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Title: Application of a New Ensemble Conserving Quantum Dynamics Simulation Algorithm to Liquid para-Hydrogen and ortho-Deuterium

Here, we apply the Feynman-Kleinert Quasi-Classical Wigner (FK-QCW) method developed in our previous work [Smith et al., J. Chem. Phys. 142, 244112 (2015)] for the determination of the dynamic structure factor of liquid para-hydrogen and ortho-deuterium at state points of (T = 20.0 K, n = 21.24 nm -3) and (T = 23.0 K, n = 24.61 nm -3), respectively. When applied to this challenging system, it is shown that this new FK-QCW method consistently reproduces the experimental dynamic structure factor reported by Smith et al. [J. Chem. Phys. 140, 034501 (2014)] for all momentum transfers considered. Moreover, this shows that FK-QCW provides a substantial improvement over the Feynman-Kleinert linearized path-integral method, in which purely classical dynamics are used. Furthermore, for small momentum transfers, it is shown that FK-QCW provides nearly the same results as ring-polymer molecular dynamics (RPMD), thus suggesting that FK-QCW provides a potentially more appealing algorithm than RPMD since it is not formally limited to correlation functions involving linear operators.
Authors:
 [1] ;  [2] ;  [2] ;  [3] ;  [4]
  1. Univ. of Texas, Austin, TX (United States)
  2. Univ. of Gothenburg (Sweden)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States)
  4. Rice Univ., Houston, TX (United States)
Publication Date:
Report Number(s):
BNL-108296-2015-JA
Journal ID: ISSN 0021-9606; R&D Project: LS001
Grant/Contract Number:
SC00112704
Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 142; Journal Issue: 24; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE
OSTI Identifier:
1237171

Smith, Kyle K.G., Poulsen, Jens Aage, Nyman, Gunnar, Cunsolo, Alessandro, and Rossky, Peter J.. Application of a New Ensemble Conserving Quantum Dynamics Simulation Algorithm to Liquid para-Hydrogen and ortho-Deuterium. United States: N. p., Web. doi:10.1063/1.4922888.
Smith, Kyle K.G., Poulsen, Jens Aage, Nyman, Gunnar, Cunsolo, Alessandro, & Rossky, Peter J.. Application of a New Ensemble Conserving Quantum Dynamics Simulation Algorithm to Liquid para-Hydrogen and ortho-Deuterium. United States. doi:10.1063/1.4922888.
Smith, Kyle K.G., Poulsen, Jens Aage, Nyman, Gunnar, Cunsolo, Alessandro, and Rossky, Peter J.. 2015. "Application of a New Ensemble Conserving Quantum Dynamics Simulation Algorithm to Liquid para-Hydrogen and ortho-Deuterium". United States. doi:10.1063/1.4922888. https://www.osti.gov/servlets/purl/1237171.
@article{osti_1237171,
title = {Application of a New Ensemble Conserving Quantum Dynamics Simulation Algorithm to Liquid para-Hydrogen and ortho-Deuterium},
author = {Smith, Kyle K.G. and Poulsen, Jens Aage and Nyman, Gunnar and Cunsolo, Alessandro and Rossky, Peter J.},
abstractNote = {Here, we apply the Feynman-Kleinert Quasi-Classical Wigner (FK-QCW) method developed in our previous work [Smith et al., J. Chem. Phys. 142, 244112 (2015)] for the determination of the dynamic structure factor of liquid para-hydrogen and ortho-deuterium at state points of (T = 20.0 K, n = 21.24 nm-3) and (T = 23.0 K, n = 24.61 nm-3), respectively. When applied to this challenging system, it is shown that this new FK-QCW method consistently reproduces the experimental dynamic structure factor reported by Smith et al. [J. Chem. Phys. 140, 034501 (2014)] for all momentum transfers considered. Moreover, this shows that FK-QCW provides a substantial improvement over the Feynman-Kleinert linearized path-integral method, in which purely classical dynamics are used. Furthermore, for small momentum transfers, it is shown that FK-QCW provides nearly the same results as ring-polymer molecular dynamics (RPMD), thus suggesting that FK-QCW provides a potentially more appealing algorithm than RPMD since it is not formally limited to correlation functions involving linear operators.},
doi = {10.1063/1.4922888},
journal = {Journal of Chemical Physics},
number = 24,
volume = 142,
place = {United States},
year = {2015},
month = {6}
}