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Globe 1 Or; ^~;ctr\ / ~ PIN Fag SCION ~1 Sac ~# and Board of ~tmo~ph~hc icI~nc~s find C#mat Commission on P~IcaJ Seance ~ath~mabo and k~sourc~ N2tIonaI Mach CouncII N<1ONAL ACADEMY PROW #~hlngton TIC 1984

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NATIONAL ACADEMY PRESS 2101 CONSTITUTION AVE., NW WASHINGTON, DC 20418 NOTICE The project that is the subject of this report was approved by the Governing Board of the National Research Council, whose members are drawn from the councils of the National Academy of Sciences, the National Academy of Engineering, and the Institute of Medicine. The members of the committee responsible for the report were chosen for their special competences and with regard for appropriate balance. This report has been reviewed by a group other than the authors according to procedures approved by a Report Review Committee consisting of members of the National Academy of Sciences, the National Academy of Engineering, and the Institute of Medicine. The National Research Council was established by the National Academy of Sciences in 1916 to associate the broad community of science and technology with the Academy's purposes of furthering knowledge and of advising the federal government. The Council operates in accordance with general policies determined by the Academy under the authority of its congressional charter of 1863, which establishes the Academy as a private, nonprofit, self-governing membership corporation. The Coun- cil has become the principal operating agency of both the National Academy of Sciences and the National Academy of Engineering in the conduct of their services to the government, the public, and . . . ~ . . . the scenic and engineering communities. It is administered jointly by both Academies and the Institute of Medicine. The National Academy of Engineering and the Institute of Medicine were established in 1964 and 1970, respectively, under the charter of the National Academy of Sciences. This material is based upon work supported jointly by the National Science Foundation and the National Aeronautics and Space Administration under Grant Number ATM 80-24257. Library of Congress Catalog Card Number 84-61498 International Standard Book Number 0-309-03481-7 Printed in the United States of America

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Global Tropospheric Chemistry Panel ROBERT A. DUCK, University of Rhode Island, Chaim~arz RALPH CICERONE, National Center for Atmospheric Research, V'ce Chairman DOUGLAS DAVIS, Georgia Institute of Technology C. C. DELWICHE, University of California, Davis ROBERT DICKINSON, National Center for Atmospheric Research ROBERT HARRISS, National Aeronautics and Space Administration BRUCE HICKS, National Oceanic and Atmospheric Administration DONALD LENSCHOW, Nations Center for Atmospheric Research HIRAM LEVY II, Nations Oceanic and Atmospheric Administration SHAW LIU, National Oceanic and Atmospheric Administration MICHAEL McELROY, Harvard University VOLKER MOHNEN, State University of New York, Albany HIROMI NIKI, Ford Motor Company JOSEPH PROSPERO,UniversityofMi~i

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Board on Atmospheric Sciences and Climate THOMAS F. MALONE, Butler University, Chairman FERDINAND BAER, University of Maryland LOUIS ]. BATTAN, University of Arizona WERNER A. BAUM, Florida State University ROBERT A. DUCK, University of Rhode Island JOHN A. EDDY, Nations Center for Atmospheric Research PETER V. HOBBS, University of Washington FRANCIS S. JOHNSON, University of Texas, Dallas ROBERT W. KATES, Clark University MICHAEL B. McELROY, Harvard University JAMES C. MCWILLIAMS, National Center for Atmospheric Research VOLKER A. MOHNEN, State University of New York, Albany ANDREW F. NAGY,UniversityofMichigan WILLIAM A. NIERENBERG, Scripps Institution of Oceanography ROGER R. REVEELE, University of California, San Diego JUAN G. ROEDERER,Universityof~aska NORMAN J. ROSENBERG, University of Nebraska STEPHEN H. SCHNEIDER, National Center for Atmospheric Research JOHN W. TOWNSEND, Fairchild Space & Electronics Company THOMAS H. YONDER HAAR, Colorado State University JOHN S. PERRY, Sta~Director FRED D. WHITE, Staff Officer 1V

