Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 10, Issue 2, Pages 265-269Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.8b02878
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- Netherlands Organization for Scientific Research (NWO) [Rubicon 68-50-1410]
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We report an experimental study of iodomethane attosecond transient absorption spectroscopy (ATAS) in the region of iodine 4d core-to-valence/Rydberg excitation. Similar to previous atomic experiments, extreme ultraviolet near-infrared (XUV-NIR) delay-dependent absorbance changes reflect a light-induced phase due to an NIR-field driven AC Stark shift of the excited states, as well as pathway interferences arising from couplings between neighboring states. As a novel aspect of molecular ATAS, we observe pronounced differences between the ATAS signatures of valence and Rydberg states. While the core-to-valence transitions carry the majority of the XUV oscillator strength, the core-to-Rydberg transitions are dominantly affected by a moderately strong, nonionizing NIR field. Our experimental findings are corroborated by ab initio calculations and ATAS simulations.
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