CHEMISTRY OF THE LOWER ATMOSPHERE

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1 CHEMISTRY OF THE LOWER ATMOSPHERE

2 CONTRIBUTORS Richard D. Cadle National Center for Atmospheric Research Boulder, Colorado James P. Friend New York University Department of Meteorology and Oceanography New York, New York G.M.Hidy North American Rockwell Science Center Thousand Oaks, California and California Institute of Technology Pasadena, California Charles D. Keeling Scripps Institution of Oceanography University of California at San Diego La Jolla, California William W. Kellogg National Center for Atmospheric Research Boulder, Colorado Hans R. Pruppacher Department of Meteorology University of California Los Angeles, California Stephen H. Schneider National Center for Atmospheric Research Boulder, Colorado

3 CHEMISTRY OF THE LOWER ATMOSPHERE EDITED BY S. I. RASOOL Deputy Director, Planetary Programs National Aeronautics and Space Administration Washington, D. C. PLENUM PRESS NEW YORK-LONDON 1973

4 Library of Congress Catalog Card Number ISBN-13: e-isbn-13: DOl: / Plenum Press, New York Softcover reprint of the hardcover 1 st edition 1973 A Division of Plenum Publishing Corporation 227 West 17th Street, New York, N. Y United Kingdom edition published by Plenum Press, London A Division of Plenum Publishing Company, Ltd. Davis House (4th Floor), 8 Scrubs Lane, Harlesden, London, NWlO 6SE, England All rights reserved No part of this publication may be reproduced in any form without written permission from the publisher

5 PREFACE About three years ago Catherine de Berg and I published a short article in Nature in which we attempted to explain why the chemistry of the atmosphere of the Earth is today so completely different from that of our two neighboring planets, Mars and Venus. Our atmosphere is composed mainly of N2 and O2 with traces of A, H20, CO2, 0 3, etc., while the atmospheres of both Mars and Venus are almost entirely made up of CO2, Also, the Earth appears to be the only one ofthe three planets which has oceans ofliquid water on the surface. Since the presence of liquid water on Earth is probably an essential requirement for life to have originated and evolved to its present state, the question of the apparent absence ofliquid water on Mars and Venus suddenly acquires significant proportions. In our paper in Nature, and later in a more detailed discussion of the subject (Planetary Atmospheres, in Exobiology, edited by C. Ponnamperuma, North Holland Publishing Co.), we tried to describe why we believe that in the early history of the solar system all the terrestrial planets lost the atmospheres of H2 and He which they had acquired from the solar nebula at the time of their formation. These planets, completely devoid of atmospheres, like the Moon today, started accumulating new gases which were exhumed from the interior by the commencement of volcanic activity. On the Earth we know that these gases were largely water vapor (steam), carbon dioxide, and nitrogen, with a number of other constituents like chlorine, hydrogen, sulfur, etc. The Earth soon acquired a thin atmosphere of water vapor and CO2 with traces of N2, H 2, and other constituents. The temperature at the surface of the Earth at this time was probably about 260 o K, mainly governed by the Earth's distance from the Sun and the albedo of the solid surface. However, both H 2 0 and CO2 are extremely efficient in trapping infrared radiation so that the surface temperature of the Earth began to rise. Because of continued replenishment of the atmosphere from the interior, the temperature soon rose above 273 K and the pressure above 6.1 mb so that atmospheric water vapor started to condense. This marked the beginning of the accumulation of the oceans on the surface of the Earth. With the atmosphere now containing nitrogen, hydrogen, oxides of carbon, and traces of water vapor (or NH 3, CH 4,and H20, depending on the amount of hydrogen relative to nitrogen, carbon, and oxygen), the solar ultraviolet v

6 vi Preface radiation could penetrate close to the surface of the Earth and deposit enough energy to allow synthesis of organic molecules like HCN and HCHO. These, when dissolved in the oceans, continued to combine and form more complex molecules, ultimately producing the complex array of molecules which gave rise to the first "living" systems, and started the train of biological evolution. The presence of liquid water on Earth was therefore a key in determining the subsequent evolution of the atmosphere and of life itself. Gradually, biological activity changed the chemistry of the atmosphere by adding to it substantial amounts of oxygen, paving the way to the highly oxidized atmosphere of today. As the atmosphere became more and more oxidized, the methane and carbon monoxide were converted to carbon dioxide, which, being highly soluble in water at these temperatures, dissolved in the oceans, reacted with the silicates in the rocks, and was deposited on the ocean floor as limestone. Only N z and Oz therefore accumulated in the atmosphere and gave rise to the present-day conditions. Venus, being about 30 % closer to the Sun than Earth is, was initially at a higher temperature, and therefore the first emanations of steam from the early volcanoes were not condensed at the surface to form oceans. Water accumulated in the atmosphere as vapor and, being an extremely efficient absorber of infrared radiation, accentuated the greenhouse effect and raised the ground temperature to such high values that oceans could never accumulate. The absence of oceans and the relatively high temperature of the surface prevented COz from entering the crust as limestone, and therefore it continued to accumulate in the atmosphere. Water, a light molecule, eventually thermally evaporated from a rather hot exosphere, leaving behind an atmosphere predominantly made up of COz, as observed today. Mars, being further away from the Sun than the Earth, was initially too cold for the volcanic steam to liquefy; rather, it froze. This again inhibited the transfer ofcoz from the atmosphere to the crust. At the same time Mars is only half the size of Venus and Earth, and that is why, although Mars is volcanically active, the rate of emanation is slow and has so far accumulated only a very thin atmosphere of COz. In summary, therefore, it seems to us that the size of the planet and its distance from the Sun are the two crucial parameters which determine the nature of the atmosphere and the oceans and therefore the nature of the living organisms that originate and evolve on the planet. To illustrate this point we showed in our paper that if Earth were only 6 % closer to the Sun, the increased solar radiation would not have allowed the volcanic steam to condense at the surface as oceans, and today we would probably have conditions on the surface of the Earth just as hostile as they are on Venus: a 7000K temperature at the surface, heavy COz atmosphere, and probably no life at all. This is my view of the evolution of our atmosphere during its long

