scholarly journals High humidity tandem differential mobility analyzer for accurate determination of aerosol hygroscopic growth, microstructure and activity coefficients over a wide range of relative humidity

2019 ◽  
Author(s):  
Eugene F. Mikhailov ◽  
Sergey S. Vlasenko
Keyword(s):  
Growth Factors ◽  
Relative Humidity ◽  
Activity Coefficients ◽  
Aerosol Particles ◽  
Accurate Determination ◽  
Spherical Shape ◽  
High Humidity ◽  
Optimal Parameters ◽  
Hygroscopic Growth ◽  
Wide Range

Abstract. Interactions with water are crucial for the properties, transformation and climate effects of atmospheric aerosols. Here we present high humidity tandem differential hygroscopicity analyzer (HHTDMA) and a new method to measure the hygroscopic growth of aerosol particles with in-situ restructuring to minimize the influence of particle shape. With this approach, growth factors can be measured with an uncertainty 0.3–0.9 % over a relative humidity (RH) range of 2–99.6 % and with an RH measurement accuracy better than 0.4 %. The HHTDMA instrument can be used in hydration, dehydration and restructuring modes of operation. The restructuring mode allows to investigate the effects of drying conditions on the initial microstructure of aerosol particles and specified the optimal parameters that provide their rearrangements into compact structures with near-spherical shape. These optimal parameters were then used in hygroscopic growth experiments by combining restructuring mode with conventional hydration or dehydration mode. The tandem of two modes allowed us to measure the particle growth factors with high precision as well as to determine the thickness of the water adsorption layer on the surface of compact crystalline particles. To verify HHTDMA instrument we compared the measured ammonium sulfate growth factors with these obtained from E-AIM-based Köhler model. Averaged over the range of 38–96 % RH, the mean relative deviations between measurement and model results is less than 0.5 %. We demonstrate this precision by presenting data for glucose for which bulk thermodynamic coefficients are available. The HHTDMA-derived activity coefficients of water and glucose were obtained for both dilute and supersaturated solutions and are in a good agreement with these reported in literature. Averaged deviation between the measured activity coefficients and these obtained by bulk method is less than 4 %. For dilute solution in water activity range of 0.98–0.99 the hygroscopicity parameter of glucose and molal osmotic coefficient were obtained with uncertainty of 0.4 % and 2.5 %, respectively.

scholarly journals High-humidity tandem differential mobility analyzer for accurate determination of aerosol hygroscopic growth, microstructure, and activity coefficients over a wide range of relative humidity

2020 ◽  
Vol 13 (4) ◽  
pp. 2035-2056 ◽  
Author(s):  
Eugene F. Mikhailov ◽  
Sergey S. Vlasenko
Keyword(s):  
Growth Factors ◽  
Relative Humidity ◽  
Activity Coefficients ◽  
Aerosol Particles ◽  
Accurate Determination ◽  
High Humidity ◽  
Optimal Parameters ◽  
Hygroscopic Growth ◽  
Average Deviation ◽  
Wide Range

Abstract. Interactions with water are crucial for the properties, transformation, and climate effects of atmospheric aerosols. Here we present the high-humidity tandem differential hygroscopicity analyzer (HHTDMA) and a new method to measure the hygroscopic growth of aerosol particles with in situ restructuring to minimize the influence of particle shape. With this approach, growth factors can be measured with an uncertainty of 0.3 %–0.9 % over a relative humidity (RH) range of 2 %–99.6 % and with an RH measurement accuracy better than 0.4 %. The HHTDMA instrument can be used in hydration, dehydration, and restructuring modes of operation. The restructuring mode allows us to investigate the effects of drying conditions on the initial microstructure of aerosol particles and specifies the optimal parameters that provide their rearrangements into compact structures with a nearly spherical shape. These optimal parameters were used in hygroscopic growth experiments by combining the restructuring mode with a conventional hydration or dehydration mode. The tandem of two modes allowed us to measure the particle growth factors with high precision as well as to determine the thickness of the water adsorption layer on the surface of compact crystalline particles. To verify the HHTDMA instrument we compared the measured ammonium sulfate growth factors with those obtained from the E-AIM-based Köhler model (E-AIM: Extended Aerosol Inorganics Model). Averaged over the range of 38 %–96 % RH, the mean relative deviations between measurements and model results is less than 0.5 %. We demonstrate this precision by presenting data for glucose, for which bulk thermodynamic coefficients are available. The HHTDMA-derived activity coefficients of water and glucose were obtained for both dilute and supersaturated solutions and are in good agreement with those reported in the literature. The average deviation between the measured activity coefficients and those obtained by the bulk method is less than 4 %. For dilute solution in water with an activity range of 0.98–0.99, the hygroscopicity parameter of glucose and the molal osmotic coefficient were obtained with an uncertainty of 0.4 % and 2.5 %, respectively.

