Roaming in highly excited states : The central atom elimination of triatomic molecule decomposition
Chemical reactions are generally assumed to proceed from reactants to products along the minimum energy path (MEP). However, straying from the MEP-roaming-has been recognized as an unconventional reaction mechanism and found to occur in both the ground and first excited states. Its existence in highly excited states is however not yet established. We report a dissociation channel to produce electronically excited fragments, S(1D)+O2(a1Δg), from SO2 photodissociation in highly excited states. The results revealed two dissociation pathways: One proceeds through the MEP to produce vibrationally colder O2(a1Δg) and the other yields vibrationally hotter O2(a1Δg) by means of a roaming pathway involving an intramolecular O abstraction during reorientation motion. Such roaming dynamics may well be the rule rather than the exception for molecular photodissociation through highly excited states.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2024 |
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| Erschienen: |
2024 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:383 |
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| Enthalten in: |
Science (New York, N.Y.) - 383(2024), 6684 vom: 16. Feb., Seite 746-750 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Li, Zhenxing [VerfasserIn] |
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| Links: |
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| Anmerkungen: |
Date Revised 15.02.2024 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
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| doi: |
10.1126/science.adn3357 |
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| funding: |
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| Förderinstitution / Projekttitel: |
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NLM368492400 |
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| 520 | |a Chemical reactions are generally assumed to proceed from reactants to products along the minimum energy path (MEP). However, straying from the MEP-roaming-has been recognized as an unconventional reaction mechanism and found to occur in both the ground and first excited states. Its existence in highly excited states is however not yet established. We report a dissociation channel to produce electronically excited fragments, S(1D)+O2(a1Δg), from SO2 photodissociation in highly excited states. The results revealed two dissociation pathways: One proceeds through the MEP to produce vibrationally colder O2(a1Δg) and the other yields vibrationally hotter O2(a1Δg) by means of a roaming pathway involving an intramolecular O abstraction during reorientation motion. Such roaming dynamics may well be the rule rather than the exception for molecular photodissociation through highly excited states | ||
| 650 | 4 | |a Journal Article | |
| 700 | 1 | |a Fu, Yan-Lin |e verfasserin |4 aut | |
| 700 | 1 | |a Luo, Zijie |e verfasserin |4 aut | |
| 700 | 1 | |a Yang, Shuaikang |e verfasserin |4 aut | |
| 700 | 1 | |a Wu, Yucheng |e verfasserin |4 aut | |
| 700 | 1 | |a Wu, Hao |e verfasserin |4 aut | |
| 700 | 1 | |a Wu, Guorong |e verfasserin |4 aut | |
| 700 | 1 | |a Zhang, Weiqing |e verfasserin |4 aut | |
| 700 | 1 | |a Fu, Bina |e verfasserin |4 aut | |
| 700 | 1 | |a Yuan, Kaijun |e verfasserin |4 aut | |
| 700 | 1 | |a Zhang, Donghui |e verfasserin |4 aut | |
| 700 | 1 | |a Yang, Xueming |e verfasserin |4 aut | |
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