Semi-Analytical Study of Aerosol Washout by Rain

Author(s):  
Pascal Lemaitre ◽  
Amandine Nuboer ◽  
Arnaud Querel ◽  
Guillaume Depuydt ◽  
Emmanuel Porcheron

The accidents of Chernobyl and Fukushima have shown the necessity to better understand all the mechanisms implied in the scavenging of aerosol particles released to the atmosphere during a nuclear accident. Among all the phenomena involved in the deposition of aerosol particles, we focus here on the aerosol particles scavenging by the raindrops below the clouds, also called washout (as opposed to the rainout, which concerns scavenging inside the clouds). The strategy of IRSN to enhance the knowledge and the modelling of any mechanism involved in the washout of aerosol particles by rain spans from environmental studies, to analytical ones. The semi-analytical approach chosen here is halfway between these two modes of reasoning. A companion paper is also submitted to the conference to present the microphysical approach chosen at IRSN. In order to perform this study, aerosol particles were dispersed in the TOSQAN chamber, which is a large cylindrical enclosure (4.8 m height with 1.5 m internal diameter). The aerosol particles once dispersed, synthetic rains of different kinds (from stratiform to convective rains) can be activated. Finally, the instantaneous spectral scavenging coefficients are determined from the spectral decrease of aerosol particles concentration in the chamber as a function of time. In order to be able to produce synthetic rains representative of any tropospheric events, a special generator has been designed; it is based on a vibro-rotative disk. This generator is able to produce monodispersed rains at the top of the TOSQAN chamber with rainfall rates from 7 to 15 mm/h and drops diameters from 0.5 to 2.5 mm injected at velocities close to their terminal one. During these tests, the spectral aerosol concentration is measured in line with the help of a Welas granulometer. This instrument is based on white light scattering. The results of these experiments highlight the influence of “meteorological” conditions inside the chamber on the washout of the chamber atmosphere, especially when the relative humidity is reaching saturation.

2010 ◽  
Vol 10 (8) ◽  
pp. 3875-3890 ◽  
Author(s):  
P. Zieger ◽  
R. Fierz-Schmidhauser ◽  
M. Gysel ◽  
J. Ström ◽  
S. Henne ◽  
...  

Abstract. Aerosol particles experience hygroscopic growth in the ambient atmosphere. Their optical properties – especially the aerosol light scattering – are therefore strongly dependent on the ambient relative humidity (RH). In-situ light scattering measurements of long-term observations are usually performed under dry conditions (RH>30–40%). The knowledge of this RH effect is of eminent importance for climate forcing calculations or for the comparison of remote sensing with in-situ measurements. This study combines measurements and model calculations to describe the RH effect on aerosol light scattering for the first time for aerosol particles present in summer and fall in the high Arctic. For this purpose, a field campaign was carried out from July to October 2008 at the Zeppelin station in Ny-Ålesund, Svalbard. The aerosol light scattering coefficient σsp(λ) was measured at three distinct wavelengths (λ=450, 550, and 700 nm) at dry and at various, predefined RH conditions between 20% and 95% with a recently developed humidified nephelometer (WetNeph) and with a second nephelometer measuring at dry conditions with an average RH<10% (DryNeph). In addition, the aerosol size distribution and the aerosol absorption coefficient were measured. The scattering enhancement factor f(RH, λ) is the key parameter to describe the RH effect on σsp(λ) and is defined as the RH dependent σsp(RH, λ) divided by the corresponding dry σsp(RHdry, λ). During our campaign the average f(RH=85%, λ=550 nm) was 3.24±0.63 (mean ± standard deviation), and no clear wavelength dependence of f(RH, λ) was observed. This means that the ambient scattering coefficients at RH=85% were on average about three times higher than the dry measured in-situ scattering coefficients. The RH dependency of the recorded f(RH, λ) can be well described by an empirical one-parameter equation. We used a simplified method to retrieve an apparent hygroscopic growth factor g(RH), defined as the aerosol particle diameter at a certain RH divided by the dry diameter, using the WetNeph, the DryNeph, the aerosol size distribution measurements and Mie theory. With this approach we found, on average, g(RH=85%) values to be 1.61±0.12 (mean±standard deviation). No clear seasonal shift of f(RH, λ) was observed during the 3-month period, while aerosol properties (size and chemical composition) clearly changed with time. While the beginning of the campaign was mainly characterized by smaller and less hygroscopic particles, the end was dominated by larger and more hygroscopic particles. This suggests that compensating effects of hygroscopicity and size determined the temporal stability of f(RH, λ). During sea salt influenced periods, distinct deliquescence transitions were observed. At the end we present a method on how to transfer the dry in-situ measured aerosol scattering coefficients to ambient values for the aerosol measured during summer and fall at this location.


