Sequential two photon excitation of the C2 Swan transitions and C2 relaxation dynamics in rare gas solids

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Abstract

The C2 d 3Πg-a 3Π u emission in solid Ar and Ne is excited both by sequential absorption of two identical photons and by two unlike photons using two separately tunable lasers. It is shown that excitation of guest molecules by sequential absorption should be a useful technique for populating levels unaccessible in a single step absorption process. The different phonon band shapes observed for the X 1Σg+-A 1Πu and d 3Πg-a 3Πu transitions are interpreted in terms of the electronic structure of the states involved. The vibrational relaxation in the d 3Πg state is fast and shows erratic variation with ν. The lifetimes of the low a 3Πu levels vary from 65 μs for ν = 0 to less than 0.5 μs for ν = 3. The rate of the spin and symmetry forbidden radiationless crossing into the ground state shows a strong temperature dependence expected by theory. The efficient two photon excitation of the low d 3Πg levels leads to population inversion and stimulated emission on the d 3Πg→a 3Πu Swan bands.

Original languageEnglish
Pages (from-to)2296-2304
Number of pages9
JournalJournal of Chemical Physics
Volume65
Issue number6
DOIs
StatePublished - 1976
Externally publishedYes

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