scholarly journals A parameterization of sub-grid particle formation in sulphur-rich plumes for global and regional-scale models

2013 ◽  
Vol 13 (7) ◽  
pp. 19583-19623 ◽  
Author(s):  
R. G. Stevens ◽  
J. R. Pierce

Abstract. New-particle formation in the plumes of coal-fired power plants and other anthropogenic sulphur sources may be an important source of particles in the atmosphere. It remains unclear, however, how best to reproduce this formation in global and regional aerosol models with grid-box lengths that are tens of kilometres and larger. Based on the results of the System for Atmospheric Modelling (SAM), a Large-Eddy Simulation/Cloud-Resolving Model (LES/CRM) with online TwO Moment Aerosol Sectional (TOMAS) microphysics, we have developed a computationally efficient, but physically based, parameterization that predicts the characteristics of aerosol formed within sulphur-rich plumes based on parameters commonly available in global- and regional-scale models. Given large-scale mean meteorological parameters ((1) wind speed, (2) boundary-layer height and (3) downward shortwave radiative flux), (4) emissions of SO2 and (5) NOx from the source, (6) mean background condensation sink, (7) background SO2 and (8) NOx concentrations, and (9) the desired distance from the source; the parameterization will predict: (1) the fraction of the emitted SO2 that is oxidized to H2SO4, (2) the fraction of that H2SO4 that forms new particles instead of condensing onto preexisting particles, (3) the mean mass per particle of the newly formed particles, and (4) the number of newly formed particles per kilogram SO2 emitted. The parameterization we describe here should allow for more accurate predictions of aerosol size distributions and a greater confidence in the effects of aerosols in climate and health studies.

2013 ◽  
Vol 13 (23) ◽  
pp. 12117-12133 ◽  
Author(s):  
R. G. Stevens ◽  
J. R. Pierce

Abstract. New-particle formation in the plumes of coal-fired power plants and other anthropogenic sulfur sources may be an important source of particles in the atmosphere. It remains unclear, however, how best to reproduce this formation in global and regional aerosol models with grid-box lengths that are tens of kilometres and larger. Based on the results of the System for Atmospheric Modelling (SAM), a large-eddy simulation/cloud-resolving model (LES/CRM) with online two-moment aerosol sectional (TOMAS) microphysics, we have developed a computationally efficient, but physically based, parameterization that predicts the characteristics of aerosol formed within sulfur-rich plumes based on parameters commonly available in global- and regional-scale models. Given large-scale mean meteorological parameters ((1) wind speed, (2) boundary-layer height and (3) downward shortwave radiative flux), (4) emissions of SO2 and (5) NOx from the source, (6) mean background condensation sink, (7) background SO2 and (8) NOx concentrations, and (9) the desired distance from the source, the parameterization will predict (1) the fraction of the emitted SO2 that is oxidized to H2SO4, (2) the fraction of that H2SO4 that forms new particles instead of condensing onto pre-existing particles, (3) the mean mass per particle of the newly formed particles, and (4) the number of newly formed particles per kilogram SO2 emitted. The parameterization we describe here should allow for more accurate predictions of aerosol size distributions and a greater confidence in the effects of aerosols in climate and health studies.


2020 ◽  
Vol 20 (3) ◽  
pp. 1301-1316
Author(s):  
Georgia Sotiropoulou ◽  
Sylvia Sullivan ◽  
Julien Savre ◽  
Gary Lloyd ◽  
Thomas Lachlan-Cope ◽  
...  

Abstract. In situ measurements of Arctic clouds frequently show that ice crystal number concentrations (ICNCs) are much higher than the number of available ice-nucleating particles (INPs), suggesting that secondary ice production (SIP) may be active. Here we use a Lagrangian parcel model (LPM) and a large-eddy simulation (LES) to investigate the impact of three SIP mechanisms (rime splintering, break-up from ice–ice collisions and drop shattering) on a summer Arctic stratocumulus case observed during the Aerosol-Cloud Coupling And Climate Interactions in the Arctic (ACCACIA) campaign. Primary ice alone cannot explain the observed ICNCs, and drop shattering is ineffective in the examined conditions. Only the combination of both rime splintering (RS) and collisional break-up (BR) can explain the observed ICNCs, since both of these mechanisms are weak when activated alone. In contrast to RS, BR is currently not represented in large-scale models; however our results indicate that this may also be a critical ice-multiplication mechanism. In general, low sensitivity of the ICNCs to the assumed INP, to the cloud condensation nuclei (CCN) conditions and also to the choice of BR parameterization is found. Finally, we show that a simplified treatment of SIP, using a LPM constrained by a LES and/or observations, provides a realistic yet computationally efficient way to study SIP effects on clouds. This method can eventually serve as a way to parameterize SIP processes in large-scale models.


