Introduction to Atmospheric Photochemistry AOSC 433/633 & CHEM 433 Ross Salawitch
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1 Introduction to Atmospheric Photochemistry AOSC 433/633 & CHEM 433 Ross Salawitch Class Web Site: Lecture 9 9 March
2 Chapman Chemistry Production of stratospheric O 3 initiated when O 2 is photodissociated by UV sunlight O 3 formed when resulting O atom reacts with O 2 : hν + O 2 O + O (1) O + O 2 + M O 3 + M (2) O 3 removed by photodissociation (UV sunlight) or by reaction with O : hν + O 3 O + O 2 (3) O + O 3 O 2 + O 2 (4) This reaction sequence was first worked out in the 1930s by Sydney Chapman, an English mathematician and geophysicist 2
3 Chapman Chemistry The cycling between O and O 2 (rxns 2 and 3) occurs much more rapidly than leakage into (rxn 1) or out of the system (rxn 4) The sum O + O 3 is commonly called odd oxygen (1) (2) (3) (4) (4) Rxn (1) produces two odd oxygen molecules Rxn (4) consumes two odd oxygen molecules and reactions 2 and 3 recycle odd oxygen molecules 3
4 Chapman Chemistry The concentration of odd oxygen reflects a balance between production and consumption: 2 k 4 [O] [O 3 ] = 2 J 1 [O 2 ] (5) Similarly the abundance of O3 (or O) reflects a balance between P & L of fast inner cycle: k 2 [O] [O 2 ] [M] = J 3 [O 3 ] (6) Rearranging (6) yields: [O] = k J 3[O 3] [O ][M] 2 2 (7) Subbing this expression into (5) yields: 1/2 J1 k 2 3/2 [O 3] = fo2[m] (8) J3 k4 where f O2 = O 2 mixing ratio, or ~0.21 4
5 Chapman Chemistry 1/2 J1 k 2 [O 3] = fo2[m] J3 k4 3/2 [O 3 ] falls off with increasing altitude (high in stratosphere), at a rate determined by [M] 3/ 2, because: [O 3 ] falls off with decreasing altitude (low in stratosphere) due to a rapid drop in J 1, reflecting: Observed [O 3 ] < Chapman [O 3 ] : why?!? 5
6 Chapman Chemistry [Ο] + [Ο 3] [Ο3] Lifetime of Odd Oxygen = (9) 2 J [O ] 2 J [O ] Chapman Profile Observed Profile Warneck, Chemistry of the Natural Atmosphere, 2000 Analysis of (9) and dynamical models shows that transport exerts a major influence on odd oxygen (e.g., ozone) below about 30 km altitude 6
7 The real stratosphere is a bit more complex: Stratospheric Photochemistry McElroy, The Atmospheric Environment,
8 Stratospheric Photochemistry plus these : McElroy, The Atmospheric Environment,
9 and these as well : Stratospheric Photochemistry McElroy, The Atmospheric Environment,
10 Stratospheric Photochemistry: Odd Oxygen Loss By Families Calculated fraction of odd oxygen loss due to various families of radicals After Osterman et al., GRL, 24, 1107, 1997; Sen et al., JGR, 103, ; Sen et al., JGR, 104, 26653,
11 One Atmosphere One Photochemistry Stratosphere HO 2 formation: OH + O 3 HO 2 + O 2 HO 2 loss: HO 2 + O 3 OH + 2 O 2 Net: O 3 + O 3 3 O 2 Troposphere HO 2 formation: O 2 OH + CO HO 2 + CO 2 HO 2 loss: HO 2 + NO OH + NO 2 Followed by: NO 2 + hν NO +O O+ O 2 + M O 3 + M Tropopause Net: CO + 2 O 2 CO 2 + O 3 Above Tropopause: Lots of O 3, little CO Below Tropopause: Lots of CO, little O 3 Courtesy of Laura Pan, NCAR 11
12 One Atmosphere One Photochemistry Stratosphere HO 2 formation: OH + O 3 HO 2 + O 2 HO 2 loss: HO 2 + O 3 OH + 2 O 2 Net: O 3 + O 3 3 O 2 Troposphere HO 2 formation: O 2 OH + CO HO 2 + CO 2 HO 2 loss: HO 2 + NO OH + NO 2 Followed by: NO 2 + hν NO +O O+ O 2 + M O 3 + M Net: CO + 2 O 2 CO 2 + O 3 Above Tropopause: Lots of O 3 results in conversion of OH to HO 2 happening via reaction with O 3 Below Tropopause: Lots of CO results in conversion of OH to HO 2 happening via reaction with CO Lanzendorf et al., JPC,
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