DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Real-Space Local Dynamics of Molten Inorganic Salts Using Van Hove Correlation Function

Abstract

Molten inorganic salts are attracting resurgent attention because of their unique physicochemical properties, making them promising media for next-generation concentrating solar power systems and molten salt reactors. The dynamics of these highly disordered ionic media is largely studied by theoretical simulations, while the robust experimental techniques capable of observing local dynamics are not well-developed. To provide fundamental insights into the atomic-scale transport properties of molten salts, we report the real-space dynamics of molten magnesium chloride at high temperatures employing the Van Hove correlation function obtained by inelastic neutron scattering. Overall, our results directly depict the distance-dependent dynamics of a molten salt on the picosecond time scale. This study demonstrates the capability of the developed approach to describe the locally correlated- and self-dynamics in molten salts, significantly improving our understanding of the interplay between microscopic structural parameters and their dynamics that ultimately control physical properties of condensed matter in extreme environments.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [1];  [1];  [1]; ORCiD logo [2]; ORCiD logo [2]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1875347
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 13; Journal Issue: 25; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; energy; ions; neutron scattering; salts; scattering

Citation Formats

Shinohara, Yuya, Ivanov, Alexander S., Maltsev, Dmitry, Granroth, Garrett E., Abernathy, Douglas L., Dai, Sheng, and Egami, Takeshi. Real-Space Local Dynamics of Molten Inorganic Salts Using Van Hove Correlation Function. United States: N. p., 2022. Web. doi:10.1021/acs.jpclett.2c01230.
Shinohara, Yuya, Ivanov, Alexander S., Maltsev, Dmitry, Granroth, Garrett E., Abernathy, Douglas L., Dai, Sheng, & Egami, Takeshi. Real-Space Local Dynamics of Molten Inorganic Salts Using Van Hove Correlation Function. United States. https://doi.org/10.1021/acs.jpclett.2c01230
Shinohara, Yuya, Ivanov, Alexander S., Maltsev, Dmitry, Granroth, Garrett E., Abernathy, Douglas L., Dai, Sheng, and Egami, Takeshi. Thu . "Real-Space Local Dynamics of Molten Inorganic Salts Using Van Hove Correlation Function". United States. https://doi.org/10.1021/acs.jpclett.2c01230. https://www.osti.gov/servlets/purl/1875347.
@article{osti_1875347,
title = {Real-Space Local Dynamics of Molten Inorganic Salts Using Van Hove Correlation Function},
author = {Shinohara, Yuya and Ivanov, Alexander S. and Maltsev, Dmitry and Granroth, Garrett E. and Abernathy, Douglas L. and Dai, Sheng and Egami, Takeshi},
abstractNote = {Molten inorganic salts are attracting resurgent attention because of their unique physicochemical properties, making them promising media for next-generation concentrating solar power systems and molten salt reactors. The dynamics of these highly disordered ionic media is largely studied by theoretical simulations, while the robust experimental techniques capable of observing local dynamics are not well-developed. To provide fundamental insights into the atomic-scale transport properties of molten salts, we report the real-space dynamics of molten magnesium chloride at high temperatures employing the Van Hove correlation function obtained by inelastic neutron scattering. Overall, our results directly depict the distance-dependent dynamics of a molten salt on the picosecond time scale. This study demonstrates the capability of the developed approach to describe the locally correlated- and self-dynamics in molten salts, significantly improving our understanding of the interplay between microscopic structural parameters and their dynamics that ultimately control physical properties of condensed matter in extreme environments.},
doi = {10.1021/acs.jpclett.2c01230},
journal = {Journal of Physical Chemistry Letters},
number = 25,
volume = 13,
place = {United States},
year = {Thu Jun 23 00:00:00 EDT 2022},
month = {Thu Jun 23 00:00:00 EDT 2022}
}

Works referenced in this record:

Generalized Gradient Approximation Made Simple
journal, October 1996

  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865

Experimental Test of Properties of KCl–MgCl2 Eutectic Molten Salt for Heat Transfer and Thermal Storage Fluid in Concentrated Solar Power Systems
journal, May 2018

  • Xu, Xiankun; Wang, Xiaoxin; Li, Peiwen
  • Journal of Solar Energy Engineering, Vol. 140, Issue 5
  • DOI: 10.1115/1.4040065