scholarly journals MOPSMAP v0.9: A versatile tool for modeling of aerosol optical properties

2018 ◽  
Author(s):  
Josef Gasteiger ◽  
Matthias Wiegner
Keyword(s):  
Remote Sensing ◽  
Optical Properties ◽  
Aerosol Particles ◽  
Particle Orientation ◽  
Spherical Particles ◽  
Refractive Indices ◽  
Hygroscopic Growth ◽  
Web Interface ◽  
Optical Modeling ◽  
Wide Range

Abstract. The spatiotemporal distribution and characterization of aerosol particles are usually determined by remote sensing and optical in-situ measurements. These measurements are indirect with respect to microphysical properties and thus inversion techniques are required to determine the aerosol microphysics. Scattering theory provides the link between microphysical and optical properties; it is not only needed for such inversions but also for radiative budget calculations and climate modeling. However, optical modeling can be very time consuming, in particular if non-spherical particles or complex ensembles are involved. In this paper we present the MOPSMAP package (modeled optical properties of ensembles of aerosol particles) which is computationally fast for optical modeling even in case of complex aerosols. The package consists of a data set of pre-calculated optical properties of single aerosol particles, a Fortran program to calculate the properties of user-defined aerosol ensembles, and a user-friendly web interface for online calculations. Spheres, spheroids, and a small set of irregular particle shapes are considered over a wide range of sizes and refractive indices. MOPSMAP provides the fundamental optical properties assuming random particle orientation, including the scattering matrix for the selected wavelengths. Moreover, the output includes tables of frequently used properties such as the single scattering albedo, the asymmetry parameter or the lidar ratio. To demonstrate the wide range of possible MOPSMAP applications a selection of examples is presented, e.g., dealing with hygroscopic growth, mixtures of absorbing and non-absorbing particles, the relevance of the size equivalence in case of non-spherical particles, and the variability of volcanic ash microphysics. The web interface is designed to be intuitive for expert and non-expert users. To support users a large set of default settings is available, e.g., several wavelength-dependent refractive indices, climatologically representative size distributions, and a parameterization of hygroscopic growth. Calculations are possible for single wavelengths or user-defined sets (e.g., of specific remote sensing application). For expert users more options for the microphysics are available. Plots for immediate visualization of the results are shown. The complete output can be downloaded for further applications. All input parameters and results are stored in the user’s personal folder so that calculations can easily be reproduced. The MOPSMAP package is available on request for offline calculations, e.g., when large numbers of different runs for sensitivity studies shall be made.

scholarly journals Accurate Measurements of Aerosol Hygroscopic Growth over a Wide Range in Relative Humidity

2016 ◽  
Vol 120 (25) ◽  
pp. 4376-4388 ◽  
Author(s):  
Grazia Rovelli ◽  
Rachael E. H. Miles ◽  
Jonathan P. Reid ◽  
Simon L. Clegg
Keyword(s):  
Relative Humidity ◽  
Hygroscopic Growth ◽  
Wide Range

Hygroscopic Growth of Multicomponent Aerosol Particles Influenced by Several Cycles of Relative Humidity

2008 ◽  
Vol 112 (11) ◽  
pp. 2378-2385 ◽  
Author(s):  
Thomas Rosenoern ◽  
Julie C. Schlenker ◽  
Scot T. Martin
Keyword(s):  
Relative Humidity ◽  
Aerosol Particles ◽  
Hygroscopic Growth

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

2010 ◽  
Vol 10 (8) ◽  
pp. 3875-3890 ◽  
Author(s):  
P. Zieger ◽  
R. Fierz-Schmidhauser ◽  
M. Gysel ◽  
J. Ström ◽  
S. Henne ◽  
...  
Keyword(s):  
Standard Deviation ◽  
Light Scattering ◽  
Relative Humidity ◽  
Aerosol Particles ◽  
Aerosol Size Distribution ◽  
Hygroscopic Growth ◽  
Scattering Coefficients ◽  
Dry Conditions ◽  
Hygroscopic Particles

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.

scholarly journals Optical particle counter measurement of marine aerosol hygroscopic growth

