Ligand-field helical luminescence in a 2D ferromagnetic insulator

Seyler, Kyle L.; Zhong, Ding; Klein, Dahlia R.; Gao, Shiyuan; Zhang, Xiaoou; Huang, Bevin; Navarro-Moratalla, Efren; Yang, Li; Cobden, David H.; McGuire, Michael A.; Yao, Wang; Xiao, Di; Jarillo-Herrero, Pablo; Xu, Xiaodong

doi:10.1038/s41567-017-0006-7

Ligand-field helical luminescence in a 2D ferromagnetic insulator

Journal Article · Mon Dec 04 00:00:00 UTC 2017 · Nature Physics

DOI:https://doi.org/10.1038/s41567-017-0006-7· OSTI ID:1430601

Seyler, Kyle L. ^[1]; Zhong, Ding ^[1]; Klein, Dahlia R. ^[2]; Gao, Shiyuan ^[3]; Zhang, Xiaoou ^[4]; Huang, Bevin ^[1]; Navarro-Moratalla, Efren ^[2]; Yang, Li ^[3]; ^[1]; ^[5]; ^[6]; Xiao, Di ^[4]; Jarillo-Herrero, Pablo ^[2]; ^[7]

Univ. of Washington, Seattle, WA (United States). Dept. of Physics
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Physics
Washington Univ., St. Louis, MO (United States). Dept. of Physics
Carnegie Mellon Univ., Pittsburgh, PA (United States). Dept. of Physics
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
Univ. of Hong Kong (China). Dept. of Physics and Center of Theoretical and Computational Physics
Univ. of Washington, Seattle, WA (United States). Dept. of Physics, and Dept. of Materials Science and Engineering

Bulk chromium tri-iodide (CrI₃) has long been known as a layered van der Waals ferromagnet. However, its monolayer form was only recently isolated and confirmed to be a truly two-dimensional (2D) ferromagnet, providing a new platform for investigating light–matter interactions and magneto-optical phenomena in the atomically thin limit. Here in this paper, we report spontaneous circularly polarized photoluminescence in monolayer CrI₃ under linearly polarized excitation, with helicity determined by the monolayer magnetization direction. In contrast, the bilayer CrI₃ photoluminescence exhibits vanishing circular polarization, supporting the recently uncovered anomalous antiferromagnetic interlayer coupling in CrI₃ bilayers. Distinct from the Wannier–Mott excitons that dominate the optical response in well-known 2D van der Waals semiconductors, our absorption and layer-dependent photoluminescence measurements reveal the importance of ligand-field and charge-transfer transitions to the optoelectronic response of atomically thin CrI₃. We attribute the photoluminescence to a parity-forbidden d–d transition characteristic of Cr³⁺ complexes, which displays broad linewidth due to strong vibronic coupling and thickness-independent peak energy due to its localized molecular orbital nature.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Excitonics (CE); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1430601

Journal Information:: Nature Physics, Journal Name: Nature Physics Journal Issue: 3 Vol. 14; ISSN 1745-2473

Publisher:: Nature Publishing Group (NPG)Copyright Statement

Country of Publication:: United States

Language:: English

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