  Nanoparticles in solution acquire charge through dissociation or association
of surface groups. Thus, a proper description of their electrostatic
interactions requires the use of charge-regulating boundary conditions rather
than the commonly employed constant-charge approximation. We implement a hybrid
Monte Carlo/Molecular Dynamics scheme that dynamically adjusts the charges of
individual surface groups of objects while evolving their trajectories.
Charge-regulation effects are shown to qualitatively change self-assembled
structures due to global charge redistribution, stabilizing asymmetric
constructs. We delineate under which conditions the conventional
constant-charge approximation may be employed and clarify the interplay between
charge regulation and dielectric polarization.
