scholarly journals An advanced scheme for wet scavenging and liquid-phase chemistry in a regional online-coupled chemistry transport model

2013 ◽  
Vol 13 (3) ◽  
pp. 1177-1192 ◽  
Author(s):  
C. Knote ◽  
D. Brunner
Keyword(s):  
Aqueous Phase ◽  
Climate Model ◽  
Transport Model ◽  
Measurement Data ◽  
Coupled System ◽  
Cloud Microphysics ◽  
Microphysics Scheme ◽  
Meteorological Model ◽  
Wet Scavenging ◽  
Phase Chemistry

Abstract. Clouds are reaction chambers for atmospheric trace gases and aerosols, and the associated precipitation is a major sink for atmospheric constituents. The regional chemistry-climate model COSMO-ART has been lacking a description of wet scavenging of gases and aqueous-phase chemistry. In this work we present a coupling of COSMO-ART with a wet scavenging and aqueous-phase chemistry scheme. The coupling is made consistent with the cloud microphysics scheme of the underlying meteorological model COSMO. While the choice of the aqueous-chemistry mechanism is flexible, the effects of a simple sulfur oxidation scheme are shown in the application of the coupled system in this work. We give details explaining the coupling and extensions made, then present results from idealized flow-over-hill experiments in a 2-D model setup and finally results from a full 3-D simulation. Comparison against measurement data shows that the scheme efficiently reduces SO2 trace gas concentrations by 0.3 ppbv (−30%) on average, while leaving O3 and NOx unchanged. PM10 aerosol mass was increased by 10% on average. While total PM2.5 changes only little, chemical composition is improved notably. Overestimations of nitrate aerosols are reduced by typically 0.5–1 μg m−3 (up to −2 μg m−3 in the Po Valley) while sulfate mass is increased by 1–1.5 μg m−3 on average (up to 2.5 μg m−3 in Eastern Europe). The effect of cloud processing of aerosols on its size distribution, i.e. a shift towards larger diameters, is observed. Compared against wet deposition measurements the system tends to underestimate the total wet deposited mass for the simulated case study.

scholarly journals An advanced scheme for wet scavenging and liquid-phase chemistry in a regional online-coupled chemistry transport model

2012 ◽  
Vol 12 (10) ◽  
pp. 26099-26142
Author(s):  
C. Knote ◽  
D. Brunner
Keyword(s):  
Aqueous Phase ◽  
Climate Model ◽  
Transport Model ◽  
Measurement Data ◽  
Coupled System ◽  
Cloud Microphysics ◽  
Microphysics Scheme ◽  
Meteorological Model ◽  
Wet Scavenging ◽  
Phase Chemistry

Abstract. Clouds are reaction chambers for atmospheric trace gases and aerosols, and the associated precipitation is a major sink for atmospheric constituents. The regional chemistry-climate model COSMO-ART has been lacking a description of wet scavenging of gases and aqueous-phase chemistry. In this work we present a coupling of COSMO-ART with a wet scavenging and aqueous-phase chemistry scheme. The coupling is made consistent with the cloud microphysics scheme of the underlying meteorological model COSMO. While the choice of the aqueous-chemistry mechanism is flexible, the effects of a simple sulfur oxidation scheme are shown in the application of the coupled system in this work. We give details explaining the coupling and extensions made, then present results from idealized flow-over-hill experiments in a 2-D model setup and finally results from a full 3-D simulation. Comparison against measurement data shows that the scheme efficiently reduces SO2 trace gas concentrations by 0.3 ppbv (−30%) on average, while leaving O3 and NOx unchanged. PM10 aerosol mass, which has been overestimated previously, is now in much better agreement with measured values due to a stronger scavenging of coarse particles. While total PM2.5 changes only little, chemical composition is improved notably. Overestimations of nitrate aerosols are reduced by typically 0.5–1 μg m−3 (up to −2 μg m−3 in the Po Valley) while sulfate mass is increased by 1–1.5 μg m−3 on average (up to 2.5 μg m−3 in Eastern Europe). The effect of cloud processing of aerosols on its size distribution, i. e. a shift towards larger diameters, is observed. Compared against wet deposition measurements the system underestimates the total wet deposited mass for the simulated case study. We find that while evaporation of cloud droplets dominates in higher altitudes, evaporation of precipitation can contribute up to 50% of total evaporated mass near the surface.

