scholarly journals Impact of mixing state and hygroscopicity on CCN activity of biomass burning aerosol in Amazonia

2017 ◽  
Vol 17 (3) ◽  
pp. 2373-2392 ◽  
Author(s):  
Madeleine Sánchez Gácita ◽  
Karla M. Longo ◽  
Julliana L. M. Freire ◽  
Saulo R. Freitas ◽  
Scot T. Martin

Abstract. Smoke aerosols prevail throughout Amazonia because of widespread biomass burning during the dry season, and external mixing, low variability in the particle size distribution and low particle hygroscopicity are typical. There can be profound effects on cloud properties. This study uses an adiabatic cloud model to simulate the activation of smoke particles as cloud condensation nuclei (CCN) for three hypothetical case studies, chosen as to resemble biomass burning aerosol observations in Amazonia. The relative importance of variability in hygroscopicity, mixing state, and activation kinetics for the activated fraction and maximum supersaturation is assessed. For a population with κp = 0.04, an overestimation of the cloud droplet number concentration Nd for the three selected case studies between 22.4 ± 1.4 and 54.3 ± 3.7 % was obtained when assuming a hygroscopicity parameter κp = 0.20. Assuming internal mixing of the aerosol population led to overestimations of up to 20 % of Nd when a group of particles with medium hygroscopicity was present in the externally mixed population cases. However, the overestimations were below 10 % for external mixtures between very low and low-hygroscopicity particles, as seems to be the case for Amazon smoke particles. Kinetic limitations were significant for medium- and high-hygroscopicity particles, and much lower for very low and low-hygroscopicity particles. When particles were assumed to be at equilibrium and to respond instantly to changes in the air parcel supersaturation, the overestimation of the droplet concentration was up to  ∼  100 % in internally mixed populations, and up to  ∼  250 % in externally mixed ones, being larger for the higher values of hygroscopicity. In addition, a perceptible delay between the times when maximum supersaturation and maximum aerosol activated fraction are reached was noticed and, for aerosol populations with effective hygroscopicity κpeff higher than a certain threshold value, the delay in particle activation was such that no particles were activated at the time of maximum supersaturation. Considering internally mixed populations, for an updraft velocity W = 0.5 m s−1 this threshold of no activation varied between κpeff = 0.35 and κpeff = 0.5 for the different case studies. However, for low hygroscopicity, kinetic limitations played a weaker role for CCN activation of particles, even when taking into account the large aerosol mass and number concentrations. For the very low range of hygroscopicities, the overestimation of the droplet concentration due to the equilibrium assumption was lowest and the delay between the times when maximum supersaturation and maximum activated fraction were reached was greatly reduced or no longer observed (depending on the case study). These findings on uncertainties and sensitivities provide guidance on appropriate simplifications that can be used for modeling of smoke aerosols within general circulation models. The use of medium values of hygroscopicity representative of smoke aerosols for other biomass burning regions on Earth can lead to significant errors compared to the use of low hygroscopicity for Amazonia (between 0.05 and 0.13, according to available observations). Also in this region, consideration of the biomass burning population as internally mixed will lead to small errors in the droplet concentration, while significantly increasing the computational burden. Regardless of the large smoke aerosol loads in the region during the dry season, kinetic limitations are expected to be low.

2016 ◽  
Author(s):  
Madeleine Sánchez Gácita ◽  
Karla M. Longo ◽  
Julliana L. M. Freire ◽  
Saulo R. Freitas ◽  
Scot T. Martin

Abstract. Smoke aerosols prevail throughout Amazonia because of widespread biomass burning during the dry season. External mixing, low variability in the particle size distribution and low particle hygroscopicity are typical. There can be profound effects on cloud properties. This study uses an adiabatic cloud model to simulate the activation of smoke particles as cloud condensation nuclei (CCN) and to assess the relative importance of variability in hygroscopicity, mixing state, and activation kinetics for the activated fraction and maximum supersaturation. The analysis shows that use of medium values of hygroscopicity representative of smoke aerosols for other biomass burning regions on Earth can lead to significant errors, compared to the use of low hygroscopicity reported for Amazonia. Kinetic limitations, which can be significant for medium and high hygroscopicity, did not play a strong role for CCN activation of particles representative of Amazonia smoke aerosols, even when taking into account the large aerosol mass and number concentrations typical of the region. Internal compared to external mixing of particle components of variable hygroscopicity resulted in a significant overestimation of the activated fraction. These findings on uncertainties and sensitivities provide guidance on appropriate simplifications that can be used for modeling of smoke aerosols within general circulation models.