7 Preface vii history of 3 or 4 billion years. However, when I expounded this thesis at various seminars and colloquia around the country, the questions that were invariably asked were not so much concerned with the history of our atmosphere but with its future. What is the effect of man's input to the atmosphere with regard to the total picture of atmospheric evolution? Is man undoing what nature did by creating Earth where it is located in the solar system? Will the increasing pollution of the atmosphere change the course of atmospheric evolution and will Earth become like Venus? What is its impact on the climate? Although at times I have tried to answer these questions, both the questions and the answers have left me very uneasy. The reason is very simple. We do not know enough about the subject because it involves complex~ interaction among a number of disciplines: atmospheric dynamics, chemical processes, radiative transfer, and-most significantly-the exchange of gas between the crust, oceans, and the atmosphere. Talking with some of my colleagues in these fields, I realized that many of the questions I had attempted to answer cannot even be formulated properly because we do not know enough about, for example, the physics, chemistry, and dynamics of atmospheric aerosols, the CO 2 and sulfur cycles, and the total interaction of these constituents with the radiation environment of the planet. On one thing, however, all of us did agree, that the literature in this field desperately needs a thorough review of the state of art in each of the above areas, and this is what this book is all about. s. I. RASOOL

8 CONTENTS Chapter 1 The Role of Natural and Anthropogenic Pollutants in Cloud and Precipitation Formation HANS R. PRUPPACHER I. Introduction If There Were No Aerosols in the Atmosphere : The Role of Aerosols in Nucleating Cloud Drops The Role oflons The Role of Water-Soluble, Hygroscopic Particles The Role of Water-Insoluble Particles The Role of Aerosols in the Formation of Precipitation in Warm Clouds The Role of Aerosols in Nucleating Ice Crystals The Role of Aerosols in the Formation of Precipitation in Supercooled Clouds References Chapter 2 Particulate Matter in the Lower Atmosphere RICHARD D. CADLE I. Introduction The Troposphere Sources of Particles Composition of Particles Collected from the Atmosphere Particle Concentrations and Size Distributions Mechanisms of Removal and Residence Times The Lower Stratosphere The Sulfate Layer Mechanisms of Removal and Residence Times References ix

9 x Contents Chapter 3 Removal Processes of Gaseous and Particulate Pollutants G. M. HIDY 1. Introduction The Physical Chemistry of Removal of Trace Gases Water-Insoluble Constituents Water-Soluble Constituents Chemical Reactivity and Sulfur Dioxide Removal Mechanisms for Aerosols Dynamical Processes and Aerosol Removal Summary and Conclusions Acknowledgment References Chapter 4 The Global Sulfur Cycle JAMES P. FRIEND 1. Introduction The Nature of the Sulfur Cycle The Chemistry of Sulfur in the Global Environment Concentrations of Sulfur The Atmosphere Crustal Sulfur Contents of the Reservoirs Transfer Mechanisms and Rates The Atmosphere The Pedosphere The Hydrosphere River Runoff Lithosphere Mantle The Global Sulfur Cycle Discussion Comparison with the Cycles Background Concentrations of Atmospheric Sulfur Mobilization of Sulfur by Man..., Pollution Sulfur in River Waters References Bibliography of Sulfur Cycles Chapter 5 The Chemical Basis for Climate Change STEPHEN H. SCHNEIDER AND WILLIAM W. KELLOGG 1. Introduction Lessons to be Learned from the Past

10 Contents xi 3. Approach to a Theory of Climate: Interactions Among Atmospheric Chemistry, Radiation, Radiation, and Dynamics Summary of Factors Affecting the Climate Physical and Mathematical Formulations of the Theory of Climate Natural and Man-Made Influences on Atmospheric Composition Carbon Dioxide from Fossil Fuels Particles in the Atmosphere Changes in the Stratosphere Acknowledgment References Chapter 6 The Carbon Dioxide Cycle: Reservoir Models to Depict the Exchange of Atmospheric Carbon Dioxide with the Oceans and Land Plants CHARLES D. KEELING Preface PART I. FORMULATION AND MATHEMATICAL SOLUTION OF THE MODEL EQUATIONS I. Introduction Introductory Remarks Review of Previous Work Preliminary Modeling Considerations Physical Basis for the Models Three-Reservoir Atmosphere-Ocean Tandem Model Four-Reservoir Tandem Model with Land Biota Five-Reservoir Branched Model with Divided Land Biota PART II. CHEMICAL SPECIFICATION AND NUMERICAL RESULTS Preface Derivation of Transfer Coefficients for the Land Biota Derivation of Transfer Coefficients for Air-Sea Exchange Influence of the Buffer Factor Steady-State Exchange Transient Exchange Derivation of Transfer Coefficients for Exchange Within the Ocean Steady-State Exchange Transient Exchange Observational Data Global Summaries Carbon Fluxes and Masses of the Land Biota

11 xii Contents 9. Numerical Results and Discussion Additional Observational Data Comparison of Three- and Five-Reservoir Models Search for a Best Fit with Observed Atmospheric Variations 317 Appendix A. Factors to Solve Four-Reservoir Model Appendix B. Equations for Five-Reservoir Model References Index

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