Elucidating the origins of multimode vibrational coherences of polyatomic molecules induced by intense laser fields

Zhengrong Wei, Jialin Li, Lin Wang, Soo Teck See, Mark Hyunpong Jhon, Yingfeng Zhang, Fan Shi, Minghui Yang and Zhi-Heng Loh ()
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Zhengrong Wei: Nanyang Technological University
Jialin Li: Nanyang Technological University
Lin Wang: Nanyang Technological University
Soo Teck See: Nanyang Technological University
Mark Hyunpong Jhon: Institute of High Performance Computing A*STAR
Yingfeng Zhang: Chinese Academy of Sciences
Fan Shi: Chinese Academy of Sciences
Minghui Yang: Chinese Academy of Sciences
Zhi-Heng Loh: Nanyang Technological University

Nature Communications, 2017, vol. 8, issue 1, 1-7

Abstract: Abstract Strong-field laser–molecule interaction forms much of the basis for initiating and probing ultrafast quantum dynamics. Previous studies aimed at elucidating the origins of vibrational coherences induced by intense laser fields have been confined to diatomic molecules. Furthermore, in all cases examined to date, vibrational wave packet motion is found to be induced by R-selective depletion; wave packet motion launched by bond softening, though theoretically predicted, remains hitherto unobserved. Here we employ the exquisite sensitivity of femtosecond extreme ultraviolet absorption spectroscopy to sub-picometer structural changes to observe both bond softening-induced vibrational wave packets, launched by the interaction of intense laser pulses with iodomethane, as well as multimode vibrational motion of the parent ion produced by strong-field ionization. In addition, we show that signatures of coherent vibrational motion in the time-dependent extreme ultraviolet absorption spectra directly furnish vibronic coupling strengths involving core-level transitions, from which geometrical parameters of transient core-excited states are extracted.

Date: 2017
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DOI: 10.1038/s41467-017-00848-2

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