{"title":"可编程螺旋波动力学:反应扩散系统中由时间调制驱动的不稳定级联。","authors":"Tarpan Maiti,Achal Jadhav,Pushpita Ghosh","doi":"10.1021/acs.jctc.5c01230","DOIUrl":null,"url":null,"abstract":"Spiral waves are iconic structures and are striking hallmarks of self-organization in chemical and biological systems. While their instabilities under spatial inhomogeneities have been widely studied, the response of spirals to temporal modulations particularly near the Turing threshold yet away from Hopf bifurcation, remains underexplored. In this study, we reveal how periodic forcing of a kinetic parameter in the Chlorine Dioxide-Iodine-Malonic Acid model unlocks a diverse and tunable landscape of spiral wave instabilities in a regime that is spatially stable yet temporally unstable. Starting from a robust single-arm spiral, we observe a cascade of modulation-induced phenomena: breathing spirals, core drift, spiral breakup and turbulence, as well as transitions to oscillating clusters, Ising-front-like patterns, and spatially uniform bulk oscillations. Remarkably, we identify spiral regeneration with altered arm width and chirality reversal, along with asymmetric spirals and multiphase cluster states arising from amplitude-phase interactions. Our findings are systematically mapped onto a two-dimensional phase diagram, revealing resonance-driven bifurcation cascades. Our results illuminate how simple temporal inputs can steer complex pattern selection in nonlinear media, offering conceptual advances for systems chemistry, chemical wave control, and the design of responsive self-organizing systems.","PeriodicalId":45,"journal":{"name":"Journal of Chemical Theory and Computation","volume":"18 1","pages":""},"PeriodicalIF":5.5000,"publicationDate":"2025-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Programmable Spiral Wave Dynamics: Instability Cascades Driven by Temporal Modulation in a Reaction-Diffusion System.\",\"authors\":\"Tarpan Maiti,Achal Jadhav,Pushpita Ghosh\",\"doi\":\"10.1021/acs.jctc.5c01230\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Spiral waves are iconic structures and are striking hallmarks of self-organization in chemical and biological systems. While their instabilities under spatial inhomogeneities have been widely studied, the response of spirals to temporal modulations particularly near the Turing threshold yet away from Hopf bifurcation, remains underexplored. In this study, we reveal how periodic forcing of a kinetic parameter in the Chlorine Dioxide-Iodine-Malonic Acid model unlocks a diverse and tunable landscape of spiral wave instabilities in a regime that is spatially stable yet temporally unstable. Starting from a robust single-arm spiral, we observe a cascade of modulation-induced phenomena: breathing spirals, core drift, spiral breakup and turbulence, as well as transitions to oscillating clusters, Ising-front-like patterns, and spatially uniform bulk oscillations. Remarkably, we identify spiral regeneration with altered arm width and chirality reversal, along with asymmetric spirals and multiphase cluster states arising from amplitude-phase interactions. Our findings are systematically mapped onto a two-dimensional phase diagram, revealing resonance-driven bifurcation cascades. Our results illuminate how simple temporal inputs can steer complex pattern selection in nonlinear media, offering conceptual advances for systems chemistry, chemical wave control, and the design of responsive self-organizing systems.\",\"PeriodicalId\":45,\"journal\":{\"name\":\"Journal of Chemical Theory and Computation\",\"volume\":\"18 1\",\"pages\":\"\"},\"PeriodicalIF\":5.5000,\"publicationDate\":\"2025-09-19\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Chemical Theory and Computation\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1021/acs.jctc.5c01230\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Chemical Theory and Computation","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acs.jctc.5c01230","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Programmable Spiral Wave Dynamics: Instability Cascades Driven by Temporal Modulation in a Reaction-Diffusion System.
Spiral waves are iconic structures and are striking hallmarks of self-organization in chemical and biological systems. While their instabilities under spatial inhomogeneities have been widely studied, the response of spirals to temporal modulations particularly near the Turing threshold yet away from Hopf bifurcation, remains underexplored. In this study, we reveal how periodic forcing of a kinetic parameter in the Chlorine Dioxide-Iodine-Malonic Acid model unlocks a diverse and tunable landscape of spiral wave instabilities in a regime that is spatially stable yet temporally unstable. Starting from a robust single-arm spiral, we observe a cascade of modulation-induced phenomena: breathing spirals, core drift, spiral breakup and turbulence, as well as transitions to oscillating clusters, Ising-front-like patterns, and spatially uniform bulk oscillations. Remarkably, we identify spiral regeneration with altered arm width and chirality reversal, along with asymmetric spirals and multiphase cluster states arising from amplitude-phase interactions. Our findings are systematically mapped onto a two-dimensional phase diagram, revealing resonance-driven bifurcation cascades. Our results illuminate how simple temporal inputs can steer complex pattern selection in nonlinear media, offering conceptual advances for systems chemistry, chemical wave control, and the design of responsive self-organizing systems.
期刊介绍:
The Journal of Chemical Theory and Computation invites new and original contributions with the understanding that, if accepted, they will not be published elsewhere. Papers reporting new theories, methodology, and/or important applications in quantum electronic structure, molecular dynamics, and statistical mechanics are appropriate for submission to this Journal. Specific topics include advances in or applications of ab initio quantum mechanics, density functional theory, design and properties of new materials, surface science, Monte Carlo simulations, solvation models, QM/MM calculations, biomolecular structure prediction, and molecular dynamics in the broadest sense including gas-phase dynamics, ab initio dynamics, biomolecular dynamics, and protein folding. The Journal does not consider papers that are straightforward applications of known methods including DFT and molecular dynamics. The Journal favors submissions that include advances in theory or methodology with applications to compelling problems.