Magnetically brightened dark electron-phonon bound states in a van der Waals antiferromagnet

Emre Ergeçen, Batyr Ilyas, Dan Mao, Hoi Chun Po, Mehmet Burak Yilmaz, Junghyun Kim, Je-Geun Park, T. Senthil and Nuh Gedik ()
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Emre Ergeçen: Massachusetts Institute of Technology
Batyr Ilyas: Massachusetts Institute of Technology
Dan Mao: Massachusetts Institute of Technology
Hoi Chun Po: Massachusetts Institute of Technology
Mehmet Burak Yilmaz: Massachusetts Institute of Technology
Junghyun Kim: Seoul National University
Je-Geun Park: Seoul National University
T. Senthil: Massachusetts Institute of Technology
Nuh Gedik: Massachusetts Institute of Technology

Nature Communications, 2022, vol. 13, issue 1, 1-7

Abstract: Abstract In van der Waals (vdW) materials, strong coupling between different degrees of freedom can hybridize elementary excitations into bound states with mixed character1–3. Correctly identifying the nature and composition of these bound states is key to understanding their ground state properties and excitation spectra4,5. Here, we use ultrafast spectroscopy to reveal bound states of d-orbitals and phonons in 2D vdW antiferromagnet NiPS3. These bound states manifest themselves through equally spaced phonon replicas in frequency domain. These states are optically dark above the Néel temperature and become accessible with magnetic order. By launching this phonon and spectrally tracking its amplitude, we establish the electronic origin of bound states as localized d–d excitations. Our data directly yield electron-phonon coupling strength which exceeds the highest known value in 2D systems6. These results demonstrate NiPS3 as a platform to study strong interactions between spins, orbitals and lattice, and open pathways to coherent control of 2D magnets.

Date: 2022
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DOI: 10.1038/s41467-021-27741-3

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