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
2012 ◽  
Vol 12 (12) ◽  
pp. 5429-5446 ◽  
Author(s):  
S. Metzger ◽  
B. Steil ◽  
L. Xu ◽  
J. E. Penner ◽  
J. Lelieveld

Abstract. Water activity is a key factor in aerosol thermodynamics and hygroscopic growth. We introduce a new representation of water activity (aw), which is empirically related to the solute molality (μs) through a single solute specific constant, νi. Our approach is widely applicable, considers the Kelvin effect and covers ideal solutions at high relative humidity (RH), including cloud condensation nuclei (CCN) activation. It also encompasses concentrated solutions with high ionic strength at low RH such as the relative humidity of deliquescence (RHD). The constant νi can thus be used to parameterize the aerosol hygroscopic growth over a wide range of particle sizes, from nanometer nucleation mode to micrometer coarse mode particles. In contrast to other aw-representations, our νi factor corrects the solute molality both linearly and in exponent form x · ax. We present four representations of our basic aw-parameterization at different levels of complexity for different aw-ranges, e.g. up to 0.95, 0.98 or 1. νi is constant over the selected aw-range, and in its most comprehensive form, the parameterization describes the entire aw range (0–1). In this work we focus on single solute solutions. νi can be pre-determined with a root-finding method from our water activity representation using an aw−μs data pair, e.g. at solute saturation using RHD and solubility measurements. Our aw and supersaturation (Köhler-theory) results compare well with the thermodynamic reference model E-AIM for the key compounds NaCl and (NH4)2SO4 relevant for CCN modeling and calibration studies. Envisaged applications include regional and global atmospheric chemistry and climate modeling.


2020 ◽  
Vol 13 (4) ◽  
pp. 2035-2056 ◽  
Author(s):  
Eugene F. Mikhailov ◽  
Sergey S. Vlasenko

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.


2019 ◽  
Author(s):  
Eugene F. Mikhailov ◽  
Sergey S. Vlasenko

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.


2011 ◽  
Vol 11 (9) ◽  
pp. 24813-24855 ◽  
Author(s):  
S. Metzger ◽  
B. Steil ◽  
L. Xu ◽  
J. E. Penner ◽  
J. Lelieveld

Abstract. Water is a main component of atmospheric aerosols and its amount depends on the particle chemical composition. We introduce a new parameterization for the aerosol hygroscopic growth factor (HGF), based on an empirical relation between water activity (aw) and solute molality (μs) through a single solute specific coefficient νi. Three main advantages are: (1) wide applicability, (2) simplicity and (3) analytical nature. (1) Our approach considers the Kelvin effect and covers ideal solutions at large relative humidity (RH), including CCN activation, as well as concentrated solutions with high ionic strength at low RH such as the relative humidity of deliquescence (RHD). (2) A single νi coefficient suffices to parameterize the HGF for a wide range of particle sizes, from nanometer nucleation mode to micrometer coarse mode particles. (3) In contrast to previous methods, our analytical aw parameterization depends not only on a linear correction factor for the solute molality, instead νi also appears in the exponent in form x · ax. According to our findings, νi can be assumed constant for the entire aw range (0–1). Thus, the νi based method is computationally efficient. In this work we focus on single solute solutions, where νi is pre-determined with the bisection method from our analytical equations using RHD measurements and the saturation molality μssat. The computed aerosol HGF and supersaturation (Köhler-theory) compare well with the results of the thermodynamic reference model E-AIM for the key compounds NaCl and (NH4)2SO4 relevant for CCN modeling and calibration studies. The equations introduced here provide the basis of our revised gas-liquid-solid partitioning model, i.e. version 4 of the EQuilibrium Simplified Aerosol Model (EQSAM4), described in a companion paper.


Sensors ◽  
2021 ◽  
Vol 21 (10) ◽  
pp. 3338
Author(s):  
Ivan Vajs ◽  
Dejan Drajic ◽  
Nenad Gligoric ◽  
Ilija Radovanovic ◽  
Ivan Popovic

Existing government air quality monitoring networks consist of static measurement stations, which are highly reliable and accurately measure a wide range of air pollutants, but they are very large, expensive and require significant amounts of maintenance. As a promising solution, low-cost sensors are being introduced as complementary, air quality monitoring stations. These sensors are, however, not reliable due to the lower accuracy, short life cycle and corresponding calibration issues. Recent studies have shown that low-cost sensors are affected by relative humidity and temperature. In this paper, we explore methods to additionally improve the calibration algorithms with the aim to increase the measurement accuracy considering the impact of temperature and humidity on the readings, by using machine learning. A detailed comparative analysis of linear regression, artificial neural network and random forest algorithms are presented, analyzing their performance on the measurements of CO, NO2 and PM10 particles, with promising results and an achieved R2 of 0.93–0.97, 0.82–0.94 and 0.73–0.89 dependent on the observed period of the year, respectively, for each pollutant. A comprehensive analysis and recommendations on how low-cost sensors could be used as complementary monitoring stations to the reference ones, to increase spatial and temporal measurement resolution, is provided.


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.


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.


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