2019 ◽  
Vol 19 (14) ◽  
pp. 9181-9208 ◽  
Author(s):  
Kristina Pistone ◽  
Jens Redemann ◽  
Sarah Doherty ◽  
Paquita Zuidema ◽  
Sharon Burton ◽  
...  

Abstract. The total effect of aerosols, both directly and on cloud properties, remains the biggest source of uncertainty in anthropogenic radiative forcing on the climate. Correct characterization of intensive aerosol optical properties, particularly in conditions where absorbing aerosol is present, is a crucial factor in quantifying these effects. The southeast Atlantic Ocean (SEA), with seasonal biomass burning smoke plumes overlying and mixing with a persistent stratocumulus cloud deck, offers an excellent natural laboratory to make the observations necessary to understand the complexities of aerosol–cloud–radiation interactions. The first field deployment of the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) campaign was conducted in September of 2016 out of Walvis Bay, Namibia. Data collected during ORACLES-2016 are used to derive aerosol properties from an unprecedented number of simultaneous measurement techniques over this region. Here, we present results from six of the eight independent instruments or instrument combinations, all applied to measure or retrieve aerosol absorption and single-scattering albedo. Most but not all of the biomass burning aerosol was located in the free troposphere, in relative humidities typically ranging up to 60 %. We present the single-scattering albedo (SSA), absorbing and total aerosol optical depth (AAOD and AOD), and absorption, scattering, and extinction Ångström exponents (AAE, SAE, and EAE, respectively) for specific case studies looking at near-coincident and near-colocated measurements from multiple instruments, and SSAs for the broader campaign average over the month-long deployment. For the case studies, we find that SSA agrees within the measurement uncertainties between multiple instruments, though, over all cases, there is no strong correlation between values reported by one instrument and another. We also find that agreement between the instruments is more robust at higher aerosol loading (AOD400>0.4). The campaign-wide average and range shows differences in the values measured by each instrument. We find the ORACLES-2016 campaign-average SSA at 500 nm (SSA500) to be between 0.85 and 0.88, depending on the instrument considered (4STAR, AirMSPI, or in situ measurements), with the interquartile ranges for all instruments between 0.83 and 0.89. This is consistent with previous September values reported over the region (between 0.84 and 0.90 for SSA at 550nm). The results suggest that the differences observed in the campaign-average values may be dominated by instrument-specific spatial sampling differences and the natural physical variability in aerosol conditions over the SEA, rather than fundamental methodological differences.


2020 ◽  
Vol 47 (19) ◽  
Author(s):  
Cyrielle Denjean ◽  
Joel Brito ◽  
Quentin Libois ◽  
Marc Mallet ◽  
Thierry Bourrianne ◽  
...  

2019 ◽  
Author(s):  
Kristina Pistone ◽  
Jens Redemann ◽  
Sarah Doherty ◽  
Paquita Zuidema ◽  
Sharon Burton ◽  
...  

