Atomic-scale visualization of the interlayer Rydberg exciton complex in moiré heterostructures

Meng Zhao, Zhongjie Wang (), Lu Liu, Chunzheng Wang, Cheng-Yen Liu, Fang Yang, Hua Wu () and Chunlei Gao ()
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Meng Zhao: Fudan University
Zhongjie Wang: Fudan University
Lu Liu: Fudan University
Chunzheng Wang: Fudan University
Cheng-Yen Liu: Fudan University
Fang Yang: Fudan University
Hua Wu: Fudan University
Chunlei Gao: Fudan University

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract Excitonic systems, facilitated by optical pumping, electrostatic gating or magnetic field, sustain composite particles with fascinating physics. Although various intriguing excitonic phases have been revealed via global measurements, the atomic-scale accessibility towards excitons has yet to be established. Here, we realize the ground-state interlayer exciton complexes through the intrinsic charge transfer in monolayer YbCl3/graphite heterostructure. Combining scanning tunneling microscope and theoretical calculations, the excitonic in-gap states are directly profiled. The out-of-plane excitonic charge clouds exhibit oscillating Rydberg nodal structure, while their in-plane arrangements are determined by moiré periodicity. Exploiting the tunneling probe to reflect the shape of charge clouds, we reveal the principal quantum number hierarchy of Rydberg series, which points to an excitonic energy-level configuration with unusually large binding energy. Our results demonstrate the feasibility of mapping out the charge clouds of excitons microscopically and pave a brand-new way to directly investigate the nanoscale order of exotic correlated phases.

Date: 2024
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DOI: 10.1038/s41467-024-47770-y

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