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Commission on Physical Sciences, Mathematics, and Resources ., HERBERT FRIEDMAN, Nations Research Council, Chai~n ELKAN R. BLOUT, Harvard Medical School WILLIAM BROWDER, Princeton University BERNARD F. BURKE, Massachusetts Institute of Technology HERMAN CHERNOFF, Massachusetts Institute of Technology MILDRED S. DRESSELHAUS, Massachusetts Institute of Technology WALTER R. ECKELMANN, Sohio Petroleum Company, Dallas, Texas JOSEPH L. FISHER, Secretary of Human Resources, Of lice of the Governor, Richmond, Virginia JAMES C. FLETCHER, Burroughs Corporation, McLean, Virginia WILLIAM A. FOWLER, California Institute of Technology GERHART FRIEDLANDER, Brookhaven National Laboratory EDWARD A. FRIEMAN, Science Applications, Inc., La iolla, California EDWARD D. GOLDBERG, Scripps Institution of Oceanography CHARLES L. HOSLER,JR.,PennsylvaniaStateuniversity KONRAD B. KRAUSKOPF, Stanford University CHARLES ]. MANKIN, Oklahoma Geologic Survey WALTER H. MUNK, University of California, San Diego GEORGE E. PAKE, Xerox Research Center ROBERT E. SIEVERS, University of Colorado, Boulder HOWARD E. SIMMONS,JR., E.I. du Pont de Nemours & Co., Inc. JOHN D. SPENGLER, Haward School of Public Health HATTEN S. YODER, Carnegie Institution of Washington RAPHAEL G. KASPER, Executive Director LAWRENCE MCCRAY, Associate Executive Director

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Foreword As the world approaches the threshoIc! of the twenty-first century, higher levels of unclerstancT- ing of the physical environment are becoming attainable and more necessary. Just as science and technology have permitted worIcT human population to grow and life expectancy to increase through modern industry ant] agriculture, so they permit more rigorous investigations into how the earth's planetary life support system works. Prudent management will become imperative if the general health ant] stability of human life on this planet are to be assured. Effective manage- ment will require a good understanding of the complex physical, chemical, and biological proc- esses in that system that enables it to combine solar radiant energy with the cycling of chemical nutrients through the biosphere to sustain plant, animal, ant! human life. The important role of chemical and physical processes in the troposphere in the planetary life support system has been brought into sharp focus in recent years not only by research discoveries, but also by a (disturbing, recurring sequence of problem identification and response, e.g., impacts of smog on health, of acid rain on lakes, forests, and agriculture, of increasing carbon dioxide and other trace gases on climate, ant! of chemicals moving upwarc! through the troposphere to the stratosphere. It has become clear that the troposphere is an integral component of the planetary life support system-receiving, transporting, transforming, and depositing substances that either contribute to the efficiency of the system or cleleteriously perturb it. Yet relatively little effort has been expencled on obtaining a funciamental understanding of the global troposphere and its clynamical behavior ancT cycles. Perturbations can be expecter] to increase in frequency and variety during the next several clecacles, ant! their significant economic impact will grow. Because the atmosphere is a moving ant! restless continuum enveloping the planet, the issues are interna- tional; since physical, chemical, and biological processes are inextricably intertwined, the effort to understand! them must be interclisciplinary. Accordingly, it was timely that a panel of atmospheric chemists and meteorologists be convened . . V11

