Bichromatic Moiré Superlattices for Tunable Quadrupolar Trions and Correlated States

Abstract: Moir\'{e} superlattices in transition metal dichalcogenide heterostructures provide a platform to engineer many-body interactions. Here, we realize a bichromatic moir\'{e} superlattice in an asymmetric WSe$_2$/WS$_2$/WSe$_2$ heterotrilayer by combining R- and H-stacked bilayers with mismatched moir\'{e} wavelengths. This structure hosts fermionic quadrupolar moir\'{e} trions--interlayer excitons bound to an opposite-layer hole--with vanishing dipole moments. These trions arise from hybridized moir\'{e} potentials enabling multiple excitonic orbitals with tunable interlayer coupling, allowing control of excitonic and electronic ground states. We show that an out-of-plane electric field could effectively reshape moir\'{e} excitons and interlayer-intralayer electron correlations, driving a transition from interlayer to intralayer Mott states with enhanced Coulomb repulsion. The asymmetric stacking further enriches excitonic selection rules, broadening opportunities for spin-photon engineering. Our results demonstrate bichromatic moir\'{e} superlattices as a reconfigurable platform for emergent quantum states, where quadrupolar moir\'{e} trion emission may enable coherent and entangled quantum light manipulation.