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This study presents a new method for calculating local diffusion coefficients in spherical systems, crucial for understanding aerosol and cell membrane processes. The method accurately estimates diffusion near interfaces, showing it increases towards the droplet surface.

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Area of Science:

  • Physical Chemistry
  • Computational Chemistry

Background:

  • Accurate estimation of local self-diffusion coefficients is vital for understanding interfacial systems.
  • Spherical interfacial systems are common in nature, influencing processes like atmospheric partitioning and biological transport.

Purpose of the Study:

  • To extend a method for estimating local diffusion coefficients from flat to spherically symmetric interfaces.
  • To provide an accurate and validated computational approach for analyzing diffusion in spherical systems.

Main Methods:

  • Derived an analytical solution to the linearized Smoluchowski equation in spherical coordinates.
  • Utilized molecular dynamics simulations to obtain necessary parameters.
  • Validated the solution against numerical solutions and experimental data for SPC/E water.

Main Results:

  • The derived analytical solution accurately estimates local self-diffusion coefficients in spherical systems.
  • The method was validated in bulk SPC/E water and applied to a water droplet in vapor.
  • Observed an increase in diffusion coefficient from the droplet center to the interface.

Conclusions:

  • The developed method provides a reliable tool for studying diffusion in spherical interfacial systems.
  • The findings are consistent with previous studies on flat interfaces, confirming the method's applicability.
  • This research enhances our understanding of molecular transport in complex, naturally occurring systems.