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

Shinohara, Yuya; Ivanov, Alexander S.; Maltsev, Dmitry; Granroth, Garrett E.; Abernathy, Douglas L.; Dai, Sheng; Egami, Takeshi

doi:10.1021/acs.jpclett.2c01230

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

Journal Article · Thu Jun 23 00:00:00 EDT 2022 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.2c01230· OSTI ID:1875347

^[1]; ^[1]; Maltsev, Dmitry ^[1]; Granroth, Garrett E. ^[1]; Abernathy, Douglas L. ^[1]; ^[2]; ^[2]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)

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.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1875347

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 25 Vol. 13; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (48)

High-Resolution Inelastic X-Ray Scattering I: Context, Spectrometers, Samples, and Superconductors Baron, Alfred Q. R. Synchrotron Light Sources and Free-Electron Lasers https://doi.org/10.1007/978-3-319-14394-1_41	book	January 2016
Electrochemical studies of magnesium ions in magnesium chloride containing chloride melt at 710 ± 10°C Rao, Gopalakrishna M. Journal of Electroanalytical Chemistry and Interfacial Electrochemistry, Vol. 249, Issue 1-2 https://doi.org/10.1016/0022-0728(88)80359-0	journal	July 1988
Molten salts and nuclear energy production Le Brun, Christian Journal of Nuclear Materials, Vol. 360, Issue 1 https://doi.org/10.1016/j.jnucmat.2006.08.017	journal	January 2007
Mantid—Data analysis and visualization package for neutron scattering and μ SR experiments 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 https://doi.org/10.1016/j.nima.2014.07.029	journal	November 2014
Molten salt reactors: A new beginning for an old idea LeBlanc, David Nuclear Engineering and Design, Vol. 240, Issue 6 https://doi.org/10.1016/j.nucengdes.2009.12.033	journal	June 2010
The Spallation Neutron Source in Oak Ridge: A powerful tool for materials research Mason, T. E.; Abernathy, D.; Anderson, I. Physica B: Condensed Matter, Vol. 385-386 https://doi.org/10.1016/j.physb.2006.05.281	journal	November 2006
Anomaly of structural relaxation in complex liquid metal of bismuth - Dynamic correlation function of coherent quasi-elastic neutron scattering Kawakita, Yukinobu; Kikuchi, Tatsuya; Inamura, Yasuhiro Physica B: Condensed Matter, Vol. 551 https://doi.org/10.1016/j.physb.2017.12.037	journal	December 2018
Potential scalability of a cost-effective purification method for MgCl2-Containing salts for next-generation concentrating solar power technologies Zhao, Youyang; Vidal, Judith Solar Energy Materials and Solar Cells, Vol. 215 https://doi.org/10.1016/j.solmat.2020.110663	journal	September 2020
Development of robust neural-network interatomic potential for molten salt Li, Qing-Jie; Küçükbenli, Emine; Lam, Stephen Cell Reports Physical Science https://doi.org/10.1016/j.xcrp.2021.100359	journal	March 2021
Investigating the Accuracy of Water Models through the Van Hove Correlation Function Matsumoto, Ray A.; Thompson, Matthew W.; Vuong, Van Quan Journal of Chemical Theory and Computation, Vol. 17, Issue 10 https://doi.org/10.1021/acs.jctc.1c00637	journal	September 2021
Unraveling Local Structure of Molten Salts via X-ray Scattering, Raman Spectroscopy, and Ab Initio Molecular Dynamics Roy, Santanu; Brehm, Martin; Sharma, Shobha The Journal of Physical Chemistry B https://doi.org/10.1021/acs.jpcb.1c03786	journal	May 2021
Neutron Spin–Echo Studies of the Structural Relaxation of Network Liquid ZnCl ₂ at the Structure Factor Primary Peak and Prepeak Luo, Peng; Zhai, Yanqin; Leao, Juscelino B. The Journal of Physical Chemistry Letters, Vol. 12, Issue 1 https://doi.org/10.1021/acs.jpclett.0c03146	journal	December 2020
Automated Development of Molten Salt Machine Learning Potentials: Application to LiCl Sivaraman, Ganesh; Guo, Jicheng; Ward, Logan The Journal of Physical Chemistry Letters, Vol. 12, Issue 17 https://doi.org/10.1021/acs.jpclett.1c00901	journal	April 2021
