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Pressure and Temperature Dependence of Local Structure and Dynamics in an Ionic Liquid

[Image: see text] A detailed understanding of the local dynamics in ionic liquids remains an important aspect in the design of new ionic liquids as advanced functional fluids. Here, we use small-angle X-ray scattering and quasi-elastic neutron spectroscopy to investigate the local structure and dyna...

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Autores principales: Lundin, Filippa, Hansen, Henriette Wase, Adrjanowicz, Karolina, Frick, Bernhard, Rauber, Daniel, Hempelmann, Rolf, Shebanova, Olga, Niss, Kristine, Matic, Aleksandar
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2021
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8034775/
https://www.ncbi.nlm.nih.gov/pubmed/33656344
http://dx.doi.org/10.1021/acs.jpcb.1c00147
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author Lundin, Filippa
Hansen, Henriette Wase
Adrjanowicz, Karolina
Frick, Bernhard
Rauber, Daniel
Hempelmann, Rolf
Shebanova, Olga
Niss, Kristine
Matic, Aleksandar
author_facet Lundin, Filippa
Hansen, Henriette Wase
Adrjanowicz, Karolina
Frick, Bernhard
Rauber, Daniel
Hempelmann, Rolf
Shebanova, Olga
Niss, Kristine
Matic, Aleksandar
author_sort Lundin, Filippa
collection PubMed
description [Image: see text] A detailed understanding of the local dynamics in ionic liquids remains an important aspect in the design of new ionic liquids as advanced functional fluids. Here, we use small-angle X-ray scattering and quasi-elastic neutron spectroscopy to investigate the local structure and dynamics in a model ionic liquid as a function of temperature and pressure, with a particular focus on state points (P,T) where the macroscopic dynamics, i.e., conductivity, is the same. Our results suggest that the initial step of ion transport is a confined diffusion process, on the nanosecond timescale, where the motion is restricted by a cage of nearest neighbors. This process is invariant considering timescale, geometry, and the participation ratio, at state points of constant conductivity, i.e., state points of isoconductivity. The connection to the nearest-neighbor structure is underlined by the invariance of the peak in the structure factor corresponding to nearest-neighbor correlations. At shorter timescales, picoseconds, two localized relaxation processes of the cation can be observed, which are not directly linked to ion transport. However, these processes also show invariance at isoconductivity. This points to that the overall energy landscape in ionic liquids responds in the same way to density changes and is mainly governed by the nearest-neighbor interactions.
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spelling pubmed-80347752021-04-13 Pressure and Temperature Dependence of Local Structure and Dynamics in an Ionic Liquid Lundin, Filippa Hansen, Henriette Wase Adrjanowicz, Karolina Frick, Bernhard Rauber, Daniel Hempelmann, Rolf Shebanova, Olga Niss, Kristine Matic, Aleksandar J Phys Chem B [Image: see text] A detailed understanding of the local dynamics in ionic liquids remains an important aspect in the design of new ionic liquids as advanced functional fluids. Here, we use small-angle X-ray scattering and quasi-elastic neutron spectroscopy to investigate the local structure and dynamics in a model ionic liquid as a function of temperature and pressure, with a particular focus on state points (P,T) where the macroscopic dynamics, i.e., conductivity, is the same. Our results suggest that the initial step of ion transport is a confined diffusion process, on the nanosecond timescale, where the motion is restricted by a cage of nearest neighbors. This process is invariant considering timescale, geometry, and the participation ratio, at state points of constant conductivity, i.e., state points of isoconductivity. The connection to the nearest-neighbor structure is underlined by the invariance of the peak in the structure factor corresponding to nearest-neighbor correlations. At shorter timescales, picoseconds, two localized relaxation processes of the cation can be observed, which are not directly linked to ion transport. However, these processes also show invariance at isoconductivity. This points to that the overall energy landscape in ionic liquids responds in the same way to density changes and is mainly governed by the nearest-neighbor interactions. American Chemical Society 2021-03-03 2021-03-18 /pmc/articles/PMC8034775/ /pubmed/33656344 http://dx.doi.org/10.1021/acs.jpcb.1c00147 Text en © 2021 The Authors. Published by American Chemical Society Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Lundin, Filippa
Hansen, Henriette Wase
Adrjanowicz, Karolina
Frick, Bernhard
Rauber, Daniel
Hempelmann, Rolf
Shebanova, Olga
Niss, Kristine
Matic, Aleksandar
Pressure and Temperature Dependence of Local Structure and Dynamics in an Ionic Liquid
title Pressure and Temperature Dependence of Local Structure and Dynamics in an Ionic Liquid
title_full Pressure and Temperature Dependence of Local Structure and Dynamics in an Ionic Liquid
title_fullStr Pressure and Temperature Dependence of Local Structure and Dynamics in an Ionic Liquid
title_full_unstemmed Pressure and Temperature Dependence of Local Structure and Dynamics in an Ionic Liquid
title_short Pressure and Temperature Dependence of Local Structure and Dynamics in an Ionic Liquid
title_sort pressure and temperature dependence of local structure and dynamics in an ionic liquid
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8034775/
https://www.ncbi.nlm.nih.gov/pubmed/33656344
http://dx.doi.org/10.1021/acs.jpcb.1c00147
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