Journal
NATURE NANOTECHNOLOGY
Volume 15, Issue 9, Pages 750-+Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41565-020-0728-z
Keywords
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Funding
- DoD Vannevar Bush Faculty Fellowship [N00014-16-1-2825, N00014-18-1-2877]
- NSF [PHY-1506284]
- NSF CUA [PHY-1125846]
- AFOSR MURI [FA9550-17-1-0002]
- ARL [W911NF1520067]
- Gordon and Betty Moore Foundation [GBMF4543]
- ONR MURI [N00014-15-1-2761]
- EPSRC [EP/S019367/1, EP/S030719/1, EP/N010345/1]
- ERC Synergy Grant Hetero2D, Lloyd's Register Foundation Nanotechnology Grant
- European Graphene Flagship Project
- European Quantum Technologies Project 2D-SIPC
- Elemental Strategy Initiative by the MEXT, Japan and the CREST, JST [JPMJCR15F3]
- Summer Undergraduate Research Fellowship at Caltech
- Samsung Electronics
- EPSRC [EP/N010345/1, EP/S030719/1, EP/K005014/1] Funding Source: UKRI
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Domain-resolved spectroscopy reveals the impact of local atomic registry and crystal symmetry on the exciton properties of individual domains in near-0 degrees-twist-angle MoSe2/MoSe2. Van der Waals heterostructures obtained via stacking and twisting have been used to create moire superlattices(1), enabling new optical and electronic properties in solid-state systems. Moire lattices in twisted bilayers of transition metal dichalcogenides (TMDs) result in exciton trapping(2-5), host Mott insulating and superconducting states(6)and act as unique Hubbard systems(7-9)whose correlated electronic states can be detected and manipulated optically. Structurally, these twisted heterostructures feature atomic reconstruction and domain formation(10-14). However, due to the nanoscale size of moire domains, the effects of atomic reconstruction on the electronic and excitonic properties have not been systematically investigated. Here we use near-0 degrees-twist-angle MoSe2/MoSe(2)bilayers with large rhombohedral AB/BA domains(15)to directly probe the excitonic properties of individual domains with far-field optics. We show that this system features broken mirror/inversion symmetry, with the AB and BA domains supporting interlayer excitons with out-of-plane electric dipole moments in opposite directions. The dipole orientation of ground-state Gamma-K interlayer excitons can be flipped with electric fields, while higher-energy K-K interlayer excitons undergo field-asymmetric hybridization with intralayer K-K excitons. Our study reveals the impact of crystal symmetry on TMD excitons and points to new avenues for realizing topologically non-trivial systems(16,17), exotic metasurfaces(18), collective excitonic phases(19)and quantum emitter arrays(20,21)via domain-pattern engineering.
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