Elucidating Ionic Correlations Beyond Simple Charge Alternation in Molten MgCl ₂ –KCl Mixtures Wu, Fei; Roy, Santanu; Ivanov, Alexander S. The Journal of Physical Chemistry Letters, Vol. 10, Issue 24 https://doi.org/10.1021/acs.jpclett.9b02845	journal	November 2019
Identifying Water–Anion Correlated Motion in Aqueous Solutions through Van Hove Functions Shinohara, Yuya; Matsumoto, Ray; Thompson, Matthew W. The Journal of Physical Chemistry Letters, Vol. 10, Issue 22 https://doi.org/10.1021/acs.jpclett.9b02891	journal	October 2019
Complex Structure of Molten NaCl–CrCl ₃ Salt: Cr–Cl Octahedral Network and Intermediate-Range Order Li, Qing-Jie; Sprouster, David; Zheng, Guiqiu ACS Applied Energy Materials, Vol. 4, Issue 4 https://doi.org/10.1021/acsaem.0c02678	journal	March 2021
Structure of Molten CaSiO ₃ : Neutron Diffraction Isotope Substitution with Aerodynamic Levitation and Molecular Dynamics Study Skinner, L. B.; Benmore, C. J.; Weber, J. K. R. The Journal of Physical Chemistry B, Vol. 116, Issue 45 https://doi.org/10.1021/jp3066019	journal	November 2012
Structure and dynamics of the molten alkali-chloride salts from an X-ray, simulation, and rate theory perspective Roy, Santanu; Wu, Fei; Wang, Haimeng Physical Chemistry Chemical Physics, Vol. 22, Issue 40 https://doi.org/10.1039/D0CP03672B	journal	January 2020
A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu Grimme, Stefan; Antony, Jens; Ehrlich, Stephan The Journal of Chemical Physics, Vol. 132, Issue 15 https://doi.org/10.1063/1.3382344	journal	April 2010
Design and operation of the wide angular-range chopper spectrometer ARCS at the Spallation Neutron Source Abernathy, D. L.; Stone, M. B.; Loguillo, M. J. Review of Scientific Instruments, Vol. 83, Issue 1 https://doi.org/10.1063/1.3680104	journal	January 2012
A comparison of four direct geometry time-of-flight spectrometers at the Spallation Neutron Source Stone, M. B.; Niedziela, J. L.; Abernathy, D. L. Review of Scientific Instruments, Vol. 85, Issue 4 https://doi.org/10.1063/1.4870050	journal	April 2014
Design and operating characteristic of a vacuum furnace for time-of-flight inelastic neutron scattering measurements Niedziela, J. L.; Mills, R.; Loguillo, M. J. Review of Scientific Instruments, Vol. 88, Issue 10 https://doi.org/10.1063/1.5007089	journal	October 2017
Experimental determination of the temperature-dependent Van Hove function in a Zr ₈₀ Pt ₂₀ liquid Ashcraft, R.; Wang, Z.; Abernathy, D. L. The Journal of Chemical Physics, Vol. 152, Issue 7 https://doi.org/10.1063/1.5144256	journal	February 2020
Molten salts: Volume 4, part 2, chlorides and mixtures—electrical conductance, density, viscosity, and surface tension data Janz, G. J.; Tomkins, R. P. T.; Allen, C. B. Journal of Physical and Chemical Reference Data, Vol. 4, Issue 4 https://doi.org/10.1063/1.555527	journal	October 1975
Viscosity of liquid water in the range −8 °C to 150 °C Kestin, Joseph; Sokolov, Mordechai; Wakeham, William A. Journal of Physical and Chemical Reference Data, Vol. 7, Issue 3 https://doi.org/10.1063/1.555581	journal	July 1978
Molten Salts Data: Diffusion Coefficients in Single and Multi‐Component Salt Systems Janz, G. J.; Bansal, N. P. Journal of Physical and Chemical Reference Data, Vol. 11, Issue 3 https://doi.org/10.1063/1.555665	journal	July 1982
Neutron scattering lengths and cross sections Sears, Varley F. Neutron News, Vol. 3, Issue 3 https://doi.org/10.1080/10448639208218770	journal	January 1992
Comments on the structure of molten salts Biggin, S.; Enderby, J. E. Journal of Physics C: Solid State Physics, Vol. 15, Issue 11 https://doi.org/10.1088/0022-3719/15/11/001	journal	April 1982
The structures of molten magnesium and manganese (II) chlorides Biggin, S.; Gay, M.; Enderby, J. E. Journal of Physics C: Solid State Physics, Vol. 17, Issue 6 https://doi.org/10.1088/0022-3719/17/6/006	journal	February 1984
