Pressure-induced liquid-liquid transition in a family of ionic materials

Zaneta Wojnarowska; Shinian Cheng; Beibei Yao; Malgorzata Swadzba-Kwasny; Shannon McLaughlin; Anne McGrogan; Yoan Delavoux; Marian Paluch

doi:10.1038/s41467-022-29021-0

Pressure-induced liquid-liquid transition in a family of ionic materials

Zaneta Wojnarowska
, Shinian Cheng
, Beibei Yao
, Malgorzata Swadzba-Kwasny
, Shannon McLaughlin
, Anne McGrogan
, Yoan Delavoux
, Marian Paluch

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

37 Scopus citations

Abstract

Liquid−liquid transition (LLT) between two disordered phases of single-component material remains one of the most intriguing physical phenomena. Here, we report a first-order LLT in a series of ionic liquids containing trihexyl(tetradecyl)phosphonium cation [P_666,14]⁺ and anions of different sizes and shapes, providing an insight into the structure-property relationships governing LLT. In addition to calorimetric proof of LLT, we report that ion dynamics exhibit anomalous behavior during the LLT, i.e., the conductivity relaxation times (τ_σ) are dramatically elongated, and their distribution becomes broader. This peculiar behavior is induced by isobaric cooling and isothermal compression, with the τ_σ(T_LL,P_LL) constant for a given system. The latter observation proves that LLT, in analogy to liquid-glass transition, has an isochronal character. Finally, the magnitude of discontinuity in a specific volume at LLT was estimated using the Clausius-Clapeyron equation.

Original language	English
Article number	1342
Journal	Nature Communications
Volume	13
Issue number	1
DOIs	https://doi.org/10.1038/s41467-022-29021-0
State	Published - Dec 2022
Externally published	Yes

Funding

Authors acknowledge M. Musiał for the density measurements of [P][TCM]. The authors Z.W., S.C. and M.P. are deeply grateful for the financial support by the National Science Centre within the framework of the Opus15 project (grant nr DEC- 2018/29/B/ST3/00889 M.P.). Solvay is acknowledged for kindly providing trihexyl(tetradecyl)phosphonium chloride. 666,14

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abstract = "Liquid−liquid transition (LLT) between two disordered phases of single-component material remains one of the most intriguing physical phenomena. Here, we report a first-order LLT in a series of ionic liquids containing trihexyl(tetradecyl)phosphonium cation [P666,14]+ and anions of different sizes and shapes, providing an insight into the structure-property relationships governing LLT. In addition to calorimetric proof of LLT, we report that ion dynamics exhibit anomalous behavior during the LLT, i.e., the conductivity relaxation times (τσ) are dramatically elongated, and their distribution becomes broader. This peculiar behavior is induced by isobaric cooling and isothermal compression, with the τσ(TLL,PLL) constant for a given system. The latter observation proves that LLT, in analogy to liquid-glass transition, has an isochronal character. Finally, the magnitude of discontinuity in a specific volume at LLT was estimated using the Clausius-Clapeyron equation.",

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AU - Wojnarowska, Zaneta

AU - Cheng, Shinian

AU - Yao, Beibei

AU - Swadzba-Kwasny, Malgorzata

AU - McLaughlin, Shannon

AU - McGrogan, Anne

AU - Delavoux, Yoan

AU - Paluch, Marian

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N2 - Liquid−liquid transition (LLT) between two disordered phases of single-component material remains one of the most intriguing physical phenomena. Here, we report a first-order LLT in a series of ionic liquids containing trihexyl(tetradecyl)phosphonium cation [P666,14]+ and anions of different sizes and shapes, providing an insight into the structure-property relationships governing LLT. In addition to calorimetric proof of LLT, we report that ion dynamics exhibit anomalous behavior during the LLT, i.e., the conductivity relaxation times (τσ) are dramatically elongated, and their distribution becomes broader. This peculiar behavior is induced by isobaric cooling and isothermal compression, with the τσ(TLL,PLL) constant for a given system. The latter observation proves that LLT, in analogy to liquid-glass transition, has an isochronal character. Finally, the magnitude of discontinuity in a specific volume at LLT was estimated using the Clausius-Clapeyron equation.

AB - Liquid−liquid transition (LLT) between two disordered phases of single-component material remains one of the most intriguing physical phenomena. Here, we report a first-order LLT in a series of ionic liquids containing trihexyl(tetradecyl)phosphonium cation [P666,14]+ and anions of different sizes and shapes, providing an insight into the structure-property relationships governing LLT. In addition to calorimetric proof of LLT, we report that ion dynamics exhibit anomalous behavior during the LLT, i.e., the conductivity relaxation times (τσ) are dramatically elongated, and their distribution becomes broader. This peculiar behavior is induced by isobaric cooling and isothermal compression, with the τσ(TLL,PLL) constant for a given system. The latter observation proves that LLT, in analogy to liquid-glass transition, has an isochronal character. Finally, the magnitude of discontinuity in a specific volume at LLT was estimated using the Clausius-Clapeyron equation.

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Pressure-induced liquid-liquid transition in a family of ionic materials

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