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. ~ . V111 FOREWORD to clevelop the conceptual framework and propose a scientific strategy for a study of the chemistry of the global troposphere. Rapid advances in the theoretical understanding of chemical reactions in the troposphere, fielcI-measurement capabilities, laboratory techniques, ciata handing, and numerical modeling capacities strongly support the conviction that a coordinated international effort can lead, before the end of the century, to the kind of unclerstancling that would provide the predictive capability necessary to anticipate the impact on the planetary ecosystem of conscious or inadvertent changes in the chemistry of the Tower atmosphere. The institutional framework for such a study exists in the International Council of Scientific Unions. Atmospheric scientists in the United States anti around the world are enthusiastic. Now is a propitious time to act. The panelists have presented a challenging but tractable scientific endeavor, with highly attractive societal benefits. It might well constitute an important element of an international program declicated to unclerstancling the behavior ofthe geosphere ant! biosphere as an integrated system. THOMAS F. MALONE, Chairman Board on Atmospheric Sciences and Climate

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Preface Prompted by an increasing awareness ofthe influence of human activity on the chemistry ofthe global troposphere, a meeting of 10 atmospheric chemists and meteorologists was held at the National Center for Atmospheric Research in the spring of 1981 . In a letter report to the National Science Foundation (NSF) following this meeting, this group called for the development of a comprehensive plan for a coordinated study oftropospheric chemistry on a global scale. They also recognized the complexities of tropospheric biogeochemical cycles and the difficulties in predict- ing tropospheric responses to both natural and anthropogenic perturbations but expressed confi- dence that the necessary research is feasible. In response, the NSF asked the National Research Council to form a Panel on Global Tropospheric Chemistry. This panel was formed by the NRC 's Committee on Atmospheric Sciences (now the Board on Atmospheric Sciences and Climate) curing the summer of 1982; the panel's work has been supported by the NSF and by the National Aeronautics and Space Administration. The panel was given the following charge: 1. assess the requirement for a global study of the chemistry of the troposphere; 2. develop a scientific strategy for a comprehensive plan taking into account the existing and projected programs of the government; 3. assess the requirements of a global study in terms of theoretical knowledge, numerical modeling, instrumentation, observing platforms, ground-level observational techniques, and other related needs; and 4. outline the appropriate sequence and coordination required to achieve the most effective utilization of available resources. The entire panel held meetings at Kingston, Rhode Island, in September 1982; at Santa Monica, California, in December 1982; and at Boulder, Colorado, in April 1983. Subgroups of 1X

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x PREFAC E the pane} met at other times. During these meetings a scientific framework was cleveloped for the proposer! program based on the fundamental processes controlling biogeochemical cycles in the troposphere: sources, transport, transformations, and removal. Efforts were made to keep both the U.S. and the international atmospheric chemistry commu- nity aware ofthe panel's deliberations, and comments and suggestions from this community were solicited. Many thoughtful ant! helpful responses were received and used by the panel in prepar- ing its report. Chapters ~ through 4 (Part I) of this report present the details of the rationale and framework for the proposed Global Tropospheric Chern~stry Program. The overall program includes intensive fielcI, laboratory, and modeling investigations in four areas: biological sources for tropospheric constituents, global distribution and long-range transport of trace species, fast-photochemical cycles and transformations, and wet and dry removal processes. Instrument ant] platform devel- opment requirements are assessed, ant! the neecI for strong international cooperation is stressed. Chapters 5 through 9 (Part Il) present the background information from which the proposal program was developed. Briefreviews are given of current understanding ant! gaps in knowlecige concerning sources, transport, transformation, ant! removal of trace species in the troposphere. Reviews of the primary chemical cycles in the troposphere and the role of modeling in under- standing tropospheric chemical processes are presented along with community surveys ant] reviews of currently available chemical instrumentation techniques used in atmospheric studies as well as aircraft, ship, ant! spaceborne sampling platforms. Current research programs in tropo- spheric chemistry in the United States are also reviewed in an appencI~x. Development of this program was a joint effort involving every pane} member. Without this cooperative involvement, it would not have been possible to complete this task. The panel expresses its gratitude to a number of individuals who contributed time, effort, and enthusiasm to the development of this report. The pane} thanks Dieter Ehhait, William Chameides, and Dan Albritton for their detailed reviews of early sections of the report, and the anonymous National Research Council reviewers ofthis report for their constructive criticism ant! suggestions. Robert CharIson, Paul Crutzen, Leonard Newman, Frank AlIario, and Roger Tanner contributed significantly to the panel's efforts through participation in some panel or subpane! meetings or extensive discussions with pane} members. Global Tropospheric Chemistry Parzel ROBERT A. DUCK, Chairman RALPH CICERONE, Vice Chairrna?: DOUGLAS DAVIS C. C. DELWICHE ROBERT DICKINSON ROBERT HARRISS BRUCE HICKS DONALD LENSCHOW HIRAM LEVY II . SHAW LIU MICHAEL MCELROY VOLKER MOHNEN HIROMI NIKI JOSEPH PROSPERO

