scholarly journals Aerosol water parameterization: a single parameter framework

2015 ◽  
Vol 15 (22) ◽  
pp. 33493-33553
Author(s):  
S. Metzger ◽  
B. Steil ◽  
M. Abdelkader ◽  
K. Klingmüller ◽  
L. Xu ◽  
...  
Keyword(s):  
Ammonium Nitrate ◽  
Water Uptake ◽  
Climate Model ◽  
Mixed Solution ◽  
Hygroscopic Growth ◽  
Simple Method ◽  
Aerosol Model ◽  
Kohler Theory ◽  
Comprehensive Comparison ◽  
Term Evaluation

Abstract. We introduce a framework to efficiently parameterize the aerosol water uptake for mixtures of semi-volatile and non-volatile compounds, based on the coefficient, νi. This solute specific coefficient was introduced in Metzger et al. (2012) to accurately parameterize the single solution hygroscopic growth, considering the Kelvin effect – accounting for the water uptake of concentrated nanometer sized particles up to dilute solutions, i.e., from the compounds relative humidity of deliquescence (RHD) up to supersaturation (Köhler-theory). Here we extend the νi-parameterization from single to mixed solutions. We evaluate our framework at various levels of complexity, by considering the full gas-liquid-solid partitioning for a comprehensive comparison with reference calculations using the E-AIM, EQUISOLV II, ISORROPIA II models as well as textbook examples. We apply our parameterization in EQSAM4clim, the EQuilibrium Simplified Aerosol Model V4 for climate simulations, implemented in a box model and in the global chemistry-climate model EMAC. Our results show: (i) that the νi-approach enables to analytically solve the entire gas-liquid-solid partitioning and the mixed solution water uptake with sufficient accuracy, (ii) that, e.g., pure ammonium nitrate and mixed ammonium nitrate – ammonium sulfate mixtures can be solved with a simple method, and (iii) that the aerosol optical depth (AOD) simulations are in close agreement with remote sensing observations for the year 2005. Long-term evaluation of the EMAC results based on EQSAM4clim and ISORROPIA II will be presented separately.

scholarly journals Aerosol water parameterisation: a single parameter framework

2016 ◽  
Vol 16 (11) ◽  
pp. 7213-7237 ◽  
Author(s):  
Swen Metzger ◽  
Benedikt Steil ◽  
Mohamed Abdelkader ◽  
Klaus Klingmüller ◽  
Li Xu ◽  
...  
Keyword(s):  
Ammonium Nitrate ◽  
Water Uptake ◽  
Climate Model ◽  
Mixed Solution ◽  
Hygroscopic Growth ◽  
Simple Method ◽  
Aerosol Model ◽  
Kohler Theory ◽  
Comprehensive Comparison ◽  
Term Evaluation

Abstract. We introduce a framework to efficiently parameterise the aerosol water uptake for mixtures of semi-volatile and non-volatile compounds, based on the coefficient, νi. This solute-specific coefficient was introduced in Metzger et al. (2012) to accurately parameterise the single solution hygroscopic growth, considering the Kelvin effect – accounting for the water uptake of concentrated nanometer-sized particles up to dilute solutions, i.e. from the compounds relative humidity of deliquescence (RHD) up to supersaturation (Köhler theory). Here we extend the νi parameterisation from single to mixed solutions. We evaluate our framework at various levels of complexity, by considering the full gas–liquid–solid partitioning for a comprehensive comparison with reference calculations using the E-AIM, EQUISOLV II and ISORROPIA II models as well as textbook examples. We apply our parameterisation in the EQuilibrium Simplified Aerosol Model V4 (EQSAM4clim) for climate simulations, implemented in a box model and in the global chemistry–climate model EMAC. Our results show (i) that the νi approach enables one to analytically solve the entire gas–liquid–solid partitioning and the mixed solution water uptake with sufficient accuracy, (ii) that ammonium sulfate mixtures can be solved with a simple method, e.g. pure ammonium nitrate and mixed ammonium nitrate and (iii) that the aerosol optical depth (AOD) simulations are in close agreement with remote sensing observations for the year 2005. Long-term evaluation of the EMAC results based on EQSAM4clim and ISORROPIA II will be presented separately.

