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Cover |
1 |
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Title Page |
5 |
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Copyright |
6 |
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Dedication |
7 |
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Content |
9 |
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Preface to the First Edition |
25 |
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Preface to the Third Edition |
27 |
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Part I: The Atmosphere and Its Constituents |
29 |
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Chapter 1: The Atmosphere |
31 |
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1.1 History and Evolution of Earth's Atmosphere |
31 |
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1.2 Climate |
33 |
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1.3 Layers of the Atmosphere |
33 |
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1.4 Pressure in the Atmosphere |
35 |
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1.4.1 Units of Pressure |
35 |
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1.4.2 Variation of Pressure with Height in the Atmosphere |
35 |
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1.5 Temperature in the Atmosphere |
38 |
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1.6 Expressing the Amount of a Substance in the Atmosphere |
38 |
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1.7 Airborne Particles |
42 |
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1.8 Spatial and Temporal Scales of Atmospheric Processes |
42 |
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Problems |
44 |
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References |
45 |
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Chapter 2: Atmospheric Trace Constituents |
46 |
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2.1 Atmospheric Lifetime |
47 |
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2.2 Sulfur-Containing Compounds |
51 |
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2.2.1 Dimethyl Sulfide (CH3SCH3) |
54 |
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2.2.2 Carbonyl Sulfide (OCS) |
54 |
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2.2.3 Sulfur Dioxide (SO2) |
55 |
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2.3 Nitrogen-Containing Compounds |
55 |
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2.3.1 Nitrous Oxide (N2O) |
56 |
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2.3.2 Nitrogen Oxides (NOx = NO + NO2) |
57 |
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2.3.3 Reactive Odd Nitrogen (NOy) |
58 |
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2.3.4 Ammonia (NH3) |
59 |
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2.3.5 Amines |
60 |
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2.4 Carbon-Containing Compounds |
60 |
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2.4.1 Classification of Hydrocarbons |
60 |
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2.4.2 Methane |
62 |
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2.4.3 Volatile Organic Compounds |
64 |
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2.4.4 Biogenic Hydrocarbons |
64 |
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2.4.5 Carbon Monoxide |
67 |
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2.4.6 Carbon Dioxide |
68 |
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2.5 Halogen-Containing Compounds |
68 |
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2.5.1 Methyl Chloride (CH3Cl) |
70 |
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2.5.2 Methyl Bromide (CH3Br) |
70 |
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2.6 Atmospheric Ozone |
72 |
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2.7 Particulate Matter (Aerosols) |
75 |
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2.7.1 Stratospheric Aerosol |
76 |
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2.7.2 Chemical Components of Tropospheric Aerosol |
76 |
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2.7.3 Cloud Condensation Nuclei (CCN) |
77 |
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2.7.4 Sizes of Atmospheric Particles |
77 |
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2.7.5 Carbonaceous Particles |
79 |
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2.7.6 Mineral Dust |
81 |
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2.7.7 Biomass Burning |
81 |
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2.7.8 Summary of Atmospheric Particulate Matter |
82 |
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2.8 Mercury |
83 |
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2.9 Emission Inventories |
83 |
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Appendix 2.1 Us Air Pollution Legislation |
84 |
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Appendix 2.2 Hazardous Air Pollutants (Air Toxics) |
85 |
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Problems |
87 |
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References |
89 |
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Part II: Atmospheric Chemistry |
95 |
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Chapter 3: Chemical Kinetics |
97 |
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3.1 Order of Reaction |
97 |
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3.2 Theories of Chemical Kinetics |
99 |
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3.2.1 Collision Theory |
99 |
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3.2.2 Transition State Theory |
102 |
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3.2.3 Potential Energy Surface for a Bimolecular Reaction |
103 |
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3.3 The Pseudo-Steady-State Approximation |
104 |
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3.4 Reactions of Excited Species |
105 |
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3.5 Termolecular Reactions |
106 |
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3.6 Chemical Families |
109 |
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3.7 Gas-Surface Reactions |
111 |
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Problems |
112 |
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References |
115 |
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Chapter 4: Atmospheric Radiation and Photochemistry |
116 |