2009 ◽  
Vol 2 (5) ◽  
pp. 2161-2190 ◽  
Author(s):  
R. Fierz-Schmidhauser ◽  
P. Zieger ◽  
G. Wehrle ◽  
A. Jefferson ◽  
J. A. Ogren ◽  
...  

Abstract. Relative humidity (RH) influences the water content of aerosol particles and therefore has an important impact on the particles' ability to scatter visible light. The RH dependence of the particle light scattering coefficient (σsp) is therefore an important measure for climate forcing calculations. We built a humidification system for a nephelometer which allows the measurement of σsp at a defined RH in the range of 40–90%. This RH conditioner consists of a humidifier followed by a dryer, which enables us to measure the hysteresis behavior of deliquescent aerosol particles. In this paper we present the set-up of a new humidified nephelometer, a detailed characterization with well defined laboratory generated aerosols, and a first application in the field by comparing our instrument to another humidified nephelometer. Monodisperse ammonium sulfate and sodium chloride particles were measured at four different dry particle sizes. Agreement between measurement and prediction based on Mie theory was found for both σsp and f(RH)=σsp(RH)/σsp(dry) within the range of uncertainty. The two humidified nephelometers measuring at a rural site in the Black Forest (Germany) often detected different f(RH), probably caused by the aerosol hysteresis behavior: when the aerosol was metastable, therefore was scattering more light, only one instrument detected the higher f(RH).


2010 ◽  
Vol 10 (2) ◽  
pp. 3659-3698 ◽  
Author(s):  
P. Zieger ◽  
R. Fierz-Schmidhauser ◽  
M. Gysel ◽  
J. Ström ◽  
S. Henne ◽  
...  

Abstract. Aerosol particles experience hygroscopic growth in the ambient atmosphere. Their optical properties – especially the aerosol light scattering – are therefore strongly dependent on the ambient relative humidity (RH). In-situ light scattering measurements of long-term observations are usually performed under dry conditions (RH<30–40%). The knowledge of this RH effect is of eminent importance for climate forcing calculations or for the comparison of remote sensing with in-situ measurements. This study combines measurements and model calculations to describe the RH effect on aerosol light scattering for the first time of aerosol particles present in summer and fall at the high Arctic. For this purpose, a field campaign was carried out from July to October 2008 at the Zeppelin station in Ny-Ålesund, Svalbard. The aerosol light scattering coefficient σsp(λ) was measured at three distinct wavelengths (λ=450, 550, and 700 nm) at dry and at various, predefined RH conditions between 20% and 95% with a recently developed humidified nephelometer (WetNeph) and with a second nephelometer measuring at dry conditions (DryNeph). In addition, the aerosol size distribution and the aerosol absorption coefficient were measured. The scattering enhancement factor f(RH,λ) is the key parameter to describe the RH effect on σsp(λ) and is defined as the RH dependent σsp(RH,λ) divided by the corresponding dry σsp(RHdry,λ). During our campaign the average f(RH=85%, λ=550 nm) was 3.24±0.63 (mean ± standard deviation), and no clear wavelength dependence of f(RH,λ) was observed. This means that the ambient scattering coefficients at RH=85% were on average about three times higher than the dry measured in-situ scattering coefficients. The RH dependency of the recorded f(RH,λ) can be well described by an empirical one-parameter equation. We used a simplified method to retrieve an apparent hygroscopic growth factor g, defined as the aerosol particle diameter at a certain RH divided by the dry diameter, using the WetNeph, the DryNeph, the aerosol size distribution measurements and Mie theory. With this approach we found on average for g values of 1.61±0.12 (mean ± standard deviation). No clear seasonal shift of f(RH,λ) was observed during the 3-month period, while aerosol properties (size and chemical composition) clearly changed with time. While the beginning of the campaign was mainly characterized by smaller and less hygroscopic particles, the end was dominated by larger and more hygroscopic particles. This suggests that compensating effects of hygroscopicity and size determined the temporal stability of f(RH,λ). During sea salt influenced periods, distinct deliquescence transitions were observed. At the end we give a method on how to transfer the dry in-situ measured aerosol scattering coefficients to ambient values for the aerosol measured during summer and fall at this location.


