Surface Charge Relaxation Controls the Lifetime of Out-of-Equilibrium Colloidal Crystals

Abstract

Interactions between charged colloidal particles are profoundly influenced by charge regulation and charge renormalization, rendering the effective potential highly sensitive to local particle density. In this work, we investigate how a dynamically evolving, density-dependent Yukawa interaction affects the stability of out-of-equilibrium colloidal structures. Motivated by a series of experiments where unexpectedly long-lived colloidal crystals have suggested the presence of like-charged attractions, we systematically explore the role of charge regulation and charge renormalization. Using Poisson-Boltzmann cell theory, we compute the effective colloidal charge and screening length as a function of packing fraction. These results are subsequently incorporated into Brownian dynamics simulations that dynamically resolve the evolving colloid charge as a function of time and local density. In the case of slow relaxation dynamics, our results show that incorporating these charging effects significantly prolongs the lifetimes of out-of-equilibrium colloidal crystals, providing an explanation for the experimental observation of long-lived crystals. These findings demonstrate that the interplay of surface charge dynamics and colloidal interactions can give rise to complex and rich nonequilibrium behavior in charged colloidal suspensions, opening new pathways for tuning colloidal stability through electrostatic feedback mechanisms.

14 pages, 5 figures (supplementary: 9 pages, 5 figures)

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