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Generation and Control of Electrohydrodynamic Flows in Aqueous Electrolyte Solutions
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Collective dipole effects in ionic transport under electric fields.

N Salles1,2, L Martin-Samos3, S de Gironcoli4

  • 1CNR-IOM/Democritos National Simulation Center, Istituto Officina dei Materiali, c/o SISSA, via Bonomea 265, Trieste, 34136, Italy. nsalles33@gmail.com.

Nature Communications
|July 5, 2020
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Summary
This summary is machine-generated.

The classical model for ionic transport under electric fields is unreliable due to collective dipole effects. This study introduces an equivalent polarization-work charge, revealing new insights into migration barrier variations.

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Area of Science:

  • Solid-state physics
  • Materials science
  • Computational materials science

Background:

  • Traditional models assume electric field effects on migration barriers equal classical point charge work.
  • The reliability of this phenomenological approach compared to the Modern Theory of Polarization is questioned.

Purpose of the Study:

  • To investigate the validity of the classical model for electric field effects on ionic migration barriers in solids.
  • To explore the role of collective dipole effects in ionic transport.
  • To derive a new theoretical framework for understanding these phenomena.

Main Methods:

  • Developed a polarization decomposition technique.
  • Derived an expression for the equivalent polarization-work charge.
  • Applied the theory to study oxygen charged defects in MgO and SiO2.

Main Results:

  • Demonstrated that the classical picture of migration barrier variation is not universally applicable.
  • Identified critical collective dipole effects influencing ionic transport.
  • Showed that the equivalent polarization-work charge is determined by the total polarization change at the transition state, not solely by the transported or Born effective charge.

Conclusions:

  • The classical phenomenological model for electric field effects on ionic migration barriers is insufficient.
  • Collective dipole effects are crucial and must be considered for accurate modeling.
  • The derived equivalent polarization-work charge provides a more robust theoretical basis for understanding ionic transport under electric fields.