Merkl PYong C.-KLiebich MHofmeister IBergh?user GMalic EHuber R.CHAW-KEONG YONG2022-04-252022-04-25202120411723https://www.scopus.com/inward/record.uri?eid=2-s2.0-85102678854&doi=10.1038%2fs41467-021-21780-6&partnerID=40&md5=a85e6acf349f893f86541046cdb9ad7ahttps://scholars.lib.ntu.edu.tw/handle/123456789/606454Van 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. ? 2021, The Author(s).calcium sulfate; quantum dot; tungsten derivative; correlation; eigenvalue; electron; hybridization; lattice dynamics; spatial analysis; tungsten; Article; chemical structure; dynamics; electron; hybridization; phonon; photoluminescence; spectroscopy; vibration; waveformjournal article10.1038/s41467-021-21780-6337419062-s2.0-85102678854