2011 ◽  
Vol 11 (9) ◽  
pp. 24765-24812 ◽  
Author(s):  
R. G. Stevens ◽  
J. R. Pierce ◽  
C. A. Brock ◽  
M. K. Reed ◽  
J. H. Crawford ◽  
...  

Abstract. New-particle formation in the plumes of coal-fired power plants and other anthropogenic sulfur sources may be an important source of particles in the atmosphere. It remains unclear, however, how best to reproduce this formation in global and regional aerosol models with grid-box lengths that are 10 s of kilometers and larger. The predictive power of these models is thus limited by the resultant uncertainties in aerosol size distributions. In this paper, we focus on sub-grid sulfate aerosol processes within coal-fired power plant plumes: the sub-grid oxidation of SO2 with condensation of H2SO4 onto newly-formed and pre-existing particles. We have developed a modeling framework with aerosol microphysics in the System for Atmospheric Modelling (SAM), a Large-Eddy Simulation/Cloud-Resolving Model (LES/CRM). The model is evaluated against aircraft observations of new-particle formation in two different power-plant plumes and reproduces the major features of the observations. We show how the downwind plume aerosols can be greatly modified by both meteorological and background aerosol conditions. In general, new-particle formation and growth is greatly reduced during polluted conditions due to the large pre-existing aerosol surface area for H2SO4 condensation and particle coagulation. The new-particle formation and growth rates are also a strong function of the amount of sunlight and NOx since both control OH concentrations. The results of this study highlight the importance for improved sub-grid particle formation schemes in regional and global aerosol models.


2012 ◽  
Vol 12 (1) ◽  
pp. 189-206 ◽  
Author(s):  
R. G. Stevens ◽  
J. R. Pierce ◽  
C. A. Brock ◽  
M. K. Reed ◽  
J. H. Crawford ◽  
...  

Abstract. New-particle formation in the plumes of coal-fired power plants and other anthropogenic sulfur sources may be an important source of particles in the atmosphere. It remains unclear, however, how best to reproduce this formation in global and regional aerosol models with grid-box lengths that are 10s of kilometers and larger. The predictive power of these models is thus limited by the resultant uncertainties in aerosol size distributions. In this paper, we focus on sub-grid sulfate aerosol processes within coal-fired power plant plumes: the sub-grid oxidation of SO2 with condensation of H2SO4 onto newly-formed and pre-existing particles. We have developed a modeling framework with aerosol microphysics in the System for Atmospheric Modelling (SAM), a Large-Eddy Simulation/Cloud-Resolving Model (LES/CRM). The model is evaluated against aircraft observations of new-particle formation in two different power-plant plumes and reproduces the major features of the observations. We show how the downwind plume aerosols can be greatly modified by both meteorological and background aerosol conditions. In general, new-particle formation and growth is greatly reduced during polluted conditions due to the large pre-existing aerosol surface area for H2SO4 condensation and particle coagulation. The new-particle formation and growth rates are also a strong function of the amount of sunlight and NOx since both control OH concentrations. The results of this study highlight the importance for improved sub-grid particle formation schemes in regional and global aerosol models.


