Large‐scale chemical evolution of the Arctic vortex during the 1999/2000 winter: HALOE/POAM III Lagrangian photochemical modeling for the SAGE III—Ozone Loss and Validation Experiment (SOLVE) campaign

Abstract : The LaRC Lagrangian Chemical Transport Model (LaRC LCTM) is used to simulate the kinematic and chemical evolution of an ensemble of trajectories initialized from Halogen Occultation Experiment (HALOE) and Polar Ozone and Aerosol Measurement (POAM) III atmospheric soundings over the SAGE III-Ozone Loss and Validation Experiment (SOLVE) campaign period. Initial mixing ratios of species which are not measured by HALOE or POAM III are specified using sunrise and sunset constituent CH(4) and constituent PV regressions obtained from the LaRC IMPACT model, a global three dimensional general circulation and photochemical model. Ensemble averaging of the trajectory chemical characteristics provides a vortex-average perspective of the photochemical state of the Arctic vortex. The vortex-averaged evolution of ozone, chlorine, nitrogen species, and ozone photochemical loss rates is presented. Enhanced chlorine catalyzed ozone loss begins in mid-January above 500 K, and the altitude of the peak loss gradually descends during the rest of the simulation. Peak vortex averaged loss rates of over 60 ppbv/day occur in early March at 450 K. Vortex averaged loss rates decline after mid- March. The accumulated photochemical ozone loss during the period from 1 December 1999 to 30 March 2000 peaks at 450 K with net losses of near 2.2 ppmv. The predicted distributions of CH4, O(3), denitrification, and chlorine activation are compared to the distributions obtained from in situ measurements to evaluate the accuracy of the simulations. The comparisons show best agreement when diffusive tendencies are included in the model calculations, highlighting the importance of this process in the Arctic vortex. Sensitivity tests examining the large-scale influence of orographically generated gravity wave temperature anomalies are also presented. Results from this sensitivity study show that mountain-wave temperature perturbations contribute an additional 2-8% O(3) loss during the 1999/2000 winter.

[1]  Richard Swinbank,et al.  Lower stratospheric temperature differences between meteorological analyses in two cold Arctic winters and their impact on polar processing studies , 2003 .

[2]  M. Chipperfield,et al.  Tracer-Based Determination of Vortex Descent in the 1999-2000 Arctic Winter , 2013 .

[3]  M. Chipperfield,et al.  A vortex‐scale simulation of the growth and sedimentation of large nitric acid hydrate particles , 2002 .

[4]  Jerry Lumpe,et al.  Reconstruction of three-dimensional ozone fields using POAM III during SOLVE , 2002 .

[5]  C. Voigt,et al.  Dehydration in the Arctic stratosphere during the SOLVE/THESEO-2000 campaigns , 2002 .

[6]  M. Chipperfield,et al.  Chemical depletion of Arctic ozone in winter 1999/2000 , 2002 .

[7]  D. Fahey,et al.  An analysis of large HNO3‐containing particles sampled in the Arctic stratosphere during the winter of 1999/2000 , 2002 .

[8]  K. Hoppel,et al.  Interaction between dynamics and chemistry of ozone in the setup phase of the Northern Hemisphere polar vortex: OZONE IN THE SETUP PHASE OF THE POLAR VORTEX , 2002 .

[9]  M. Chipperfield,et al.  Modeling the effect of denitrification on Arctic ozone depletion during winter 1999/2000 , 2002 .

[10]  E. Browell,et al.  Microphysical modeling of the 1999–2000 Arctic winter: 1. Polar stratospheric clouds, denitrification, and dehydration , 2002 .

[11]  E. Atlas,et al.  Hydration, dehydration, and the total hydrogen budget of the 1999/2000 winter Arctic stratosphere , 2002 .

[12]  W. Grose,et al.  Response of middle atmosphere chemistry and dynamics to volcanically elevated sulfate aerosol: Three‐dimensional coupled model simulations , 2001 .

[13]  Costas A. Varotsos,et al.  Arctic ozone loss in threshold conditions: Match observations in 1997/1998 and 1998/1999 , 2001 .

[14]  T. L. Thompson,et al.  The Detection of Large HNO3-Containing Particles in the Winter Arctic Stratosphere , 2001, Science.

[15]  W. Grose,et al.  Dynamical climatology of the NASA Langley Research Center interactive modeling Project for Atmospheric Chemistry and Transport (IMPACT) model , 2000 .

