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Title: Refinement of the experimental dynamic structure factor for liquid para-hydrogen and ortho-deuterium using semi-classical quantum simulation

Abstract

The dynamic structure factor of liquid para-hydrogen and ortho-deuterium in corresponding thermodynamic states (T = 20.0 K, n = 21.24 nm{sup −3}) and (T = 23.0 K, n = 24.61 nm{sup −3}), respectively, has been computed by both the Feynman-Kleinert linearized path-integral (FK-LPI) and Ring-Polymer Molecular Dynamics (RPMD) methods and compared with Inelastic X Ray Scattering spectra. The combined use of computational and experimental methods enabled us to reduce experimental uncertainties in the determination of the true sample spectrum. Furthermore, the refined experimental spectrum of para-hydrogen and ortho-deuterium is consistently reproduced by both FK-LPI and RPMD results at momentum transfers lower than 12.8 nm{sup −1}. At larger momentum transfers the FK-LPI results agree with experiment much better for ortho-deuterium than for para-hydrogen. More specifically we found that for k ∼ 20.0 nm{sup −1} para-hydrogen provides a test case for improved approximations to quantum dynamics.

Authors:
;  [1];  [2];  [3]
  1. Institute for Computational Engineering and Sciences and Department of Chemistry, University of Texas at Austin, Austin, Texas 78712 (United States)
  2. Department of Physical Chemistry, Goteborg University, S-412-96 Goteborg (Sweden)
  3. Photon Sciences Directorate, Brookhaven National Laboratory, P.O. Box 5000, Upton, New York 11973 (United States)
Publication Date:
OSTI Identifier:
22255283
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 140; Journal Issue: 3; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; DEUTERIUM; HYDROGEN; LIQUIDS; MOLECULAR DYNAMICS METHOD; POLYMERS; SIMULATION; SPECTRA; STRUCTURE FACTORS; X-RAY DIFFRACTION

Citation Formats

Smith, Kyle K. G., E-mail: kylesmith@utexas.edu, Rossky, Peter J., E-mail: peter.rossky@austin.utexas.edu, Poulsen, Jens Aage, E-mail: jens72@chem.gu.se, and Cunsolo, A., E-mail: acunsolo@bnl.gov. Refinement of the experimental dynamic structure factor for liquid para-hydrogen and ortho-deuterium using semi-classical quantum simulation. United States: N. p., 2014. Web. doi:10.1063/1.4851997.
Smith, Kyle K. G., E-mail: kylesmith@utexas.edu, Rossky, Peter J., E-mail: peter.rossky@austin.utexas.edu, Poulsen, Jens Aage, E-mail: jens72@chem.gu.se, & Cunsolo, A., E-mail: acunsolo@bnl.gov. Refinement of the experimental dynamic structure factor for liquid para-hydrogen and ortho-deuterium using semi-classical quantum simulation. United States. doi:10.1063/1.4851997.
Smith, Kyle K. G., E-mail: kylesmith@utexas.edu, Rossky, Peter J., E-mail: peter.rossky@austin.utexas.edu, Poulsen, Jens Aage, E-mail: jens72@chem.gu.se, and Cunsolo, A., E-mail: acunsolo@bnl.gov. Tue . "Refinement of the experimental dynamic structure factor for liquid para-hydrogen and ortho-deuterium using semi-classical quantum simulation". United States. doi:10.1063/1.4851997.
@article{osti_22255283,
title = {Refinement of the experimental dynamic structure factor for liquid para-hydrogen and ortho-deuterium using semi-classical quantum simulation},
author = {Smith, Kyle K. G., E-mail: kylesmith@utexas.edu and Rossky, Peter J., E-mail: peter.rossky@austin.utexas.edu and Poulsen, Jens Aage, E-mail: jens72@chem.gu.se and Cunsolo, A., E-mail: acunsolo@bnl.gov},
abstractNote = {The dynamic structure factor of liquid para-hydrogen and ortho-deuterium in corresponding thermodynamic states (T = 20.0 K, n = 21.24 nm{sup −3}) and (T = 23.0 K, n = 24.61 nm{sup −3}), respectively, has been computed by both the Feynman-Kleinert linearized path-integral (FK-LPI) and Ring-Polymer Molecular Dynamics (RPMD) methods and compared with Inelastic X Ray Scattering spectra. The combined use of computational and experimental methods enabled us to reduce experimental uncertainties in the determination of the true sample spectrum. Furthermore, the refined experimental spectrum of para-hydrogen and ortho-deuterium is consistently reproduced by both FK-LPI and RPMD results at momentum transfers lower than 12.8 nm{sup −1}. At larger momentum transfers the FK-LPI results agree with experiment much better for ortho-deuterium than for para-hydrogen. More specifically we found that for k ∼ 20.0 nm{sup −1} para-hydrogen provides a test case for improved approximations to quantum dynamics.},
doi = {10.1063/1.4851997},
journal = {Journal of Chemical Physics},
number = 3,
volume = 140,
place = {United States},
year = {Tue Jan 21 00:00:00 EST 2014},
month = {Tue Jan 21 00:00:00 EST 2014}
}