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Role of aerosol chemical composition on the formation of cloud condensation nuclei during biomass burning periods
Role of aerosol chemical composition on the formation of cloud condensation nuclei during biomass burning periods
Swen Metzger1, Ivonne Trebs1, Laurens Ganzeveld1,
Jos Lelieveld1, Philip Stier2, Franz X. Meixner1, Meinrat O. Andreae1, Paulo Artaxo3
Swen Metzger1, Ivonne Trebs1, Laurens Ganzeveld1,
Jos Lelieveld1, Philip Stier2, Franz X. Meixner1, Meinrat O. Andreae1, Paulo Artaxo3
Wednesday, 28/07/04, III LBA Scientific Conference - Brasília, July 27-29, 2004
Wednesday, 28/07/04, III LBA Scientific Conference - Brasília, July 27-29, 2004
11Max-Planck Institute for Chemistry, Mainz, GermanyMax-Planck Institute for Chemistry, Mainz, Germany22Max-Planck Institute for Meteorology, Hamburg, GermanyMax-Planck Institute for Meteorology, Hamburg, Germany
33Instituto de Fisica, Universidade de Sao Paulo, BrasilInstituto de Fisica, Universidade de Sao Paulo, Brasil
© Greg Roberts
Introduction
The chemical composition of atmospheric aerosols plays an The chemical composition of atmospheric aerosols plays an
important role for the hygroscopic growth and the aerosol-important role for the hygroscopic growth and the aerosol-
associated water mass. associated water mass.
Biomass burning events are likely to alter the chemical Biomass burning events are likely to alter the chemical
composition due to the emission of inorganic cations, such as composition due to the emission of inorganic cations, such as
potassium, and organic acids.potassium, and organic acids.
We therefore investigate their impact on the chemical We therefore investigate their impact on the chemical
composition and on the aerosol water mass, which is important composition and on the aerosol water mass, which is important
for the cloud formation.for the cloud formation.
Thermodynamical aerosol model: EQSAM;
Gas/liquid/solid partitioning
HNO3, NH3, H2SO4, HCl,
organic acids (g) Ions, liquid phase
NO3-, NH4
+, SO42-, Cl-,
lumped Low Molecular Weight (LMW) organic acids (e.g., HCOOH), Na+, K+, Ca2+, Mg2+,
H2O, pH
Salts, Solid phase
NH4NO3, NH4HSO4, (NH4)2SO4,
NH4 & organic acids
Temperature & relative humidityTemperature & relative humidity
R1
NH4NO3, NH4HSO4, (NH4)2SO4,
NH4 & organic acids
NO3-, NH4
+, SO42-, Cl-,
LMW organic acids (e.g., HCOOH), Na+, K+, Ca2+, Mg2+, H2O,
pH
R2
Model Application - SMOCC Data
Na/Cl-NH3/NH4-HNO3/NO3-H2SO4/SO4-H2O-System
Reduced aerosol systems compare relatively good for the wrong reason !Reduced aerosol systems compare relatively good for the wrong reason !
Model simulations:
box model constrained with observed T, RH & total gas-particulate mass (Trebs et al., in prep.)
K-Ca-Mg-Na/Cl-NH3/NH4-HNO3/NO3-H2SO4/SO4-H2O-Systemwith K-Ca-Mg as equivalent Na
All models compare reasonable well when applied with the same complexityAll models compare reasonable well when applied with the same complexity
Model Application - SMOCC Data
But they all underestimate the But they all underestimate the observed aerosol NHobserved aerosol NH44
++ concentration!concentration!
Model Application - SMOCC Data
K-Ca-Mg-Na/Cl-NH3/NH4-HNO3/NO3-H2SO4/SO4-H2O-Systemwith K-Ca-Mg considered explicitly in EQSAM/SCAPE2
Crustal elements considered in EQSAM; same ammonium loss as SCAPE2Crustal elements considered in EQSAM; same ammonium loss as SCAPE2KK++ drives NH4 drives NH4++ out of the aerosol phase, out of the aerosol phase, in contrast to the observationsin contrast to the observations! !
Reduced aerosol systems for Isorropia Reduced aerosol systems for Isorropia compares relatively good for the compares relatively good for the
wrong reason !wrong reason !
