Spectroscopic studies of OCS-doped 4He clusters with 9-72 helium atoms : observation of broad oscillations in the rotational moment of inertia

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DOIResolve DOI: http://doi.org/10.1021/jp070618w
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TypeArticle
Journal titleThe Journal of Physical Chemistry A
ISSN1089-5639
Volume111
Issue31
Pages73297337; # of pages: 9
AbstractHigh-resolution spectra of HeN-OCS clusters with N up to 39 in the microwave region and up to 72 in the infrared region were observed with apparatus-limited line widths of about 15 kHz and 0.001 cm-1, respectively. The cold (~0.2 K) clusters were produced in pulsed supersonic jet expansions of very dilute OCS + He mixtures and probed using a microwave Fourier transform spectrometer or a tunable infrared diode laser spectrometer. Consistent analyses of the microwave and infrared data yield band origins for the carbonyl stretching vibration, together with rotational parameters for the ground and excited vibrational states. The rotational constant, B, passes through a minimum at N = 9 and then rises as the He atoms uncouple from the OCS rotational motion as a result of superfluid effects. There are broad unexpected oscillations in B, with maxima at N = 24 and 47 and minima at N = 36 and 62. The change in B upon vibrational excitation, which is negative for the OCS molecule, converges to positive values for N > 15. These results help to bridge the gap between individual molecules and bulk matter with atom-by-atom resolution over a significant range of cluster sizes.
Publication date
LanguageEnglish
AffiliationNational Research Council Canada; NRC Steacie Institute for Molecular Sciences
Peer reviewedYes
Identifier16891788
NPARC number12339036
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Record identifiereec7c859-2e39-45f0-a667-8c171e74b4d6
Record created2009-09-11
Record modified2017-03-23
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