Abstract. The total effect of aerosols, both directly and on cloud properties, remains the biggest source of uncertainty in anthropogenic radiative forcing on the climate. Correct characterization of intensive aerosol optical properties, particularly in conditions where absorbing aerosol is present, is a crucial factor in quantifying these effects. The Southeast Atlantic Ocean (SEA), with seasonal biomass burning smoke plumes overlying and mixing with a persistent stratocumulus cloud deck, offers an excellent natural laboratory to make the observations necessary to understand the complexities of aerosol-cloud-radiation interactions. The first field deployment of the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) campaign was conducted in September of 2016 out of Walvis Bay, Namibia. Data collected during ORACLES-2016 are used to derive aerosol properties from an unprecedented number of simultaneous measurement techniques over this region. Here we present results from six of the eight independent instruments or instrument combinations, all applied to measure or retrieve aerosol absorption and single scattering albedo. Most but not all of the biomass-burning aerosol was located in the free troposphere, in relative humidities typically ranging up to 60 %. We present the single scattering albedo (SSA), absorbing and total aerosol optical depth (AOD and AAOD), and absorption, scattering, and extinction Ångström exponents (AAE, SAE, EAE) for specific case studies looking at near-coincident and -colocated measurements from multiple instruments, and SSAs for the broader campaign average over the monthlong deployment. For the case studies, we find that SSA agrees within the measurement uncertainties between multiple instruments, though, over all cases, there is no strong correlation between values reported by one instrument and another. We also find that agreement between the instruments is more robust at higher aerosol loading (AOD400 > 0.4). The campaign-wide average and range shows differences in the values measured by each instrument. We find the ORACLES-2016 campaign-average SSA at 500 nm (SSA500) to be between 0.85 and 0.88, depending on the instrument considered (4STAR, AirMSPI, or in situ measurements), with the inter-quartile ranges for all instruments between 0.83 and 0.89. This is consistent with previous September values reported over the region (between 0.84 and 0.90 for SSA at 550 nm). The results suggest that the differences observed in the campaign-average values may be dominated by instrument-specific spatial sampling differences and the natural physical variability in aerosol conditions over the SEA, rather than fundamental methodological differences.


2010 ◽  
Vol 10 (24) ◽  
pp. 12005-12023 ◽  
Author(s):  
O. Cavalieri ◽  
F. Cairo ◽  
F. Fierli ◽  
G. Di Donfrancesco ◽  
M. Snels ◽  
...  

Abstract. In this work, we have studied the seasonal and inter-annual variability of the aerosol vertical distribution over Sahelian Africa for the years 2006, 2007 and 2008, characterizing the different kind of aerosols present in the atmosphere in terms of their optical properties observed by ground-based and satellite instruments, and their sources searched for by using trajectory analysis. This study combines data acquired by three ground-based micro lidar systems located in Banizoumbou (Niger), Cinzana (Mali) and M'Bour (Senegal) in the framework of the African Monsoon Multidisciplinary Analysis (AMMA), by the AEROsol RObotic NETwork (AERONET) sun-photometers and by the space-based Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) onboard the CALIPSO satellite (Cloud-Aerosol Lidar and Infrared Pathfinder Observations). During winter, the lower levels air masses arriving in the Sahelian region come mainly from North, North-West and from the Atlantic area, while in the upper troposphere air flow generally originates from West Africa, crossing a region characterized by the presence of large biomass burning sources. The sites of Cinzana, Banizoumbou and M'Bour, along a transect of aerosol transport from East to West, are in fact under the influence of tropical biomass burning aerosol emission during the dry season, as revealed by the seasonal pattern of the aerosol optical properties, and by back-trajectory studies. Aerosol produced by biomass burning are observed mainly during the dry season and are confined in the upper layers of the atmosphere. This is particularly evident for 2006, which was characterized by a large presence of biomass burning aerosols in all the three sites. Biomass burning aerosol is also observed during spring when air masses originating from North and East Africa pass over sparse biomass burning sources, and during summer when biomass burning aerosol is transported from the southern part of the continent by the monsoon flow. During summer months, the entire Sahelian region is under the influence of Saharan dust aerosols: the air masses in low levels arrive from West Africa crossing the Sahara desert or from the Southern Hemisphere crossing the Guinea Gulf while in the upper layers air masses still originate from North, North-East. The maximum of the desert dust activity is observed in this period which is characterized by large AOD (above 0.2) and backscattering values. It also corresponds to a maximum in the extension of the aerosol vertical distribution (up to 6 km of altitude). In correspondence, a progressive cleaning up of the lowermost layers of the atmosphere is occurring, especially evident in the Banizoumbou and Cinzana sites. Summer is in fact characterized by extensive and fast convective phenomena. Lidar profiles show at times large dust events loading the atmosphere with aerosol from the ground up to 6 km of altitude. These events are characterized by large total attenuated backscattering values, and alternate with very clear profiles, sometimes separated by only a few hours, indicative of fast removal processes occurring, likely due to intense convective and rain activity. The inter-annual variability in the three year monitoring period is not very significant. An analysis of the aerosol transport pathways, aiming at detecting the main source regions, revealed that air originated from the Saharan desert is present all year long and it is observed in the lower levels of the atmosphere at the beginning and at the end of the year. In the central part of the year it extends upward and the lower levels are less affected by air masses from Saharan desert when the monsoon flow carries air from the Guinea Gulf and the Southern Hemisphere inland.