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4.1 Radiation |
116 |
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4.2 Radiative Flux in the Atmosphere |
119 |
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4.3 Beer-Lambert Law and Optical Depth |
121 |
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4.4 Actinic Flux |
123 |
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4.5 Atmospheric Photochemistry |
125 |
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4.6 Absorption of Radiation By Atmospheric Gases |
128 |
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4.7 Absorption By O2 and O3 |
133 |
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4.8 Photolysis Rate As a Function of Altitude |
137 |
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4.9 Photodissociation of O3 to Produce O and O(D) |
140 |
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4.10 Photodissociation of No2 |
142 |
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Problems |
145 |
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References |
145 |
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Chapter 5: Chemistry of the Stratosphere |
147 |
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5.1 Chapman Mechanism |
150 |
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5.2 Nitrogen Oxide Cycles |
157 |
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5.2.1 Stratospheric Source of NOx from N2O |
157 |
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5.2.2 NOx Cycles |
159 |
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5.3 Hox Cycles |
162 |
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5.4 Halogen Cycles |
167 |
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5.4.1 Chlorine Cycles |
168 |
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5.4.2 Bromine Cycles |
171 |
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5.5 Reservoir Species and Coupling of the Cycles |
172 |
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5.6 Ozone Hole |
174 |
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5.6.1 Polar Stratospheric Clouds (PSCs) |
177 |
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5.6.2 PSCs and the Ozone Hole |
178 |
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5.6.3 Arctic Ozone Hole |
181 |
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5.7 Heterogeneous (Nonpolar) Stratospheric Chemistry |
183 |
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5.7.1 The Stratospheric Aerosol Layer |
183 |
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5.7.2 Heterogeneous Hydrolysis of N2O5 |
183 |
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5.7.3 Effect of Volcanoes on Stratospheric Ozone |
188 |
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5.8 Summary of Stratospheric Ozone Depletion |
190 |
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5.9 Transport and Mixing in the Stratosphere |
193 |
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5.10 Ozone Depletion Potential |
195 |
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Problems |
196 |
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References |
201 |
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Chapter 6: Chemistry of the Troposphere |
203 |
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6.1 Production of Hydroxyl Radicals in the Troposphere |
204 |
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6.2 Basic Photochemical Cycle of No2, No, and O3 |
207 |
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6.3 Atmospheric Chemistry of Carbon Monoxide |
209 |
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6.3.1 Low-NOx Limit |
211 |
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6.3.2 High-NOx Limit |
212 |
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6.3.3 Ozone Production Efficiency |
212 |
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6.3.4 Theoretical Maximum Yield of Ozone from CO Oxidation |
216 |
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6.4 Atmospheric Chemistry of Methane |
216 |
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6.5 The Nox and Noy Families |
220 |
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6.5.1 Daytime Behavior |
220 |
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6.5.2 Nighttime Behavior |
221 |
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6.6 Ozone Budget of the Troposphere and Role of Nox |
223 |
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6.6.1 Ozone Budget of the Troposphere |
223 |
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6.6.2 Role of NOx |
223 |
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6.6.3 Global Hydroxyl Radical Budget |
225 |
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6.7 Tropospheric Reservoir Molecules |
231 |
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6.7.1 H2O2, CH3OOH, and Hydroperoxides |
231 |
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6.7.2 Nitrous Acid (HONO) |
232 |
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6.7.3 Peroxyacyl Nitrates (PANs) |
232 |
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6.8 Relative Roles of Voc and Nox in Ozone Formation |
236 |
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6.8.1 Importance of the VOC/NOx Ratio |
236 |
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6.8.2 Ozone Isopleth Plot |
237 |
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6.8.3 Weekend Ozone Effect |
239 |
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6.9 Simplified Organic/Nox Chemistry |
240 |
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6.10 Chemistry of Nonmethane Organic Compounds in the Troposphere |
242 |
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6.10.1 Alkanes |
243 |
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6.10.2 Alkenes |
250 |
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6.10.2.1 OH Reaction |
251 |
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6.10.2.2 NO3 Reaction |
253 |
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6.10.2.3 Ozone Reaction |
255 |
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6.10.3 Aromatics |
256 |
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6.10.4 Aldehydes |
258 |
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6.10.5 Ketones |
258 |
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6.10.6 Ethers |
259 |
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6.10.7 Alcohols |
259 |
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6.10.8 Tropospheric Lifetimes of Organic Compounds |
