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- W4385628654 endingPage "7173" @default.
- W4385628654 startingPage "7162" @default.
- W4385628654 abstract "Traditionally, deviation from Stokes–Einstein–Debye (SED) relation in terms of viscosity dependence of medium dynamics, i.e., τx∝(ηT)p with p ≠ 1, is taken as a signature of dynamic heterogeneity. However, it does not guarantee medium heterogeneity, as the decoupling may also originate from the deviation of the basic assumption of SED. Here, we developed a method to find a stronger relation between viscosity decoupling (p ≠ 1) and dynamic heterogeneity in terms of rotational motion. Our approach exploited the fact that in heterogeneous media, a solvatochromic probe will be solvated to a different extent at different microdomains (subpopulations), and photoselection of these subpopulations can be achieved by excitation or emission wavelength-dependent measurements. We hypothesized that the dynamics of a homogeneous system might show viscosity decoupling, but the extent of decoupling at different excitations (or at different emissions) should not be different. On the other hand, in a heterogeneous medium, this extent of viscosity decoupling (p-value) should be different at different excitations (or at different emissions). As proof of concept, we investigated three versatile solvent media: squalane (viscous molecular liquid), 1-ethyle-3-methylimidazolium ethyl sulfate ionic liquid (IL), and [0.78 acetamide + 0.22 LiNO3] deep eutectic solvent (DES). We found that squalane is homogeneous, although it shows fractional viscosity dependence (p ≠ 1). Interestingly, mild heterogeneity in IL and significant heterogeneity in the DES were observed. Overall, we conclude that the difference in the p-value as a function of excitation (or emission) wavelength-dependent might be a superior way for the detection of dynamic heterogeneity." @default.
- W4385628654 created "2023-08-08" @default.
- W4385628654 creator A5027686302 @default.
- W4385628654 creator A5081493365 @default.
- W4385628654 date "2023-08-07" @default.
- W4385628654 modified "2023-10-03" @default.
- W4385628654 title "Does Viscosity Decoupling Guarantee Dynamic Heterogeneity? A Clue through an Excitation and Emission Wavelength-Dependent Time-Resolved Fluorescence Anisotropy Study" @default.
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- W4385628654 doi "https://doi.org/10.1021/acs.jpcb.3c00334" @default.
- W4385628654 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/37549044" @default.