Coherent many-body exciton in van der Waals antiferromagnet NiPS3

Soonmin Kang, Kangwon Kim, Beom Hyun Kim, Jonghyeon Kim, Kyung Ik Sim, Jae-Ung Lee, Sungmin Lee, Kisoo Park, Seokhwan Yun, Taehun Kim, Abhishek Nag, Andrew Walters, Mirian Garcia-Fernandez, Jiemin Li, Laurent Chapon, Ke-Jin Zhou (), Young-Woo Son (), Jae Hoon Kim (), Hyeonsik Cheong () and Je-Geun Park ()
Additional contact information
Soonmin Kang: Institute for Basic Science
Kangwon Kim: Sogang University
Beom Hyun Kim: Korea Institute for Advanced Study
Jonghyeon Kim: Yonsei University
Kyung Ik Sim: Yonsei University
Jae-Ung Lee: Sogang University
Sungmin Lee: Institute for Basic Science
Kisoo Park: Institute for Basic Science
Seokhwan Yun: Institute for Basic Science
Taehun Kim: Institute for Basic Science
Abhishek Nag: Diamond Light Source
Andrew Walters: Diamond Light Source
Mirian Garcia-Fernandez: Diamond Light Source
Jiemin Li: Diamond Light Source
Laurent Chapon: Diamond Light Source
Ke-Jin Zhou: Diamond Light Source
Young-Woo Son: Korea Institute for Advanced Study
Jae Hoon Kim: Yonsei University
Hyeonsik Cheong: Sogang University
Je-Geun Park: Institute for Basic Science

Nature, 2020, vol. 583, issue 7818, 785-789

Abstract: Abstract An exciton is the bosonic quasiparticle of electron–hole pairs bound by the Coulomb interaction1. Bose–Einstein condensation of this exciton state has long been the subject of speculation in various model systems2,3, and examples have been found more recently in optical lattices and two-dimensional materials4–9. Unlike these conventional excitons formed from extended Bloch states4–9, excitonic bound states from intrinsically many-body localized states are rare. Here we show that a spin–orbit-entangled exciton state appears below the Néel temperature of 150 kelvin in NiPS3, an antiferromagnetic van der Waals material. It arises intrinsically from the archetypal many-body states of the Zhang–Rice singlet10,11, and reaches a coherent state assisted by the antiferromagnetic order. Using configuration-interaction theory, we determine the origin of the coherent excitonic excitation to be a transition from a Zhang–Rice triplet to a Zhang–Rice singlet. We combine three spectroscopic tools—resonant inelastic X-ray scattering, photoluminescence and optical absorption—to characterize the exciton and to demonstrate an extremely narrow excitonic linewidth below 50 kelvin. The discovery of the spin–orbit-entangled exciton in antiferromagnetic NiPS3 introduces van der Waals magnets as a platform to study coherent many-body excitons.

Date: 2020
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DOI: 10.1038/s41586-020-2520-5

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