scholarly journals Aerosol water parameterization: long-term evaluation and importance for climate studies

2018 ◽  
Vol 18 (22) ◽  
pp. 16747-16774 ◽  
Author(s):  
Swen Metzger ◽  
Mohamed Abdelkader ◽  
Benedikt Steil ◽  
Klaus Klingmüller
Keyword(s):  
Water Uptake ◽  
Climate Model ◽  
Climate Modeling ◽  
Mixed Solution ◽  
Hygroscopic Growth ◽  
Computationally Efficient ◽  
Aerosol Model ◽  
Term Evaluation ◽  
Climate Studies

Abstract. We scrutinize the importance of aerosol water for the aerosol optical depth (AOD) calculations using a long-term evaluation of the EQuilibrium Simplified Aerosol Model v4 for climate modeling. EQSAM4clim is based on a single solute coefficient approach that efficiently parameterizes hygroscopic growth, accounting for aerosol water uptake from the deliquescence relative humidity up to supersaturation. EQSAM4clim extends the single solute coefficient approach to treat water uptake of multicomponent mixtures. The gas–aerosol partitioning and the mixed-solution water uptake can be solved analytically, preventing the need for iterations, which is computationally efficient. EQSAM4clim has been implemented in the global chemistry climate model EMAC and compared to ISORROPIA II on climate timescales. Our global modeling results show that (I) our EMAC results of the AOD are comparable to modeling results that have been independently evaluated for the period 2000–2010, (II) the results of various aerosol properties of EQSAM4clim and ISORROPIA II are similar and in agreement with AERONET and EMEP observations for the period 2000–2013, and (III) the underlying assumptions on the aerosol water uptake limitations are important for derived AOD calculations. Sensitivity studies of different levels of chemical aging and associated water uptake show larger effects on AOD calculations for the year 2005 compared to the differences associated with the application of the two gas–liquid–solid partitioning schemes. Overall, our study demonstrates the importance of aerosol water for climate studies.

scholarly journals Aerosol water parameterization: long-term evaluation and importance

2018 ◽  
Author(s):  
Swen Metzger ◽  
Mohamed Abdelkader ◽  
Benedikt Steil ◽  
Klaus Klingmüller
Keyword(s):  
Aerosol Optical Depth ◽  
Optical Depth ◽  
Water Uptake ◽  
Climate Model ◽  
Climate Modeling ◽  
Mixed Solution ◽  
Hygroscopic Growth ◽  
Aerosol Model ◽  
Term Evaluation

Abstract. We scrutinize the importance of aerosol water for the aerosol optical depth (AOD) calculations by a long-term evaluation of the EQuilibrium Simplified Aerosol Model V4 for climate modeling, which was introduced by Metzger et al. (2016a). EQSAM4clim is based on a sin-gle solute coefficient approach that efficiently parameterizes hygroscopic growth, account- ing for aerosol water uptake from the deliquescence relative humidity up to supersaturation. EQSAM4clim extends the single solute coefficient approach to treat water uptake of multi- component mixtures. The gas-aerosol partitioning and the mixed solution water uptake can be solved analytically, preventing the need for iterations, which is computationally efficient. EQSAM4clim has been implemented in the global chemistry climate model EMAC and com- pared to ISORROPIA II (Fountoukis and Nenes, 2007) at climate time-scales. Our global modeling results show that (I) our EMAC results of the aerosol optical depth (AOD) are comparable to independent results of Pozzer et al. (2015) for the period 2000–2010, (II) the results of various aerosol properties of EQSAM4clim and ISORROPIA II are similar and in agreement with AERONET and EMEP observations for the period 2000–2013, and (III) that the underlying assumptions on the aerosol water uptake limitations are important for derived AOD calculations. Sensitivity studies of different levels of chemical aging and associated water uptake show larger effects on AOD calculations for the year 2005 compared to the differences associated with the application of the two gas-liquid-solid partitioning schemes. Altogether, our study reveals the importance of the aerosol water for climate applications.

