References

ACPD

Atmospheric Chemistry and Physics Discussions

ACPD

1680-7375

Copernicus GmbH

Göttingen, Germany

10.5194/acpd-12-10331-2012

Improvements of organic aerosol representations and their effects in large-scale atmospheric models

Tost

¹ Pringle

K. J.

Institut für Physik der Atmosphäre, Johannes Gutenberg Universität, Mainz, Germany

School of Earth and Environment, University of Leeds, Woodhouse Lane, Leeds, UK

20 04 2012

12 4 10331 10379

This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited.

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Organics dominate the composition of the atmospheric aerosol, especially in the fine mode, influencing some of its characteristics such as the hygroscopicity, which is of climatic relevance for the Earth system. This study targets an improvement in the description of organic aerosols suitable for large-scale modelling, making use of recent developments based on laboratory and field measurements. In addition to the organic mass and particle number distribution, the proposed method keeps track of the oxidation state of the aerosol based on the OH exposure time, describing some of its chemical characteristics. This study presents the application of the method in a global chemistry climate model, investigates the sensitivity to process formulations and emission assignments, provides a comparison with observations and analyses the climate impact. <br><br> Even though the organic aerosol mass distribution is hardly affected by the new formulation, it shows impacts (regionally of the order of 10% to 20%) on parameters directly influencing climate via the direct and indirect aerosol effects. Furthermore, the global distribution of the organic O:C ratio is analysed in detail, leading to different regimes in the oxidation state: low O:C ratios over the tropical continents due to small OH concentrations caused by OH depletion in chemical reactions, and enhanced oxidation states over the tropical oceans based on the OH abundance and at high altitudes due to longer atmospheric residence time. Due to the relation between O:C ratio and the aerosol hygroscopicity the ageing results in a more accurate description of aerosol water uptake by the organic aerosol. In comparison with observations reasonable agreement within the limits of a global model of the simulations is achieved.

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% Taraborrelli,~D., Lawrence,~M G., Butler,~T M., Sander,~R., and % Lelieveld,~J.: Mainz Isoprene Mechanism 2 (MIM2): an isoprene % oxidation mechanism for regional and global atmospheric modelling, % Atmos. Chem. Phys., 9, 2751–2777, http://dx.doi.org/10.5194/acp-9-2751-2009doi:10.5194/acp-9-2751-2009, % 2009. ### SELF-REFERENCE ### Taraborrelli,~D., Lawrence,~M G., Butler,~T M., Sander,~R., and Lelieveld,~J.: Mainz Isoprene Mechanism 2 (MIM2): an isoprene oxidation mechanism for regional and global atmospheric modelling, Atmos. Chem. Phys., 9, 2751–2777, http://dx.doi.org/10.5194/acp-9-2751-2009doi:10.5194/acp-9-2751-2009, 2009.

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% Tost,~H., Jöckel,~P., Kerkweg,~A., Sander,~R., and % Lelieveld,~J.: Technical Note: A new comprehensive SCAVenging % submodel for global atmospheric chemistry modelling, % Atmos. Chem. Phys., 6, 565–574, 2006. ### SELF-REFERENCE ### Tost,~H., Jöckel,~P., Kerkweg,~A., Sander,~R., and Lelieveld,~J.: Technical note: A new comprehensive SCAVenging submodel for global atmospheric chemistry modelling, Atmos. Chem. Phys., 6, 565–574, http://dx.doi.org/10.5194/acp-6-565-2006doi:10.5194/acp-6-565-2006, 2006.

% Tost,~H., Jöckel,~P., Kerkweg,~A., Pozzer,~A., Sander,~R., and % Lelieveld,~J.: Global cloud and precipitation chemistry and wet % deposition: tropospheric model simulations with ECHAM5/MESSy1, % Atmos. Chem. Phys., 7, 2733–2757, 2007a. ### SELF-REFERENCE ### Tost,~H., Jöckel,~P., Kerkweg,~A., Pozzer,~A., Sander,~R., and Lelieveld,~J.: Global cloud and precipitation chemistry and wet deposition: tropospheric model simulations with ECHAM5/MESSy1, Atmos. Chem. Phys., 7, 2733–2757, http://dx.doi.org/10.5194/acp-7-2733-2007doi:10.5194/acp-7-2733-2007, 2007a.

% Tost,~H., Jöckel,~P., and Lelieveld,~J.: Lightning and % convection parameterisations – uncertainties in global modelling, % Atmos. Chem. Phys., 7, 4553–4568, 2007b. ### SELF-REFERENCE ### Tost,~H., Jöckel,~P., and Lelieveld,~J.: Lightning and convection parameterisations – uncertainties in global modelling, Atmos. Chem. Phys., 7, 4553–4568, http://dx.doi.org/10.5194/acp-7-4553-2007doi:10.5194/acp-7-4553-2007, 2007b.

% Tost,~H., Lawrence,~M G., Brühl,~C., Jöckel,~P., % GABRIEL-Team, and SCOUT-O3-DARWIN/ACTIVE-Team: Uncertainties in % atmospheric chemistry modelling due to convection % parameterisations and subsequent scavenging, Atmos. Chem. Phys., % 10, 1931–1951, http://dx.doi.org/10.5194/acp-10-1931-2010doi:10.5194/acp-10-1931-2010, 2010. ### % SELF-REFERENCE ### Tost,~H., Lawrence,~M G., Brühl,~C., Jöckel,~P., The~GABRIEL~Team, and The~SCOUT-O3-DARWIN/ACTIVE~Team: Uncertainties in atmospheric chemistry modelling due to convection parameterisations and subsequent scavenging, Atmos. Chem. Phys., 10, 1931–1951, http://dx.doi.org/10.5194/acp-10-1931-2010doi:10.5194/acp-10-1931-2010, 2010a.

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% Wex,~H., Petters,~M D., Carrico,~C M., Hallbauer,~E., % Massling,~A., McMeeking,~G R., Poulain,~L., Wu,~Z., % Kreidenweis,~S M., and Stratmann,~F.: Towards closing the gap % between hygroscopic growth and activation for secondary organic % aerosol: Part 1 – Evidence from measurements, Atmos. Chem. Phys., % 9, 3987–3997, http://dx.doi.org/10.5194/acp-9-3987-2009doi:10.5194/acp-9-3987-2009, 2009. ### % SELF-REFERENCE ### Wex,~H., Petters,~M D., Carrico,~C M., Hallbauer,~E., Massling,~A., McMeeking,~G R., Poulain,~L., Wu,~Z., Kreidenweis,~S M., and Stratmann,~F.: Towards closing the gap between hygroscopic growth and activation for secondary organic aerosol: Part 1 – Evidence from measurements, Atmos. Chem. Phys., 9, 3987–3997, http://dx.doi.org/10.5194/acp-9-3987-2009doi:10.5194/acp-9-3987-2009, 2009.