Experimental Observation of the Autler-Townes Splitting in Polyatomic Molecules

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Autler-Townes (AT) splitting has been experimentally observed in the optical transition between the zero-point levels of S-1 and S(0 )for supersonically cooled 2-methoxythiophenol, 2-fluorothiophenol, and 2-chlorothiophenol. This is the first experimental observation of the light-dressed quantum states of polyatomic molecules (N > 3) in the electronic transition. In the resonance-enhanced ionization process involving the optically coupled states, if Rabi cycling is ensured within the nanosecond laser pulse, AT splitting is clearly observed for the open system for which the excited-state lifetime is shorter than hundreds of picoseconds. Semiclassical optical Bloch equations and a dressed-atom approach based on the three-level atomic model describe the experiment quite well, giving deep insights into the light-matter interaction in polyatomic molecular systems.
Publisher
AMER CHEMICAL SOC
Issue Date
2020-08
Language
English
Article Type
Article
Citation

JOURNAL OF PHYSICAL CHEMISTRY LETTERS, v.11, no.16, pp.6791 - 6795

ISSN
1948-7185
DOI
10.1021/acs.jpclett.0c01918
URI
http://hdl.handle.net/10203/281931
Appears in Collection
CH-Journal Papers(저널논문)
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