Identifying Water-Anion Correlated Motion in Aqueous Solutions through Van Hove Functions

Yuya Shinohara; Ray Matsumoto; Matthew W. Thompson; Chae Woo Ryu; Wojciech Dmowski; Takuya Iwashita; Daisuke Ishikawa; Alfred Q.R. Baron; Peter T. Cummings; Takeshi Egami

doi:10.1021/acs.jpclett.9b02891

Identifying Water-Anion Correlated Motion in Aqueous Solutions through Van Hove Functions

Yuya Shinohara, Ray Matsumoto, Matthew W. Thompson, Chae Woo Ryu, Wojciech Dmowski, Takuya Iwashita, Daisuke Ishikawa, Alfred Q.R. Baron, Peter T. Cummings, Takeshi Egami

Neutron & X-Ray Scattering, & Thermophys

Research output: Contribution to journal › Article › peer-review

16 Scopus citations

Abstract

Electrolyte solutions are ubiquitous in materials in daily use and in biological systems. However, the understanding of their molecular and ionic dynamics, particularly those of their correlated motions, are elusive despite extensive experimental, theoretical, and numerical studies. Here we report the real-space observations of the molecular/ionic-correlated dynamics of aqueous salt (NaCl, NaBr, and NaI) solutions using the Van Hove functions obtained by high-resolution inelastic X-ray scattering measurement and molecular dynamics simulation. Our results directly depict the distance-dependent dynamics of aqueous salt solutions on the picosecond time scale and identify the changes in the anion-water correlations. This study demonstrates the capability of the real-space Van Hove function analysis to describe the local correlated dynamics in aqueous salt solutions.

Original language	English
Pages (from-to)	7119-7125
Number of pages	7
Journal	Journal of Physical Chemistry Letters
Volume	10
Issue number	22
DOIs	https://doi.org/10.1021/acs.jpclett.9b02891
State	Published - Nov 21 2019

Funding

Inelastic X-ray scattering work by Y.S. and T.E. was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials and Science and Engineering Division. High-energy X-ray diffraction work by C.W.R. and W.D. and MD simulation work by R.M., M.W.T., and P.T.C. were supported as part of the Fluid Interface Reactions, Structures and Transport (FIRST) Center, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences. IXS experiments at BL43LXU, SPring-8 were conducted under the approval of RIKEN (Proposal No. 20170075, 20180069, and 20190002). This research used resources of the Advanced Photon Source, a U.S. DOE Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH1135.

Funders	Funder number
Advanced Photon Source
DOE Office of Science User Facility operated
Energy Frontier Research Center
Office of Basic Energy Sciences
Office of Basic Energy Sciences, Materials and Science and Engineering Division
U.S. DOE Office of Science
U.S. Department of Energy
Foundation for Ichthyosis and Related Skin Types
Interface
Office of Science
Argonne National Laboratory

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10.1021/acs.jpclett.9b02891

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title = "Identifying Water-Anion Correlated Motion in Aqueous Solutions through Van Hove Functions",

abstract = "Electrolyte solutions are ubiquitous in materials in daily use and in biological systems. However, the understanding of their molecular and ionic dynamics, particularly those of their correlated motions, are elusive despite extensive experimental, theoretical, and numerical studies. Here we report the real-space observations of the molecular/ionic-correlated dynamics of aqueous salt (NaCl, NaBr, and NaI) solutions using the Van Hove functions obtained by high-resolution inelastic X-ray scattering measurement and molecular dynamics simulation. Our results directly depict the distance-dependent dynamics of aqueous salt solutions on the picosecond time scale and identify the changes in the anion-water correlations. This study demonstrates the capability of the real-space Van Hove function analysis to describe the local correlated dynamics in aqueous salt solutions.",

author = "Yuya Shinohara and Ray Matsumoto and Thompson, {Matthew W.} and Ryu, {Chae Woo} and Wojciech Dmowski and Takuya Iwashita and Daisuke Ishikawa and Baron, {Alfred Q.R.} and Cummings, {Peter T.} and Takeshi Egami",

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doi = "10.1021/acs.jpclett.9b02891",

language = "English",

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T1 - Identifying Water-Anion Correlated Motion in Aqueous Solutions through Van Hove Functions

AU - Shinohara, Yuya

AU - Matsumoto, Ray

AU - Thompson, Matthew W.

AU - Ryu, Chae Woo

AU - Dmowski, Wojciech

AU - Iwashita, Takuya

AU - Ishikawa, Daisuke

AU - Baron, Alfred Q.R.

AU - Cummings, Peter T.

AU - Egami, Takeshi

PY - 2019/11/21

Y1 - 2019/11/21

N2 - Electrolyte solutions are ubiquitous in materials in daily use and in biological systems. However, the understanding of their molecular and ionic dynamics, particularly those of their correlated motions, are elusive despite extensive experimental, theoretical, and numerical studies. Here we report the real-space observations of the molecular/ionic-correlated dynamics of aqueous salt (NaCl, NaBr, and NaI) solutions using the Van Hove functions obtained by high-resolution inelastic X-ray scattering measurement and molecular dynamics simulation. Our results directly depict the distance-dependent dynamics of aqueous salt solutions on the picosecond time scale and identify the changes in the anion-water correlations. This study demonstrates the capability of the real-space Van Hove function analysis to describe the local correlated dynamics in aqueous salt solutions.

AB - Electrolyte solutions are ubiquitous in materials in daily use and in biological systems. However, the understanding of their molecular and ionic dynamics, particularly those of their correlated motions, are elusive despite extensive experimental, theoretical, and numerical studies. Here we report the real-space observations of the molecular/ionic-correlated dynamics of aqueous salt (NaCl, NaBr, and NaI) solutions using the Van Hove functions obtained by high-resolution inelastic X-ray scattering measurement and molecular dynamics simulation. Our results directly depict the distance-dependent dynamics of aqueous salt solutions on the picosecond time scale and identify the changes in the anion-water correlations. This study demonstrates the capability of the real-space Van Hove function analysis to describe the local correlated dynamics in aqueous salt solutions.

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Identifying Water-Anion Correlated Motion in Aqueous Solutions through Van Hove Functions

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