260 |
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6.11 Atmospheric Chemistry of Biogenic Hydrocarbons |
261 |
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6.11.1 Atmospheric Chemistry of Isoprene |
261 |
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6.11.1.1 Isoprene + OH |
262 |
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6.11.1.2 Isoprene + O3 |
266 |
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6.11.1.3 Isoprene + NO3 |
266 |
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6.11.1.4 Chemistry of Isoprene Oxidation Products: Methacrolein and Methyl Vinyl Ketone |
267 |
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6.11.2 Monoterpenes (?-Pinene) |
269 |
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6.11.2.1 ?-Pinene + O3 |
270 |
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6.11.2.2 ?-Pinene + OH |
270 |
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6.12 Atmospheric Chemistry of Reduced Nitrogen Compounds |
272 |
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6.12.1 Amines |
273 |
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6.12.2 Nitriles |
274 |
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6.12.3 Nitrites |
274 |
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6.13 Atmospheric Chemistry (Gas Phase) of Sulfur Compounds |
274 |
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6.13.1 Sulfur Oxides |
274 |
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6.13.2 Reduced Sulfur Compounds (Dimethyl Sulfide) |
275 |
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6.14 Tropospheric Chemistry of Halogen Compounds |
277 |
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6.14.1 Chemical Cycles of Halogen Species |
277 |
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6.14.2 Tropospheric Chemistry of CFC Replacements: Hydrofluorocarbons (HFCs) and Hydrochlorofluorocarbons (HCFCs) |
279 |
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6.15 Atmospheric Chemistry of Mercury |
281 |
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Appendix 6 Organic Functional Groups |
282 |
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Problems |
284 |
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References |
287 |
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Chapter 7: Chemistry of the Atmospheric Aqueous Phase |
293 |
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7.1 Liquid Water in the Atmosphere |
293 |
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7.2 Absorption Equilibria and Henry's Law |
296 |
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7.3 Aqueous-Phase Chemical Equilibria |
299 |
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7.3.1 Water |
299 |
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7.3.2 Carbon Dioxide-Water Equilibrium |
300 |
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7.3.3 Sulfur Dioxide-Water Equilibrium |
302 |
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7.3.4 Ammonia-Water Equilibrium |
306 |
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7.3.5 Nitric Acid-Water Equilibrium |
308 |
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7.3.6 Equilibria of Other Important Atmospheric Gases |
309 |
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7.3.6.1 Hydrogen Peroxide |
309 |
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7.3.6.2 Ozone |
310 |
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7.3.6.3 Oxides of Nitrogen |
310 |
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7.3.6.4 Formaldehyde |
310 |
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7.3.6.5 Formic and Other Atmospheric Acids |
311 |
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7.3.6.6 OH and HO2 Radicals |
312 |
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7.4 Aqueous-Phase Reaction Rates |
312 |
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7.5 S(IV)-S(VI) Transformation and Sulfur Chemistry |
314 |
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7.5.1 Oxidation of S(IV) by Dissolved O3 |
314 |
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7.5.2 Oxidation of S(IV) by Hydrogen Peroxide |
317 |
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7.5.3 Oxidation of S(IV) by Organic Peroxides |
318 |
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7.5.4 Uncatalyzed Oxidation of S(IV) by O2 |
319 |
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7.5.5 Oxidation of S(IV) by O2 Catalyzed by Iron and Manganese |
319 |
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7.5.5.1 Iron Catalysis |
319 |
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7.5.5.2 Manganese Catalysis |
321 |
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7.5.5.3 Iron/Manganese Synergism |
321 |
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7.5.6 Comparison of Aqueous-Phase S(IV) Oxidation Paths |
321 |
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7.6 Dynamic Behavior of Solutions With Aqueous-Phase Chemical Reactions |
323 |
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7.6.1 Closed System |
324 |
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7.6.2 Calculation of Concentration Changes in a Droplet with Aqueous-Phase Reactions |
326 |
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Appendix 7.1 Thermodynamic and Kinetic Data |
329 |
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Appendix 7.2 Additional Aqueous-Phase Sulfur Chemistry |
333 |
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7A.1 S(IV) Oxidation by the OH Radical |
333 |
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7A.2 Oxidation of S(IV) by Oxides of Nitrogen |
336 |
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7A.3 Reaction of Dissolved SO2 with HCHO |
337 |
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Appendix 7.3 Aqueous-Phase Nitrite and Nitrate Chemistry |
339 |
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7A.4 NOx Oxidation |
339 |
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7A.5 Nitrogen Radicals |
339 |
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Appendix 7.4 Aqueous-Phase Organic Chemistry |
340 |
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Appendix 7.5 Oxygen and Hydrogen Chemistry |
341 |
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Problems |
342 |
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References |
345 |
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Part III: Aerosols |
351 |
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Chapter 8: Properties of the Atmospheric Aerosol |
