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Solution-Tunable Interfacial Interaction Landscape Governs Anomalous Nanoparticle Diffusion in Liquid-Phase Electron

Isabel Panicker1, Zain Shabeeb1, Cory Hargus2

  • 1School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, United States of America.

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Summary

We discovered how ion concentration controls nanoparticle movement at interfaces. By adjusting salt levels, we can switch nanoparticle diffusion between fractional Brownian motion and annealed transient time motion, enabling precise control over their mobility.

Keywords:
anomalous diffusioninterfacial transportliquid-phase transmission electron microscopypassive nanorheologysingle-particle tracking

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Area of Science:

  • Nanoscale science and engineering
  • Surface chemistry and physics
  • Soft matter physics

Background:

  • Understanding nanoparticle behavior at liquid-solid interfaces is crucial for applications in catalysis, biology, and materials science.
  • Anomalous diffusion near interfaces presents complex challenges for predicting and controlling nanoscale transport.

Purpose of the Study:

  • To investigate the physical mechanisms governing the surface diffusion of PEG-coated gold nanorods (AuNRs) near silicon nitride (SiNx) membranes.
  • To determine how ionic environment modulates nanoparticle-interface interactions and diffusion dynamics.
  • To introduce and validate a passive nanorheology framework for characterizing interfacial properties.

Main Methods:

  • Systematic tuning of the ionic environment (deionized H2O, H2SO4, NaCl, PBS) for PEG-AuNRs near SiNx membranes in liquid-phase transmission electron microscopy (LPTEM).
  • Statistical analysis and deep learning classification of nanoparticle trajectories to identify diffusion mechanisms (fractional Brownian motion - FBM, annealed transient time motion - ATTM).
  • Development of a passive nanorheology framework using particle trajectories to probe the viscoelastic properties of the near-surface environment.

Main Results:

  • Electrostatic screening and ion-specific interactions significantly alter the binding site landscape, affecting nanoparticle confinement and mobility.
  • A tunable transition in diffusion mechanisms from FBM to ATTM was observed by varying ionic strength and composition.
  • The nanorheology framework successfully extracted viscoelastic moduli, revealing insights into interfacial interaction strengths.

Conclusions:

  • Ionic environment acts as an external control to program near-surface nanoparticle transport, shifting diffusion mechanisms and tuning mobility.
  • LPTEM, combined with nanorheology, provides a quantitative platform for diagnosing interfacial mechanical responses and probing nanoscale transport.
  • These findings offer a pathway to control nanoparticle dynamics in complex interfacial systems.