Low frequency temperature forcing of chemical oscillations

Abstract

The low frequency forcing of chemical oscillations by temperature is investigated experimentally in the Belousov-Zhabotinsky (BZ) reaction and in simulations of the Oregonator model with Arrhenius temperature dependence of the rate constants. Forcing with temperature leads to modulation of the chemical frequency. The number of response cycles per forcing cycle is given by the ratio of the natural frequency to the forcing frequency and phase locking is only observed in simulations when this ratio is a whole number and the forcing amplitude is small. The global temperature forcing of flow-distributed oscillations in a tubular reactor is also investigated and synchronisation is observed in the variation of band position with the external signal, reflecting the periodic modulation of chemical oscillations by temperature.

Dynamic Environments as a Tool to Preserve Desired Output in a Chemical Reaction Network

“…Although temperature forcing has been demonstrated in the BZ system, our results experimentally demonstrate period‐locking (only observed in simulations of temperature‐forced BZ reactions) and show that, in these minimal systems with a single negative feedback loop, periodic temperature oscillations can be used as a variable, instead of a fixed experimental parameter.…”

“…We draw inspiration fromn ature, [26][27][28][29][30] in whichfluctuating environmentsa re the norm (e.g.,d ay/night cycles, tidal waves, seasons),a nd from theoretical and experimentalw ork on simplified model systems [31,32] and studies on inorganic oscillators, such as the Belousov-Zhabotinsky (BZ) reaction, [33][34][35][36][37][38][39][40][41][42][43] which show ar ange of phenomena can emerge when operatedi na dynamic environment, for example, synchronisation through periodic variations in feed concentration, [33] entrainment of spatiotemporalw ave generation with temperature forcing, [34] spiral and standing spatiotemporal waves through periodic spiking withl ight, [37,38] noise-induced oscillations, [39] and chaotic oscillations. We draw inspiration fromn ature, [26][27][28][29][30] in whichfluctuating environmentsa re the norm (e.g.,d ay/night cycles, tidal waves, seasons),a nd from theoretical and experimentalw ork on simplified model systems [31,32] and studies on inorganic oscillators, such as the Belousov-Zhabotinsky (BZ) reaction, [33][34][35][36][37][38][39][40][41][42][43] which show ar ange of phenomena can...…”

“…Here, we demonstrate as imple way to enable robustb ehaviour by coupling the network to ad ynamic environment. We draw inspiration fromn ature, [26][27][28][29][30] in whichfluctuating environmentsa re the norm (e.g.,d ay/night cycles, tidal waves, seasons),a nd from theoretical and experimentalw ork on simplified model systems [31,32] and studies on inorganic oscillators, such as the Belousov-Zhabotinsky (BZ) reaction, [33][34][35][36][37][38][39][40][41][42][43] which show ar ange of phenomena can emerge when operatedi na dynamic environment, for example, synchronisation through periodic variations in feed concentration, [33] entrainment of spatiotemporalw ave generation with temperature forcing, [34] spiral and standing spatiotemporal waves through periodic spiking withl ight, [37,38] noise-induced oscillations, [39] and chaotic oscillations. [40] We use our previously designed enzymatic reaction network ( Figure 1) [5,44,45] to show how the behaviour of an etwork, in this case oscillations, varies upon ac hange in the environment.…”

MRI of chemical reactions and processes

“…Of course, the observed periodic changes in colour do not break the second law of thermodynamics, because they are caused by oscillations in the concentration of reaction intermediates as the reaction progresses towards equilibrium. Since its initially contentious beginnings, this reaction has become the most studied pattern-forming reaction, and provides a useful device for observing the coupling between reaction with molecular transport [21] and other environmental factors or external stimuli [27]. The chemical waves formed in the BZ reaction, and other autocatalytic reactions, are particularly useful for characterising transport and mixing behaviour within complex flow environments [28][29][30][31][32], because only small amounts of the autocatalyst are required to enter a region, before there is a rapid amplification of the concentration of that, and associated, species.…”

Noise induced oscillations and coherence resonance in a generic model of the nonisothermal chemical oscillator

“…For example, it has been suggested that the oscillatory Belousov-Zhabotinsky reaction could have some temperature compensation mechanism35. Effects of temperature on this system were studied both experimentally and theoretically363738. However, a common feature of these studies is that temperature was considered as a parameter, not a variable.…”