2010 ◽  
Vol 3 (1) ◽  
pp. 39-50 ◽  
Author(s):  
R. Fierz-Schmidhauser ◽  
P. Zieger ◽  
G. Wehrle ◽  
A. Jefferson ◽  
J. A. Ogren ◽  
...  

Abstract. Relative humidity (RH) influences the water content of aerosol particles and therefore has an important impact on the particles' ability to scatter visible light. The RH dependence of the particle light scattering coefficient (σsp is therefore an important measure for climate forcing calculations. We built a humidification system for a nephelometer which allows the measurement of σsp at a defined RH in the range of 40–90%. This RH conditioner consists of a humidifier followed by a dryer, which enables us to measure the hysteresis behavior of deliquescent aerosol particles. In this paper we present the set-up of a new humidified nephelometer, a detailed characterization with well defined laboratory generated aerosols, and a first application in the field by comparing our instrument to another humidified nephelometer. Monodisperse ammonium sulfate and sodium chloride particles were measured at four different dry particle sizes. Agreement between measurement and prediction based on Mie theory was found for both σsp and f(RH)=σsp(RH)/σsp(dry) within the range of uncertainty. The two humidified nephelometers measuring at a rural site in the Black Forest (Germany) often detected different f(RH), probably caused by the aerosol hysteresis behavior: when the aerosol was metastable, therefore was scattering more light, only one instrument detected the higher f(RH).


2016 ◽  
Author(s):  
Sara D. Forestieri ◽  
Gavin C. Cornwell ◽  
Taylor M. Helgestad ◽  
Kathryn A. Moore ◽  
Christopher Lee ◽  
...  

Abstract. The extent to which water uptake influences the light scattering ability of marine sea spray aerosol (SSA) particles depends critically on SSA chemical composition. The organic fraction of SSA can increase during phytoplankton blooms, decreasing the salt content and therefore the hygroscopicity of the particles. In this study, subsaturated hygroscopic growth factors at 85 % relative humidity (GF(85 %)) of SSA particles were quantified during two induced phytoplankton blooms in marine aerosol reference tanks (MARTs). One MART was illuminated with fluorescent lights and the other was illuminated with sunlight, referred to as the "indoor" and "outdoor" MARTs, respectively. GF(85 %) values for SSA particles were derived from measurements of light scattering and particle size distributions, concurrently with online single particle and bulk aerosol composition measurements. During both microcosm experiments, the observed bulk average GF(85 %) values were depressed substantially relative to pure, inorganic sea salt, by 10 to 19 %, with a one (indoor MART) and six (outdoor MART) day lag between GF(85 %) depression and the peak chlorophyll-a concentrations. The fraction of organiccontaining SSA particles generally increased after the peak of the phytoplankton blooms. The GF(85 %) values were inversely correlated with the fraction of particles containing organic or other biological markers. This indicates these particles were less hygroscopic than the particles identified as predominately sea salt containing and demonstrates a clear relationship between SSA particle composition and the sensitivity of light scattering to variations in relative humidity. The implications of these observations to the direct climate effects of SSA particles are discussed.


Micromachines ◽  
2021 ◽  
Vol 12 (4) ◽  
pp. 466
Author(s):  
Aimable Kalume ◽  
Chuji Wang ◽  
Yongle Pan

We present a broad assessment on the studies of optically-trapped single airborne aerosol particles, particularly chemical aerosol particles, using laser technologies. To date, extensive works have been conducted on ensembles of aerosols as well as on their analogous bulk samples, and a decent general description of airborne particles has been drawn and accepted. However, substantial discrepancies between observed and expected aerosols behavior have been reported. To fill this gap, single-particle investigation has proved to be a unique intersection leading to a clear representation of microproperties and size-dependent comportment affecting the overall aerosol behavior, under various environmental conditions. In order to achieve this objective, optical-trapping technologies allow holding and manipulating a single aerosol particle, while offering significant advantages such as contactless handling, free from sample collection and preparation, prevention of contamination, versatility to any type of aerosol, and flexibility to accommodation of various analytical systems. We review spectroscopic methods that are based on the light-particle interaction, including elastic light scattering, light absorption (cavity ring-down and photoacoustic spectroscopies), inelastic light scattering and emission (Raman, laser-induced breakdown, and laser-induced fluorescence spectroscopies), and digital holography. Laser technologies offer several benefits such as high speed, high selectivity, high accuracy, and the ability to perform in real-time, in situ. This review, in particular, discusses each method, highlights the advantages and limitations, early breakthroughs, and recent progresses that have contributed to a better understanding of single particles and particle ensembles in general.


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