Manipulating Charge Distribution in Moiré Superlattices by Light

In ordinary solids, nonlinear optical responses are typically studied in terms of unit-cell averages due to the ångström-scale lattice constants. In contrast, moiré superlattices, characterized by a large length scale, unlock an often-overlooked degree of freedom: intrasupercell spatial variations of local observables. Here, we formulate the second-order direct current (dc) charge response in a spatially resolved manner, showing that even uniform optical illumination can drive a static, spatially nonuniform charge redistribution within a supercell. This effect is ubiquitous and cannot be forbidden by any crystalline symmetries. Furthermore, we identify a dominant contribution arising from diverging analytical response coefficients, which leads to linear-in-time growth of the redistribution in the absence of relaxation. This growth is driven by the convergence or divergence of local dc photocurrents. Applying our theory to twisted bilayer MoTe_{2}, we demonstrate strong, highly tunable charge modulation controlled by light intensity and frequency, opening a route to in situ, all-optical control of moiré-periodic electrostatic potentials. Our Letter underscores the importance of intracell degrees of freedom, which enable a qualitatively richer class of nonlinear optical responses in moiré superlattices.