2016 ◽  
Author(s):  
Rogier Westerhoff ◽  
Paul White ◽  
Zara Rawlinson

Abstract. Large-scale models and satellite data are increasingly used to characterise groundwater and its recharge at the global scale. Although these models have the potential to fill in data gaps and solve trans-boundary issues, they are often neglected in smaller-scale studies, since data are often coarse or uncertain. Large-scale models and satellite data could play a more important role in smaller-scale (i.e., national or regional) studies, if they could be adjusted to fit that scale. In New Zealand, large-scale models and satellite data are not used for groundwater recharge estimation at the national scale, since regional councils (i.e., the water managers) have varying water policy and models are calibrated at the local scale. Also, some regions have many localised ground observations (but poor record coverage), whereas others are data-sparse. Therefore, estimation of recharge is inconsistent at the national scale. This paper presents an approach to apply large-scale, global, models and satellite data to estimate rainfall recharge at the national to regional scale across New Zealand. We present a model, NGRM, that is largely inspired by the global-scale WaterGAP recharge model, but is improved and adjusted using national data. The NGRM model uses MODIS-derived ET and vegetation satellite data, and the available nation-wide datasets on rainfall, elevation, soil and geology. A valuable addition to the recharge estimation is the model uncertainty estimate, based on variance, covariance and sensitivity of all input data components in the model environment. This research shows that, with minor model adjustments and use of improved input data, large-scale models and satellite data can be used to derive rainfall recharge estimates, including their uncertainty, at the smaller scale, i.e., national and regional scale of New Zealand. The estimated New Zealand recharge of the NGRM model compare well to most local and regional lysimeter data and recharge models. The NGRM is therefore assumed to be capable to fill in gaps in data-sparse areas and to create more consistency between datasets from different regions, i.e., to solve trans-boundary issues. This research also shows that smaller-scale recharge studies in New Zealand should include larger boundaries than only a (sub-)aquifer, and preferably the whole catchment. This research points out the need for improved collaboration on the international to national to regional levels to further merge large-scale (global) models to smaller (i.e., national or regional) scales. Future research topics should, collaboratively, focus on: improvement of rainfall-runoff and snowmelt methods; inclusion of river recharge; further improvement of input data (rainfall, evapotranspiration, soil and geology); and the impact of recharge uncertainty in mountainous and irrigated areas.


2018 ◽  
Vol 18 (5) ◽  
pp. 3839-3864 ◽  
Author(s):  
Christian Hogrefe ◽  
Peng Liu ◽  
George Pouliot ◽  
Rohit Mathur ◽  
Shawn Roselle ◽  
...  

Abstract. This study analyzes simulated regional-scale ozone burdens both near the surface and aloft, estimates process contributions to these burdens, and calculates the sensitivity of the simulated regional-scale ozone burden to several key model inputs with a particular emphasis on boundary conditions derived from hemispheric or global-scale models. The Community Multiscale Air Quality (CMAQ) model simulations supporting this analysis were performed over the continental US for the year 2010 within the context of the Air Quality Model Evaluation International Initiative (AQMEII) and Task Force on Hemispheric Transport of Air Pollution (TF-HTAP) activities. CMAQ process analysis (PA) results highlight the dominant role of horizontal and vertical advection on the ozone burden in the mid-to-upper troposphere and lower stratosphere. Vertical mixing, including mixing by convective clouds, couples fluctuations in free-tropospheric ozone to ozone in lower layers. Hypothetical bounding scenarios were performed to quantify the effects of emissions, boundary conditions, and ozone dry deposition on the simulated ozone burden. Analysis of these simulations confirms that the characterization of ozone outside the regional-scale modeling domain can have a profound impact on simulated regional-scale ozone. This was further investigated by using data from four hemispheric or global modeling systems (Chemistry – Integrated Forecasting Model (C-IFS), CMAQ extended for hemispheric applications (H-CMAQ), the Goddard Earth Observing System model coupled to chemistry (GEOS-Chem), and AM3) to derive alternate boundary conditions for the regional-scale CMAQ simulations. The regional-scale CMAQ simulations using these four different boundary conditions showed that the largest ozone abundance in the upper layers was simulated when using boundary conditions from GEOS-Chem, followed by the simulations using C-IFS, AM3, and H-CMAQ boundary conditions, consistent with the analysis of the ozone fields from the global models along the CMAQ boundaries. Using boundary conditions from AM3 yielded higher springtime ozone columns burdens in the middle and lower troposphere compared to boundary conditions from the other models. For surface ozone, the differences between the AM3-driven CMAQ simulations and the CMAQ simulations driven by other large-scale models are especially pronounced during spring and winter where they can reach more than 10 ppb for seasonal mean ozone mixing ratios and as much as 15 ppb for domain-averaged daily maximum 8 h average ozone on individual days. In contrast, the differences between the C-IFS-, GEOS-Chem-, and H-CMAQ-driven regional-scale CMAQ simulations are typically smaller. Comparing simulated surface ozone mixing ratios to observations and computing seasonal and regional model performance statistics revealed that boundary conditions can have a substantial impact on model performance. Further analysis showed that boundary conditions can affect model performance across the entire range of the observed distribution, although the impacts tend to be lower during summer and for the very highest observed percentiles. The results are discussed in the context of future model development and analysis opportunities.


2017 ◽  
Author(s):  
Christian Hogrefe ◽  
Peng Liu ◽  
George Pouliot ◽  
Rohit Mathur ◽  
Shawn Roselle ◽  
...  

