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Excitonic insulators are long-sought-after quantum materials predicted tospontaneously open a gap by the Bose condensation of bound electron-hole pairs,namely, excitons, in their ground state. Since the theoretical conjecture,extensive efforts have been devoted to pursuing excitonic insulator platformsfor exploring macroscopic quantum phenomena in real materials. Reliableevidences of excitonic character have been obtained in layered chalcogenides aspromising candidates. However, owing to the interference of intrinsic latticeinstabilities, it is still debatable whether those features, such as chargedensity wave and gap opening, are primarily driven by the excitonic effect orby the lattice transition. Herein, we develop a novel charge-transfer excitonicinsulator in organic-inorganic superlattice interfaces, which serves as anideal platform to decouple the excitonic effect from the lattice effect. Inthis system, we observe the narrow gap opening and the formation of a chargedensity wave without periodic lattice distortion, providing visualized evidenceof exciton condensation occurring in thermal equilibrium. Our findings identifyspontaneous interfacial charge transfer as a new strategy for developing novelexcitonic insulators and investigating their correlated many-body physics.

Interfacial Charge-transfer Excitonic Insulator in a Two-dimensional Organic-inorganic Superlattice