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Globe 1
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N<1ONAL ACADEMY PROW
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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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