scholarly journals Description of EQSAM4: gas-liquid-solid partitioning model for global simulations

2011 ◽  
Vol 4 (4) ◽  
pp. 2791-2847 ◽  
Author(s):  
S. Metzger ◽  
B. Steil ◽  
L. Xu ◽  
J. E. Penner ◽  
J. Lelieveld
Keyword(s):  
Water Uptake ◽  
Atmospheric Aerosols ◽  
Atmospheric Chemistry ◽  
Large Scale ◽  
Climate Model ◽  
Reference Model ◽  
Climate Modeling ◽  
Box Model ◽  
Hygroscopic Growth ◽  
Aerosol Model

Abstract. We introduce version 4 of the EQuilibrium Simplified Aerosol Model (EQSAM4), which is part of our aerosol chemistry-microphysics module (GMXe) and chemistry-climate model (EMAC). We focus on the relative humidity of deliquescence (RHD) based water uptake of atmospheric aerosols, as this is important for atmospheric chemistry and climate modeling, e.g. to calculate the aerosol optical depth (AOD). Since the main EQSAM4 applications will involve large-scale, long-term and high-resolution atmospheric chemistry-climate modeling with EMAC, computational efficiency is an important requirement. EQSAM4 parameterizes the composition and water uptake of multicomponent atmospheric aerosols by considering the gas-liquid-solid partitioning of single and mixed solutes. EQSAM4 builds on analytical, and hence CPU efficient, aerosol hygroscopic growth parameterizations to compute the aerosol liquid water content (AWC). The parameterizations are described in the companion paper (Metzger et al., 2011) and only require a compound specific coefficient νi to derive the single solute molality and the AWC for the whole range of water activity (aw). νi is pre-calculated and applied during runtime by using internal look-up tables. Here, the EQSAM4 equilibrium model is described and compared to the more explicit thermodynamic model ISORROPIA II. Both models are imbedded in EMAC/GMXe. Box model inter-comparisons, including the reference model E-AIM, and global simulations with EMAC show that gas-particle partitioning, including semi-volatiles and water, is in good agreement. A more comprehensive box model inter-comparison of EQSAM4 with EQUISOLV II is subject of the revised publication of Xu et al. (2009), i.e. Xu et al. (2011).

scholarly journals Effects of relative humidity on aerosol light scattering: results from different European sites

2013 ◽  
Vol 13 (21) ◽  
pp. 10609-10631 ◽  
Author(s):  
P. Zieger ◽  
R. Fierz-Schmidhauser ◽  
E. Weingartner ◽  
U. Baltensperger
Keyword(s):  
Light Scattering ◽  
Relative Humidity ◽  
Water Uptake ◽  
Swiss Alps ◽  
The Arctic ◽  
Rural Site ◽  
Hygroscopic Growth ◽  
Aerosol Model ◽  
Arctic Aerosol ◽  
Measurement Results

