Journal Title
Title of Journal: J Chem Sci
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Abbravation: Journal of Chemical Sciences
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Authors: SARMISTHA SARKAR SAIKAT BANERJEE SUSMITA ROY RIKHIA GHOSH PARTHA PRATIM RAY BIMAN BAGCHI
Publish Date: 2015/02/14
Volume: 127, Issue: 1, Pages: 49-59
Abstract
We explore the potential energy landscape of structure breaking binary mixtures SBBM where two constituents dislike each other yet remain macroscopically homogeneous at intermediate to high temperatures Interestingly we find that the origin of strong composition dependent nonideal behaviour lies in its phase separated inherent structure The inherent structure IS of SBBM exhibits bicontinuous phase as is usually formed during spinodal decomposition We draw analogy of this correlation between nonideality and phase separation in IS to explain observation of nonideality in real aqueous mixtures of small amphiphilic solutes containing both hydrophilic and hydrophobic groups Although we have not been able to obtain IS of these liquids we find that even at room temperature these liquids sustain formation of fluctuating transient bicontinuous phase with limited lifetime τ≲20 ps While in the model A B binary mixture the nonideal composition dependence can be considered as a fluctuation from a phase separated state a similar scenario is expected to be responsible for the unusually strong nonideality in these aqueous binary mixturesOur main observation is that the occurrence of strong nonideality in many binary mixtures is due to the existence of a transient phase separation The presence of the interpenetrating percolating networks provides a striking resemblance to spinodal decompositionSingle particle potential energy distribution of parent liquid for structure former binary mixture Model I at mole fraction xB=04 and temperature T = 1 is shown in figure S1 and the corresponding single particle inherent structure energy distribution is shown in figure S2 Supplementary information is available at wwwiasacin/chemsci
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