Mantid—Data analysis and visualization package for neutron scattering and μ SR experiments
journal, November 2014

  • Arnold, O.; Bilheux, J. C.; Borreguero, J. M.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 764
  • DOI: 10.1016/j.nima.2014.07.029

The Spallation Neutron Source in Oak Ridge: A powerful tool for materials research
journal, November 2006


Atomic Dynamics in Simple Liquid: de Gennes Narrowing Revisited
journal, March 2018


Neutron Spin–Echo Studies of the Structural Relaxation of Network Liquid ZnCl 2 at the Structure Factor Primary Peak and Prepeak
journal, December 2020

  • Luo, Peng; Zhai, Yanqin; Leao, Juscelino B.
  • The Journal of Physical Chemistry Letters, Vol. 12, Issue 1
  • DOI: 10.1021/acs.jpclett.0c03146

A comparison of four direct geometry time-of-flight spectrometers at the Spallation Neutron Source
journal, April 2014

  • Stone, M. B.; Niedziela, J. L.; Abernathy, D. L.
  • Review of Scientific Instruments, Vol. 85, Issue 4
  • DOI: 10.1063/1.4870050

Van Hove correlation functions from coherent neutron inelastic scattering
journal, September 1989

  • Dahlborg, U.; Gudowski, W.; Davidovic, M.
  • Journal of Physics: Condensed Matter, Vol. 1, Issue 35
  • DOI: 10.1088/0953-8984/1/35/016

Short- and intermediate-range order in MCl 2 melts: the importance of anionic polarization
journal, September 1993


Time-Dependent Pair Correlations in Liquid Lead
journal, September 1959


Electrochemical studies of magnesium ions in magnesium chloride containing chloride melt at 710 ± 10°C
journal, July 1988

  • Rao, Gopalakrishna M.
  • Journal of Electroanalytical Chemistry and Interfacial Electrochemistry, Vol. 249, Issue 1-2
  • DOI: 10.1016/0022-0728(88)80359-0

Elucidating Ionic Correlations Beyond Simple Charge Alternation in Molten MgCl 2 –KCl Mixtures
journal, November 2019

  • Wu, Fei; Roy, Santanu; Ivanov, Alexander S.
  • The Journal of Physical Chemistry Letters, Vol. 10, Issue 24
  • DOI: 10.1021/acs.jpclett.9b02845

Development of robust neural-network interatomic potential for molten salt
journal, March 2021


Anomaly of structural relaxation in complex liquid metal of bismuth - Dynamic correlation function of coherent quasi-elastic neutron scattering
journal, December 2018


Collective modes in molten alkaline earth chlorides: III. Inelastic neutron scattering from molten MgCl 2 and CaCl 2
journal, February 1985


Design and operation of the wide angular-range chopper spectrometer ARCS at the Spallation Neutron Source
journal, January 2012

  • Abernathy, D. L.; Stone, M. B.; Loguillo, M. J.
  • Review of Scientific Instruments, Vol. 83, Issue 1
  • DOI: 10.1063/1.3680104

Molten salts and nuclear energy production
journal, January 2007


Complex Structure of Molten NaCl–CrCl 3 Salt: Cr–Cl Octahedral Network and Intermediate-Range Order
journal, March 2021

  • Li, Qing-Jie; Sprouster, David; Zheng, Guiqiu
  • ACS Applied Energy Materials, Vol. 4, Issue 4
  • DOI: 10.1021/acsaem.0c02678

Coherent- and Incoherent-Scattering Laws of Liquid Argon
journal, September 1972


Structure and dynamics of the molten alkali-chloride salts from an X-ray, simulation, and rate theory perspective
journal, January 2020

  • Roy, Santanu; Wu, Fei; Wang, Haimeng
  • Physical Chemistry Chemical Physics, Vol. 22, Issue 40
  • DOI: 10.1039/D0CP03672B

Investigating the Accuracy of Water Models through the Van Hove Correlation Function
journal, September 2021

  • Matsumoto, Ray A.; Thompson, Matthew W.; Vuong, Van Quan
  • Journal of Chemical Theory and Computation, Vol. 17, Issue 10
  • DOI: 10.1021/acs.jctc.1c00637

