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Coherent multistep rovibrational excitation using intense midinfrared pulses

Hiroki Tsusaka, Ikki Morichika, and Satoshi Ashihara

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Phys. Rev. Research 6, L042058 – Published 9 December, 2024

DOI: https://doi.org/10.1103/PhysRevResearch.6.L042058

Abstract

We experimentally demonstrate coherent multistep rovibrational excitation in gas-phase carbon dioxide using intense midinfrared laser pulses. Ultrafast pump-probe spectroscopy directly observes excited-state rovibrational lines up to V=11 state with rotational quantum numbers of J=0−40. The observed signal for each transition line is found to oscillate with the pump-probe delay time, attributed to rotational beats based on higher-order nonlinear response function theory. These results indicate generation of rotational wave packets in the high-lying vibrational states, which paves the way toward mode-selective stereochemistry at the electronic ground-state.

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Phys. Rev. Research 6, L042058– Published 9 December, 2024
  • Received 31 May 2024
  • Accepted 20 November 2024
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Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.

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