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OCS in para-hydrogen clusters: rotational dynamics and superfluidity.

F Paesani1, R E Zillich, Y Kwon

  • 1Department of Chemistry and Pitzer Center for Theoretical Chemistry, University of California, Berkeley, California 94720, USA. fpaesani@holmium.cchem.berkeley.edu

The Journal of Chemical Physics
|May 28, 2005
PubMed
Summary

The study reveals how para-hydrogen molecules influence OCS molecule rotation. Initially rigid, the cluster becomes more flexible, showing partial superfluidity in para-hydrogen as more molecules are added.

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Area of Science:

  • Quantum Chemistry
  • Molecular Spectroscopy
  • Condensed Matter Physics

Background:

  • Understanding molecular interactions in clusters is key to solvation studies.
  • Para-hydrogen (pH2) clusters offer a unique system to probe quantum effects like superfluidity.

Purpose of the Study:

  • To analyze the rotational excitations of OCS molecules within pH2 clusters.
  • To investigate the influence of cluster size (9-17 pH2 molecules) on OCS rotational behavior.
  • To explore the onset and nature of para-hydrogen superfluidity in these clusters.

Main Methods:

  • Analysis of rotational energy levels of OCS in pH2 clusters.
  • Fitting experimental data to extract effective rotational constants.
  • Path-integral Monte Carlo (PIMC) simulations to model cluster dynamics.

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Main Results:

  • Effective rotational constant decreases up to N=13, indicating near-rigid coupling.
  • Rigidity is lost for clusters with 14-17 pH2 molecules.
  • PIMC calculations explain the observed behavior through partial para-hydrogen superfluid response.

Conclusions:

  • Para-hydrogen exhibits a partial superfluid response to OCS rotations perpendicular to the OCS axis.
  • Complete superfluid response is observed for rotations along the OCS axis when N >= 10.
  • Cluster size dictates the transition from rigid coupling to superfluid behavior.