[16]  G. Manney,et al.  Development of the polar vortex in the 1999–2000 Arctic winter stratosphere , 2000 .

[17]  J. Russell,et al.  The contribution of mixing in Lagrangian photochemical predictions of polar ozone loss over the Arctic in summer 1997 , 1999 .

[18]  J. Russell,et al.  Large‐scale stratospheric ozone photochemistry and transport during the POLARIS Campaign , 1999 .

[19]  P. Preusse,et al.  Global Measurements of Stratospheric Mountain Waves from Space. , 1999, Science.

[20]  Gert König-Langlo,et al.  The Polar Ozone and Aerosol Measurement (POAM) III instrument and early validation results , 1999 .

[21]  Stanley C. Solomon,et al.  Stratospheric ozone depletion: A review of concepts and history , 1999 .

[22]  Martyn P. Chipperfield,et al.  Multiannual simulations with a three‐dimensional chemical transport model , 1999 .

[23]  J. Bacmeister,et al.  Widespread solid particle formation by mountain waves in the Arctic stratosphere , 1999 .

[24]  James F. Gleason,et al.  Anomalously low ozone over the Arctic , 1997 .

[25]  P. Crutzen,et al.  Photochemical calculations along air mass trajectories during ASHOE/MAESA , 1997 .

[26]  P. Crutzen,et al.  Chlorine activation and ozone depletion in the Arctic vortex: Observations by the Halogen Occultation Experiment on the Upper Atmosphere Research Satellite , 1996 .

[27]  P. Newman,et al.  An objective determination of the polar vortex using Ertel's potential vorticity , 1996 .

[28]  S. J. Ciciora,et al.  Airborne gas chromatograph for in situ measurements of long‐lived species in the upper troposphere and lower stratosphere , 1996 .

[29]  L. Froidevaux,et al.  Stratospheric trace constituents simulated by a three‐dimensional general circulation model: Comparison with UARS data , 1995 .

[30]  B. Luo,et al.  An analytic expression for the composition of aqueous HNO3‐H2SO4 stratospheric aerosols including gas phase removal of HNO3 , 1995 .

[31]  S. Wofsy,et al.  Removal of Stratospheric O3 by Radicals: In Situ Measurements of OH, HO2, NO, NO2, ClO, and BrO , 1994, Science.

[32]  A. O'Neill,et al.  Mixing processes within the polar night jet , 1994 .

[33]  J. Bacmeister,et al.  An Algorithm for Forecasting Mountain Wave–Related Turbulence in the Stratosphere , 1994 .

[34]  Richard Swinbank,et al.  A Stratosphere-Troposphere Data Assimilation System , 1994 .

[35]  R. May,et al.  Aircraft (ER-2) laser infrared absorption spectrometer (ALIAS) for in-situ stratospheric measurements of HCI, N(2)O, CH(4), NO(2), and HNO(3). , 1994, Applied optics.

[36]  Richard B. Rood,et al.  An assimilated dataset for Earth science applications , 1993 .

[37]  W. Grose,et al.  The Interaction of Radiative and Dynamical Processes during a Simulated Sudden Stratospheric Warming , 1993 .

[38]  R. Pierce,et al.  Chaotic advection in the stratosphere: Implications for the dispersal of chemically perturbed air from the polar vortex , 1993 .

[39]  M. Loewenstein,et al.  Ozone Loss Inside the Northern Polar Vortex During the 1991-1992 Winter , 1993, Science.

[40]  James M. Russell,et al.  The Halogen Occultation Experiment , 1993 .

[41]  G. Toon.  The JPL MkIV interferometer , 1991 .

[42]  D. Hofmann,et al.  Evidence from balloon measurements for chemical depletion of stratospheric ozone in the Arctic winter of 1989–90 , 1991, Nature.

[43]  S. Wofsy,et al.  Loss of ozone in the Arctic vortex for the winter of 1989 , 1990 .

[44]  Roderic L. Jones,et al.  Calculations of ozone destruction during the 1988/89 Arctic winter , 1990 .

[45]  R. Turco,et al.  Physical processes in polar stratospheric ice clouds , 1989 .

[46]  D. Fahey,et al.  In situ measurements of total reactive nitrogen, total water, and aerosol in a polar stratospheric cloud in the Antarctic , 1989 .

[47]  D. Fahey,et al.  In-situ measurements of total reactive nitrogen, total water vapor, and aerosols in polar stratospheric clouds in the Antarctic stratosphere , 1988 .

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