Quadrupolar–dipolar excitonic transition in a tunnel-coupled van der Waals 
heterotrilayer

Li, W.; Hadjri, Z.; Devenica, L. M.; Zhang, J.; Liu, S.; Hone, J.; Watanabe, K.; Taniguchi, T.; Rubio, A.; Srivastava, A.

doi:10.1038/s41563-023-01667-1

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Journal Article

Quadrupolar–dipolar excitonic transition in a tunnel-coupled van der Waals heterotrilayer

MPS-Authors

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Zhang, J.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free-Electron Laser Science;

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Rubio, A.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free-Electron Laser Science;
Center for Computational Quantum Physics, Simons Foundation Flatiron Institute;
Nano-Bio Spectroscopy Group, Departamento de Fisica de Materiales, Universidad del Paìs Vasco;

External Resource

https://arxiv.org/abs/2208.05490
(Preprint)

https://doi.org/10.1038/s41563-023-01667-1
(Publisher version)

https://doi.org/10.1038/s41563-023-01741-8
(Supplementary material)

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2208.05490.pdf
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suppl.zip
(Supplementary material), 41MB

Citation

Li, W., Hadjri, Z., Devenica, L. M., Zhang, J., Liu, S., Hone, J., et al. (2023). Quadrupolar–dipolar excitonic transition in a tunnel-coupled van der Waals heterotrilayer. Nature Materials, 22(12), 1478-1484. doi:10.1038/s41563-023-01667-1.

Cite as: https://hdl.handle.net/21.11116/0000-000A-D878-C

Abstract

Strongly bound excitons determine light–matter interactions in van der Waals heterostructures of two-dimensional semiconductors. Unlike fundamental particles, quasiparticles in condensed matter, such as excitons, can be tailored to alter their interactions and realize emergent quantum phases. Here, using a WS₂/WSe₂/WS₂ heterotrilayer, we create a quantum superposition of oppositely oriented dipolar excitons—a quadrupolar exciton—wherein an electron is layer-hybridized in WS₂ layers while the hole localizes in WSe₂. In contrast to dipolar excitons, symmetric quadrupolar excitons only redshift in an out-of-plane electric field. At higher densities and a finite electric field, the nonlinear Stark shift of quadrupolar excitons becomes linear, signalling a transition to dipolar excitons resulting from exciton–exciton interactions, while at a vanishing electric field, the reduced exchange interaction suggests antiferroelectric correlations between dipolar excitons. Our results present van der Waals heterotrilayers as a field-tunable platform to engineer light–matter interactions and explore quantum phase transitions between spontaneously ordered many-exciton phases.