2009 ◽  
Vol 9 (20) ◽  
pp. 8017-8038 ◽  
Author(s):  
S.-W. Kim ◽  
P. Chazette ◽  
F. Dulac ◽  
J. Sanak ◽  
B. Johnson ◽  
...  

Abstract. We present observations of tropospheric aerosol and water vapor transport over West Africa and the associated meteorological conditions during the AMMA SOP-0 dry season experiment, which was conducted in West Africa in January–February 2006. This study combines data from ultra-light aircraft (ULA)-based lidar, airborne in-situ aerosol and gas measurements, standard meteorological measurements, satellite-based aerosol measurements, airmass trajectories, and radiosonde measurements. At Niamey (13.5° N, 2.2° E) the prevailing surface wind (i.e. Harmattan) was from the northeast bringing dry dusty air from the Sahara desert. High concentrations of mineral dust aerosol were typically observed from the surface to 1.5 or 2 km associated with the Saharan airmasses. At higher altitudes the prevailing wind veered to the south or southeast bringing relatively warm and humid airmasses from the biomass burning regions to the Sahel (<10° N). These elevated layers had high concentrations of biomass burning aerosol and were typically observed between altitudes of 2–5 km. Meteorological analyses show these airmasses were advected upwards over the biomass burning regions through ascent in Inter-Tropical Discontinuity (ITD) zone. Aerosol vertical profiles obtained from the space-based lidar CALIOP onboard CALIPSO during January 2007 also showed the presence of dust particles (particle depolarization (δ)~30%, lidar Ångström exponent (LAE)<0, aerosol backscatter to extinction ratio (BER): 0.026~0.028 sr−1) at low levels (<1.5 km) and biomass burning smoke aerosol (δ<10%, LAE: 0.6~1.1, BER: 0.015~0.018 sr−1) between 2 and 5 km. CALIOP data indicated that these distinct continental dust and biomass burning aerosol layers likely mixed as they advected further south over the tropical Atlantic Ocean, as indicated an intermediate values of δ (10~17%), LAE (0.16~0.18) and BER (0.0021~0.0022 sr−1).


2009 ◽  
Vol 9 (1) ◽  
pp. 1831-1871
Author(s):  
S.-W. Kim ◽  
P. Chazette ◽  
F. Dulac ◽  
J. Sanak ◽  
B. Johnson ◽  
...  

Abstract. We present observations of tropospheric aerosol and water vapor transport over West Africa and the associated meteorological conditions during the AMMA SOP-0 dry season experiment, which was conducted in West Africa in January–February 2006. This study combines data from ultra-light aircraft (ULA)-based lidar, airborne in-situ aerosol and gas measurements, standard meteorological measurements, satellite-based aerosol measurements, airmass trajectories, and radiosonde measurements. At Niamey (13.5° N, 2.2° E) the prevailing surface wind was from the northeast bringing dry dusty air from the Sahara desert. High concentrations of mineral dust aerosol were typically observed from the surface to 1.5 or 2 km associated with the Saharan airmasses. At higher altitudes the prevailing wind veered to the south or southeast bringing relatively warm and humid airmasses from the biomass burning regions to the Sahel (<10° N). These elevated layers had high concentrations of biomass burning aerosol and were typically observed between altitudes of 2–5 km. Meteorological analyses show these airmasses were advected upwards over the biomass burning regions through large-scale ascent, presumably driven by surface heating rather than pyro-convection. Aerosol vertical profiles obtained from the space-based lidar CALIOP onboard CALIPSO during January 2007 also showed the presence of dust particles (depolarization ~30%, color ratio <0) at low levels (<1.5 km) and biomass burning smoke aerosol (depolarization ratio <10%) between 2 and 5 km. CALIOP data indicated that these distinct continental dust and biomass burning aerosol layers likely mixed as they advected further south over the tropical Atlantic Ocean.


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