scholarly journals Effects of relative humidity on aerosol light scattering in the Arctic

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 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.


2014 ◽  
Vol 14 (6) ◽  
pp. 7067-7111 ◽  
Author(s):  
N. Rastak ◽  
S. Silvergren ◽  
P. Zieger ◽  
U. Wideqvist ◽  
J. Ström ◽  
...  

Abstract. In this study we investigated the impact of water uptake by aerosol particles in ambient atmosphere on their optical properties and their direct radiative effect (ADRE, W m−2) in the Arctic at Ny-Ålesund, Svalbard, during 2008. To achieve this, we combined three models, a hygroscopic growth model, Mie model and a radiative transfer model, with an extensive set of observational data. We found that the seasonal variation of dry aerosol scattering coefficients showed minimum values during the summer season and the beginning of fall (July, August and September), when small particles (< 100 nm in diameter) dominate the aerosol size distribution. The maximum scattering by dry particles was observed during Arctic haze period (March, April and May) when average size of the particles was larger. Considering the hygroscopic growth of aerosol particles in the ambient atmosphere had a significant impact on the aerosol scattering coefficients: the aerosol scattering coefficients were enhanced by on average a factor of 4.30 ± 2.26 (mean ± standard deviation), with lower values during the haze period (March, April, May) as compared to summer and fall. Hygroscopic growth of aerosol particles was found to cause 1.6 to 3.7 times more negative ADRE on the surface, with the smallest effect during the haze period (March, April and May) and the highest during late summer and beginning of fall (July, August and September).


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.


2021 ◽  
Author(s):  
Maria Ángeles Burgos Simón ◽  
Elisabeth Andrews ◽  
Gloria Titos ◽  
Angela Benedetti ◽  
Huisheng Bian ◽  
...  

&lt;p&gt;The particle hygroscopic growth impacts the optical properties of aerosols and, in turn, affects the aerosol-radiation interaction and calculation of the Earth&amp;#8217;s radiative balance. The dependence of particle light scattering on relative humidity (RH) can be described by the scattering enhancement factor f(RH), defined as the ratio between the particle light scattering coefficient at a given RH divided by its dry value.&lt;/p&gt;&lt;p&gt;The first effort of the AeroCom Phase III &amp;#8211; INSITU experiment was to develop an observational dataset of scattering enhancement values at 26 sites to study the uptake of water by atmospheric aerosols, and evaluate f(RH) globally (Burgos et al., 2019). Model outputs from 10 Earth System Models (CAM, CAM-ATRAS, CAM-Oslo, GEOS-Chem, GEOS-GOCART, MERRAero, TM5, OsloCTM3, IFS-AER, and ECMWF) were then evaluated against this in-situ dataset. Building on these results, we investigate f(RH) in the context of other aerosol optical and chemical properties, making use of the same 10 Earth System Models (ESMs) and in-situ measurements as in Burgos et al. (2020) and Titos et al. (2021).&lt;/p&gt;&lt;p&gt;Given the difficulties of deploying and maintaining instrumentation for long-term, accurate and comprehensive f(RH) observations, it is desirable to find an observational proxy for f(RH). This observation-based proxy would also need to be reproduced in modelling space. Our aim here is to evaluate how ESMs currently represent the relationship between f(RH), scattering &amp;#197;ngstr&amp;#246;m exponent (SAE), and single scattering albedo (SSA). This work helps to identify current challenges in modelling water-uptake by aerosols and their impact on aerosol optical properties within Earth system models.&lt;/p&gt;&lt;p&gt;We start by analyzing the behavior of SSA with RH, finding the expected increase with RH for all site types and models. Then, we analyze the three variables together (f(RH)-SSA-SAE relationship). Results show that hygroscopic particles tend to be bigger and scatter more than non-hygroscopic small particles, though variability within models is noticeable. This relationship can be further studied by relating SAE to model chemistry, by selecting those grid points dominated by a single chemical component (mass mixing ratios &gt; 90%). Finally, we analyze model performance at three specific sites representing different aerosol types: Arctic, marine and rural. At these sites, the model data can be exactly temporally and spatially collocated with the observations, which should help to identify the models which exhibit better agreement with measurements and for which aerosol type.&lt;/p&gt;&lt;p&gt;&amp;#160;&lt;/p&gt;&lt;p&gt;Burgos, M.A.&amp;#160;et al.:&amp;#160;A global view on the effect of water uptake on aerosol particle light scattering.&amp;#160;Sci Data&amp;#160;6,&amp;#160;157. https://doi.org/10.1038/s41597-019-0158-7, 2019.&lt;/p&gt;&lt;p&gt;Burgos, M.A. et al.: A global model&amp;#8211;measurement evaluation of particle light scattering coefficients at elevated relative humidity, Atmos. Chem. Phys., 20, 10231&amp;#8211;10258, https://doi.org/10.5194/acp-20-10231-2020, 2020.&lt;/p&gt;&lt;p&gt;Titos, G. et al.: A global study of hygroscopicity-driven light scattering enhancement in the context of other in-situ aerosol optical properties, Atmos. Chem. Phys. Discuss. [preprint], https://doi.org/10.5194/acp-2020-1250, in review, 2020.&lt;/p&gt;


