Correlated excitonic signatures of individual van der Waals NiPS3 antiferromagnet nanoflakes

Vigneshwaran Chandrasekaran; Christopher R. DeLaney; Cong Tai Trinh; David Parobek; Christopher A. Lane; Jian Xin Zhu; Xiangzhi Li; Huan Zhao; Marshall A. Campbell; Laura Martin; Edward F. Wyckoff; Andrew C. Jones; Matthew M. Schneider; John Watt; Michael T. Pettes; Sergei A. Ivanov; Andrei Piryatinski; David H. Dunlap; Han Htoon

doi:10.1039/d4nh00390j

Correlated excitonic signatures of individual van der Waals NiPS₃ antiferromagnet nanoflakes

Vigneshwaran Chandrasekaran, Christopher R. DeLaney, Cong Tai Trinh, David Parobek, Christopher A. Lane, Jian Xin Zhu, Xiangzhi Li, Huan Zhao, Marshall A. Campbell, Laura Martin, Edward F. Wyckoff, Andrew C. Jones, Matthew M. Schneider, John Watt, Michael T. Pettes, Sergei A. Ivanov, Andrei Piryatinski, David H. Dunlap, Han Htoon

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

Abstract

Composite quasi-particles with emergent functionalities in spintronic and quantum information science can be realized in correlated materials due to entangled charge, spin, orbital, and lattice degrees of freedom. Here we show that by reducing the lateral dimension of correlated antiferromagnet NiPS₃ flakes to tens of nanometers and thickness to less than ten nanometers, we can switch-off the bulk spin-orbit entangled exciton in the near-infrared (1.47 eV) and activate visible-range (1.8-2.2 eV) transitions. These ultra-sharp lines (<120 μeV at 4.2 K) share the spin-correlated nature of the bulk exciton by displaying a strong linear polarization below Néel temperature. Furthermore, exciton photoluminescence lineshape analysis indicates a polaronic character via coupling with at-least 3 phonon modes and a comb-like Stark effect through discretization of charges in each layer. These findings augment the knowledge on the many-body nature of excitonic quasi-particles in correlated antiferromagnets and also establish the nanoscale correlated antiferromagnets as a promising platform for integrated magneto-optic devices.

Original language	English
Pages (from-to)	150-157
Number of pages	8
Journal	Nanoscale Horizons
Volume	10
Issue number	1
DOIs	https://doi.org/10.1039/d4nh00390j
State	Published - Oct 29 2024
Externally published	Yes

Funding

This work was performed at the Center for Integrated Nanotechnologies, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science (OS). Los Alamos National Laboratory (LANL), an affirmative action equal opportunity employer, is managed by Triad National Security, LLC for the U.S. Department of Energy's NNSA, under contract 89233218CNA000001. C. R. D., D. P., C. A. L., J.-X. Z., M. A. C., and A. P. acknowledge support for the works from Laboratory Directed Research and Development (LDRD) program 20200104DR. S. A. I., and C. T. T. are supported by LDRD 20220757ER. H. H., V. C., X. L., and H. Z. acknowledge partial support by Quantum Science Center, a National QIS Research Center supported by DOE, OS. M. T. P. acknowledges support from LDRD awards 20210782ER and 20210640ECR. A. C. J. is supported by DOE BES QIS program LANLE3QR.

Access to Document

10.1039/d4nh00390j

Cite this

Chandrasekaran, V., DeLaney, C. R., Trinh, C. T., Parobek, D., Lane, C. A., Zhu, J. X., Li, X., Zhao, H., Campbell, M. A., Martin, L., Wyckoff, E. F., Jones, A. C., Schneider, M. M., Watt, J., Pettes, M. T., Ivanov, S. A., Piryatinski, A., Dunlap, D. H., & Htoon, H. (2024). Correlated excitonic signatures of individual van der Waals NiPS₃ antiferromagnet nanoflakes. Nanoscale Horizons, 10(1), 150-157. https://doi.org/10.1039/d4nh00390j

@article{ab4524b6a93c41649aea82ce1a35fa74,

title = "Correlated excitonic signatures of individual van der Waals NiPS3 antiferromagnet nanoflakes",

abstract = "Composite quasi-particles with emergent functionalities in spintronic and quantum information science can be realized in correlated materials due to entangled charge, spin, orbital, and lattice degrees of freedom. Here we show that by reducing the lateral dimension of correlated antiferromagnet NiPS3 flakes to tens of nanometers and thickness to less than ten nanometers, we can switch-off the bulk spin-orbit entangled exciton in the near-infrared (1.47 eV) and activate visible-range (1.8-2.2 eV) transitions. These ultra-sharp lines (<120 μeV at 4.2 K) share the spin-correlated nature of the bulk exciton by displaying a strong linear polarization below N{\'e}el temperature. Furthermore, exciton photoluminescence lineshape analysis indicates a polaronic character via coupling with at-least 3 phonon modes and a comb-like Stark effect through discretization of charges in each layer. These findings augment the knowledge on the many-body nature of excitonic quasi-particles in correlated antiferromagnets and also establish the nanoscale correlated antiferromagnets as a promising platform for integrated magneto-optic devices.",

