Abstract
We studied the solute-induced perturbation of the solvent environment around a solute species from a microscopic viewpoint and propose a novel approach to the understanding of the structure-making/breaking process, regardless of the type and nature of the solute-solvent interactions. Based on the Kirkwood-Buff fluctuation formalism, we present a rigorous statistical mechanics description of the evolution of the solvent structure around the solute, analyze its response to small perturbations of the ( TP) state conditions and composition of the system, and make direct connections between a few equivalent micro- and macroscopic manifestations as probes for, and targets of, experimental measurements. We illustrate the analysis with theoretical results from integral equation calculations of model fluids and experimental evidence from available data for a variety of aqueous electrolyte and nonelectrolyte real fluid solutions. Finally, we provide a critical discussion about the inadequacy underlying a widely used de facto criterion for the classification of structure-making/breaking solutes.
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