2018 ◽  
Vol 18 (10) ◽  
pp. 7001-7017 ◽  
Author(s):  
Andrés Esteban Bedoya-Velásquez ◽  
Francisco Navas-Guzmán ◽  
María José Granados-Muñoz ◽  
Gloria Titos ◽  
Roberto Román ◽  
...  

Abstract. This study focuses on the analysis of aerosol hygroscopic growth during the Sierra Nevada Lidar AerOsol Profiling Experiment (SLOPE I) campaign by using the synergy of active and passive remote sensors at the ACTRIS Granada station and in situ instrumentation at a mountain station (Sierra Nevada, SNS). To this end, a methodology based on simultaneous measurements of aerosol profiles from an EARLINET multi-wavelength Raman lidar (RL) and relative humidity (RH) profiles obtained from a multi-instrumental approach is used. This approach is based on the combination of calibrated water vapor mixing ratio (r) profiles from RL and continuous temperature profiles from a microwave radiometer (MWR) for obtaining RH profiles with a reasonable vertical and temporal resolution. This methodology is validated against the traditional one that uses RH from co-located radiosounding (RS) measurements, obtaining differences in the hygroscopic growth parameter (γ) lower than 5 % between the methodology based on RS and the one presented here. Additionally, during the SLOPE I campaign the remote sensing methodology used for aerosol hygroscopic growth studies has been checked against Mie calculations of aerosol hygroscopic growth using in situ measurements of particle number size distribution and submicron chemical composition measured at SNS. The hygroscopic case observed during SLOPE I showed an increase in the particle backscatter coefficient at 355 and 532 nm with relative humidity (RH ranged between 78 and 98 %), but also a decrease in the backscatter-related Ångström exponent (AE) and particle linear depolarization ratio (PLDR), indicating that the particles became larger and more spherical due to hygroscopic processes. Vertical and horizontal wind analysis is performed by means of a co-located Doppler lidar system, in order to evaluate the horizontal and vertical dynamics of the air masses. Finally, the Hänel parameterization is applied to experimental data for both stations, and we found good agreement on γ measured with remote sensing (γ532=0.48±0.01 and γ355=0.40±0.01) with respect to the values calculated using Mie theory (γ532=0.53±0.02 and γ355=0.45±0.02), with relative differences between measurements and simulations lower than 9 % at 532 nm and 11 % at 355 nm.


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.


