A modified band approach for the accurate calculation of online photolysis rates in stratospheric-tropospheric Chemical Transport Models

Here we present an efficient and accurate method for the online calculation of photolysis rates relevant to both the stratosphere and troposphere for use in global Chem- istry Transport Models and General Circulation Models. The method is a modified version of the band model introduced by Landgraf and Crutzen (1998) which has been updated to improve the performance of the approach for solar zenith an- gles >72 without the use of any implicit parameterisations. For this purpose, additional sets of band parameters have been defined for instances where the incident angle of the light beam is between 72-93 , in conjunction with a scaling component for the far UV region of the spectrum ( =178.6- 202.0 nm). For incident angles between 85-93 we introduce a modification for pseudo-sphericity that improves the accu- racy of the 2-stream approximation. We show that this mod- ified version of the Practical Improved Flux Method (PIFM) is accurate for angles <93 by comparing the resulting height resolved actinic fluxes with a recently developed full spher- ical reference model. We also show that the modified band method is more accurate than the original, with errors gener- ally being less than ±10% throughout the atmospheric col- umn for a diverse range of chemical species. Moreover, we perform certain sensitivity studies that indicate it is robust and performs well over a wide range of conditions relevant to the atmosphere.

[1]  Benjamin M. Herman,et al.  Evaluation of the pseudo‐spherical approximation for backscattered ultraviolet radiances and ozone retrieval , 1997 .

[2]  Oliver Wild,et al.  Fast-J: Accurate Simulation of In- and Below-Cloud Photolysis in Tropospheric Chemical Models , 2000 .

[3]  W. Kouker,et al.  The Karlsruhe simulation model of the middle atmosphere (KASIMA). Version 1 , 1995 .

[4]  H. Bovensmann,et al.  Impact of Accurate Photolysis Calculations on the Simulation of Stratospheric Chemistry , 2003 .

[5]  Veronika Eyring,et al.  Impact of large solar zenith angles on lower stratospheric dynamical and chemical processes in a coupled chemistry-climate model , 2003 .

[6]  Donal P. Murtagh,et al.  Model studies of the influence of O2 photodissociation parameterizations in the Schumann-Runge bands on ozone related photolysis in the upper atmosphere , 1996 .

[7]  J. Landgraf,et al.  Linearization of a radiative transfer model in spherical geometry , 2006 .

[8]  A. Ravishankara,et al.  Quantum yields for production of O(1D) in the ultraviolet photolysis of ozone: Recommendation based on evaluation of laboratory data , 2002 .

[9]  William D. Collins,et al.  Effect of clouds on photolysis and oxidants in the troposphere , 2003 .

[10]  Wissenschaftliche Berichte,et al.  The Karlsruhe Simulation Model of the Middle Atmosphere (KASIMA) Version 2 , 1999 .

[11]  Simon Chabrillat,et al.  Simple parameterization of the absorption of the solar Lyman‐alpha line , 1997 .

[12]  A. T. Young,et al.  Revised optical air mass tables and approximation formula. , 1989, Applied optics.

[13]  P. Crutzen,et al.  Scenarios of possible changes in atmospheric temperatures and ozone concentrations due to man's activities, estimated with a one-dimensional coupled photochemical climate model , 1988 .

[14]  G. Rybicki Radiative transfer , 2019, Climate Change and Terrestrial Ecosystem Modeling.

[15]  D. Murcray Optical Properties of the Atmosphere , 1968 .

[16]  Mark Lawrence,et al.  A model for studies of tropospheric photochemistry: Description, global distributions, and evaluation , 1999 .

[17]  K. Stamnes,et al.  A reliable and efficient two-stream algorithm for spherical radiative transfer: Documentation of accuracy in realistic layered media , 1995 .

[18]  J. Feather The Printing Office , 1985 .

[19]  C. Bohren,et al.  An introduction to atmospheric radiation , 1981 .

[20]  A. Slingo A GCM Parameterization for the Shortwave Radiative Properties of Water Clouds , 1989 .

[21]  David J. Lary,et al.  Refraction and atmospheric photochemistry , 1997 .