2007 ◽  
Vol 7 (4) ◽  
pp. 12381-12415 ◽  
Author(s):  
J. R. Snider ◽  
M. D. Petters
Keyword(s):  
Growth Factors ◽  
Relative Humidity ◽  
Scattered Light ◽  
Particle Diameter ◽  
Mie Scattering ◽  
Size Spectrum ◽  
Hygroscopic Growth ◽  
Marine Stratocumulus ◽  
Ambient Relative Humidity ◽  
Light Scattering Detection

Abstract. A technique is developed for the determination of the hygroscopic growth factor of dry particles with diameter between 0.3 and 0.6 µm and is applied to measurements made during the second Dynamics and Chemistry of Marine Stratocumulus experiment. Two optical particle counters are utilized, one measures the aerosol size spectrum at ambient relative humidity and the other simultaneously dries the aerosol prior to light scattering detection. Growth factors are based on measurements made in the region of the Mie scattering curve where scattered light intensity increases monotonically with dry and wet particle diameter, i.e. D<0.9 µm. Factors influencing the accuracy of the measurement are evaluated, including particle drying, refractive index and shape. Growth factors at 90±3% ambient relative humidity in marine airmasses 400 km west of San Diego, California range between 1.5 and 1.8. This suggests that a significant fraction of the particle mass, between 40 and 70%, is either non-hygroscopic or weakly hygroscopic.

scholarly journals Effect of mixing structure on the water uptake of mixtures of ammonium sulfate and phthalic acid particles

2021 ◽  
Vol 21 (3) ◽  
pp. 2179-2190
Author(s):  
Weigang Wang ◽  
Ting Lei ◽  
Andreas Zuend ◽  
Hang Su ◽  
Yafang Cheng ◽  
...  
Keyword(s):  
Growth Factor ◽  
Relative Humidity ◽  
Water Uptake ◽  
Phthalic Acid ◽  
Aerosol Particles ◽  
Core Shell ◽  
Hygroscopic Growth ◽  
The Core ◽  
Mass Fractions ◽  
Mixing States

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.

scholarly journals MOPSMAP v1.0: a versatile tool for the modeling of aerosol optical properties

2018 ◽  
Vol 11 (7) ◽  
pp. 2739-2762 ◽  
Author(s):  
Josef Gasteiger ◽  
Matthias Wiegner
Keyword(s):  
Optical Properties ◽  
Aerosol Particles ◽  
Fortran Program ◽  
Refractive Indices ◽  
Nonspherical Particles ◽  
Hygroscopic Growth ◽  
Web Interface ◽  
Data Set ◽  
Optical Modeling ◽  
Wide Range

Abstract. The spatiotemporal distribution and characterization of aerosol particles are usually determined by remote-sensing and optical in situ measurements. These measurements are indirect with respect to microphysical properties, and thus inversion techniques are required to determine the aerosol microphysics. Scattering theory provides the link between microphysical and optical properties; it is not only needed for such inversions but also for radiative budget calculations and climate modeling. However, optical modeling can be very time-consuming, in particular if nonspherical particles or complex ensembles are involved. In this paper we present the MOPSMAP package (Modeled optical properties of ensembles of aerosol particles), which is computationally fast for optical modeling even in the case of complex aerosols. The package consists of a data set of pre-calculated optical properties of single aerosol particles, a Fortran program to calculate the properties of user-defined aerosol ensembles, and a user-friendly web interface for online calculations. Spheres, spheroids, and a small set of irregular particle shapes are considered over a wide range of sizes and refractive indices. MOPSMAP provides the fundamental optical properties assuming random particle orientation, including the scattering matrix for the selected wavelengths. Moreover, the output includes tables of frequently used properties such as the single-scattering albedo, the asymmetry parameter, or the lidar ratio. To demonstrate the wide range of possible MOPSMAP applications, a selection of examples is presented, e.g., dealing with hygroscopic growth, mixtures of absorbing and non-absorbing particles, the relevance of the size equivalence in the case of nonspherical particles, and the variability in volcanic ash microphysics. The web interface is designed to be intuitive for expert and nonexpert users. To support users a large set of default settings is available, e.g., several wavelength-dependent refractive indices, climatologically representative size distributions, and a parameterization of hygroscopic growth. Calculations are possible for single wavelengths or user-defined sets (e.g., of specific remote-sensing application). For expert users more options for the microphysics are available. Plots for immediate visualization of the results are shown. The complete output can be downloaded for further applications. All input parameters and results are stored in the user's personal folder so that calculations can easily be reproduced. The web interface is provided at https://mopsmap.net (last access: 9 July 2018) and the Fortran program including the data set is freely available for offline calculations, e.g., when large numbers of different runs for sensitivity studies are to be made.

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