Abstract. The effect of aerosol water uptake on the aerosol particle light scattering coefficient (σsp) is described in this study by comparing measurements from five European sites: the Jungfraujoch, located in the Swiss Alps at 3580 m a.s.l.; Ny-Ålesund, located on Spitsbergen in the Arctic; Mace Head, a coastal site in Ireland; Cabauw, a rural site in the Netherlands; and Melpitz, a regional background site in Eastern Germany. These sites were selected according to the aerosol type usually encountered at that location. The scattering enhancement factor f(RH, λ) is the key parameter to describe the effect of water uptake on the particle light scattering. It is defined as the σsp(RH) at a certain relative humidity (RH) and wavelength λ divided by its dry value. f(RH) at the five sites varied widely, starting at very low values of f(RH = 85%, λ = 550 nm) around 1.28 for mineral dust, and reaching up to 3.41 for Arctic aerosol. Hysteresis behavior was observed at all sites except at the Jungfraujoch (due to the absence of sea salt). Closure studies and Mie simulations showed that both size and chemical composition determine the magnitude of f(RH). Both parameters are also needed to successfully predict f(RH). Finally, the measurement results were compared to the widely used aerosol model, OPAC (Hess et al., 1998). Significant discrepancies were seen, especially at intermediate RH ranges; these were mainly attributed to inappropriate implementation of hygroscopic growth in the OPAC model. Replacement of the hygroscopic growth with values from the recent literature resulted in a clear improvement of the OPAC model.

scholarly journals Effects of relative humidity on aerosol light scattering: results from different European sites

2013 ◽  
Vol 13 (4) ◽  
pp. 8939-8984 ◽  
Author(s):  
P. Zieger ◽  
R. Fierz-Schmidhauser ◽  
E. Weingartner ◽  
U. Baltensperger
Keyword(s):  
Light Scattering ◽  
Relative Humidity ◽  
Water Uptake ◽  
Swiss Alps ◽  
The Arctic ◽  
Rural Site ◽  
Hygroscopic Growth ◽  
Aerosol Model ◽  
Arctic Aerosol ◽  
Measurement Results

Abstract. The effect of aerosol water uptake on the aerosol particle light scattering coefficient (σsp) is described in this study by comparing measurements from five European sites: the Jungfraujoch, located in the Swiss Alps at 3580 m a.s.l., Ny-Ålesund, located on Spitsbergen in the Arctic, Mace Head, a coastal site in Ireland, Cabauw, a rural site in the Netherlands and Melpitz, a regional background site in Eastern Germany. These sites were selected according to the aerosol type usually encountered at that location. The scattering enhancement factor f(RH,λ) is the key parameter to describe the effect of water uptake on the particle light scattering. It is defined as the σsp(RH) at a certain relative humidity (RH) and wavelength λ divided by its dry value. f(RH) largely varied at the five sites starting from very low values of f(RH = 85%,λ = 550 nm) around 1.28 for mineral dust to 3.41 for Arctic aerosol. Hysteresis behavior was observed at all sites except at the Jungfraujoch due to the absence of sea salt. Closure studies and Mie simulations showed that both size and chemical composition determine the magnitude of f(RH). Both parameters are also needed to successfully predict f(RH). Finally, the measurement results were compared to the widely used aerosol model OPAC (Hess et al., 1998). Significant discrepancies were seen especially at intermediate RH ranges, which were mainly attributed to inappropriate implemented hygroscopic growth within OPAC. Replacement of the hygroscopic growth with recent literature values showed a clear improvement of the OPAC model.

Water uptake of humic and fulvic acid: measurements and modelling using single parameter Köhler theory

2009 ◽  
Vol 6 (5) ◽  
pp. 380 ◽  
Author(s):  
Courtney D. Hatch ◽  
Kelly M. Gierlus ◽  
James Zahardis ◽  
Jennifer Schuttlefield ◽  
Vicki H. Grassian
Keyword(s):  
Thin Films ◽  
Surface Tension ◽  
Ftir Spectroscopy ◽  
Fulvic Acid ◽  
Water Uptake ◽  
Fulvic Acids ◽  
Single Parameter ◽  
Critical Parameters ◽  
Hygroscopic Growth ◽  
Kohler Theory

