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Title: V-T theory for the Self-Intermediate Scattering Function in a Monatomic Liquid

In V-T theory the atomic motion is harmonic vibrations in a liquid-specific potential energy valley, plus transits, which move the system rapidly among the multitude of such valleys. Here, in its first application to the self intermediate scattering function (SISF), V-T theory produced an accurate account of molecular dynamics (MD) data at all wave numbers q and time t. Recently, analysis of the mean square displacement (MSD) resolved a crossover behavior that was not observed in the SISF study. Our purpose here is to apply the more accurate MSD calibration to the SISF, and assess the results. We derive and discuss the theoretical equations for vibrational and transit contributions to the SISF. The time evolution is divided into three successive intervals: the vibrational interval when the vibrational contribution alone accurately accounts for the MD data; the crossover when the vibrational contribution saturates and the transit contribution becomes resolved; and the diffusive interval when the transit contribution alone accurately accounts for the MD data. Finally, the resulting theoretical error is extremely small at all q and t. V-T theory is compared to mode-coupling theories for the MSD and SISF, and to recent developments in Brownian motion experiments and theory.
Authors:
 [1] ;  [1] ;  [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Report Number(s):
LA-UR-16-26145
Journal ID: ISSN 0953-8984; TRN: US1800654
Grant/Contract Number:
AC52-06NA25396
Type:
Accepted Manuscript
Journal Name:
Journal of Physics. Condensed Matter
Additional Journal Information:
Journal Volume: 29; Journal Issue: 5; Journal ID: ISSN 0953-8984
Publisher:
IOP Publishing
Research Org:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Liquid Theory; Liquid Dynamics; Time Correlation Functions; Liquid Structure; Diffusion, Atomic Motion
OSTI Identifier:
1414129
Alternate Identifier(s):
OSTI ID: 1335200

Wallace, Duane C., Chisolm, Eric D., and De Lorenzi-Venneri, Giulia. V-T theory for the Self-Intermediate Scattering Function in a Monatomic Liquid. United States: N. p., Web. doi:10.1088/1361-648X/29/5/055101.
Wallace, Duane C., Chisolm, Eric D., & De Lorenzi-Venneri, Giulia. V-T theory for the Self-Intermediate Scattering Function in a Monatomic Liquid. United States. doi:10.1088/1361-648X/29/5/055101.
Wallace, Duane C., Chisolm, Eric D., and De Lorenzi-Venneri, Giulia. 2016. "V-T theory for the Self-Intermediate Scattering Function in a Monatomic Liquid". United States. doi:10.1088/1361-648X/29/5/055101. https://www.osti.gov/servlets/purl/1414129.
@article{osti_1414129,
title = {V-T theory for the Self-Intermediate Scattering Function in a Monatomic Liquid},
author = {Wallace, Duane C. and Chisolm, Eric D. and De Lorenzi-Venneri, Giulia},
abstractNote = {In V-T theory the atomic motion is harmonic vibrations in a liquid-specific potential energy valley, plus transits, which move the system rapidly among the multitude of such valleys. Here, in its first application to the self intermediate scattering function (SISF), V-T theory produced an accurate account of molecular dynamics (MD) data at all wave numbers q and time t. Recently, analysis of the mean square displacement (MSD) resolved a crossover behavior that was not observed in the SISF study. Our purpose here is to apply the more accurate MSD calibration to the SISF, and assess the results. We derive and discuss the theoretical equations for vibrational and transit contributions to the SISF. The time evolution is divided into three successive intervals: the vibrational interval when the vibrational contribution alone accurately accounts for the MD data; the crossover when the vibrational contribution saturates and the transit contribution becomes resolved; and the diffusive interval when the transit contribution alone accurately accounts for the MD data. Finally, the resulting theoretical error is extremely small at all q and t. V-T theory is compared to mode-coupling theories for the MSD and SISF, and to recent developments in Brownian motion experiments and theory.},
doi = {10.1088/1361-648X/29/5/055101},
journal = {Journal of Physics. Condensed Matter},
number = 5,
volume = 29,
place = {United States},
year = {2016},
month = {12}
}