Response to “Comment on ‘Relative Diffusivities of Bound and Unbound Protein Can Control Chemotactic Directionality’”

Mandal, Niladri Sekhar; Sen, Ayusman

doi:10.1021/acs.langmuir.1c03446

Langmuir

2022

DOI: 10.1021/acs.langmuir.1c03446

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Response to “Comment on ‘Relative Diffusivities of Bound and Unbound Protein Can Control Chemotactic Directionality’”

Niladri Sekhar Mandal

Ayusman Sen

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2023

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Relating the artificial chemotaxis of catalysts to a gradient descent of the free energy

Krist

Noid

2023

The Journal of Chemical Physics

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Recent experiments suggest that mesoscale catalysts are active materials that power their motion with chemical free energy from their environment and also “chemotax” with respect to substrate gradients. In the present work, we explore a thermodynamic framework for relating this chemotaxis to the evolution of a system down the gradient of its free energy. This framework builds upon recent studies that have employed the Wasserstein metric to describe diffusive processes within the Onsager formalism for irreversible thermodynamics. In this work, we modify the Onsager dissipation potential to explicitly couple the reactive flux to the diffusive flux of catalysts. The corresponding gradient flow is a modified reaction-diffusion equation with an advective term that propels the chemotaxis of catalysts with the free energy released by chemical reactions. In order to gain first insights into this framework, we numerically simulate a simplified model for spherical catalysts undergoing artificial chemotaxis in one dimension. These simulations investigate the thermodynamic forces and fluxes that drive this chemotaxis, as well as the resulting dissipation of free energy. Additionally, they demonstrate that chemotaxis can delay the relaxation to equilibrium and, equivalently, prolong the duration of nonequilibrium conditions. Although future simulations should consider a more realistic coupling between reactive and diffusive fluxes, this work may provide insight into the thermodynamics of artificial chemotaxis. More generally, we hope that this work may bring attention to the importance of the Wasserstein metric for relating nonequilibrium relaxation to the thermodynamic free energy and to large deviation principles.

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Relating the artificial chemotaxis of catalysts to a gradient descent of the free energy

Krist

Noid

2023

The Journal of Chemical Physics

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Response to “Comment on ‘Relative Diffusivities of Bound and Unbound Protein Can Control Chemotactic Directionality’”

Cited by 1 publication

References 4 publications

Relating the artificial chemotaxis of catalysts to a gradient descent of the free energy

Relating the artificial chemotaxis of catalysts to a gradient descent of the free energy

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