Viscosity of liquid water in the range −8 °C to 150 °C
journal, July 1978

  • Kestin, Joseph; Sokolov, Mordechai; Wakeham, William A.
  • Journal of Physical and Chemical Reference Data, Vol. 7, Issue 3
  • DOI: 10.1063/1.555581

The structure of molten sodium chloride
journal, November 1975

  • Edwards, F. G.; Enderby, J. E.; Howe, R. A.
  • Journal of Physics C: Solid State Physics, Vol. 8, Issue 21
  • DOI: 10.1088/0022-3719/8/21/018

Neutron scattering lengths and cross sections
journal, January 1992


The structures of molten magnesium and manganese (II) chlorides
journal, February 1984


Structure and dynamics of molten salts
journal, September 1986


Design and operating characteristic of a vacuum furnace for time-of-flight inelastic neutron scattering measurements
journal, October 2017

  • Niedziela, J. L.; Mills, R.; Loguillo, M. J.
  • Review of Scientific Instruments, Vol. 88, Issue 10
  • DOI: 10.1063/1.5007089

Scattering of Slow Neutrons by a Liquid
journal, June 1958


Molten Salts Data: Diffusion Coefficients in Single and Multi‐Component Salt Systems
journal, July 1982

  • Janz, G. J.; Bansal, N. P.
  • Journal of Physical and Chemical Reference Data, Vol. 11, Issue 3
  • DOI: 10.1063/1.555665

Local self-motion of water through the Van Hove function
journal, September 2020


Experimental determination of the temperature-dependent Van Hove function in a Zr 80 Pt 20 liquid
journal, February 2020

  • Ashcraft, R.; Wang, Z.; Abernathy, D. L.
  • The Journal of Chemical Physics, Vol. 152, Issue 7
  • DOI: 10.1063/1.5144256

Electrochemistry of MgCl2 in LiCl-KCl Eutectic Melts
journal, January 2013


Structure of Molten CaSiO 3 : Neutron Diffraction Isotope Substitution with Aerodynamic Levitation and Molecular Dynamics Study
journal, November 2012

  • Skinner, L. B.; Benmore, C. J.; Weber, J. K. R.
  • The Journal of Physical Chemistry B, Vol. 116, Issue 45
  • DOI: 10.1021/jp3066019

Seeing real-space dynamics of liquid water through inelastic x-ray scattering
journal, December 2017


Molten salt reactors: A new beginning for an old idea
journal, June 2010


Identifying Water–Anion Correlated Motion in Aqueous Solutions through Van Hove Functions
journal, October 2019

  • Shinohara, Yuya; Matsumoto, Ray; Thompson, Matthew W.
  • The Journal of Physical Chemistry Letters, Vol. 10, Issue 22
  • DOI: 10.1021/acs.jpclett.9b02891

Comments on the structure of molten salts
journal, April 1982


A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu
journal, April 2010

  • Grimme, Stefan; Antony, Jens; Ehrlich, Stephan
  • The Journal of Chemical Physics, Vol. 132, Issue 15
  • DOI: 10.1063/1.3382344

Automated Development of Molten Salt Machine Learning Potentials: Application to LiCl
journal, April 2021

  • Sivaraman, Ganesh; Guo, Jicheng; Ward, Logan
  • The Journal of Physical Chemistry Letters, Vol. 12, Issue 17
  • DOI: 10.1021/acs.jpclett.1c00901

The Molten Salt Reactor Adventure
journal, August 1985

  • MacPherson, H. G.
  • Nuclear Science and Engineering, Vol. 90, Issue 4
  • DOI: 10.13182/NSE90-374

Molten salts: Volume 4, part 2, chlorides and mixtures—electrical conductance, density, viscosity, and surface tension data
journal, October 1975

  • Janz, G. J.; Tomkins, R. P. T.; Allen, C. B.
  • Journal of Physical and Chemical Reference Data, Vol. 4, Issue 4
  • DOI: 10.1063/1.555527

Unraveling Local Structure of Molten Salts via X-ray Scattering, Raman Spectroscopy, and Ab Initio Molecular Dynamics
journal, May 2021


Local correlated motions in aqueous solution of sodium chloride
journal, June 2019