Improving the Accuracy of Atomistic Simulations of the Electrochemical Interface

Ravishankar Sundaraman, Derek Vigil-Fowler, Kathleen Schwarz

Research output: Contribution to journalArticlepeer-review

38 Scopus Citations


Atomistic simulation of the electrochemical double layer is an ambitious undertaking, requiring quantum mechanical description of electrons, phase space sampling of liquid electrolytes, and equilibration of electrolytes over nanosecond time scales. All models of electrochemistry make different trade-offs in the approximation of electrons and atomic configurations, from the extremes of classical molecular dynamics of a complete interface with point-charge atoms to correlated electronic structure methods of a single electrode configuration with no dynamics or electrolyte. Here, we review the spectrum of simulation techniques suitable for electrochemistry, focusing on the key approximations and accuracy considerations for each technique.

Original languageAmerican English
Pages (from-to)10651-10674
Number of pages24
JournalChemical Reviews
Issue number12
StatePublished - 22 Jun 2022

Bibliographical note

Publisher Copyright:
© 2022 American Chemical Society.

NREL Publication Number

  • NREL/JA-2C00-82948


  • atomistic simulation
  • electrochemistry
  • electrode configuration
  • electronic methods
  • enhanced sampling
  • molecular dynamics


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