Abstract. This study analyzes simulated regional-scale ozone burdens both near the surface and aloft, estimates process contributions to these burdens, and calculates the sensitivity of the simulated regional-scale ozone burden to several key model inputs with a particular emphasis on boundary conditions derived from hemispheric or global scale models. The Community Multiscale Air Quality (CMAQ) model simulations supporting this analysis were performed over the continental U.S. for the year 2010 within the context of the Air Quality Model Evaluation International Initiative (AQMEII) and Task Force on Hemispheric Transport of Air Pollution (TF-HTAP) activities. CMAQ Process Analysis (PA) results highlight the dominant role of horizontal and vertical advection on the ozone burden in the mid-to-upper troposphere and lower stratosphere. Vertical mixing, including mixing by convective clouds, couple fluctuations in free tropospheric ozone to ozone in lower layers. Hypothetical bounding scenarios were performed to quantify the effects of emissions, boundary conditions, and ozone dry deposition on the simulated ozone burden. Analysis of these simulations confirms that the characterization of ozone outside the regional-scale modeling domain can have a profound impact on simulated regional-scale ozone. This was further investigated by using data from four hemispheric or global modeling systems (Chemistry – Integrated Forecasting Model (C-IFS), CMAQ extended for hemispheric applications (H-CMAQ), GEOS-Chem, and AM3) to derive alternate boundary conditions for the regional-scale CMAQ simulations. The regional-scale CMAQ simulations using these four different boundary conditions showed that the largest ozone abundance in the upper layers was simulated when using boundary conditions from GEOS-Chem, followed by the simulations using C-IFS, AM3, and H-CMAQ boundary conditions, consistent with the analysis of the ozone fields from the global models along the CMAQ boundaries. Using boundary conditions from AM3 yielded higher springtime ozone columns burdens in the mid- and lower troposphere compared to boundary conditions from the other models. For surface ozone, the differences between the AM3-driven CMAQ simulations and the CMAQ simulations driven by other large-scale models are especially pronounced during spring and winter where they can reach more than 10 ppb for seasonal mean ozone mixing ratios and as much as 15 ppb for domain-averaged daily maximum 8-hr average ozone on individual days. In contrast, the differences between the C-IFS, GEOS-Chem, and H-CMAQ driven regional-scale CMAQ simulations are typically smaller. Comparing simulated surface ozone mixing ratios to observations and computing seasonal and regional model performance statistics revealed that boundary conditions can have a substantial impact on model performance. Further analysis showed that boundary conditions can affect model performance across the entire range of the observed distribution, although the impacts tend to be lower during summer and for the very highest observed percentiles. The results are discussed in the context of future model development and analysis opportunities.


2021 ◽  
Author(s):  
Christopher ODell ◽  
Annmarie Eldering ◽  
Michael Gunson ◽  
David Crisp ◽  
Brendan Fisher ◽  
...  

<p>While initial plans for measuring carbon dioxide from space hoped for 1-2 ppm levels of accuracy (bias) and precision in the CO<sub>2</sub> column mean dry air mole fraction (XCO<sub>2</sub>), in the past few years it has become clear that accuracies better than 0.5 ppm are required for most current science applications.  These include measuring continental (1000+ km) and regional scale (100s of km) surface fluxes of CO<sub>2</sub> at monthly-average timescales.  Considering the 400+ ppm background, this translates to an accuracy of roughly 0.1%, an incredibly challenging target to hit. </p><p>Improvements in both instrument calibration and retrieval algorithms have led to significant improvements in satellite XCO<sub>2</sub> accuracies over the past decade.  The Atmospheric Carbon Observations from Space (ACOS) retrieval algorithm, including post-retrieval filtering and bias correction, has demonstrated unprecedented accuracy with our latest algorithm version as applied to the Orbiting Carbon Observatory-2 (OCO-2) satellite sensor.   This presentation will discuss the performance of the v10 XCO<sub>2</sub> product by comparisons to TCCON and models, and showcase its performance with some recent examples, from the potential to infer large-scale fluxes to its performance on individual power plants.  The v10 product yields better agreement with TCCON over land and ocean, plus reduced biases over tropical oceans and desert areas as compared to a median of multiple global carbon inversion models, allowing better accuracy and faith in inferred regional-scale fluxes.  More specifically, OCO-2 has single sounding precision of ~0.8 ppm over land and ~0.5 ppm over water, and RMS biases of 0.5-0.7 ppm over both land and water.  Given the six-year and growing length of the OCO-2 data record, this also enables new studies on carbon interannual variability, while at the same time allowing identification of more subtle and temporally-dependent errors.  Finally, we will discuss the prospects of future improvements in the next planned version (v11), and the long-term prospects of greenhouse gas retrievals in the coming years. </p><p> </p>


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