2008 ◽  
Vol 112 (11) ◽  
pp. 2378-2385 ◽  
Author(s):  
Thomas Rosenoern ◽  
Julie C. Schlenker ◽  
Scot T. Martin

2020 ◽  
Author(s):  
Paolo Laj ◽  
Clémence Rose ◽  
Alessandro Bigi ◽  
Martine Collaud Coen ◽  
Elisabeth Andrews ◽  
...  

&lt;p&gt;Aerosol particles are essential constituents of the Earth&amp;#8217;s atmosphere, impacting the earth radiation balance directly by scattering and absorbing solar radiation, and indirectly by acting as cloud condensation nuclei. In contrast to most greenhouse gases, aerosol particles have short atmospheric residence time resulting in a highly heterogeneous distribution in space and time. There is a clear need to document this variability at regional scale through observations involving, in particular, the in-situ near-surface segment of the atmospheric observations system. This paper will provide the widest effort so far to document variability of climate-relevant in-situ aerosol properties (namely wavelength dependent particle light scattering and absorption coefficients, particle number concentration and particle number size distribution) from all sites connected to the Global Atmosphere Watch network. High quality data from more than 90 stations worldwide have been collected and controlled for quality and are reported for a reference year in 2017, providing a very extended and robust view of the variability of these variables worldwide. The range of variability observed worldwide for light scattering and absorption coefficients, single scattering albedo and particle number concentration are presented together with preliminary information on their long-term trends and comparison with model simulation for the different stations. The scope of the present paper is also to provide the necessary suite of information including data provision procedures, quality control and analysis, data policy and usage of the ground-based aerosol measurements network. It delivers to users of the World Data Centre on Aerosol, the required confidence in data products in the form of a fully-characterized value chain, including uncertainty estimation and requirements for contributing to the global climate monitoring system.&lt;/p&gt;


2021 ◽  
Vol 21 (3) ◽  
pp. 2179-2190
Author(s):  
Weigang Wang ◽  
Ting Lei ◽  
Andreas Zuend ◽  
Hang Su ◽  
Yafang Cheng ◽  
...  

Abstract. Aerosol mixing state regulates the interactions between water molecules and particles and thus controls aerosol activation and hygroscopic growth, which thereby influences visibility degradation, cloud formation, and its radiative forcing. There are, however, few current studies on the mixing structure effects on aerosol hygroscopicity. Here, we investigated the hygroscopicity of ammonium sulfate / phthalic acid (AS / PA) aerosol particles with different mass fractions of PA in different mixing states in terms of initial particle generation. Firstly, the effect of PA coatings on the hygroscopic behavior of the core-shell-generated mixtures of AS with PA was studied using a coating hygroscopicity tandem differential mobility analyzer (coating HTDMA). The slow increase in the hygroscopic growth factor of core-shell-generated particles is observed with increasing thickness of the coating PA prior to the deliquescence relative humidity (DRH) of AS. At relative humidity (RH) above 80 %, a decrease in the hygroscopic growth factor of particles occurs as the thickness of the PA shell increases, which indicates that the increase of PA mass fractions leads to a reduction of the overall core-shell-generated particle hygroscopicity. In addition, the use of the Zdanovskii–Stokes–Robinson (ZSR) relation leads to the underestimation of the measured growth factors of core-shell-generated particles without consideration of the morphological effect of core-shell-generated particles, especially at higher RH. Secondly, in the case of the AS / PA initially well-mixed particles, a shift of the DRH of AS (∼80 %, Tang and Munkelwitz, 1994) to lower RH is observed due to the presence of PA in the initially well-mixed particles. The predicted hygroscopic growth factor using the ZSR relation is consistent with the measured hygroscopic growth factor of the initially well-mixed particles. Moreover, we compared and discussed the influence of mixing states on the water uptake of AS / PA aerosol particles. It is found that the hygroscopic growth factor of the core-shell-generated particles is slightly higher than that of the initially well-mixed particles with the same mass fractions of PA at RH above 80 %. The observation of AS / PA particles may contribute to a growing field of knowledge regarding the influence of coating properties and mixing structure on water uptake.


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