2022/09/23 by Avishek Das, Das, Avishek, David T. Limmer +1 · 1 citation
Biochemistry, Genetics and Molecular Biology · Chemistry · Engineering · #Chemical Physics (physics.chem-ph) #Diffusion and Search Dynamics #Electrostatics and Colloid Interactions #FOS: Physical sciences #Nanopore and Nanochannel Transport Studies #Soft Condensed Matter (cond-mat.soft) #Statistical Mechanics (cond-mat.stat-mech)
paper · pdf · doi:10.48550/arxiv.2209.11538
openalex publication_date 2022/09/23 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/28
We use a nonequilibrium variational principle to optimize the steady-state, shear-induced interconversion of self-assembled nanoclusters of DNA-coated colloids. Employing this principle within a stochastic optimization algorithm allows us to discover design strategies for functional materials. We find that far-from-equilibrium shear flow can significantly enhance the flux between specific colloidal states by decoupling trade-offs between stability and reactivity required by systems in equilibrium. For isolated nanoclusters, we find nonequilibrium strategies for amplifying transition rates by coupling a given reaction coordinate to the background shear flow. We also find that shear flow can be made to selectively break detailed balance and maximize probability currents by coupling orientational degrees of freedom to conformational transitions. For a microphase consisting of many nanoclusters, we study the flux of colloids hopping between clusters. We find that a shear flow can amplify the flux without a proportional compromise on the microphase structure. This approach provides a general means of uncovering design principles for nanoscale, autonomous, functional materials driven far from equilibrium.