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We study the loss of coherence of electrochemical oscillations on meso- andnanosized electrodes with numeric simulations of the electrochemical masterequation for a prototypical electrochemical oscillator, the hydrogen peroxidereduction on Pt electrodes in the presence of halides. On nanoelectrodes, theelectrode potential changes whenever a stochastic electron-transfer event takesplace. Electrochemical reaction rate coefficients depend exponentially on theelectrode potential and become thus fluctuating quantities as well. Therefore,also the transition rates between system states become time-dependent whichconstitutes a fundamental difference to purely chemical nanoscale oscillators.Three implications are demonstrated: (a) oscillations and steady states shiftin phase space with decreasing system size, thereby also decreasingconsiderably the oscillating parameter regions; (b) the minimal number ofmolecules necessary to support correlated oscillations is more than 10 times aslarge as for nanoscale chemical oscillators; (c) the relation betweencorrelation time and variance of the period of the oscillations predicted forchemical oscillators in the weak noise limit is only fulfilled in a veryrestricted parameter range for the electrochemical nano-oscillator.

Destructive Impact of Molecular Noise on Nanoscale Electrochemical Oscillators