Photodissociation of sulfur dioxide clusters: Excitation to the e state

Kenneth Knappenberger, A. W. Castleman

Research output: Contribution to journalConference article

Abstract

Due to its ubiquitous nature, SO2 has been a chromophore of spectroscopic interest for some time. However, its potential energy surface is very complex and many details of SO2 photolysis remain unknown. A femtosecond pump-probe technique was used to elucidate the temporal evolution of photoinduced wavepacket motion of this chromophore. The monomer transient rapidly decayed, exhibiting an excited state lifetime of 230 fsec. The corresponding product, SO, displayed a growth of 225 fsec in accord with the proposed mechanism resulting in S-O cleavage. The addition of sequential SO2 molecules to the cluster significantly altered the lifetime associated with the E state, resulting in an increase from 230 to 435 fsec for one to four SO2 units, respectively. This trend was consistent with the proposed dissociation mechanism. Molecular SO2 clusters were formed through van der Waals forces and as additional units are accommodated a steric force was exerted on the bending SO2, thereby impeding its achievement of a linear geometry. Dissociation of the molecular clusters proceeded differently than the SO2 molecule itself. This is an abstract of a paper presented at the 228th ACS National Meeting (Philadelphia, PA 8/22-26/2004).

Original languageEnglish (US)
Pages (from-to)81-83
Number of pages3
JournalACS, Division of Environmental Chemistry - Preprints of Extended Abstracts
Volume44
Issue number2
StatePublished - Dec 1 2004
Event228th ACS National Meeting - Philadelphia, PA, United States
Duration: Aug 22 2004Aug 26 2004

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Photodissociation
Sulfur dioxide
Chromophores
Van der Waals forces
Potential energy surfaces
Molecules
Photolysis
Excited states
Monomers
Pumps
Geometry

All Science Journal Classification (ASJC) codes

  • Energy(all)

Cite this

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abstract = "Due to its ubiquitous nature, SO2 has been a chromophore of spectroscopic interest for some time. However, its potential energy surface is very complex and many details of SO2 photolysis remain unknown. A femtosecond pump-probe technique was used to elucidate the temporal evolution of photoinduced wavepacket motion of this chromophore. The monomer transient rapidly decayed, exhibiting an excited state lifetime of 230 fsec. The corresponding product, SO, displayed a growth of 225 fsec in accord with the proposed mechanism resulting in S-O cleavage. The addition of sequential SO2 molecules to the cluster significantly altered the lifetime associated with the E state, resulting in an increase from 230 to 435 fsec for one to four SO2 units, respectively. This trend was consistent with the proposed dissociation mechanism. Molecular SO2 clusters were formed through van der Waals forces and as additional units are accommodated a steric force was exerted on the bending SO2, thereby impeding its achievement of a linear geometry. Dissociation of the molecular clusters proceeded differently than the SO2 molecule itself. This is an abstract of a paper presented at the 228th ACS National Meeting (Philadelphia, PA 8/22-26/2004).",
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Photodissociation of sulfur dioxide clusters : Excitation to the e state. / Knappenberger, Kenneth; Castleman, A. W.

In: ACS, Division of Environmental Chemistry - Preprints of Extended Abstracts, Vol. 44, No. 2, 01.12.2004, p. 81-83.

Research output: Contribution to journalConference article

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