Quantum Solvation of CO_2 by he Atoms: from Onset to Nanodroplet

Details Quantum Solvation of CO_2 by he Atoms: from Onset to Nanodroplet Quantum Solvation of CO_2 by he Atoms: from Onset to Nanodroplet

Jun 2009

adsabs.harvard.edu/cgi-bin/nph-data_query?bibcode=2009mss..confefb01l&link_type=abstract

"International Symposium On Molecular Spectroscopy, 64th Meeting, Held 22-26 June, 2009 at Ohio State University. http://molspec

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Spectroscopic studies of molecules embedded in helium droplets provide a unique opportunity to investigate a superfluid. High-resolution infrared spectra of CO_2-(He)_N clusters ranging in size from `small' (N≃q 1-17) to `intermediate' (N˜ 60) have been reported recently by McKellar and co-workers. However, they have not yet been able to extend this range to clusters large enough that the observed vibrational band origins shifts Δν_3 and rotational constants B_0 and D_0 approached the nanodroplet limit values. This paper describes the use of modeling techniques to explore the domain between intermediate and `larger' (N˜10^2-10^3) clusters, seeking to characterize the onset of nanodroplet behaviour. Path integral Monte Carlo (PIMC) simulations using the worm algorithm can in principle provide reliable quantitative results for ``larger'' clusters approaching the nanodroplet limit. We have recently determined a three-dimensional analytical `Morse/Long-Range' potential energy surface for CO_2-He, which explicitly depends on the Q_3 asymmetric-stretch vibrational motion of CO_2, and takes account of change in the average value of Q_1 when ν_3 is excited. Using this potential, predicted vibrational frequency shifts have been found to be in excellent agreement with experiment across the range N=1-40,^d so it is expected to provides a good description of larger clusters. This paper describes results obtained on using this potential in PIMC simulations to predict the effective rotational constant B_0 and the Δν_3 band-origin shift for CO_2 in (He)_N clusters with N > 10^2. The importance of identical-particle exchange effects will be examined by comparing results obtained using both Boltzmann and Bose-Einstein statistics.
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