Abstract
Moiré superlattices in transition metal dichalcogenide heterostructures provide a platform to engineer many-body interactions. Here, we realize a bichromatic moiré superlattice in an asymmetric WSe2/WS2/WSe2 heterotrilayer by combining R- and H-stacked bilayers with mismatched moiré wavelengths. This structure hosts fermionic quadrupolar moiré trions—interlayer excitons bound to an opposite-layer hole—with vanishing dipole moments. These trions arise from hybridized moiré 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 moiré 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 moiré superlattices as a reconfigurable platform for emergent quantum states, where quadrupolar moiré trion emission may enable coherent and entangled quantum light manipulation.
| Original language | English |
|---|---|
| Article number | 10359 |
| Journal | Nature Communications |
| Volume | 16 |
| Issue number | 1 |
| DOIs | |
| State | Published - Dec 2025 |
Funding
This work was mainly supported by the Wang Start-up funding, funded by the College of Arts & Sciences at Washington University in St. Louis (WUSTL). The fabrication is partially supported by Ralph E. Powe Junior Faculty Enhancement Awards, partially supported by the Gordon and Betty Moore Foundation, grant https://doi.org/10.37807/gbmf11560. X.W. acknowledges equipment support by the Center for Quantum Leaps at WUSTL. X.W. acknowledges the use of the Cypher S atomic force microscope for high-resolution PFM characterization of the moiré superlattices. The fabrication used instruments in the Institute of Materials Science and Engineering (IMSE) at WUSTL, with partial financial support from IMSE. Bulk WSe2 crystals were grown and characterized by C.H., J.C., and J.Y. Materials synthesis by C.H. and J.C. was supported as part of Programmable Quantum Materials, an Energy Frontier Research Center funded by the U.S. DOE, Office of Science, BES, under award DE-SC0019443. J.Y. is supported by the US Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. K.W. and T.T. acknowledge support from the Elemental Strategy Initiative conducted by the MEXT, Japan (Grant Number JPMXP0112101001) and JSPS KAKENHI (Grant Numbers 19H05790, 20H00354 and 21H05233). C.Z. is supported by the Air Force Office of Scientific Research under Grant No. FA9550-20-1-0220 and the National Science Foundation under Grant No. PHY-2409943, OSI-2228725, ECCS-2411394. H.W. and L.Y. are supported by the National Science Foundation (NSF) grant No. DMR-2124934. The simulation used Anvil at Purdue University through allocation DMR100005 from the Advanced Cyberinfrastructure Coordination Ecosystem: Services & Support (ACCESS) program, which is supported by National Science Foundation grants #2138259, #2138286, #2138307, #2137603, and #2138296. E. H. acknowledges support by the Gordon and Betty Moore Foundation, grant https://doi.org/10.37807/gbmf11560. This work was mainly supported by the Wang Start-up funding, funded by the College of Arts & Sciences at Washington University in St. Louis (WUSTL). The fabrication is partially supported by Ralph E. Powe Junior Faculty Enhancement Awards, partially supported by the Gordon and Betty Moore Foundation, grant https://doi.org/10.37807/gbmf11560 . X.W. acknowledges equipment support by the Center for Quantum Leaps at WUSTL. X.W. acknowledges the use of the Cypher S atomic force microscope for high-resolution PFM characterization of the moiré superlattices. The fabrication used instruments in the Institute of Materials Science and Engineering (IMSE) at WUSTL, with partial financial support from IMSE. Bulk WSe crystals were grown and characterized by C.H., J.C., and J.Y. Materials synthesis by C.H. and J.C. was supported as part of Programmable Quantum Materials, an Energy Frontier Research Center funded by the U.S. DOE, Office of Science, BES, under award DE-SC0019443. J.Y. is supported by the US Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. K.W. and T.T. acknowledge support from the Elemental Strategy Initiative conducted by the MEXT, Japan (Grant Number JPMXP0112101001) and JSPS KAKENHI (Grant Numbers 19H05790, 20H00354 and 21H05233). C.Z. is supported by the Air Force Office of Scientific Research under Grant No. FA9550-20-1-0220 and the National Science Foundation under Grant No. PHY-2409943, OSI-2228725, ECCS-2411394. H.W. and L.Y. are supported by the National Science Foundation (NSF) grant No. DMR-2124934. The simulation used Anvil at Purdue University through allocation DMR100005 from the Advanced Cyberinfrastructure Coordination Ecosystem: Services & Support (ACCESS) program, which is supported by National Science Foundation grants #2138259, #2138286, #2138307, #2137603, and #2138296. E. H. acknowledges support by the Gordon and Betty Moore Foundation, grant https://doi.org/10.37807/gbmf11560 . 2