Model Application - SMOCC Data
LMW organic acids gets the ammonium back in the aerosol phaseLMW organic acids gets the ammonium back in the aerosol phase
Including LMW organic acids in EQSAM
Reduced aerosol systems for Isorropia Reduced aerosol systems for Isorropia compares relatively good for the compares relatively good for the
wrong reason !wrong reason ! Consistent inclusion of KConsistent inclusion of K++ and LMW and LMW organic acids in EQSAMorganic acids in EQSAM
MModular odular EEarth arth SSubmodel ubmodel SySystem (MESSy) coupled to GCM stem (MESSy) coupled to GCM ECHAM5ECHAM5
http://www.messy-interface.orghttp://www.messy-interface.org
MModular odular EEarth arth SSubmodel ubmodel SySystem (MESSy) coupled to GCM stem (MESSy) coupled to GCM ECHAM5ECHAM5
http://www.messy-interface.orghttp://www.messy-interface.org
ECHAM5ECHAM5
Polar Stratospheric Cloudsmicro-physics and sedimentation
Polar Stratospheric Cloudsmicro-physics and sedimentation
Aerosol Physics (& chemistry) Thermodynamical aerosol
composition module and size-resolving dynamical module
Aerosol Physics (& chemistry) Thermodynamical aerosol
composition module and size-resolving dynamical module
14CO / Radonnatural atmospheric tracer, evaluation
of tropospheric OH. STE / PBL transport
14CO / Radonnatural atmospheric tracer, evaluation
of tropospheric OH. STE / PBL transport
Eulerian Transport Schemes Eulerian Transport Schemes
Lagrangian Transport Scheme
Lagrangian Transport Scheme
Natural and Anthropogenic Emissionsbiogenic surface emissions and anthropogenic emissions
Natural and Anthropogenic Emissionsbiogenic surface emissions and anthropogenic emissions
Gas-phase and Heterogeneous Chemistry
using Kinetic PreProcessor (KPP)
Gas-phase and Heterogeneous Chemistry
using Kinetic PreProcessor (KPP)
MBL Chemistryswitchable extension with chemistry
scheme
MBL Chemistryswitchable extension with chemistry
scheme
Photolysisfast on-line scheme
Photolysisfast on-line scheme
Diagnostic and Output(e.g., PBL and tropopause height)
Diagnostic and Output(e.g., PBL and tropopause height)
ScavengingBelow and in-cloud scavenging of
gases and aerosols
ScavengingBelow and in-cloud scavenging of
gases and aerosols
Dry Depositiondry deposition of gases and aerosols
Dry Depositiondry deposition of gases and aerosols
Convection & Tracer Transport
Convection & Tracer Transport
Stratospheric Water VaporStratospheric Water Vapor
Lightning NOxLightning NOx
Coupled chemistry-GCM
G: 6N: 7M: 34total: 471. N
2. BC-OA1a3. BC-OA2a4. NO3 5.NH4 6. SO4
7. SOA1 8. SOA2
1. N2. SO43. BC => BC-OA1a, BC-OA2a4. OC => SOA1 8. SOA25. SS => SS-Na 12.SS-Cl6. DU => DU1, DU27./8./9. NO3, NH4, H2O
1. N2. BC-OA1a3. BC-OA2a4. NO3 5. NH4 6. SO4
7. SOA1 8. SOA29. DU1 10.DU2 11. SS-Na 12.SS-Cl
1. N2. H2SO4Nucleation
Aitken
Accumulation
Coarse
H2SO4
NH3
HNO3
SOA1SOA2HCl
soluble (liquid/solid)
1. N 2. BC-OA1 (primary) 3. BC-OA2 (primary)
1. N 2. DU3 (solid Si-core)
1. N 2. DU3 (solid Si-core)
insoluble (solid)
2.
1.
3.
4.
5.
6.
7.
<=>
GasphaseNew M7/EQSAM Structure
Coupled chemistry-GCM: Aerosol modeling
As an example:
EQSAM-M7: Aerosol Water [1e-9 kg/kg] (ug/kg) (PBL monthly mean, august)
Coupled chemistry-GCM: Aerosol modeling
M7: Aerosol Water [1e-9 kg/kg]
Coupled chemistry-GCM: Aerosol modeling
ECHAM5: Cloud Water [1e-6 kg/kg]
Coupled chemistry-GCM: Aerosol modeling
EQSAM-M7: Aerosol Water [1e-9 kg/kg] M7: Aerosol Water [1e-9 kg/kg]
Qualitive comparison of cloud and aerosol water spatial distributionQualitive comparison of cloud and aerosol water spatial distribution
There is a larger spatial variability in the global distribution of the EQSAM-M7 There is a larger spatial variability in the global distribution of the EQSAM-M7 aerosol water compared to M7, which only includes non-volatile sodium and aerosol water compared to M7, which only includes non-volatile sodium and sulfatesulfate
Conclusion/Outlook
Comparison of the aerosol NHComparison of the aerosol NH44++ content simulated with EQSAM and LBA- content simulated with EQSAM and LBA-
SMOCC observations shows the aerosol chemical composition needs to be SMOCC observations shows the aerosol chemical composition needs to be included consistently, e.g., for biomass burning including not only potassium included consistently, e.g., for biomass burning including not only potassium but also LMW acids.but also LMW acids.