[22]  L. J. Cox Optical Properties of the Atmosphere , 1979 .

[23]  Finite element method for the two-dimensional atmospheric radiative transfer , 2005 .

[24]  K. Stamnes,et al.  Numerically stable algorithm for discrete-ordinate-method radiative transfer in multiple scattering and emitting layered media. , 1988, Applied optics.

[25]  Vladimir V. Rozanov,et al.  A numerical radiative transfer model for a spherical planetary atmosphere: combined differential-integral approach involving the Picard iterative approximation , 2001 .

[26]  R. A. Cox,et al.  Evaluated kinetic and photochemical data for atmospheric chemistry: Supplement V , 1996 .

[27]  O. Boucher,et al.  Estimates of the direct and indirect radiative forcing due to tropospheric aerosols: A review , 2000 .

[28]  S. Koch,et al.  Photochemistry of Methylglyoxal in the Vapor Phase , 1998 .

[29]  Roger Atkinson,et al.  Evaluated kinetic and photochemical data for atmospheric chemistry: Supplement IV: IUPAC subcommittee on gas kinetic data evaluation for atmospheric chemistry , 1992 .

[30]  S. Madronich Photodissociation in the atmosphere: 1. Actinic flux and the effects of ground reflections and clouds , 1987 .

[31]  R. A. Cox,et al.  Evaluated kinetic and photochemical data for atmospheric chemistry: Volume III - gas phase reactions of inorganic halogens , 2006 .

[32]  Sasha Madronich,et al.  Numerical integration errors in calculated tropospheric photodissociation rate coefficients , 1990 .

[33]  Otto P. Hasekamp,et al.  Linearization of a pseudo-spherical vector radiative transfer model , 2004 .

[34]  M. Nicolet,et al.  On the molecular scattering in the terrestrial atmosphere : An empirical formula for its calculation in the homosphere , 1984 .

[35]  R. A. Cox,et al.  Evaluated Kinetic, Photochemical and Heterogeneous Data for Atmospheric Chemistry: Supplement V. IUPAC Subcommittee on Gas Kinetic Data Evaluation for Atmospheric Chemistry , 1997 .

[36]  G. Carmichael,et al.  Sensitivity of photolysis rates and ozone production in the troposphere to aerosol properties , 1999 .

[37]  A. Ravishankara,et al.  Quantum yields of O(¹D) in the photolysis of ozone between 289 and 329 nm as a function of temperature , 1998 .

[38]  J. Frederick,et al.  Effective photodissociation cross sections for molecular oxygen and nitric oxide in the Schumann-Runge bands , 1982 .

[39]  Y. Yung,et al.  Atmospheric Radiation: Theoretical Basis , 1989 .

[40]  E. Shettle,et al.  Models for the aerosols of the lower atmosphere and the effects of humidity variations on their optical properties , 1979 .

[41]  J. Lelieveld,et al.  N2O and O3 relationship in the lowermost stratosphere: A diagnostic for mixing processes as represented by a three-dimensional chemistry-transport model , 2000 .

[42]  Paul J. Crutzen,et al.  An efficient method for online calculations of photolysis and heating rates , 1998 .

[43]  M. Prather,et al.  Fast-J2: Accurate Simulation of Stratospheric Photolysis in Global Chemical Models , 2002 .

[44]  Philip J. Rasch,et al.  MOZART, a global chemical transport model for ozone and related chemical tracers: 1. Model description , 1998 .

[45]  J. Lenoble Radiative transfer in scattering and absorbing atmospheres: Standard computational procedures , 1985 .

[46]  A Linearized Discrete Ordinate Radiative Transfer Model for Atmospheric Retrieval , 2001 .

[47]  J. Burrows,et al.  Combined differential‐integral approach for the radiation field computation in a spherical shell atmosphere: Nonlimb geometry , 2000 .

[48]  D. Shemansky,et al.  CO2 Extinction Coefficient 1700–3000 Å , 1972 .

[49]  Jacqueline Lenoble,et al.  Atmospheric Radiative Transfer , 1993 .

[50]  M. Molina,et al.  Absolute absorption cross sections of ozone in the 185- to 350-nm wavelength range , 1986 .