353 |
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8.1 The Size Distribution Function |
353 |
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8.1.1 The Number Distribution nN(Dp) |
356 |
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8.1.2 The Surface Area, Volume, and Mass Distributions |
358 |
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8.1.3 Distributions Based on ln Dp and log Dp |
359 |
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8.1.4 Relating Size Distributions Based on Different Independent Variables |
361 |
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8.1.5 Properties of Size Distributions |
362 |
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8.1.6 Definition of the Lognormal Distribution |
363 |
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8.1.7 Plotting the Lognormal Distribution |
366 |
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8.1.8 Properties of the Lognormal Distribution |
367 |
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8.2 Ambient Aerosol Size Distributions |
370 |
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8.2.1 Urban Aerosols |
371 |
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8.2.2 Marine Aerosols |
372 |
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8.2.3 Rural Continental Aerosols |
375 |
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8.2.4 Remote Continental Aerosols |
376 |
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8.2.5 Free Tropospheric Aerosols |
376 |
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8.2.6 Polar Aerosols |
377 |
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8.2.7 Desert Aerosols |
377 |
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8.3 Aerosol Chemical Composition |
380 |
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8.4 Spatiotemporal Variation |
382 |
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Problems |
385 |
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References |
387 |
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Chapter 9: Dynamics of Single Aerosol Particles |
390 |
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9.1 Continuum and Noncontinuum Dynamics: the Mean Free Path |
390 |
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9.1.1 Mean Free Path of a Pure Gas |
391 |
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9.1.2 Mean Free Path of a Gas in a Binary Mixture |
393 |
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9.2 The Drag on a Single Particle: Stokes' Law |
396 |
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9.2.1 Corrections to Stokes' Law: The Drag Coefficient |
399 |
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9.2.2 Stokes' Law and Noncontinuum Effects: Slip Correction Factor |
399 |
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9.3 Gravitational Settling of an Aerosol Particle |
400 |
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9.4 Motion of an Aerosol Particle in an External Force Field |
404 |
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9.5 Brownian Motion of Aerosol Particles |
404 |
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9.5.1 Particle Diffusion |
407 |
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9.5.2 Aerosol Mobility and Drift Velocity |
409 |
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9.5.3 Mean Free Path of an Aerosol Particle |
412 |
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9.6 Aerosol and Fluid Motion |
413 |
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9.6.1 Motion of a Particle in an Idealized Flow (90° Corner) |
414 |
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9.6.2 Stop Distance and Stokes Number |
415 |
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9.7 Equivalent Particle Diameters |
416 |
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9.7.1 Volume Equivalent Diameter |
416 |
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9.7.2 Stokes Diameter |
418 |
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9.7.3 Classical Aerodynamic Diameter |
419 |
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9.7.4 Electrical Mobility Equivalent Diameter |
421 |
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Problems |
421 |
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References |
422 |
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Chapter 10: Thermodynamics of Aerosols |
424 |
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10.1 Thermodynamic Principles |
424 |
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10.1.1 Internal Energy and Chemical Potential |
424 |
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10.1.2 The Gibbs Free Energy G |
426 |
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10.1.3 Conditions for Chemical Equilibrium |
428 |
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10.1.4 Chemical Potentials of Ideal Gases and Ideal-Gas Mixtures |
430 |
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10.1.4.1 The Single Ideal Gas |
431 |
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10.1.4.2 The Ideal-Gas Mixture |
431 |
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10.1.5 Chemical Potential of Solutions |
432 |
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10.1.5.1 Ideal Solutions |
432 |
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10.1.5.2 Nonideal Solutions |
435 |
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10.1.5.3 Pure Solid Compounds |
435 |
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10.1.5.4 Solutions of Electrolytes |
436 |
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10.1.6 The Equilibrium Constant |
436 |
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10.2 Aerosol Liquid Water Content |
437 |
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10.2.1 Chemical Potential of Water in Atmospheric Particles |
439 |
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10.2.2 Temperature Dependence of the DRH |
440 |
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10.2.3 Deliquescence of Multicomponent Aerosols |
443 |
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10.2.4 Crystallization of Single- and Multicomponent Salts |
447 |
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10.3 Equilibrium Vapor Pressure Over a Curved Surface: the Kelvin Effect |
447 |
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10.4 Thermodynamics of Atmospheric Aerosol Systems |
451 |
