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Perturbation facilitated two-color four-wave-mixing spectroscopy of C-3

Type of publication Peer-reviewed
Publikationsform Original article (peer-reviewed)
Publication date 2013
Author Sych Y., Bornhauser P., Knopp G., Liu Y., Gerber T., Marquardt R., Radi P. P.,
Project Spectroscopic Characterization of Radicals by Degenerate and Two-Color Resonant Four-Wave Mixing
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Original article (peer-reviewed)

Journal JOURNAL OF CHEMICAL PHYSICS
Volume (Issue) 139(15)
Page(s) 154203
Title of proceedings JOURNAL OF CHEMICAL PHYSICS
DOI 10.1063/1.4825198

Abstract

Perturbation-facilitated two-color resonant four-wave-mixing spectroscopy is realized to access the (dark) triplet manifold of the C3 molecule from the singlet X˜1Σ+g ground state. The inherent nonlinear signal dependence and coherence of the technique result in a favorable detection of the excited triplet states of interest. The observation of a newly found 3Δu electronic state is achieved by a two-step excitation via “gate-way” levels (i.e., singlet-triplet mixed levels). Additionally, by fixing the probe laser on a transition exhibiting mainly triplet-triplet character and scanning the pump laser, we demonstrate an effective spin-filtering in a four-wave mixing measurement where only transitions to the perturber Σu−3 state appear exclusively in an otherwise congested spectral range of the Comet band. Ab initio calculations of excited triplet states complement our analysis with the electronic assignment of the observed resonances.
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