A path-integral Langevin equation treatment of low-temperature doped helium clusters.
We present an implementation of path integral molecular dynamics for sampling low temperature properties of doped helium clusters using Langevin dynamics. The robustness of the path integral Langevin equation and white-noise Langevin equation [M. Ceriotti, M. Parrinello, T. E. Markland, and D. E. Manolopoulos, J. Chem. Phys. 133, 124104 (2010)] sampling methods are considered for those weakly bound systems with comparison to path integral Monte Carlo (PIMC) in terms of efficiency and accuracy. Using these techniques, convergence studies are performed to confirm the systematic error reduction introduced by increasing the number of discretization steps of the path integral. We comment on the structural and energetic evolution of He(N)-CO(2) clusters from N = 1 to 20. To quantify the importance of both rotations and exchange in our simulations, we present a chemical potential and calculated band origin shifts as a function of cluster size utilizing PIMC sampling that includes these effects. This work also serves to showcase the implementation of path integral simulation techniques within the molecular modelling toolkit [K. Hinsen, J. Comp. Chem. 21, 79 (2000)], an open-source molecular simulation package.
Department of Chemistry, University of Waterloo, Waterloo, Canada, Ontario N2L 3G1.
Christopher
C
Ing
Konrad
K
Hinsen
Jing
J
Yang
Toby
T
Zeng
Hui
H
Li
Pierre-Nicholas
PN
Roy
D002245:Carbon Dioxide / Q000737:chemistry*; D003080:Cold Temperature; D006371:Helium / Q000737:chemistry*; D056004:Molecular Dynamics Simulation
D002245:Carbon Dioxide; D006371:Helium