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Linear solvation theories fail for nanometer solutes. Surface hydration shows nonlinear responses and dynamics slowing, impacting nanoparticle and biomolecule interfaces.

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Area of Science:

  • Physical Chemistry
  • Computational Chemistry
  • Materials Science

Background:

  • Established linear solvation theories accurately predict hydration free energy for small solutes dominated by electrostatic multipole interactions.
  • Hydration of nanometer-sized solutes is primarily governed by surface hydration effects, differing significantly from small solute behavior.

Purpose of the Study:

  • To investigate the applicability of linear-response thermodynamics, developed for small solutes, to the surface hydration of nanometer-sized solutes.
  • To explore the thermodynamic and dynamic responses of water at the interface of a model nanometer solute with varying surface polarity.

Main Methods:

  • Utilized molecular dynamics simulations to study a model C180 solute.
  • The solute surface was functionalized with radially oriented dipoles to simulate varying surface polarity without a global multipole.
  • Analyzed solvation thermodynamics and interfacial dynamics under different surface polarity conditions.

Main Results:

  • Demonstrated a dramatic violation of linear response in the solvation thermodynamics of the nanometer solute.
  • Identified two distinct crossovers in solvation thermodynamics with increasing surface polarity, indicating strongly nonlinear responses.
  • Observed a significant slowing down of interfacial water dynamics, reaching nanosecond timescales, associated with a collective crossover.

Conclusions:

  • Linear solvation theories are inadequate for describing the surface hydration of nanometer solutes.
  • Surface polarity induces nonlinear solvation responses and significantly alters interfacial water dynamics.
  • The findings suggest potential for controlling water domain flipping at nanoparticle and biomolecule interfaces.