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10.4.1 The H2SO4-H2O System |
451 |
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10.4.2 The Sulfuric Acid-Ammonia-Water System |
455 |
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10.4.3 The Ammonia-Nitric Acid-Water System |
458 |
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10.4.3.1 Ammonium Nitrate Solutions |
460 |
|
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10.4.4 The Ammonia-Nitric Acid-Sulfuric Acid-Water System |
462 |
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10.4.5 Other Inorganic Aerosol Species |
467 |
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10.4.6 Organic Aerosol |
468 |
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10.5 Aerosol Thermodynamic Models |
468 |
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Problems |
470 |
|
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References |
471 |
|
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Chapter 11: Nucleation |
476 |
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11.1 Classical Theory of Homogeneous Nucleation: Kinetic Approach |
477 |
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11.1.1 The Forward Rate Constant ?i |
480 |
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11.1.2 The Reverse Rate Constant ?i |
481 |
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11.1.3 Derivation of the Nucleation Rate |
481 |
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11.2 Classical Homogeneous Nucleation Theory: Constrained Equilibrium Approach |
485 |
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11.2.1 Free Energy of i-mer Formation |
485 |
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11.2.2 Constrained Equilibrium Cluster Distribution |
487 |
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11.2.3 The Evaporation Coefficient ?i |
489 |
|
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11.2.4 Nucleation Rate |
489 |
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11.3 Recapitulation of Classical Theory |
492 |
|
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11.4 Experimental Measurement of Nucleation Rates |
493 |
|
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11.4.1 Upward Thermal Diffusion Cloud Chamber |
494 |
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11.4.2 Fast Expansion Chamber |
494 |
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11.4.3 Turbulent Mixing Chambers |
495 |
|
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11.5 Modifications of the Classical Theory and More Rigorous Approaches |
495 |
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11.6 Binary Homogeneous Nucleation |
496 |
|
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11.7 Binary Nucleation in the H2so4-H2o System |
501 |
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11.8 Nucleation on an Insoluble Foreign Surface |
503 |
|
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11.9 Ion-Induced Nucleation |
506 |
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11.10 Atmospheric New-Particle Formation |
508 |
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11.10.1 Molecular Constituency of New Particles |
509 |
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11.10.2 New-Particle Growth Rates |
510 |
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11.10.3 CLOUD Studies of Atmospheric Nucleation |
510 |
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11.10.4 Atmospheric Nucleation by Organic Species |
515 |
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Appendix 11 the Law of Mass Action |
515 |
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Problems |
517 |
|
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References |
518 |
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Chapter 12: Mass Transfer Aspects of Atmospheric Chemistry |
521 |
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12.1 Mass and Heat Transfer to Atmospheric Particles |
521 |
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12.1.1 The Continuum Regime |
521 |
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12.1.2 The Kinetic Regime |
525 |
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12.1.3 The Transition Regime |
525 |
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12.1.3.1 Fuchs Theory |
525 |
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12.1.3.2 Fuchs-Sutugin Approach |
526 |
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12.1.3.3 Dahneke Approach |
527 |
|
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12.1.3.4 Loyalka Approach |
527 |
|
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12.1.3.5 Sitarski-Nowakowski Approach |
527 |
|
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12.1.4 The Accommodation Coefficient |
528 |
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12.2 Mass Transport Limitations in Aqueous-Phase Chemistry |
531 |
|
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12.2.1 Characteristic Time for Gas-Phase Diffusion to a Particle |
533 |
|
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12.2.2 Characteristic Time to Achieve Equilibrium at the Gas-Liquid Interface |
534 |
|
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12.2.3 Characteristic Time of Aqueous Dissociation Reactions |
536 |
|
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12.2.4 Characteristic Time of Aqueous-Phase Diffusion in a Droplet |
538 |
|
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12.2.5 Characteristic Time for Aqueous-Phase Chemical Reactions |
539 |
|
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12.3 Mass Transport and Aqueous-Phase Chemistry |
539 |
|
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12.3.1 Gas-Phase Diffusion and Aqueous-Phase Reactions |
540 |
|
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12.3.2 Aqueous-Phase Diffusion and Reaction |
542 |
|
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12.3.3 Interfacial Mass Transport and Aqueous-Phase Reactions |
543 |
|
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12.3.4 Application to the S(IV)-Ozone Reaction |
545 |
|
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12.3.5 Application to the S(IV)-Hydrogen Peroxide Reaction |
547 |
|
|
12.3.6 Calculation of Aqueous-Phase Reaction Rates |
548 |
|
|
12.3.6.1 No Mass Transport Limitations |
548 |
|
|
12.3.6.2 Aqueous-Phase Mass Transport Limitation |
548 |
|
|
12.3.6.3 Gas-Phase Limitation |
551 |
|
|
12.3.6.4 Interfacial Limitation |
551 |
|
|
12.3.6.5 Gas-Phase Plus Interfacial Limitation |
551 |
|
|
