observations, together with ground‑based and airborne aerosol particle observations, this paper provides evidence of the influence that volcanic emissions have on the aerosol properties that have been observed in central Amazonia. Under the volcanic influence, sulfate mass concentrations reached up to 3.6 µg m−3 (hourly mean) at ground level, the highest value ever reported in the Amazon region. The hygroscopicity parameter was higher than the characteristic dry-season average, reaching a maximum of 0.36 for accumulation mode aerosol particles. Airborne measurements and satellite data indicated the transport of two different volcanic plumes reaching the Amazon Basin in September 2014 with a sulfate-enhanced layer at an altitude between 4 and 5 km. These observations show that remote volcanic sources can episodically affect the aerosol cycling over the Amazon rain forest and perturb the background conditions. Further studies should address the long-term effect of volcanogenic aerosol particles over the Amazon Basin by running long-term and intensive field measurements in the Amazon region and by monitoring African emissions and their transatlantic transport.

scholarly journals Response of CO<sub>2</sub> and H<sub>2</sub>O fluxes of a mountainous tropical rain forest in equatorial Indonesia to El Niño events

2015 ◽  
Vol 12 (6) ◽  
pp. 4405-4431 ◽  
Author(s):  
A. Olchev ◽  
A. Ibrom ◽  
O. Panferov ◽  
D. Gushchina ◽  
P. Propastin ◽  
...  
Keyword(s):  
El Niño ◽  
Rain Forest ◽  
Tropical Rain Forest ◽  
El Nino ◽  
Southern Oscillation ◽  
La Niña ◽  
Moderate Intensity ◽  
Central Pacific ◽  
Enso Events ◽  
La Nina

Abstract. The possible impact of El Niño–Southern Oscillation (ENSO) events on the main components of CO2 and H2O fluxes in a pristine mountainous tropical rainforest growing in Central Sulawesi in Indonesia is described. The fluxes were continuously measured using the eddy covariance method for the period from January 2004 to June 2008. During this period, two episodes of El Niño and one episode of La Niña were observed. All these ENSO episodes had moderate intensity and were of Central Pacific type. The temporal variability analysis of the main meteorological parameters and components of CO2 and H2O exchange showed a very high sensitivity of Evapotranspiration (ET) and Gross Primary Production (GPP) of the tropical rain forest to meteorological variations caused by both El Niño and La Niña episodes. Incoming solar radiation is the main governing factor that is responsible for ET and GPP variability. Ecosystem Respiration (RE) dynamics depend mainly on the air temperature changes and are almost insensitive to ENSO. Changes of precipitation due to moderate ENSO events did not cause any notable effect on ET and GPP, mainly because of sufficient soil moisture conditions even in periods of anomalous reduction of precipitation in the region.

scholarly journals Absorptivity of brown carbon in fresh and photo-chemically aged biomass-burning emissions

2013 ◽  
Vol 13 (5) ◽  
pp. 11509-11536 ◽  
Author(s):  
R. Saleh ◽  
C. J. Hennigan ◽  
G. R. McMeeking ◽  
W. K. Chuang ◽  
E. S. Robinson ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Light Absorption ◽  
Radiative Forcing ◽  
Uv Light ◽  
Wavelength Dependence ◽  
Organic Aerosol ◽  
The United States ◽  
Prescribed Fires ◽  
Brown Carbon ◽  
Chemical Aging

Abstract. Experiments were conducted to investigate light absorption of organic aerosol (OA) in fresh and photo-chemically aged biomass-burning emissions. The experiments considered residential hardwood fuel (oak) and fuels commonly consumed in wild-land and prescribed fires in the United States (pocosin pine and gallberry). Photo-chemical aging was performed in an environmental chamber. We constrained the light-absorption properties of the OA using conservative limiting assumptions, and found that both primary organic aerosol (POA) in the fresh emissions and secondary organic aerosol (SOA) produced by photo-chemical aging absorb light to a significant extent, and are categorized as brown carbon. This work presents the first direct evidence that SOA produced in aged biomass-burning emissions is absorptive. For the investigated fuels, SOA is less absorptive than POA in the long visible, but exhibits steeper wavelength-dependence (larger Absorption Ångström Exponent) and is more absorptive in the short visible and near-UV. Light absorption by SOA in biomass-burning emissions might be an important contributor to the global radiative forcing budget.

scholarly journals Production of particulate brown carbon during atmospheric aging of wood-burning emissions

2018 ◽  
Author(s):  
Nivedita K. Kumar ◽  
Joel C. Corbin ◽  
Emily A. Bruns ◽  
Dario Massabó ◽  
Jay G. Slowik ◽  
...  
Keyword(s):  
Black Carbon ◽  
Light Absorption ◽  
Wavelength Dependence ◽  
Organic Aerosol ◽  
Geometric Standard Deviation ◽  
Wood Combustion ◽  
Brown Carbon ◽  
Atmospheric Aging ◽  
Aerosol Absorption ◽  
Uv Visible

Abstract. We investigate the optical properties of light-absorbing organic carbon (brown carbon) from domestic wood combustion as a function of simulated atmospheric aging. At shorter wavelengths, light absorption by brown carbon from primary organic aerosol (POA) and secondary organic aerosol (SOA) formed during aging was around 10 % and 20 %, respectively, of the total aerosol absorption (brown carbon plus black carbon). The mass absorption cross-section (MAC) determined for black carbon (BC, 13.7 m2 g−1 (geometric standard deviation GSD = 1.1) at 370 nm) was consistent with that recommended by Bond et al. (2006). The corresponding MAC of POA (5.5 m2 g−1 (GSD = 1.2)) was higher than that of SOA (2.4 m2 g−1 (GSD = 1.3)) at 370 nm. However, SOA presents a substantial mass fraction, with a measured average SOA / POA mass ratio after aging of ~ 5 and therefore contributes significantly to the overall light absorption, highlighting the importance of wood-combustion SOA as a source of atmospheric brown carbon. The wavelength dependence of POA and SOA light absorption between 370 nm and 660 nm is well described with absorption Ångström exponents of 4.6 and 5.6, respectively. UV-visible absorbance measurements of water and methanol-extracted OA were also performed showing that the majority of the light-absorbing OA is water insoluble even after aging.

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