scholarly journals libcloudph++ 1.1: aqueous phase chemistry extension of the Lagrangian cloud microphysics scheme

2018 ◽  
Author(s):  
Anna Jaruga ◽  
Hanna Pawlowska
Keyword(s):  
Programming Languages ◽  
Aqueous Phase ◽  
Numerical Models ◽  
Cloud Condensation Nuclei ◽  
Cloud Microphysics ◽  
Chemical Processes ◽  
Cloud Droplets ◽  
Microphysics Scheme ◽  
Phase Oxidation ◽  
Phase Chemistry

Abstract. This paper introduces a new scheme available in the library of algorithms for representing cloud microphysics in numerical models named libcloudph++. The scheme extends the Lagrangian microphysics scheme available in libcloudph++ to the aqueous phase chemical processes occurring within cloud droplets. The representation of chemical processes focuses on the aqueous phase oxidation of the dissolved SO2 by O3 and H2O2. The Lagrangian Microphysics and Chemistry (LMC) scheme allows tracking the changes in the cloud condensation nuclei (CCN) distribution caused by both collisions between cloud droplets and aqueous phase oxidation. The scheme is implemented in C++ and equipped with bindings to Python which allow reusing the created scheme from models implemented in other programming languages. The scheme can be used on either CPU or GPU, and is distributed under the GPL3 license. Here, the LMC scheme is tested in a simple 0-dimensional adiabatic parcel model and then used in a 2-dimensional prescribed flow framework. The results are discussed with the focus on changes to the CCN sizes and compared with other model simulations discussed in the literature.

scholarly journals libcloudph++ 2.0: aqueous-phase chemistry extension of the particle-based cloud microphysics scheme

2018 ◽  
Vol 11 (9) ◽  
pp. 3623-3645 ◽  
Author(s):  
Anna Jaruga ◽  
Hanna Pawlowska
Keyword(s):  
Aqueous Phase ◽  
Numerical Models ◽  
Cloud Condensation Nuclei ◽  
Cloud Microphysics ◽  
Chemical Processes ◽  
Cloud Droplets ◽  
Microphysics Scheme ◽  
Phase Oxidation ◽  
Phase Chemistry ◽  
Phase Chemical

Abstract. This paper introduces a new scheme available in the library of algorithms for representing cloud microphysics in numerical models named libcloudph++. The scheme extends the particle-based microphysics scheme with a Monte Carlo coalescence available in libcloudph++ to the aqueous-phase chemical processes occurring within cloud droplets. The representation of chemical processes focuses on the aqueous-phase oxidation of the dissolved SO2 by O3 and H2O2. The particle-based microphysics and chemistry scheme allows for tracking of the changes in the cloud condensation nuclei (CCN) distribution caused by both collisions between cloud droplets and aqueous-phase oxidation. The scheme is implemented in C++ and equipped with bindings to Python. The scheme can be used on either a CPU or a GPU, and is distributed under the GPLv3 license. Here, the particle-based microphysics and chemistry scheme is tested in a simple 0-dimensional adiabatic parcel model and then used in a 2-dimensional prescribed flow framework. The results are discussed with a focus on changes to the CCN sizes and comparison with other model simulations discussed in the literature.

