Rotational Coherence Spectroscopy of Molecules in Helium Nanodroplets: Reconciling the Time and the Frequency Domains

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  • Adam S. Chatterley
  • ,
  • Lars Christiansen
  • ,
  • Constant A. Schouder
  • Anders V. Jørgensen
  • ,
  • Benjamin Shepperson
  • ,
  • Igor N. Cherepanov, Institute of Science and Technology Austria
  • ,
  • Giacomo Bighin, Institute of Science and Technology Austria
  • ,
  • Robert E. Zillich, Johannes Kepler University of Linz
  • ,
  • Mikhail Lemeshko, Institute of Science and Technology Austria
  • ,
  • Henrik Stapelfeldt

Alignment of OCS, CS2, and I2 molecules embedded in helium nanodroplets is measured as a function of time following rotational excitation by a nonresonant, comparatively weak ps laser pulse. The distinct peaks in the power spectra, obtained by Fourier analysis, are used to determine the rotational, B, and centrifugal distortion, D, constants. For OCS, B and D match the values known from IR spectroscopy. For CS2 and I2, they are the first experimental results reported. The alignment dynamics calculated from the gas-phase rotational Schrödinger equation, using the experimental in-droplet B and D values, agree in detail with the measurement for all three molecules. The rotational spectroscopy technique for molecules in helium droplets introduced here should apply to a range of molecules and complexes.

Original languageEnglish
Article number013001
JournalPhysical Review Letters
Number of pages6
Publication statusPublished - Jul 2020

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