Environmental context. Humic and fulvic acids are macromolecular, multifunctional, polyacidic compounds that are important proxies for humic-like substances (HULIS), which are ubiquitous components of tropospheric particulate matter. The hygroscopic nature of these substances suggests that they can contribute to direct and indirect climate forcing. Thus, the effects of water uptake in humic-like particles in the atmosphere must be well understood. Abstract. The water uptake of humic and fulvic acid aerosols was determined by hygroscopic tandem differential mobility analysis (hTDMA) and extinction Fourier transform infrared (FTIR) spectroscopy. Water uptake on humic and fulvic acid thin films was also investigated using attenuated total reflectance (ATR) FTIR spectroscopy. The hygroscopic growth of monodisperse, 100-nm (dry) Suwannee River fulvic acid (SRFA) and humic acid sodium salt (NaHA) aerosols was determined and modelled using Köhler theory. A single parameter, the ionic density (ρion), which contains physical properties that are not well established for these substances, was determined for SRFA and NaHA to be 2.1 × 10–3 and 7.0 × 10–3 mol cm–3 respectively. The hygroscopic growth was then modelled using the ρion-Köhler equation and the critical parameters determined. The critical percent supersaturation of SRFA and NaHA was determined to be 0.60 and 0.33% respectively using the surface tension of water; and 0.35 and 0.19% respectively using the surface tension of aqueous HULIS. κ-Köhler theory, was also used to calculate the critical supersaturation and was found to be in good agreement with the ρion representation. Both extinction FTIR of aerosols and ATR-FTIR absorption measurements of thin films confirm enhanced water uptake with increasing relative humidity (RH).

scholarly journals Improved tropospheric and stratospheric sulfur cycle in the aerosol–chemistry–climate model SOCOL-AERv2

2019 ◽  
Vol 12 (9) ◽  
pp. 3863-3887 ◽  
Author(s):  
Aryeh Feinberg ◽  
Timofei Sukhodolov ◽  
Bei-Ping Luo ◽  
Eugene Rozanov ◽  
Lenny H. E. Winkel ◽  
...  
Keyword(s):  
Climate Model ◽  
Model Performance ◽  
Stratospheric Aerosol ◽  
Sulfur Cycle ◽  
Sulfate Aerosol ◽  
Tropospheric Chemistry ◽  
Sulfur Deposition ◽  
Aerosol Chemistry ◽  
Deposition Fluxes ◽  
Aerosol Model

Abstract. SOCOL-AERv1 was developed as an aerosol–chemistry–climate model to study the stratospheric sulfur cycle and its influence on climate and the ozone layer. It includes a sectional aerosol model that tracks the sulfate particle size distribution in 40 size bins, between 0.39 nm and 3.2 µm. Sheng et al. (2015) showed that SOCOL-AERv1 successfully matched observable quantities related to stratospheric aerosol. In the meantime, SOCOL-AER has undergone significant improvements and more observational datasets have become available. In producing SOCOL-AERv2 we have implemented several updates to the model: adding interactive deposition schemes, improving the sulfate mass and particle number conservation, and expanding the tropospheric chemistry scheme. We compare the two versions of the model with background stratospheric sulfate aerosol observations, stratospheric aerosol evolution after Pinatubo, and ground-based sulfur deposition networks. SOCOL-AERv2 shows similar levels of agreement as SOCOL-AERv1 with satellite-measured extinctions and in situ optical particle counter (OPC) balloon flights. The volcanically quiescent total stratospheric aerosol burden simulated in SOCOL-AERv2 has increased from 109 Gg of sulfur (S) to 160 Gg S, matching the newly available satellite estimate of 165 Gg S. However, SOCOL-AERv2 simulates too high cross-tropopause transport of tropospheric SO2 and/or sulfate aerosol, leading to an overestimation of lower stratospheric aerosol. Due to the current lack of upper tropospheric SO2 measurements and the neglect of organic aerosol in the model, the lower stratospheric bias of SOCOL-AERv2 was not further improved. Model performance under volcanically perturbed conditions has also undergone some changes, resulting in a slightly shorter volcanic aerosol lifetime after the Pinatubo eruption. With the improved deposition schemes of SOCOL-AERv2, simulated sulfur wet deposition fluxes are within a factor of 2 of measured deposition fluxes at 78 % of the measurement stations globally, an agreement which is on par with previous model intercomparison studies. Because of these improvements, SOCOL-AERv2 will be better suited to studying changes in atmospheric sulfur deposition due to variations in climate and emissions.

