Medium decoupling of dynamics at temperatures ~100 K above glass-transition temperature: a case study with (acetamide + lithium bromide/nitrate) melts

The Journal of Chemical Physics
Biswajit GuchhaitRanjit Biswas

Abstract

Time-resolved fluorescence Stokes shift and anisotropy measurements using a solvation probe in [0.78CH(3)CONH(2) + 0.22{f LiBr + (1-f) LiNO(3)}] melts reveal a strong decoupling of medium dynamics from viscosity. Interestingly, this decoupling has been found to occur at temperatures ∼50-100 K above the glass transition temperatures of the above melt at various anion concentrations (f(LiBr)). The decoupling is reflected via the following fractional viscosity dependence (η) of the measured average solvation and rotation times (<τ(s)> and <τ(r)>, respectively): <τ(x)> ∝ (η∕T)(p) (x being solvation or rotation), with p covering the range, 0.20 < p < 0.70. Although this is very similar to what is known for deeply supercooled liquids, it is very surprising because of the temperature range at which the above decoupling occurs for these molten mixtures. The kinship to the supercooled liquids is further exhibited via p which is always larger for <τ(r)> than for <τ(s)>, indicating a sort of translation-rotation decoupling. Multiple probes have been used in steady state fluorescence measurements to explore the extent of static heterogeneity. Estimated experimental dynamic Stokes shift for coumarin 153 in these mixtures lies in the range, ...Continue Reading

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Citations

Jan 15, 2014·The Journal of Chemical Physics·Snehasis Daschakraborty, Ranjit Biswas
Sep 15, 2014·The Journal of Chemical Physics·Tamisra Pal, Ranjit Biswas
Mar 17, 2016·The Journal of Chemical Physics·Snehasis Daschakraborty, Ranjit Biswas
Jul 2, 2015·The Journal of Physical Chemistry. B·Suman DasBiswaroop Mukherjee
Sep 20, 2018·Physical Chemistry Chemical Physics : PCCP·Sk Saddam Hossain, Anunay Samanta
Jan 31, 2015·Journal of Physics. Condensed Matter : an Institute of Physics Journal·Zaneta Wojnarowska, Marian Paluch
Nov 10, 2018·The Journal of Chemical Physics·Adam H Turner, Doseok Kim
Dec 15, 2020·Chemical Reviews·Benworth B HansenJoshua R Sangoro
Jul 22, 2021·Physical Chemistry Chemical Physics : PCCP·Nilimesh Das, Pratik Sen
Oct 14, 2014·The Journal of Physical Chemistry. B·Aninda ChatterjeeDebabrata Seth
Nov 1, 2017·The Journal of Physical Chemistry. B·Sk Saddam Hossain, Anunay Samanta
Jul 31, 2019·The Journal of Physical Chemistry. B·Shivam DuebySnehasis Daschakraborty
Sep 11, 2021·Physical Chemistry Chemical Physics : PCCP·H SrinivasanS Mitra

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Methods Mentioned

BETA
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Software Mentioned

DMASBT

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