Modelling nitrogen transport across compartments over northern Europe

2021 ◽  
Author(s):  
Stefan Hagemann ◽  
Ute Daewel ◽  
Volker Matthias ◽  
Tobias Stacke
Keyword(s):  
Baltic Sea ◽  
Land Surface ◽  
Climate Model ◽  
Transport Model ◽  
Atmospheric Transport ◽  
Regional Climate ◽  
Marine Ecosystem ◽  
Coupled System ◽  
Nutrient Concentrations ◽  
Nutrient Loads

<p>River discharge and the associated nutrient loads are important factors that influence the functioning of the marine ecosystem. Lateral inflows from land carrying fresh, nutrient-rich water determine coastal physical conditions and nutrient concentration and, hence, dominantly influence primary production in the system. Since this forms the basis of the trophic food web, riverine nutrient concentrations impact the variability of the whole coastal ecosystem. This process becomes even more relevant in systems like the Baltic Sea, which is almost decoupled from the open ocean and land-borne nutrients play a major role for ecosystem productivity on seasonal up to decadal time scales.</p><p> </p><p>In order to represent the effects of climate or land use change on nutrient availability, a coupled system approach is required to simulate the transport of nutrients across Earth system compartments. This comprises their transport within the atmosphere, the deposition and human application at the surface, the lateral transport over the land surface into the ocean and their dynamics and transformation in the marine ecosystem. In our study, we combine these processes in a modelling chain within the GCOAST (Geesthacht Coupled cOAstal model SysTem) framework for the northern European region. This modelling chain comprises:</p><p> </p><ul><li>Simulation of emissions, atmospheric transport and deposition with the chemistry transport model CMAQ at 36 km grid resolution using atmospheric forcing from the coastDat3 data that have been generated with the regional climate model COSMO-CLM over Europe at 0.11° resolution using ERA-Interim re-analyses as boundary conditions</li> <li>Simulation of inert processes at the land surface with the global hydrology model HydroPy (former MPI-HM), i.e. considering total nitrogen without any chemical reactions</li> <li>Riverine transport with the Hydrological Discharge (HD) model at 0.0833° spatial resolution</li> <li>Simulation of the North Sea and Baltic Sea ecosystems with 3D coupled physical-biogeochemical NPZD-model ECOSMO II at about 10 km resolution</li> </ul><p> </p><p>We will present first results and their validation from this exercise.</p><p> </p>

scholarly journals Numerical framework and performance of the new multiple-phase cloud microphysics scheme in RegCM4.5: precipitation, cloud microphysics, and cloud radiative effects

2016 ◽  
Vol 9 (7) ◽  
pp. 2533-2547 ◽  
Author(s):  
Rita Nogherotto ◽  
Adrian Mark Tompkins ◽  
Graziano Giuliani ◽  
Erika Coppola ◽  
Filippo Giorgi
Keyword(s):  
Radiative Forcing ◽  
Climate Model ◽  
Regional Climate ◽  
Cloud Microphysics ◽  
Microphysics Scheme ◽  
Additional Information ◽  
Mixing Ratios ◽  
Multiple Phase ◽  
Realistic Representation ◽  
And Performance

Abstract. We implement and evaluate a new parameterization scheme for stratiform cloud microphysics and precipitation within regional climate model RegCM4. This new parameterization is based on a multiple-phase one-moment cloud microphysics scheme built upon the implicit numerical framework recently developed and implemented in the ECMWF operational forecasting model. The parameterization solves five prognostic equations for water vapour, cloud liquid water, rain, cloud ice, and snow mixing ratios. Compared to the pre-existing scheme, it allows a proper treatment of mixed-phase clouds and a more physically realistic representation of cloud microphysics and precipitation. Various fields from a 10-year long integration of RegCM4 run in tropical band mode with the new scheme are compared with their counterparts using the previous cloud scheme and are evaluated against satellite observations. In addition, an assessment using the Cloud Feedback Model Intercomparison Project (CFMIP) Observational Simulator Package (COSP) for a 1-year sub-period provides additional information for evaluating the cloud optical properties against satellite data. The new microphysics parameterization yields an improved simulation of cloud fields, and in particular it removes the overestimation of upper level cloud characteristics of the previous scheme, increasing the agreement with observations and leading to an amelioration of a long-standing problem in the RegCM system. The vertical cloud profile produced by the new scheme leads to a considerably improvement of the representation of the longwave and shortwave components of the cloud radiative forcing.