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Contents PART I A PLAN FOR ACTION Executive Summary 1 1 THE NEED FOR A PROGRAM ....... Public Policy Problems anc! Atmospheric Chemistry /8 Atmospheric Chemistry: Tool, Science, or Both? /9 Tropospheric Chemistry: The Prospectus /9 2 A FRAMEWORK Sources /12 Transport and Distribution /13 Transformation /14 Removal /15 Physical Effects of Trace Substances in the Troposphere /16 Summary /18 3 A PROPOSED PROGRAM. . Long-Term Goals ant! Objectives /19 Biological Sources of Atmospheric Chemicals /21 Global Distributions ant] Long-Range Transport /26 Photochemical Transformations /33 Conversion, Redistribution, and Removal /38 Mocleling the Tropospheric Chemical System /44 X1 7 11 . 19

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~ . X11 CONTENTS Instrument and Platform Requirements /47 International Cooperation /49 4 A CALL TO ACTION PART II ASSESSMENTS 0F CURRENT UNDERSTANDING 5 CRITICAL PROCESSES AFFECTING THE DISTRIBUTION OF CHEMICAL SPECIES ..................... Biological and Surface Sources /55 R. Cicerone, C. C. De~wiche, R. Harass, andR. Dickinson Global Distributions anti Lor~g-Range Transport /69 [. M. Prospero and H. Levy I! Homogeneous and Heterogeneous Transformations /78 D. Davis, H. Nak`; UMohner~, and S. Liu Wet ant! Dry Removal Processes /88 B. Hicks, D. [er~schow, and T:Mohnen 6 THE ROLE OF MODELING IN UNDERSTANDING TROPOSPHERIC CHEMICAL PROCESSES ....................... R. Dickinson and S. Liu Principles of Mocleling /94 Existing Models /94 Modeling in Support Of the Proposed Research Programs /96 7 TROPOSPHERIC CHEMICAL CYCLES Tropospheric Chemistry and Biogeochemical Cycles /101 C. C. De~wiche Water(HydrologicalCycle) /106 R. Dickinson Ozone /109 H. JevyIl Fixed Nitrogen Cycle /113 S. [iu and R. Cicerorze Sulfur Cycle /117 R. Harriss and H. Niki Carbon Cycle /122 H. Nik`; R. Duce, and{R. Dickinson Halogens /128 R. Cicerone Trace Elements /! 33 R. Duce Aerosol Particles /136 [. M. Prospero . 50 . 53 . 55 . . 94 101

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CONTENTS . . . X111 8 INSTRUMENTATION DEVELOPMENT NEEDS FOR USE OF MASS-BALANCE TECHNIQUE................ D. [enschow 9 INSTRUMENT AND PLATFORM SURVEY T:Mohnen, F:Aliario, D. Davis, D. [enschow, andR. Tanner Instrumentation for in situ Measurements /144 Remote Sensing Technology /145 Aircraft Platforms /145 Oceanographic Platforms /152 APPENDIXES . Appendix A Appendix B Appendix C INDEX . CURRENT TROPOSPHERIC CHEMISTRY RESEARCH IN THE UNITED STATES .................. REMOTE SENSOR TECHNOLOGY ELEMENT CYCLE MATRICES . . . . 141 . 144 . 169 171 . 175 183 189

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