Vibrational relaxation dynamics of I35Cl(B, ν′) induced by low-temperature collisions with He atoms

Joshua Paul Darr, Richard A. Loomis

Research output: Contribution to journalArticle

2 Citations (Scopus)

Abstract

Using laser-induced fluorescence and two-laser, pump-probe spectroscopy, collision-induced vibrational relaxation is observed to compete with the dissociation of electronically excited ICl in a helium carrier gas expansion. By thoroughly characterizing the expansion properties, we observe that collisions of ICl(B, ν′ = 3) molecules with He atoms in the expansion induce vibrational relaxation of the initially prepared dihalogen down to rotor states in the next lower ICl(B,ν′ = 2) level on timescales that compete with the rate for non-adiabatic transfer from the B state to the Z1 state. The resulting ICl(B,ν′ = 2,j′) product rotational distribution, along with the analogous ICl(B,ν′ = 1,j′) distribution formed by collisional relaxation of molecules in the long-lived ICl(B,ν′ = 2) level are compared to ICl(B,ν′ = 2,j′) products formed by vibrational predissociation of He⋯ICl complexes prepared in different intermolecular vibrational levels within the He + ICl(B,ν′ = 3) potential. No evidence is observed for resonance-enhanced collisional cross sections, even at the low temperatures achieved, T < 1.0 K.

Original languageEnglish (US)
Pages (from-to)3323-3330
Number of pages8
JournalPhysical Chemistry Chemical Physics
Volume7
Issue number18
DOIs
StatePublished - Sep 21 2005

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molecular relaxation
Atoms
collisions
gas expansion
atoms
Helium
Molecules
expansion
Lasers
products
laser induced fluorescence
Temperature
rotors
molecules
Rotors
Gases
Fluorescence
helium
Pumps
Spectroscopy

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

Cite this

Vibrational relaxation dynamics of I35Cl(B, ν′) induced by low-temperature collisions with He atoms. / Darr, Joshua Paul; Loomis, Richard A.

In: Physical Chemistry Chemical Physics, Vol. 7, No. 18, 21.09.2005, p. 3323-3330.

Research output: Contribution to journalArticle

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abstract = "Using laser-induced fluorescence and two-laser, pump-probe spectroscopy, collision-induced vibrational relaxation is observed to compete with the dissociation of electronically excited ICl in a helium carrier gas expansion. By thoroughly characterizing the expansion properties, we observe that collisions of ICl(B, ν′ = 3) molecules with He atoms in the expansion induce vibrational relaxation of the initially prepared dihalogen down to rotor states in the next lower ICl(B,ν′ = 2) level on timescales that compete with the rate for non-adiabatic transfer from the B state to the Z1 state. The resulting ICl(B,ν′ = 2,j′) product rotational distribution, along with the analogous ICl(B,ν′ = 1,j′) distribution formed by collisional relaxation of molecules in the long-lived ICl(B,ν′ = 2) level are compared to ICl(B,ν′ = 2,j′) products formed by vibrational predissociation of He⋯ICl complexes prepared in different intermolecular vibrational levels within the He + ICl(B,ν′ = 3) potential. No evidence is observed for resonance-enhanced collisional cross sections, even at the low temperatures achieved, T < 1.0 K.",
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N2 - Using laser-induced fluorescence and two-laser, pump-probe spectroscopy, collision-induced vibrational relaxation is observed to compete with the dissociation of electronically excited ICl in a helium carrier gas expansion. By thoroughly characterizing the expansion properties, we observe that collisions of ICl(B, ν′ = 3) molecules with He atoms in the expansion induce vibrational relaxation of the initially prepared dihalogen down to rotor states in the next lower ICl(B,ν′ = 2) level on timescales that compete with the rate for non-adiabatic transfer from the B state to the Z1 state. The resulting ICl(B,ν′ = 2,j′) product rotational distribution, along with the analogous ICl(B,ν′ = 1,j′) distribution formed by collisional relaxation of molecules in the long-lived ICl(B,ν′ = 2) level are compared to ICl(B,ν′ = 2,j′) products formed by vibrational predissociation of He⋯ICl complexes prepared in different intermolecular vibrational levels within the He + ICl(B,ν′ = 3) potential. No evidence is observed for resonance-enhanced collisional cross sections, even at the low temperatures achieved, T < 1.0 K.

AB - Using laser-induced fluorescence and two-laser, pump-probe spectroscopy, collision-induced vibrational relaxation is observed to compete with the dissociation of electronically excited ICl in a helium carrier gas expansion. By thoroughly characterizing the expansion properties, we observe that collisions of ICl(B, ν′ = 3) molecules with He atoms in the expansion induce vibrational relaxation of the initially prepared dihalogen down to rotor states in the next lower ICl(B,ν′ = 2) level on timescales that compete with the rate for non-adiabatic transfer from the B state to the Z1 state. The resulting ICl(B,ν′ = 2,j′) product rotational distribution, along with the analogous ICl(B,ν′ = 1,j′) distribution formed by collisional relaxation of molecules in the long-lived ICl(B,ν′ = 2) level are compared to ICl(B,ν′ = 2,j′) products formed by vibrational predissociation of He⋯ICl complexes prepared in different intermolecular vibrational levels within the He + ICl(B,ν′ = 3) potential. No evidence is observed for resonance-enhanced collisional cross sections, even at the low temperatures achieved, T < 1.0 K.

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