scholarly journals Towards an online-coupled chemistry-climate model: evaluation of trace gases and aerosols in COSMO-ART

2011 ◽  
Vol 4 (4) ◽  
pp. 1077-1102 ◽  
Author(s):  
C. Knote ◽  
D. Brunner ◽  
H. Vogel ◽  
J. Allan ◽  
A. Asmi ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Size Distribution ◽  
Urban Areas ◽  
Climate Model ◽  
Transport Model ◽  
Climate Impacts ◽  
Chemistry Transport Model ◽  
Pm2.5 And Pm10 ◽  
Phase Chemistry ◽  
Aerosol Chemical Composition

Abstract. The online-coupled, regional chemistry transport model COSMO-ART is evaluated for periods in all seasons against several measurement datasets to assess its ability to represent gaseous pollutants and ambient aerosol characteristics over the European domain. Measurements used in the comparison include long-term station observations, satellite and ground-based remote sensing products, and complex datasets of aerosol chemical composition and number size distribution from recent field campaigns. This is the first time these comprehensive measurements of aerosol characteristics in Europe are used to evaluate a regional chemistry transport model. We show a detailed analysis of the simulated size-resolved chemical composition under different meteorological conditions. Mean, variability and spatial distribution of the concentrations of O3 and NOx are well reproduced. SO2 is found to be overestimated, simulated PM2.5 and PM10 levels are on average underestimated, as is AOD. We find indications of an overestimation of shipping emissions. Time evolution of aerosol chemical composition is captured, although some biases are found in relative composition. Nitrate aerosol components are on average overestimated, and sulfates underestimated. The accuracy of simulated organics depends strongly on season and location. While strongly underestimated during summer, organic mass is comparable in spring and autumn. We see indications for an overestimated fractional contribution of primary organic matter in urban areas and an underestimation of SOA at many locations. Aerosol number concentrations compare well with measurements for larger size ranges, but overestimations of particle number concentration with factors of 2–5 are found for particles smaller than 50 nm. Size distribution characteristics are often close to measurements, but show discrepancies at polluted sites. Suggestions for further improvement of the modeling system consist of the inclusion of a revised secondary organic aerosols scheme, aqueous-phase chemistry and improved aerosol boundary conditions. Our work sets the basis for subsequent studies of aerosol characteristics and climate impacts with COSMO-ART, and highlights areas where improvements are necessary for current regional modeling systems in general.

scholarly journals The multi-scale aerosol-climate model PNNL-MMF: model description and evaluation

2010 ◽  
Vol 3 (4) ◽  
pp. 1625-1695 ◽  
Author(s):  
M. Wang ◽  
S. Ghan ◽  
R. Easter ◽  
M. Ovchinnikov ◽  
X. Liu ◽  
...  
Keyword(s):  
Reasonable Agreement ◽  
Large Scale ◽  
Climate Model ◽  
Cloud Microphysics ◽  
Chemical Processes ◽  
Future Climate Change ◽  
Free Troposphere ◽  
Microphysics Scheme ◽  
New Model ◽  
Multi Scale

