Atmos. Chem. Phys. Discuss., 12, 8053-8106, 2012
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This discussion paper has been under review for the journal Atmospheric Chemistry and Physics (ACP). Please refer to the corresponding final paper in ACP.
Simulations of column-average CO2 and CH4 using the NIES TM with a hybrid sigma-isentropic (σ−θ) vertical coordinate
D. A. Belikov1, S. Maksyutov1, V. Sherlock2, S. Aoki3, N. M. Deutscher4,5, S. Dohe6, D. Griffith5, E. Kyro7, I. Morino1, T. Nakazawa3, J. Notholt4, M. Rettinger8, M. Schneider6, R. Sussmann8, G. C. Toon9, P. O. Wennberg9, and D. Wunch9
1National Institute for Environmental Studies, Tsukuba, Ibaraki, Japan
2Department of Atmospheric Research, National Institute of Water and Atmospheric Research, Wellington, New Zealand
3Center for Atmospheric and Oceanic Studies, Graduate School of Science, Tohoku University, Sendai, Japan
4Institute of Environmental Physics, University of Bremen, Bremen, Germany
5School of Chemistry, University of Wollongong, Wollongong, Australia
6Institute for Meteorology and Climate Research, Karlsruhe Institute of Technology, Karlsruhe, Germany
7Arctic Research Center, Finnish Meteorological Institute, Helsinki, Finland
8Karlsruhe Institute of Technology, IMK-IFU, Garmisch-Partenkirchen, Germany
9Department of Earth Science and Engineering, California Institute of Technology, Pasadena, CA, USA

Abstract. We have developed an improved version of the National Institute for Environmental Studies (NIES) three-dimensional chemical transport model (TM) designed for accurate tracer transport simulations in the stratosphere, given the use of a hybrid sigma-isentropic (σ−θ) vertical coordinate that employs both terrain following and isentropic parts switched smoothly around the tropopause. The air-ascending rate was derived from the effective heating rate and was used to simulate vertical motion in the isentropic part of the grid (above level 350 K), which was adjusted to fit to the observed age of the air in the stratosphere. Multi-annual simulations were conducted using NIES TM to evaluate vertical profiles and dry-air column-averaged mole fractions of CO2 and CH4. Comparisons with balloon-borne observations over Sanriku (Japan) in 2000–2007 revealed that the tracer transport simulations in the upper troposphere and lower stratosphere are performed with accuracies of ~5% for CH4 and SF6, and ~1% for CO2 compared with the observed volume-mixing ratios. The simulated XCO2 and XCH4 were evaluated against daily ground-based high-resolution Fourier Transform Spectrometer (FTS) observations measured at twelve sites of the Total Carbon Column Observing Network (TCCON) (Bialystok, Bremen, Darwin, Garmisch, Izaña, Lamont, Lauder, Orleans, Park Falls, Sodankylä, Tsukuba, and Wollongong) between January 2009 and January 2011. The comparison shows the model's ability to reproduce the site-dependent seasonal cycles as observed by TCCON, with correlation coefficients typically on the order 0.8–0.9 and 0.4–0.8 for XCO2 and XCH4, respectively, and mean model biases of ±0.2% and ±0.5%, excluding Sodankylä, where strong biases are found. The capturing of tracer total column mole fractions is strongly dependent on the model's ability to reproduce seasonal variations in tracer concentrations in the planetary boundary layer (PBL). We found a marked difference in the model's ability to reproduce near-surface concentrations at sites located some distance from multiple emission sources and where high emissions play a notable role in the tracer's budget. Comparisons with aircraft observations over Surgut (West Siberia), in an area with high emissions of methane from wetlands, show contrasting model performance in the PBL and in the free troposphere. This is another instance where the representation of the PBL is critical in simulating the tracer total columns.

Citation: Belikov, D. A., Maksyutov, S., Sherlock, V., Aoki, S., Deutscher, N. M., Dohe, S., Griffith, D., Kyro, E., Morino, I., Nakazawa, T., Notholt, J., Rettinger, M., Schneider, M., Sussmann, R., Toon, G. C., Wennberg, P. O., and Wunch, D.: Simulations of column-average CO2 and CH4 using the NIES TM with a hybrid sigma-isentropic (σ−θ) vertical coordinate, Atmos. Chem. Phys. Discuss., 12, 8053-8106, doi:10.5194/acpd-12-8053-2012, 2012.
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