For detailed questions/remarks: [email protected] detailed questions/remarks: [email protected]
The spatial variability in the EQSAM-M7 aerosol water is more similar The spatial variability in the EQSAM-M7 aerosol water is more similar compared to the spatial variability in ECHAM5’s cloud water, suggesting that compared to the spatial variability in ECHAM5’s cloud water, suggesting that the more detailed representation of the aerosol chemical composition in the more detailed representation of the aerosol chemical composition in EQSAM-M7 will facilitate a direct coupling of the aerosol model to ECHAM5’s EQSAM-M7 will facilitate a direct coupling of the aerosol model to ECHAM5’s cloud representation with respect to CCN activation.cloud representation with respect to CCN activation.
Evaluation of the ECHAM5 water/cloud fields, coupled to EQSAM-M7, with Evaluation of the ECHAM5 water/cloud fields, coupled to EQSAM-M7, with satellite observations (satellite observations (R. LangR. Lang). ).
Calculations of CCN and ICN in MESSy-ECHAM5 by explicitly coupling the Calculations of CCN and ICN in MESSy-ECHAM5 by explicitly coupling the cloud- and aerosol water content based on the ionic composition that reflects cloud- and aerosol water content based on the ionic composition that reflects the actual aerosol composition (incl. gas/liquid/solid aerosol partitioning)the actual aerosol composition (incl. gas/liquid/solid aerosol partitioning)
Outlook
For detailed questions/remarks: [email protected] detailed questions/remarks: [email protected]
MESSy – coupling chemistry etc. to GCMsMax-Planck Institute for Chemistry, Mainz, Germanyin collaboration withDLR Oberpfaffenhofen, GermanyMPI for Meteorology, Hamburg, Germany
Chemistry: R. Sander, A. Kerkweg, R. von Kuhlmann, B. Steil, R. von Glasow
Lagrangian Advection: C. Reithmeier, V. Grewe,G. Erhardt, R. Sausen, P. Jöckel, M. Traub
Aerosols: S. Metzger, P. Stier, A. Kerkweg,J. Wilson+, E.Vignati+, J. Feichter
Emission/Deposition: L. Ganzeveld, P. Stier,J. van Aardenne, Y. Balkanski+, M. Schulz+,W. Guelle+, V. Grewe, P. Jöckel, S. Metzger,G. J. Roelofs+
Polar stratospheric clouds: J. Buchholz,S. Meilinger, K. Carslaw
Photolysis: J. Landgraf, C. Brühl, P. Jöckel,R. Sander
Scavenging: H. Tost, L. Ganzeveld
Convective tracer transport: M. Lawrence, H. Tost,P. Jöckel, S. Brinkop, M. Ponater, C. Kurz
14CO, 222Rn, and passive tracer diagnostics:P. Jöckel
Tropopause diagnostics: P. Jöckel, M. TraubStratospheric H2O: C. Brühl, B Steil, P. JöckelTracer assimilation: L. Ganzeveld, P. JöckelFlexible data output: A. Rhodin, R. Sander,
P. Jöckel
Automatic rediscretization of input data: P. Jöckel
http://www.messy-interface.org
+external contribution, current maintainer/coordinator
... to be extended ...
more detailed references: see web-page
Scientific Coordination: Jos LelieveldTechnical Coordination: Patrick Jöckel & Rolf Sander
Contributions to the program code:
1. Metzger, S. M., Gas/Aerosol Partitioning: A simplified Method for Global Modeling, Ph.D. Thesis,
University Utrecht, The Netherlands, 2000.
http://www.library.uu.nl/digiarchief/dip/diss/1930853/inhoud.htm
2. Metzger, S. M., F. J. Dentener, J. Lelieveld, and S. N. Pandis, Gas/aerosol Partitioning I:
A Computationally Efficient Model. J Geophys. Res., 107, D16, 10.1029/2001JD001102, 2002.
http://www.agu.org/journals/jd/jd0216/2001JD001102/index.html
3. Metzger, S. M., F. J. Dentener, A. Jeuken, and M. Krol, J. Lelieveld, Gas/aerosol Partitioning II:
Global Modeling Results. J Geophys. Res., 107, D16, 10.1029/2001JD001103, 2002.
http://www.agu.org/journals/jd/jd0216/2001JD001103/index.html
4. Metzger, S. M., Gas/aerosol partitioning III: Model development (EQSAM) and comparison (MINOS
Data), in preparation.
The new version of EQSAM has been successfully applied within the EMEP modelling framework.
Results are included in the EMEP reports, http://www.emep.int/common_publications.html, 2003.
5. Trebs, I., S. Metzger, F. X. Meixner, G. Helas, A. Hoffer, M. O. Andreae, M. A.L. Moura, R. S. da Silva
(Jr.), J. Slanina, Y. Rudich, A. Falkovich, P. Artaxo, The NH4+-NO3–-Cl–-SO42–-H2O system and its gas
phase precursors at a rural site in the Amazon Basin: How relevant are crustal species and soluble organic
compounds?, in preparation for JGR.
References