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

Abstract

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:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1237171
Report Number(s):
BNL-108296-2015-JA
Journal ID: ISSN 0021-9606; R&D Project: LS001
Grant/Contract Number:  
SC00112704
Resource Type:
Journal Article: 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)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

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., 2015. 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. https://doi.org/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. https://doi.org/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},
url = {https://www.osti.gov/biblio/1237171}, journal = {Journal of Chemical Physics},
issn = {0021-9606},
number = 24,
volume = 142,
place = {United States},
year = {Tue Jun 30 00:00:00 EDT 2015},
month = {Tue Jun 30 00:00:00 EDT 2015}
}

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Cited by: 22 works
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Works referenced in this record:

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journal, August 2004


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Works referencing / citing this record:

Approximating Matsubara dynamics using the planetary model: Tests on liquid water and ice
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Mean-field Matsubara dynamics: Analysis of path-integral curvature effects in rovibrational spectra
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Recent advances in Wigner function approaches
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Computation of static quantum triplet structure factors of liquid para -hydrogen
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Density and time scaling effects on the velocity autocorrelation function of quantum and classical dense fluid para -hydrogen
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Multi-time formulation of Matsubara dynamics
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Dynamical Origin of the Total and Zero-Point Kinetic Energy in a Quantum Fluid
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Approximating Matsubara dynamics using the planetary model: Tests on liquid water and ice.
text, January 2018


Mean-field Matsubara dynamics: analysis of path-integral curvature effects in rovibrational spectra
text, January 2018