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Camel back shaped Kirkwood-Buff integrals.

Aurélien Perera1, Martina Požar2, Bernarda Lovrinčević2

  • 1Laboratoire de Physique Théorique de la Matière Condensée (UMR CNRS 7600), Sorbonne Université, 4 Place Jussieu, F75252 Paris Cedex 05, France.

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Binary mixtures with "camel back" Kirkwood-Buff integrals (KBIs) show dual concentration fluctuations. This phenomenon arises when one component forms aggregates, creating a "meta-species" with its own KBI extremum.

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Area of Science:

  • Physical Chemistry
  • Thermodynamics
  • Solution Chemistry

Background:

  • Binary mixtures typically exhibit single extrema in Kirkwood-Buff integrals (KBIs), indicating maximum concentration fluctuations and micro-segregation.
  • Unusual "camel back" shaped KBIs, with two humps, are observed in specific mixtures like alcohol-alkane and water-tert-butanol.

Purpose of the Study:

  • To explain the occurrence of two extrema in KBIs for certain binary mixtures.
  • To elucidate the relationship between concentration fluctuations, micro-segregation, and aggregate formation in solutions.

Main Methods:

  • Analysis of Kirkwood-Buff integrals (KBIs) for binary mixtures.
  • Theoretical investigation of concentration fluctuations and micro-segregation phenomena.
  • Modeling of systems where one component forms "meta-particle" aggregates.

Main Results:

  • Two KBI extrema arise when one component forms "meta-particle" aggregates, effectively acting as a "meta-species".
  • These aggregates possess their own concentration fluctuations, leading to a distinct KBI extremum (a "meta-extremum").
  • The "meta-extremum" appears at low concentrations of the aggregate-forming species and is independent of the usual extremum at mid-volume fraction.

Conclusions:

  • The presence of two KBI extrema signifies a duality between concentration fluctuations and micro-segregation.
  • Aggregate formation by one component is key to observing this dual extremum behavior in binary mixtures.
  • These findings offer insights into the complex structural organization of solutions exhibiting unusual thermodynamic properties.