12.3.7 An Aqueous-Phase Chemistry/Mass Transport Model |
553 |
|
|
12.4 Mass Transfer to Falling Drops |
554 |
|
|
12.5 Characteristic Time for Atmospheric Aerosol Equilibrium |
555 |
|
|
12.5.1 Solid Aerosol Particles |
556 |
|
|
12.5.2 Aqueous Aerosol Particles |
557 |
|
|
12. Appendix 12 Solution of the Transient Gas-Phase Diffusion |
560 |
|
|
Problems |
561 |
|
|
References |
563 |
|
|
Chapter 13: Dynamics of Aerosol Populations |
565 |
|
|
13.1 Mathematical Representations of Aerosol Size Distributions |
565 |
|
|
13.1.1 Discrete Distribution |
565 |
|
|
13.1.2 Continuous Distribution |
566 |
|
|
13.2 Condensation |
566 |
|
|
13.2.1 The Condensation Equation |
566 |
|
|
13.2.2 Solution of the Condensation Equation |
568 |
|
|
13.3 Coagulation |
572 |
|
|
13.3.1 Brownian Coagulation |
572 |
|
|
13.3.1.1 Continuum Regime |
572 |
|
|
13.3.1.2 Transition and Free Molecular Regime |
575 |
|
|
13.3.1.3 Coagulation Rates |
576 |
|
|
13.3.1.4 Collision Efficiency |
578 |
|
|
13.3.2 The Coagulation Equation |
579 |
|
|
13.3.2.1 The Discrete Coagulation Equation |
579 |
|
|
13.3.2.2 The Continuous Coagulation Equation |
581 |
|
|
13.3.3 Solution of the Coagulation Equation |
581 |
|
|
13.3.3.1 Discrete Coagulation Equation |
581 |
|
|
13.3.3.2 Continuous Coagulation Equation |
583 |
|
|
13.4 The Discrete General Dynamic Equation |
585 |
|
|
13.5 The Continuous General Dynamic Equation |
586 |
|
|
Appendix 13.1 Additional Mechanisms of Coagulation |
588 |
|
|
13.A.1 Coagulation in Laminar Shear Flow |
588 |
|
|
13.A.2 Coagulation in Turbulent Flow |
588 |
|
|
13.A.3 Coagulation from Gravitational Settling |
589 |
|
|
13.A.4 Brownian Coagulation and External Force Fields |
590 |
|
|
13.A.4.1 Van der Waals Forces |
590 |
|
|
13.A.4.2 Coulomb Forces |
592 |
|
|
13.A.4.3 Hydrodynamic Forces |
593 |
|
|
Appendix 13.2 Solution of (13.73) |
595 |
|
|
Problems |
596 |
|
|
References |
599 |
|
|
Chapter 14: Atmospheric Organic Aerosols |
601 |
|
|
14.1 Chemistry of Secondary Organic Aerosol Formation |
602 |
|
|
14.1.1 Oxidation State of Organic Compounds |
604 |
|
|
14.1.2 Generation of Highly Oxygenated Species by Autoxidation |
607 |
|
|
14.2 Volatility of Organic Compounds |
610 |
|
|
14.3 Idealized Description of Secondary Organic Aerosol Formation |
611 |
|
|
14.3.1 Noninteracting Secondary Organic Aerosol Compounds |
611 |
|
|
14.3.2 Formation of Binary Ideal Solution with Preexisting Aerosol |
614 |
|
|
14.3.3 Formation of Binary Ideal Solution with Other Organic Vapor |
616 |
|
|
14.4 Gas-Particle Partitioning |
618 |
|
|
14.4.1 Gas-Particle Equilibrium |
618 |
|
|
14.4.2 Effect of Aerosol Water on Gas-Particle Partitioning |
622 |
|
|
14.5 Models of Soa Formation and Evolution |
624 |
|
|
14.5.1 The Volatility Basis Set |
625 |
|
|
14.5.2 Two-Dimensional SOA Models |
631 |
|
|
14.5.2.1 Two-Dimensional VBS |
631 |
|
|
14.5.2.2 Statistical Oxidation Model (SOM) |
632 |
|
|
14.5.2.3 Carbon Number-Polarity Grid (CNPG) |
633 |
|
|
14.5.2.4 Functional Group Oxidation Model (FGOM) |
633 |
|
|
14.5.2.5 Conclusion |
633 |
|
|
14.6 Primary Organic Aerosol |
633 |
|
|
14.7 The Physical State of Organic Aerosols |
636 |
|
|
14.8 Soa Particle-Phase Chemistry |
638 |
|
|
14.8.1 Particle-Phase Accretion Reactions |
640 |
|
|
14.8.2 Heterogeneous Gas-Aerosol Reactions |
640 |
|
|
14.9 Aqueous-Phase Secondary Organic Aerosol Formation |
643 |
|
|
14.9.1 Gas- versus Aqueous-Phase Routes to SOA |
644 |
|
|
14.9.2 Sources of OH Radicals in the Aqueous Phase |
646 |
|
|
14.9.3 Glyoxal as a Source of aqSOA |
647 |
|
|
14.10 Estimates of the Global Budget of Atmospheric Organic Aerosol |
650 |
|
|
14.10.1 Estimate Based on Total VOC Emissions |
650 |
|
|
14.10.2 Sulfate Lifetime and Ratio of Organic to Sulfate |
650 |
|
|
14.10.3 Atmospheric Burden and Lifetime of SOA |
651 |
|
|
14.10.4 Satellite Measurements |
651 |
|
|
Problems |
651 |
|
|
References |
654 |
|
|
Chapter 15: Interaction of Aerosols with Radiation |
661 |
|
|
15.1 Scattering and Absorption of Light By Small Particles |
661 |
|
|
15.1.1 Rayleigh Scattering Regime |
666 |
|
|
15.1.2 Geometric Scattering Regime |
668 |
|
|
15.1.3 Scattering Phase Function |
668 |
|
|
15.1.4 Extinction by an Ensemble of Particles |
668 |
|
|
15.2 Visibility |
672 |
|
|
15.3 Scattering, Absorption, and Extinction Coefficients From Mie Theory |
675 |
|
|
15.4 Calculated Visibility Reduction Based on Atmospheric Data |
679 |
|
|
Appendix 15 Calculation of Scattering and Extinction Coefficients By Mie Theory |
682 |
|
|
Problems |
682 |
|
|
References |
684 |
|
|
Part IV: Physical and Dynamic Meteorology, Cloud Physics, and Atmospheric Diffusion |
687 |
|
|
Chapter 16: Physical and Dynamic Meteorology |
689 |
|
|
16.1 Temperature in the Lower Atmosphere |
689 |
|
|
16.2 Atmospheric Stability |
693 |
|
|
16.3 The Moist Atmosphere |
698 |
|
|
16.3.1 The Gas Constant for Moist Air |
699 |
|
|
16.3.2 Level of Cloud Formation: The Lifting Condensation Level |
699 |
|
|
16.3.3 Dew-point and Wet-Bulb Temperatures |
701 |
|
|
16.3.4 The Moist Adiabatic Lapse Rate |
703 |
|
|
16.3.5 Stability of Moist Air |
707 |
|
|
16.3.6 Convective Available Potential Energy (CAPE) |
708 |
|
|
16.3.7 Thermodynamic Diagrams |
709 |
|
|
16.4 Basic Conservation Equations for the Atmospheric Surface Layer |
711 |
|
|
16.4.1 Turbulence |
715 |
|
|
16.4.2 Equations for the Mean Quantities |
716 |
|
|
16.4.3 Mixing-Length Models for Turbulent Transport |
718 |
|
|
16.5 Variation of Wind With Height in the Atmosphere |
720 |
|
|
16.5.1 Mean Velocity in the Adiabatic Surface Layer over a Smooth Surface |
721 |
|
|
16.5.2 Mean Velocity in the Adiabatic Surface Layer over a Rough Surface |
722 |
|
|
16.5.3 Mean Velocity Profiles in the Nonadiabatic Surface Layer |
723 |
|
|
16.5.4 The Pasquill Stability Classes-Estimation of L |
726 |
|
|
16.5.5 Empirical Equation for the Mean Windspeed |
728 |
|
|
Appendix 16.1 Properties of Water and Water Solutions |
729 |
|
|
16.A.1 Specific Heat of Water and Ice |
729 |
|
|
16.A.2 Latent Heats of Vaporization and Melting for Water |
729 |
|
|
16.A.3 Water Surface Tension |
729 |
|
|
Appendix 16.2 Derivation of the Basic Equations of Surface-Layer Atmospheric Fluid Mechanics |
730 |
|
|
Problems |
733 |
|
|
References |
734 |
|
|
Chapter 17: Cloud Physics |
736 |
|
|
17.1 Equilibrium of Water Droplets in the Atmosphere |
736 |
|
|
17.1.1 Equilibrium of a Pure Water Droplet |
736 |
|
|
17.1.2 Equilibrium of a Flat Water Solution |
738 |
|
|
17.1.3 Atmospheric Equilibrium of an Aqueous Solution Drop |
740 |
|
|
17.1.3.1 Stability of Atmospheric Droplets |
