Proximity control of interlayer exciton-phonon hybridization in van der Waals heterostructures

Philipp Merkl, Chaw-Keong Yong (), Marlene Liebich, Isabella Hofmeister, Gunnar Berghäuser, Ermin Malic and Rupert Huber ()
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Philipp Merkl: University of Regensburg
Chaw-Keong Yong: University of Regensburg
Marlene Liebich: University of Regensburg
Isabella Hofmeister: University of Regensburg
Gunnar Berghäuser: Philipps-Universität Marburg
Ermin Malic: Philipps-Universität Marburg
Rupert Huber: University of Regensburg

Nature Communications, 2021, vol. 12, issue 1, 1-7

Abstract: Abstract Van der Waals stacking has provided unprecedented flexibility in shaping many-body interactions by controlling electronic quantum confinement and orbital overlap. Theory has predicted that also electron-phonon coupling critically influences the quantum ground state of low-dimensional systems. Here we introduce proximity-controlled strong-coupling between Coulomb correlations and lattice dynamics in neighbouring van der Waals materials, creating new electrically neutral hybrid eigenmodes. Specifically, we explore how the internal orbital 1s-2p transition of Coulomb-bound electron-hole pairs in monolayer tungsten diselenide resonantly hybridizes with lattice vibrations of a polar capping layer of gypsum, giving rise to exciton-phonon mixed eigenmodes, called excitonic Lyman polarons. Tuning orbital exciton resonances across the vibrational resonances, we observe distinct anticrossing and polarons with adjustable exciton and phonon compositions. Such proximity-induced hybridization can be further controlled by quantum designing the spatial wavefunction overlap of excitons and phonons, providing a promising new strategy to engineer novel ground states of two-dimensional systems.

Date: 2021
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DOI: 10.1038/s41467-021-21780-6

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