author = "Vigneshwaran Chandrasekaran and DeLaney, {Christopher R.} and Trinh, {Cong Tai} and David Parobek and Lane, {Christopher A.} and Zhu, {Jian Xin} and Xiangzhi Li and Huan Zhao and Campbell, {Marshall A.} and Laura Martin and Wyckoff, {Edward F.} and Jones, {Andrew C.} and Schneider, {Matthew M.} and John Watt and Pettes, {Michael T.} and Ivanov, {Sergei A.} and Andrei Piryatinski and Dunlap, {David H.} and Han Htoon",

note = "Publisher Copyright: {\textcopyright} 2025 The Royal Society of Chemistry.",

year = "2024",

month = oct,

day = "29",

doi = "10.1039/d4nh00390j",

language = "English",

volume = "10",

pages = "150--157",

journal = "Nanoscale Horizons",

issn = "2055-6756",

publisher = "Royal Society of Chemistry",

number = "1",

}

Chandrasekaran, V, DeLaney, CR, Trinh, CT, Parobek, D, Lane, CA, Zhu, JX, Li, X, Zhao, H, Campbell, MA, Martin, L, Wyckoff, EF, Jones, AC, Schneider, MM, Watt, J, Pettes, MT, Ivanov, SA, Piryatinski, A, Dunlap, DH & Htoon, H 2024, 'Correlated excitonic signatures of individual van der Waals NiPS₃ antiferromagnet nanoflakes', Nanoscale Horizons, vol. 10, no. 1, pp. 150-157. https://doi.org/10.1039/d4nh00390j

TY - JOUR

T1 - Correlated excitonic signatures of individual van der Waals NiPS3 antiferromagnet nanoflakes

AU - Chandrasekaran, Vigneshwaran

AU - DeLaney, Christopher R.

AU - Trinh, Cong Tai

AU - Parobek, David

AU - Lane, Christopher A.

AU - Zhu, Jian Xin

AU - Li, Xiangzhi

AU - Zhao, Huan

AU - Campbell, Marshall A.

AU - Martin, Laura

AU - Wyckoff, Edward F.

AU - Jones, Andrew C.

AU - Schneider, Matthew M.

AU - Watt, John

AU - Pettes, Michael T.

AU - Ivanov, Sergei A.

AU - Piryatinski, Andrei

AU - Dunlap, David H.

AU - Htoon, Han

PY - 2024/10/29

Y1 - 2024/10/29

N2 - Composite quasi-particles with emergent functionalities in spintronic and quantum information science can be realized in correlated materials due to entangled charge, spin, orbital, and lattice degrees of freedom. Here we show that by reducing the lateral dimension of correlated antiferromagnet NiPS3 flakes to tens of nanometers and thickness to less than ten nanometers, we can switch-off the bulk spin-orbit entangled exciton in the near-infrared (1.47 eV) and activate visible-range (1.8-2.2 eV) transitions. These ultra-sharp lines (<120 μeV at 4.2 K) share the spin-correlated nature of the bulk exciton by displaying a strong linear polarization below Néel temperature. Furthermore, exciton photoluminescence lineshape analysis indicates a polaronic character via coupling with at-least 3 phonon modes and a comb-like Stark effect through discretization of charges in each layer. These findings augment the knowledge on the many-body nature of excitonic quasi-particles in correlated antiferromagnets and also establish the nanoscale correlated antiferromagnets as a promising platform for integrated magneto-optic devices.

AB - Composite quasi-particles with emergent functionalities in spintronic and quantum information science can be realized in correlated materials due to entangled charge, spin, orbital, and lattice degrees of freedom. Here we show that by reducing the lateral dimension of correlated antiferromagnet NiPS3 flakes to tens of nanometers and thickness to less than ten nanometers, we can switch-off the bulk spin-orbit entangled exciton in the near-infrared (1.47 eV) and activate visible-range (1.8-2.2 eV) transitions. These ultra-sharp lines (<120 μeV at 4.2 K) share the spin-correlated nature of the bulk exciton by displaying a strong linear polarization below Néel temperature. Furthermore, exciton photoluminescence lineshape analysis indicates a polaronic character via coupling with at-least 3 phonon modes and a comb-like Stark effect through discretization of charges in each layer. These findings augment the knowledge on the many-body nature of excitonic quasi-particles in correlated antiferromagnets and also establish the nanoscale correlated antiferromagnets as a promising platform for integrated magneto-optic devices.

UR - http://www.scopus.com/inward/record.url?scp=85209575790&partnerID=8YFLogxK

U2 - 10.1039/d4nh00390j

DO - 10.1039/d4nh00390j

M3 - Article

AN - SCOPUS:85209575790

SN - 2055-6756

VL - 10

SP - 150

EP - 157

JO - Nanoscale Horizons

JF - Nanoscale Horizons

IS - 1

ER -

Correlated excitonic signatures of individual van der Waals NiPS₃ antiferromagnet nanoflakes

Abstract

Funding

Access to Document

Other files and links

Fingerprint

Cite this