scholarly journals Secondary aerosol formation promotes water uptake by organic-rich wildfire haze particles in Equatorial Asia

2017 ◽  
Author(s):  
Jing Chen ◽  
Sri Hapsari Budisulistiorini ◽  
Takuma Miyakawa ◽  
Yuichi Komazaki ◽  
Mikinori Kuwata
Keyword(s):  
Water Uptake ◽  
Mass Fraction ◽  
Water Soluble ◽  
Submicron Particles ◽  
Chemical Information ◽  
Hygroscopic Growth ◽  
Aerosol Formation ◽  
Secondary Formation ◽  
Soluble Organic Fraction ◽  
Haze Episode

Abstract. Diameter growth factors (GF) of 100 nm haze particles at 85 % relative humidity and chemical characteristics were simultaneously monitored at Singapore in October 2015 during a pervasive wildfire haze episode, which was caused by peatland burning in Indonesia. Non-refractory submicron particles (NR-PM1) were dominated by organics (approximating 77.1 % in total mass), whereas sulfate was the most abundant inorganic constituent (11.7 % on average). A statistical analysis of the organic mass spectra showed that most of organics (36.0 % of NR-PM1 mass) were highly oxygenated. Diurnal variations of GF, number fraction of highly hygroscopic mode particles, mass fraction of sulfate, and mass fraction of oxygenated organics (OOA) synchronized well, peaking during daytime. The mean hygroscopicity parameter (κ) of haze particles was 0.189 ± 0.087, and mean κ values of organics were 0.157 ± 0.108 (κorg, bulk organics) and 0.287 ± 0.193 (κOOA, OOA), demonstrating the important roles of both sulfate and highly oxygenated organics in hygroscopic growth of wildfire haze particles. κorg was also affected by the water-soluble organic fraction to some extent. These results show the importance of secondary formation processes in promoting water uptake properties of wildfire haze particles, including both inorganic and organic species. Further detailed size-resolved as well as molecular level chemical information of organics will be necessary for more profound exploration of water uptake by wildfire haze particles in Equatorial Asia.

scholarly journals A thermodynamic description for the hygroscopic growth of atmospheric aerosol particles

2018 ◽  
Vol 18 (20) ◽  
pp. 14939-14948 ◽  
Author(s):  
Dimitri Castarède ◽  
Erik S. Thomson
Keyword(s):  
Radiative Forcing ◽  
Thermodynamic Description ◽  
Liquid Droplets ◽  
Hygroscopic Growth ◽  
Salt Particle ◽  
Aerosol Radiative Forcing ◽  
Condensation Nucleation ◽  
Kohler Theory ◽  
Kelvin Effect ◽  
Brine Layer

Abstract. The phase state of atmospheric particulate is important to atmospheric processes, and aerosol radiative forcing remains a large uncertainty in climate predictions. That said, precise atmospheric phase behavior is difficult to quantify and observations have shown that “precondensation” of water below predicted saturation values can occur. We propose a revised approach to understanding the transition from solid soluble particles to liquid droplets, typically described as cloud condensation nucleation – a process that is traditionally captured by Köhler theory, which describes a modified equilibrium saturation vapor pressure due to (i) mixing entropy (Raoult's law) and (ii) droplet geometry (Kelvin effect). Given that observations of precondensation are not predicted by Köhler theory, we devise a more complete model that includes interfacial forces giving rise to predeliquescence, i.e., the formation of a brine layer wetting a salt particle at relative humidities well below the deliquescence point.

Sign in / Sign up

Export Citation Format

Share Document