Chemical behavior of the tropopause observed during the Stratosphere-Troposphere Analyses of Regional Transport experiment

[1] During the Stratosphere-Troposphere Analyses of Regional Transport (START) experiment in December 2005, the behavior of the extratropical tropopause was examined under a variety of dynamical conditions. Using in situ measurements of ozone and water vapor, on board the new NSF/NCAR research aircraft Gulfstream V, and data from large-scale meteorological analyses, we address issues of the tropopause definitions and sharpness. Comparisons of the data from two flights show that the sharpness of chemical transitions across the tropopause varies with the sharpness of the static stability change across the tropopause. Using tracer correlations, air masses of mixed stratospheric and tropospheric characteristics are identified. The mixed air mass does not form a uniform mixing layer near the tropopause, but rather shows strong spatial variation. A depth of mixed air (∼5 km in vertical distribution) is found on the cyclonic side of the polar jet, where the thermal gradient is weak and significant separation occurs between the thermal and the dynamical tropopause. Away from the jet or on the anticyclonic side of the jet, where the stability gradient is strong, the chemical transition across the tropopause was much more abrupt and shows minimum mixing. In both cases (either significant or minimal mixing), the thermal tropopause is shown to be approximately at the center of the mixing layer, and the altitude relative to the thermal tropopause is found to be an effective coordinate for locating the chemical transition. To further understand the role of the thermal and dynamical tropopause as a chemical transport boundary, tracer correlations are used to examine the chemical characteristics, and the trajectory calculations are used to infer the fate of the air mass between the thermal and dynamic tropopauses in the region of significant separation. The tracer correlation analysis shows that the air mass in this region is a mixture of stratospheric and tropospheric air but predominantly of tropospheric characteristics. Trajectory model calculations show that a significant fraction of the air parcels in this region ended in the mid to lower troposphere, which suggest the irreversible nature of the observed stratospheric intrusion.

[1]  A. Kochanski CROSS SECTIONS OF THE MEAN ZONAL FLOW AND TEMPERATURE ALONG 8O°W , 1955 .

[2]  M. Hegglin,et al.  Seasonality and extent of extratropical TST derived from in-situ CO measurements during SPURT , 2004 .

[3]  D. McKenna,et al.  Contribution of mixing to the upward transport across the TTL , 2006 .

[4]  K. Hoinka Die Tropopause: Entdeckung, Definition, Bestimmung , 1997 .

[5]  G. Brasseur,et al.  A set of diagnostics for evaluating chemistry‐climate models in the extratropical tropopause region , 2007 .

[6]  C. Barnet,et al.  Validation of AIRS v4 ozone profiles in the UTLS using ozonesondes from Lauder, NZ and Boulder, USA , 2007 .

[7]  G. Vaughan,et al.  The potential for stratosphere‐troposphere exchange in cut‐off‐low systems , 1993 .

[8]  E. Danielsen,et al.  Stratospheric-Tropospheric Exchange Based on Radioactivity, Ozone and Potential Vorticity , 1968 .

[9]  Moustafa T. Chahine,et al.  Biases in total precipitable water vapor climatologies from Atmospheric Infrared Sounder and Advanced Microwave Scanning Radiometer , 2006 .

[10]  A. Stohl,et al.  A textbook example of long‐range transport: Simultaneous observation of ozone maxima of stratospheric and North American origin in the free troposphere over Europe , 1999 .

[11]  R. Toumi,et al.  An entropy‐based measure of mixing at the tropopause , 2006 .

[12]  E. Shuckburgh,et al.  Effective diffusivity as a diagnostic of atmospheric transport: 1. Stratosphere , 2000 .

[13]  W. Randel,et al.  Definitions and sharpness of the extratropical tropopause: A trace gas perspective , 2004 .

[14]  K. Bowman,et al.  Observations of fine‐scale transport structure in the upper troposphere from the High‐performance Instrumented Airborne Platform for Environmental Research , 2007 .

[15]  H. Wernli,et al.  A Lagrangian “1‐year climatology” of (deep) cross‐tropopause exchange in the extratropical Northern Hemisphere , 2002 .

[16]  Brian J. Hoskins Towards a PV- θ view of the general circulation , 1991 .

[17]  C. Brenninkmeijer,et al.  New directions: A chemical tropopause defined , 2003 .

[18]  V. Wirth Cyclone–Anticyclone Asymmetry Concerning the Height of the Thermal and the Dynamical Tropopause , 2001 .

[19]  Enhanced new particle formation observed in the northern midlatitude tropopause region , 2007 .

[20]  Christopher D. Barnet,et al.  Accuracy of geophysical parameters derived from Atmospheric Infrared Sounder/Advanced Microwave Sounding Unit as a function of fractional cloud cover , 2006 .

[21]  J. Holton,et al.  Stratosphere‐troposphere exchange , 1995 .