Collective modes in molten alkaline earth chlorides: III. Inelastic neutron scattering from molten MgCl ₂ and CaCl ₂ McGreevy, R. L.; Mitchell, E. W. J. Journal of Physics C: Solid State Physics, Vol. 18, Issue 6 https://doi.org/10.1088/0022-3719/18/6/011	journal	February 1985
The structure of molten sodium chloride Edwards, F. G.; Enderby, J. E.; Howe, R. A. Journal of Physics C: Solid State Physics, Vol. 8, Issue 21 https://doi.org/10.1088/0022-3719/8/21/018	journal	November 1975
Structure and dynamics of molten salts Revere, M.; Tosi, M. P. Reports on Progress in Physics, Vol. 49, Issue 9 https://doi.org/10.1088/0034-4885/49/9/002	journal	September 1986
Van Hove correlation functions from coherent neutron inelastic scattering Dahlborg, U.; Gudowski, W.; Davidovic, M. Journal of Physics: Condensed Matter, Vol. 1, Issue 35 https://doi.org/10.1088/0953-8984/1/35/016	journal	September 1989
Short- and intermediate-range order in MCl ₂ melts: the importance of anionic polarization Wilson, M.; Madden, P. A. Journal of Physics: Condensed Matter, Vol. 5, Issue 37 https://doi.org/10.1088/0953-8984/5/37/004	journal	September 1993
Scattering of Slow Neutrons by a Liquid Vineyard, George H. Physical Review, Vol. 110, Issue 5 https://doi.org/10.1103/PhysRev.110.999	journal	June 1958
Correlations in Space and Time and Born Approximation Scattering in Systems of Interacting Particles Van Hove, Léon Physical Review, Vol. 95, Issue 1 https://doi.org/10.1103/PhysRev.95.249	journal	July 1954
Coherent- and Incoherent-Scattering Laws of Liquid Argon Sköld, K.; Rowe, J. M.; Ostrowski, G. Physical Review A, Vol. 6, Issue 3 https://doi.org/10.1103/PhysRevA.6.1107	journal	September 1972
Local self-motion of water through the Van Hove function Shinohara, Yuya; Dmowski, Wojciech; Iwashita, Takuya Physical Review E, Vol. 102, Issue 3 https://doi.org/10.1103/PhysRevE.102.032604	journal	September 2020
Viscosity and real-space molecular motion of water: Observation with inelastic x-ray scattering Shinohara, Yuya; Dmowski, Wojciech; Iwashita, Takuya Physical Review E, Vol. 98, Issue 2 https://doi.org/10.1103/PhysRevE.98.022604	journal	August 2018
Elementary Excitations and Crossover Phenomenon in Liquids Iwashita, T.; Nicholson, D. M.; Egami, T. Physical Review Letters, Vol. 110, Issue 20 https://doi.org/10.1103/PhysRevLett.110.205504	journal	May 2013
Atomic Dynamics in Simple Liquid: de Gennes Narrowing Revisited Wu, Bin; Iwashita, Takuya; Egami, Takeshi Physical Review Letters, Vol. 120, Issue 13 https://doi.org/10.1103/PhysRevLett.120.135502	journal	March 2018
Time-Dependent Pair Correlations in Liquid Lead Brockhouse, B. N.; Pope, N. K. Physical Review Letters, Vol. 3, Issue 6 https://doi.org/10.1103/PhysRevLett.3.259	journal	September 1959
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Local correlated motions in aqueous solution of sodium chloride Shinohara, Yuya; Dmowski, Wojciech; Iwashita, Takuya Physical Review Materials, Vol. 3, Issue 6 https://doi.org/10.1103/PhysRevMaterials.3.065604	journal	June 2019
Experimental Test of Properties of KCl–MgCl2 Eutectic Molten Salt for Heat Transfer and Thermal Storage Fluid in Concentrated Solar Power Systems Xu, Xiankun; Wang, Xiaoxin; Li, Peiwen Journal of Solar Energy Engineering, Vol. 140, Issue 5 https://doi.org/10.1115/1.4040065	journal	May 2018
Seeing real-space dynamics of liquid water through inelastic x-ray scattering Iwashita, Takuya; Wu, Bin; Chen, Wei-Ren Science Advances, Vol. 3, Issue 12 https://doi.org/10.1126/sciadv.1603079	journal	December 2017
The Molten Salt Reactor Adventure MacPherson, H. G. Nuclear Science and Engineering, Vol. 90, Issue 4 https://doi.org/10.13182/NSE90-374	journal	August 1985
Electrochemistry of MgCl₂ in LiCl-KCl Eutectic Melts Hao, Tang; Yong-De, Yan; Mi-Lin, Zhang Acta Physico-Chimica Sinica, Vol. 29, Issue 08 https://doi.org/10.3866/PKU.WHXB201305102	journal	January 2013

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