Abstract. Anthropogenic aerosol effects on climate produce one of the largest uncertainties in estimates of radiative forcing of past and future climate change. Much of this uncertainty arises from the multi-scale nature of the interactions between aerosols, clouds and large-scale dynamics, which are difficult to represent in conventional global climate models (GCMs). In this study, we develop a multi-scale aerosol climate model that treats aerosols and clouds across different scales, and evaluate the model performance, with a focus on aerosol treatment. This new model is an extension of a multi-scale modeling framework (MMF) model that embeds a cloud-resolving model (CRM) within each grid column of a GCM. In this extension, the effects of clouds on aerosols are treated by using an explicit-cloud parameterized-pollutant (ECPP) approach that links aerosol and chemical processes on the large-scale grid with statistics of cloud properties and processes resolved by the CRM. A two-moment cloud microphysics scheme replaces the simple bulk microphysics scheme in the CRM, and a modal aerosol treatment is included in the GCM. With these extensions, this multi-scale aerosol-climate model allows the explicit simulation of aerosol and chemical processes in both stratiform and convective clouds on a global scale. Simulated aerosol budgets in this new model are in the ranges of other model studies. Simulated gas and aerosol concentrations are in reasonable agreement with observations, although the model underestimates black carbon concentrations at the surface. Simulated aerosol size distributions are in reasonable agreement with observations in the marine boundary layer and in the free troposphere, while the model underestimates the accumulation mode number concentrations near the surface, and overestimates the accumulation number concentrations in the free troposphere. Simulated cloud condensation nuclei (CCN) concentrations are within the observational variations. Simulated aerosol optical depth (AOD) and single scattering albedo (SSA) are in reasonable agreement with observations, and the spatial distribution of AOD is consistent with observations, while the model underestimates AOD over regions with strong fossil fuel and biomass burning emissions, and overestimates AOD over regions with strong dust emissions. Overall, this multi-scale aerosol climate model simulates aerosol fields as well as conventional aerosol models.

scholarly journals Functionalization and fragmentation during ambient organic aerosol aging: application of the 2-D volatility basis set to field studies

2012 ◽  
Vol 12 (4) ◽  
pp. 9857-9901 ◽  
Author(s):  
B. N. Murphy ◽  
N. M. Donahue ◽  
C. Fountoukis ◽  
M. Dall'Osto ◽  
C. O'Dowd ◽  
...  
Keyword(s):  
Organic Compounds ◽  
Aqueous Phase ◽  
Transport Model ◽  
Field Studies ◽  
Organic Aerosol ◽  
Basis Set ◽  
Base Case ◽  
Chemical Transport Model ◽  
Heterogeneous Oxidation ◽  
Phase Chemistry

Abstract. Multigenerational oxidation chemistry of atmospheric organic compounds and its effects on aerosol loadings and chemical composition is investigated by implementing the Two-Dimensional Volatility Basis Set (2-D-VBS) in a Lagrangian host chemical transport model. Three model formulations were chosen to explore the complex interactions between functionalization and fragmentation processes during gas-phase oxidation of organic compounds by the hydroxyl radical. The base case model employs a conservative transformation by assuming a reduction of one order of magnitude in effective saturation concentration and an increase of oxygen content by one or two oxygen atoms per oxidation generation. A second scheme simulates functionalization in more detail using group contribution theory to estimate the effects of oxygen addition to the carbon backbone on the compound volatility. Finally, a fragmentation scheme is added to the detailed functionalization scheme to create a functionalization-fragmentation parameterization. Two condensed-phase chemistry pathways are also implemented as additional sensitivity tests to simulate (1) heterogeneous oxidation via OH uptake to the particle-phase and (2) aqueous-phase chemistry of glyoxal and methylglyoxal. The model is applied to summer and winter periods at three sites where observations of organic aerosol (OA) mass and O:C were obtained during the European Integrated Project on Aerosol Cloud Climate and Air Quality Interactions (EUCAARI) campaigns. The base case model reproduces observed mass concentrations and O:C well, with fractional errors (FE) lower than 55% and 25%, respectively. The detailed functionalization scheme tends to overpredict OA concentrations, especially in the summertime, and also underpredicts O:C by approximately a factor of 2. The detailed functionalization model with fragmentation agrees well with the observations for OA concentration, but still underpredicts O:C. Both heterogeneous oxidation and aqueous-phase processing have small effects on OA levels but heterogeneous oxidation, as implemented here, does enhance O:C by about 0.1. The different schemes result in very different fractional attribution for OA between anthropogenic and biogenic sources.

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