[22]  Jos Lelieveld,et al.  Tracer correlations in the northern high latitude lowermost stratosphere: Influence of cross‐tropopause mass exchange , 2000 .

[23]  G. Vaughan,et al.  A comparison of ozone and thermal tropopause heights and the impact of tropopause definition on quantifying the ozone content of the troposphere , 1996 .

[24]  V. L. Orkin,et al.  Scientific Assessment of Ozone Depletion: 2010 , 2003 .

[25]  T. L. Thompson,et al.  Convective transport of reactive constituents to the tropical and mid-latitude tropopause region: I. Observations , 2004 .

[26]  E. Browell,et al.  Observations and model simulations of mixing near the extratropical tropopause , 2006 .

[27]  D. Fahey,et al.  Transport into the northern hemisphere lowermost stratosphere revealed by in situ tracer measurements , 1999 .

[28]  S. Wofsy,et al.  Troposphere‐to‐stratosphere transport in the lowermost stratosphere from measurements of H2O, CO2, N2O and O3 , 1998 .

[29]  T. L. Thompson,et al.  Quantifying Stratospheric Ozone in the Upper Troposphere with in Situ Measurements of HCl , 2004, Science.

[30]  M. Hoerling,et al.  Global objective tropopause analysis , 1991 .

[31]  J. Staehelin,et al.  Measurements of NO, NO y , N 2 O, and O 3 during SPURT: implications for transport and chemistry in the lowermost stratosphere , 2005 .

[32]  D. Seidel,et al.  Observational characteristics of double tropopauses , 2007 .

[33]  K. Cehak ReviewAtmospheric circulation systems: PALMÉN, E. and C.W. NEWTON (1969): Their Structure and Physical Interpretation 603 pp., 250 figs., 23 tables. International Geophysics Series, vol. 13. New York/ London: Academic Press. $ 26.00 , 1971 .

[34]  B. Hoskins,et al.  On the use and significance of isentropic potential vorticity maps , 2007 .

[35]  L. Horowitz,et al.  On the life cycle of a stratospheric intrusion and its dispersion into polluted warm conveyor belts , 2004 .

[36]  Kenneth P. Bowman,et al.  Large-scale isentropic mixing properties of the Antarctic polar vortex from analyzed winds , 1993 .

[37]  E. Weinstock,et al.  Mechanisms controlling water vapor in the lower stratosphere: “A tale of two stratospheres” , 1995 .

[38]  M. Shapiro Turbulent Mixing within Tropopause Folds as a Mechanism for the Exchange of Chemical Constituents between the Stratosphere and Troposphere , 1980 .

[39]  J. Lamarque,et al.  Hemispheric asymmetries and seasonal variations of the lowermost stratospheric water vapor and ozone derived from , 1997 .

[40]  M. Hegglin,et al.  Seasonal cycles and variability of O 3 and H 2 O in the UT/LMS during SPURT , 2005 .

[41]  John Y. N. Cho,et al.  Observations of convective and dynamical instabilities in tropopause folds and their contribution to stratosphere-troposphere exchange , 1999 .

[42]  P. Crutzen,et al.  Identification of extratropical two‐way troposphere‐stratosphere mixing based on CARIBIC measurements of O3, CO, and ultrafine particles , 2000 .

[43]  Michael Sprenger,et al.  A NEW PERSPECTIVE OF STRATOSPHERE-TROPOSPHERE EXCHANGE , 2003 .

[44]  D. McKenna,et al.  A new Chemical Lagrangian Model of the Stratosphere (CLaMS) 1. Formulation of advection and mixing , 2002 .

[45]  K. Hoinka The Tropopause: Discovery, Definition and Demarcation , 1997 .

[46]  M. Proffitt,et al.  Fast‐response dual‐beam UV‐absorption ozone photometer suitable for use on stratospheric balloons , 1983 .

[47]  Jennifer A. Logan,et al.  An analysis of ozonesonde data for the troposphere : recommendations for testing 3-D models and development of a gridded climatology for tropospheric ozone , 1999 .

[48]  R. K. Scott,et al.  Wave Breaking and Mixing at the Subtropical Tropopause , 2002 .

[49]  J. Lelieveld,et al.  Seasonal variations of a mixing layer in the lowermost stratosphere as identified by the CO‐O3 correlation from in situ measurements , 2002 .

[50]  Holger Vömel,et al.  The water vapour distribution in the Arctic lowermost stratosphere during the LAUTLOS campaign and related transport processes including stratosphere-troposphere exchange , 2006 .

[51]  Andrew Gettelman,et al.  Validation of satellite ozone profile retrievals using Beijing ozonesonde data , 2007 .

[52]  S. Sherwood,et al.  On the control of stratospheric humidity , 2000 .

[53]  Brian J. Hoskins,et al.  The tropical tropopause , 1998 .