743 |
|
|
17.1.4 Atmospheric Equilibrium of an Aqueous Solution Drop Containing an Insoluble Substance |
745 |
|
|
17.2 Cloud and Fog Formation |
747 |
|
|
17.2.1 Isobaric Cooling |
748 |
|
|
17.2.2 Adiabatic Cooling |
748 |
|
|
17.2.3 A Simplified Mathematical Description of Cloud Formation |
749 |
|
|
17.3 Growth Rate of Individual Cloud Droplets |
751 |
|
|
17.4 Growth of a Droplet Population |
754 |
|
|
17.5 Cloud Condensation Nuclei |
758 |
|
|
17.5.1 Ambient CCN |
761 |
|
|
17.5.2 The Hygroscopic Parameter Kappa |
761 |
|
|
17.6 Cloud Processing of Aerosols |
764 |
|
|
17.6.1 Nucleation Scavenging of Aerosols by Clouds |
764 |
|
|
17.6.2 Chemical Composition of Cloud Droplets |
765 |
|
|
17.6.3 Nonraining Cloud Effects on Aerosol Concentrations |
767 |
|
|
17.6.4 Interstitial Aerosol Scavenging by Cloud Droplets |
770 |
|
|
17.7 Other Forms of Water in the Atmosphere |
771 |
|
|
17.7.1 Ice Clouds |
771 |
|
|
17.7.1.1 Freezing-Point Depression |
772 |
|
|
17.7.1.2 Curvature Effects |
774 |
|
|
17.7.1.3 Ice Nucleating Particles (INP) |
774 |
|
|
17.7.2 Rain |
775 |
|
|
17.7.2.1 Raindrop Distributions |
778 |
|
|
Appendix 17 Extended Köhler Theory |
779 |
|
|
17.1 Modified Form of Köhler Theory for a Soluble Trace Gas |
779 |
|
|
17.2 Modified Form of Köhler Theory for a Slightly Soluble Substance |
782 |
|
|
17.3 Modified Form of Köhler Theory for a Surface-Active Solute |
783 |
|
|
17.4 Examples |
784 |
|
|
Problems |
787 |
|
|
References |
788 |
|
|
Chapter 18: Atmospheric Diffusion |
791 |
|
|
18.1 Eulerian Approach |
791 |
|
|
18.2 Lagrangian Approach |
794 |
|
|
18.3 Comparison of Eulerian and Lagrangian Approaches |
795 |
|
|
18.4 Equations Governing the Mean Concentration of Species in Turbulence |
795 |
|
|
18.4.1 Eulerian Approaches |
795 |
|
|
18.4.2 Lagrangian Approaches |
797 |
|
|
18.5 Solution of the Atmospheric Diffusion Equation For an Instantaneous Source |
799 |
|
|
18.6 Mean Concentration from Continuous Sources |
800 |
|
|
18.6.1 Lagrangian Approach |
800 |
|
|
18.6.1.1 An Alternate Derivation of (18.42) |
802 |
|
|
18.6.1.2 Still Another Derivation of (18.42) |
804 |
|
|
18.6.2 Eulerian Approach |
804 |
|
|
18.6.2.1 An Alternate Derivation of (18.55) |
805 |
|
|
18.6.3 Summary of Continuous Point Source Solutions |
805 |
|
|
18.7 Statistical Theory of Turbulent Diffusion |
806 |
|
|
18.7.1 Qualitative Features of Atmospheric Diffusion |
806 |
|
|
18.7.2 Motion of a Single Particle Relative to a Fixed Axis |
808 |
|
|
18.8 Summary of Atmospheric Diffusion Theories |
811 |
|
|
18.9 Analytical Solutions for Atmospheric Diffusion: the Gaussian Plume Equation and Others |
812 |
|
|
18.9.1 Gaussian Concentration Distributions |
812 |
|
|
18.9.1.1 Total Reflection at z = 0 |
813 |
|
|
18.9.1.2 Total Absorption at z = 0 |
813 |
|
|
18.9.2 Derivation of the Gaussian Plume Equation as a Solution of the Atmospheric Diffusion Equation |
814 |
|
|
18.9.2.1 Solution of (18.90) to (18.92) |
815 |
|
|
18.9.3 Summary of Gaussian Point Source Diffusion Formulas |
819 |
|
|
18.10 Dispersion Parameters in Gaussian Models |
819 |
|
|
18.10.1 Correlations for ?y and ?z Based on Similarity Theory |
819 |
|
|
18.10.2 Correlations for ?y and ?z Based on Pasquill Stability Classes |
823 |
|
|
18.11 Plume Rise |
824 |
|
|
18.12 Functional Forms of Mean Windspeed and Eddy Diffusivities |
826 |
|
|
18.12.1 Mean Windspeed |
828 |
|
|
18.12.2 Vertical Eddy Diffusion Coefficient Kzz |
828 |
|
|
18.12.2.1 Unstable Conditions |
828 |
|
|
18.12.2.2 Neutral Conditions |
829 |
|
|
18.12.2.3 Stable Conditions |
831 |
|
|
18.12.3 Horizontal Eddy Diffusion Coefficients Kxx and Kyy |
831 |
|
|
18.13 Solutions of The Steady-State Atmospheric Diffusion Equation |
831 |
|
|
18.13.1 Diffusion from a Point Source |
832 |
|
|
18.13.2 Diffusion from a Line Source |
833 |
|
|
APPENDIX 18.1 Further Solutions of Atmospheric Diffusion Problems |
835 |
|
|
18A.1 Solution of (18.29)–(18.31) |
835 |
|
|
18A.2 Solution of (18.50) and (18.51) |
837 |
|
|
18A.3 Solution of (18.59)–(18.61) |
838 |
|
|
APPENDIX 18.2 Analytical Properties of the Gaussian Plume Equation |
839 |
|
|
Problems |
843 |
|
|
REFERENCES |
851 |
|
|
Part V: Dry and Wet Deposition |
855 |
|
|
Chapter 19: Dry Deposition |
857 |
|
|
19.1 Deposition Velocity |
857 |
|
|
19.2 Resistance Model for Dry Deposition |
858 |
|
|
19.3 Aerodynamic Resistance |
862 |
|
|
19.4 Quasilaminar Resistance |
863 |
|
|
19.4.1 Gases |
864 |
|
|
19.4.2 Particles |
864 |
|
|
19.5 Surface Resistance |
867 |
|
|
19.5.1 Surface Resistance for Dry Deposition of Gases to Water |
869 |
|
|
19.5.2 Surface Resistance for Dry Deposition of Gases to Vegetation |
873 |
|
|
19.6 Measurement of Dry Deposition |
877 |
|
|
19.6.1 Direct Methods |
877 |
|
|
19.6.1.1 Surrogate Surfaces |
877 |
|
|
19.6.1.2 Natural Surfaces |
877 |
|
|
19.6.1.3 Chamber Method |
878 |
|
|
19.6.1.4 Eddy Correlation |
878 |
|
|
19.6.1.5 Eddy Accumulation |
878 |
|
|
19.6.2 Indirect Methods |
878 |
|
|
19.6.2.1 Gradient Method |
878 |
|
|
19.6.2.2 Inferential Method |
879 |
|
|
19.6.3 Comparison of Methods |
879 |
|
|
19.7 Some Comments on Modeling and Measurement of Dry Deposition |
879 |
|
|
Problems |
880 |
|
|
References |
882 |
|
|
Chapter 20: Wet Deposition |
884 |
|
|
20.1 General Representation of Atmospheric Wet Removal Processesƒ |
884 |
|
|
20.2 Below-Cloud Scavenging of Gases |
888 |
|
|
20.2.1 Below-Cloud Scavenging of an Irreversibly Soluble Gas |
889 |
|
|
20.2.2 Below-Cloud Scavenging of a Reversibly Soluble Gas |
892 |
|
|
20.3 Precipitation Scavenging of Particles |
896 |
|
|
20.3.1 Raindrop-Aerosol Collision Efficiency |
898 |
|
|
20.3.2 Scavenging Rates |
899 |
|
|
20.4 In-Cloud Scavenging |
901 |
|
|
20.5 Acid Deposition |
902 |
|
|
20.5.1 Acid Rain Overview |
902 |
|
|
20.5.1.1 Historical Perspective |
902 |
|
|
20.5.1.2 Definition of the Problem |
903 |
|
|
20.5.2 Surface Water Acidification |
904 |
|
|
20.5.3 Cloudwater Deposition |
905 |
|
|
20.5.4 Fogs and Wet Deposition |
905 |
|
|
20.6 Acid Deposition Process Synthesis |
906 |
|
|
20.6.1 Chemical Species Involved in Acid Deposition |
906 |
|
|
20.6.2 Dry versus Wet Deposition |
906 |
|
|
20.6.3 Chemical Pathways for Sulfate and Nitrate Production |
906 |
|
|
20.6.4 Source-Receptor Relationships |
907 |
|
|
20.6.5 Linearity |
908 |
|
|
Problems |
909 |
|
|
References |
914 |
|
|
Part VI: The Global Atmosphere, Biogeochemical Cycles, and Climate |
917 |
|
|
Chapter 21: General Circulation of the Atmosphere |
919 |
|
|
21.1 Hadley Cell |
921 |
|
|
21.2 Ferrell Cell and Polar Cell |
921 |
|
|
21.3 Coriolis Force |
923 |
|
|
