Chemical Frequency Combs in Reaction-Diffusion Oscillators

Abstract

Frequency combs, evenly spaced spectral lines locked to one fundamental frequency, are well known in optics and have also been found in phononic, magnonic, ferroelectric, and cosmological systems, but have not yet been studied in oscillating chemical reactions. In this work, we show that reaction-diffusion oscillators can also produce frequency combs. We use the Brusselator model and derive its Hopf bifurcation condition directly from the rate equations. We find that the trimolecular autocatalytic term is the only source of nonlinear harmonic content. Above the Hopf threshold, our simulations of target-wave patterns show a clear fundamental frequency followed by a long, evenly spaced ladder of harmonics, with each harmonic weaker than the one before it. We then vary the reactant concentrations and kinetic parameters one at a time and find that this comb structure holds across a wide range of values. We also test this idea experimentally using the Belousov-Zhabotinsky reaction. Intensity signals recorded at different points in a target pattern show a shared fundamental frequency with several weakening harmonics, matching the simulated pattern closely. Together, these results show that reaction-diffusion chemistry is a new platform for generating frequency combs.