Many-body quantum chaos in excitonic spectra from first principles

Abstract

We demonstrate that realistic excitonic many-body Hamiltonians obtained from first-principles GW-Bethe-Salpeter equation calculations can exhibit quantum chaos governed by random-matrix universality. Considering a prototypical van der Waals heterostructure (WS$_2$-graphene), with and without lattice disorder, we analyze their energy-resolved spectral correlations and identify a disorder-driven crossover from regular to complete chaotic dynamics. We show that while pristine samples exhibit incomplete chaos (non-ergodicity) due to an approximate valley symmetry that restricts excitonic mixing, the presence of disorder-induced electronic flat bands act as a catalyst for valley mixing to drive the system into a fully developed chaotic (ergodic) regime with reduced symmetry. Crucially, fluctuations in many-body oscillator strengths are shown to follow universal Porter-Thomas statistics, directly linking the underlying quantum chaos and experimentally accessible optical observables. Finally, by examining long-range spectral correlations, we estimate the Thouless time associated to excitonic mixing across the entire many-body bandwidth. Our results establish excitons as a highly tunable platform for probing many-body ergodicity and its spectroscopic signatures in realistic interacting 2D materials.