Multiferroic-Enabled Magnetic-Excitons in 2D Quantum-Entangled Van der Waals Antiferromagnet NiI2

Suhan Son; Youjin Lee; Jae Ha Kim; Beom Hyun Kim; Chaebin Kim; Woongki Na; Hwiin Ju; Sudong Park; Abhishek Nag; Ke Jin Zhou; Young Woo Son; Hyeongdo Kim; Woo Suk Noh; Jae Hoon Park; Jong Seok Lee; Hyeonsik Cheong; Jae Hoon Kim; Je Geun Park

doi:10.1002/adma.202109144

Multiferroic-Enabled Magnetic-Excitons in 2D Quantum-Entangled Van der Waals Antiferromagnet NiI₂

Suhan Son, Youjin Lee, Jae Ha Kim, Beom Hyun Kim, Chaebin Kim, Woongki Na, Hwiin Ju, Sudong Park, Abhishek Nag, Ke Jin Zhou, Young Woo Son, Hyeongdo Kim, Woo Suk Noh, Jae Hoon Park, Jong Seok Lee, Hyeonsik Cheong, Jae Hoon Kim, Je Geun Park

Department of Physics

Research output: Contribution to journal › Article › peer-review

3 Citations (Scopus)

Abstract

Matter–light interaction is at the center of diverse research fields from quantum optics to condensed matter physics, opening new fields like laser physics. A magnetic exciton is one such rare example found in magnetic insulators. However, it is relatively rare to observe that external variables control matter-light interaction. Here, it is reported that the broken inversion symmetry of multiferroicity can act as an external knob enabling magnetic excitons in the van der Waals antiferromagnet NiI₂. It is further discovered that this magnetic exciton arises from a transition between Zhang–Rice-triplet and Zhang–Rice-singlet fundamentally quantum-entangled states. This quantum entanglement produces an ultrasharp optical exciton peak at 1.384 eV with a 5 meV linewidth. The work demonstrates that NiI₂ is 2D magnetically ordered with an intrinsically quantum-entangled ground state.

Original language	English
Article number	2109144
Journal	Advanced Materials
Volume	34
Issue number	10
DOIs	https://doi.org/10.1002/adma.202109144
Publication status	Published - 2022 Mar 10

Bibliographical note

Funding Information:
S.S., Y.L., Jae Ha Kim, and B.H.K. contributed equally to this work. The authors acknowledge the helpful discussion with Ki‐Hoon Lee. Work at CQM and SNU was supported by the Leading Researcher Program of the National Research Foundation of Korea (Grant No. 2020R1A3B2079375). Work at Yonsei University was supported by National Research Foundation (NRF) grants funded by the Korean government (MSIT; grant 2021R1A2C3004989) and the SRC program (vdWMRC; grant 2017R1A5A1014862). Work at Sogang Univ. was supported by the National Research Foundation (NRF) grant funded by the Korean government (MSIT) (2019R1A2C3006189; 2017R1A5A1014862, SRC program: vdWMRC center). B.H.K. and Y.W.S. at KIAS were supported by KIAS Individual Grants (CG068702), and numerical computations have been performed with the Center for Advanced Computation Linux Cluster System at KIAS. The work at POSTECH and MPK was supported by the National Research Foundation of Korea (NRF), funded by the Ministry of Science and ICT (Grant No. 2016K1A4A4A01922028 and No. 2020M3H4A2084417). The work at GIST was supported by the Ministry of Science, ICT, and Future Planning (Nos. 2015R1A5A1009962, 2018R1A2B2005331). The authors acknowledge Diamond Light Source for time on beamline I21.

Publisher Copyright:
© 2022 Wiley-VCH GmbH

All Science Journal Classification (ASJC) codes

Materials Science(all)
Mechanics of Materials
Mechanical Engineering

Access to Document

10.1002/adma.202109144

Cite this

Son, S., Lee, Y., Kim, J. H., Kim, B. H., Kim, C., Na, W., Ju, H., Park, S., Nag, A., Zhou, K. J., Son, Y. W., Kim, H., Noh, W. S., Park, J. H., Lee, J. S., Cheong, H., Kim, J. H., & Park, J. G. (2022). Multiferroic-Enabled Magnetic-Excitons in 2D Quantum-Entangled Van der Waals Antiferromagnet NiI₂. Advanced Materials, 34(10), [2109144]. https://doi.org/10.1002/adma.202109144

