• Media type: Electronic Conference Proceeding
  • Title: Atomistic Modelling of Redox Reactions in Non-Equilibrium
  • Contributor: Dapp, Wolfgang [Author]; Müser, Martin [Author]
  • Published: John von Neumann Institute for Computing, 2014
  • Published in: Jülich : John von Neumann Institute for Computing, NIC Series 47, 25-32 (2014). ; NIC Symposium 2014 - Proceedings ; NIC Symposium 2014 - Proceedings NIC Symposium 2014, Jülich, Germany, 2014-02-12 - 2014-02-13
  • Language: English
  • Origination:
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  • Description: We developed a new atomistic method to model (non-equilibrium) redox reaction using empirical force fields for use in MD simulations. To this end, we added the (formal) ionisation state as a discrete variable into the “split charge equilibration” method (SQE). This extension allows atoms to swap integer charges across bonds, in addition to exchanging fractional charges. We call this method “redoxSQE”, and, in first steps, used it to study contact electrification and to set up a model rechargeable nano-battery that reproduces the generic features of the discharge of a macroscopic battery qualitatively. Other popular charge-transfer force fields fundamentallycannot describe any history-dependent effect because they calculate the charge distribution as a unique function of atomic positions. For similar reasons, state-of-the-art DFT-based methods fail to describe redox reactions in non-equilibrium.
  • Access State: Open Access