21.4 Geostrophic Windspeed |
925 |
|
|
21.4.1 Buys Ballot's Law |
927 |
|
|
21.4.2 Ekman Spiral |
928 |
|
|
21.5 The Thermal Wind Relation |
930 |
|
|
21.6 Stratospheric Dynamics |
933 |
|
|
21.7 The Hydrologic Cycle |
933 |
|
|
Problems |
934 |
|
|
References |
935 |
|
|
Chapter 22: Global Cycles: Sulfur and Carbon |
936 |
|
|
22.1 The Atmospheric Sulfur Cycle |
936 |
|
|
22.2 The Global Carbon Cycle |
940 |
|
|
22.2.1 Carbon Dioxide |
940 |
|
|
22.2.2 Compartmental Model of the Global Carbon Cycle |
942 |
|
|
22.2.3 Atmospheric Lifetime of CO2 |
949 |
|
|
22.3 Solution for a Steady-State Four-Compartment Model of the Atmosphere |
951 |
|
|
Problems |
955 |
|
|
References |
957 |
|
|
Chapter 23: Global Climate |
959 |
|
|
23.1 Earth'S Energy Balance |
959 |
|
|
23.2 Radiative Forcing |
961 |
|
|
23.2.1 Climate Sensitivity |
962 |
|
|
23.2.2 Climate Feedbacks |
963 |
|
|
23.2.3 Timescales of Climate Change |
963 |
|
|
23.3 The Greenhouse Effect |
964 |
|
|
23.4 Climate-Forcing Agents |
970 |
|
|
23.4.1 Solar Irradiance |
970 |
|
|
23.4.2 Greenhouse Gases |
973 |
|
|
23.4.3 Radiative Efficiencies of Greenhouse Gases |
974 |
|
|
23.4.4 Aerosols |
974 |
|
|
23.4.5 Summary of IPCC (2013) Estimated Forcing |
975 |
|
|
23.4.6 The Preindustrial Atmosphere |
976 |
|
|
23.5 Cosmic Rays and Climate |
977 |
|
|
23.6 Climate Sensitivity |
978 |
|
|
23.7 Simplified Dynamic Description of Climate Forcing and Responseƒ |
979 |
|
|
23.7.1 Response to a Perturbation of Earth's Radiative Equilibrium |
979 |
|
|
23.7.2 Physical Interpretation of Feedback Factors |
982 |
|
|
23.8 Climate Feedbacks |
983 |
|
|
23.8.1 Water Vapor Feedback |
983 |
|
|
23.8.2 Lapse Rate Feedback |
984 |
|
|
23.8.3 Cloud Feedback |
984 |
|
|
23.8.4 Arctic Sea Ice Feedback |
986 |
|
|
23.8.5 Summary of Feedbacks |
986 |
|
|
23.9 Relative Radiative Forcing Indices |
988 |
|
|
23.10 Atmospheric Chemistry and Climate Change |
989 |
|
|
23.10.1 Indirect Chemical Impacts |
990 |
|
|
23.10.2 Atmospheric Lifetimes and Adjustment Times |
991 |
|
|
23.11 Conclusion |
992 |
|
|
Problems |
993 |
|
|
References |
995 |
|
|
Chapter 24: Aerosols and Climate |
998 |
|
|
24.1 Scattering-Absorbing Model of an Aerosol Layer |
1000 |
|
|
24.2 Cooling Versus Heating of an Aerosol Layer |
1003 |
|
|
24.3 Scattering Model of an Aerosol Layer for a Nonabsorbing Aerosol |
1005 |
|
|
24.4 Upscatter Fraction |
1007 |
|
|
24.5 Optical Depth and Column Forcing |
1009 |
|
|
24.6 Internal and External Mixtures |
1013 |
|
|
24.7 Top-Of-The-Atmosphere Versus Surface Forcing |
1015 |
|
|
24.8 Indirect Effects of Aerosols on Climate |
1018 |
|
|
24.8.1 Stratocumulus Clouds |
1019 |
|
|
24.8.2 Simplified Model for Cloud Albedo |
1021 |
|
|
24.8.3 Albedo Susceptibility: Simplified Model |
1023 |
|
|
24.8.4 Albedo Susceptibility: Additional Considerations |
1025 |
|
|
24.8.5 A General Equation for Cloud Albedo Susceptibility |
1027 |
|
|
24.8.6 Estimating Indirect Aerosol Forcing on Climate |
1031 |
|
|
Problems |
1031 |
|
|
References |
1032 |
|
|
Part VII: Chemical Transport Models and Statistical Models |
1037 |
|
|
Chapter 25: Atmospheric Chemical Transport Models |
1039 |
|
|
25.1 Introduction |
1039 |
|
|
25.1.1 Model Types |
1040 |
|
|
25.1.2 Types of Atmospheric Chemical Transport Models |
1041 |
|
|
25.2 Box Models |
1042 |
|
|
25.2.1 The Eulerian Box Model |
1043 |
|
|
25.2.2 A Lagrangian Box Model |
1045 |
|
|
25.3 Three-Dimensional Atmospheric Chemical Transport Models |
1048 |
|
|
25.3.1 Coordinate System-Uneven Terrain |
1048 |
|
|
25.3.2 Initial Conditions |
1050 |
|
|
25.3.3 Boundary Conditions |
1051 |
|
|
25.4 One-Dimensional Lagrangian Models |
1052 |
|
|
25.5 Other Forms of Chemical Transport Models |
1054 |
|
|
25.5.1 Atmospheric Diffusion Equation Expressed in Terms of Mixing Ratio |
1054 |
|
|
25.5.2 Pressure-Based Coordinate System |
1057 |
|
|
25.5.3 Spherical Coordinates |
1059 |
|
|
25.6 Numerical Solution of Chemical Transport Models |
1059 |
|
|
25.6.1 Coupling Problem-Operator Splitting |
1060 |
|
|
25.6.1.1 Finite Difference Methods |
1060 |
|
|
25.6.1.2 Finite Element Methods |
1062 |
|
|
25.6.1.3 Operator Splitting |
1063 |
|
|
25.6.2 Chemical Kinetics |
1065 |
|
|
25.6.2.1 Backward Differentiation Methods |
1068 |
|
|
25.6.2.2 Asymptotic Methods |
1068 |
|
|
25.6.3 Diffusion |
1069 |
|
|
25.6.4 Advection |
1070 |
|
|
25.7 Model Evaluation |
1074 |
|
|
25.8 Response of Organic and Inorganic Aerosols to Changes in Emission |
1075 |
|
|
Problems |
1076 |
|
|
References |
1078 |
|
|
Chapter 26: Statistical Models |
1079 |
|
|
26.1 Receptor Modeling Methods |
1079 |
|
|
26.2 Chemical Mass Balance (Cmb) |
1082 |
|
|
26.2.1 CMB Evaluation |
1086 |
|
|
26.2.2 CMB Resolution |
1087 |
|
|
26.2.3 CMB Codes |
1087 |
|
|
26.3 Factor Analysis |
1087 |
|
|
26.3.1 Principal-Component Analysis (PCA) |
1089 |
|
|
26.3.2 Positive Matrix Factorization (PMF) |
1092 |
|
|
26.3.2.1 Uncertainties and Missing Values |
1092 |
|
|
26.3.2.2 Extreme Values |
1093 |
|
|
26.3.2.3 Choice of Number of Factors |
1093 |
|
|
26.3.2.4 Rotational Ambiguity |
1094 |
|
|
26.3.2.5 The Multilinear Engine (ME) |
1095 |
|
|
26.4 Methods Incorporating Wind Information |
1095 |
|
|
26.4.1 Potential Source Contribution Function (PSCF) |
1096 |
|
|
26.4.2 Empirical Orthogonal Function (EOF) |
1098 |
|
|
26.5 Probability Distributions for Air Pollutant Concentrations |
1100 |
|
|
26.5.1 The Lognormal Distribution |
1101 |
|
|
26.5.2 The Weibull Distribution |
1102 |
|
|
26.6 Estimation of Parameters in the Distributions |
1102 |
|
|
26.6.1 Method of Quantiles |
1103 |
|
|
26.6.2 Method of Moments |
1104 |
|
|
26.7 Order Statistics of Air Quality Data |
1106 |
|
|
26.7.1 Basic Notions and Terminology of Order Statistics |
1106 |
|
|
26.7.2 Extreme Values |
1107 |
|
|
26.8 Exceedances of Critical Levels |
1108 |
|
|
26.9 Alternative Forms of Air Quality Standards |
1108 |
|
|
26.10 Relating Current and Future Air Pollutant Statistical Distributions |
1111 |
|
|
Problems |
1113 |
|
|
References |
1115 |
|
|
Appendix A: Units and Physical Constants |
1119 |
|
|
A.1 Si Base Units |
1119 |
|
|
A.2 Si Derived Units |
1120 |
|
|
A.3 Fundamental Physical Constants |
1122 |
|
|
A.4 Properties of the Atmosphere and Water |
1122 |
|
|
A.5 Units for Representing Chemical Reactions |
1124 |
|
|
A.6 Concentrations in the Aqueous Phase |
1124 |
|
|
A.7 Symbols Denoting Concentration |
1125 |
|
|
References |
1125 |
|
|
Appendix B: Rate Constants of Atmospheric Chemical Reactions |
1126 |
|
|
References |
1134 |
|
|
Appendix C: Abbreviations |
1135 |
|
|
Index |
1140 |
|
|
EULA |
1149 |
|