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title = "Multiferroic-Enabled Magnetic-Excitons in 2D Quantum-Entangled Van der Waals Antiferromagnet NiI2",

abstract = "Matter–light interaction is at the center of diverse research fields from quantum optics to condensed matter physics, opening new fields like laser physics. A magnetic exciton is one such rare example found in magnetic insulators. However, it is relatively rare to observe that external variables control matter-light interaction. Here, it is reported that the broken inversion symmetry of multiferroicity can act as an external knob enabling magnetic excitons in the van der Waals antiferromagnet NiI2. It is further discovered that this magnetic exciton arises from a transition between Zhang–Rice-triplet and Zhang–Rice-singlet fundamentally quantum-entangled states. This quantum entanglement produces an ultrasharp optical exciton peak at 1.384 eV with a 5 meV linewidth. The work demonstrates that NiI2 is 2D magnetically ordered with an intrinsically quantum-entangled ground state.",

author = "Suhan Son and Youjin Lee and Kim, {Jae Ha} and Kim, {Beom Hyun} and Chaebin Kim and Woongki Na and Hwiin Ju and Sudong Park and Abhishek Nag and Zhou, {Ke Jin} and Son, {Young Woo} and Hyeongdo Kim and Noh, {Woo Suk} and Park, {Jae Hoon} and Lee, {Jong Seok} and Hyeonsik Cheong and Kim, {Jae Hoon} and Park, {Je Geun}",

note = "Funding Information: S.S., Y.L., Jae Ha Kim, and B.H.K. contributed equally to this work. The authors acknowledge the helpful discussion with Ki‐Hoon Lee. Work at CQM and SNU was supported by the Leading Researcher Program of the National Research Foundation of Korea (Grant No. 2020R1A3B2079375). Work at Yonsei University was supported by National Research Foundation (NRF) grants funded by the Korean government (MSIT; grant 2021R1A2C3004989) and the SRC program (vdWMRC; grant 2017R1A5A1014862). Work at Sogang Univ. was supported by the National Research Foundation (NRF) grant funded by the Korean government (MSIT) (2019R1A2C3006189; 2017R1A5A1014862, SRC program: vdWMRC center). B.H.K. and Y.W.S. at KIAS were supported by KIAS Individual Grants (CG068702), and numerical computations have been performed with the Center for Advanced Computation Linux Cluster System at KIAS. The work at POSTECH and MPK was supported by the National Research Foundation of Korea (NRF), funded by the Ministry of Science and ICT (Grant No. 2016K1A4A4A01922028 and No. 2020M3H4A2084417). The work at GIST was supported by the Ministry of Science, ICT, and Future Planning (Nos. 2015R1A5A1009962, 2018R1A2B2005331). The authors acknowledge Diamond Light Source for time on beamline I21. Publisher Copyright: {\textcopyright} 2022 Wiley-VCH GmbH",

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AU - Son, Suhan

AU - Lee, Youjin

AU - Kim, Jae Ha

AU - Kim, Beom Hyun

AU - Kim, Chaebin

AU - Na, Woongki

AU - Ju, Hwiin

AU - Park, Sudong

AU - Nag, Abhishek

AU - Zhou, Ke Jin

AU - Son, Young Woo

AU - Kim, Hyeongdo

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AU - Park, Jae Hoon

AU - Lee, Jong Seok

AU - Cheong, Hyeonsik

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AU - Park, Je Geun

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N2 - Matter–light interaction is at the center of diverse research fields from quantum optics to condensed matter physics, opening new fields like laser physics. A magnetic exciton is one such rare example found in magnetic insulators. However, it is relatively rare to observe that external variables control matter-light interaction. Here, it is reported that the broken inversion symmetry of multiferroicity can act as an external knob enabling magnetic excitons in the van der Waals antiferromagnet NiI2. It is further discovered that this magnetic exciton arises from a transition between Zhang–Rice-triplet and Zhang–Rice-singlet fundamentally quantum-entangled states. This quantum entanglement produces an ultrasharp optical exciton peak at 1.384 eV with a 5 meV linewidth. The work demonstrates that NiI2 is 2D magnetically ordered with an intrinsically quantum-entangled ground state.

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