Enhanced Direct Exchange Interaction and Hybridization by Single-Atom Linkers for High Curie Temperature and Superior Visible-Light Harvesting in Cr3(CN3)2

Xiaofeng Liu; Haidi Wang; Zhao Chen; Weiduo Zhu; Zhongjun Li; Wei Hu; Haixiao Xiao; Xiao Cheng Zeng

doi:10.1021/acs.nanolett.3c03044

Enhanced Direct Exchange Interaction and Hybridization by Single-Atom Linkers for High Curie Temperature and Superior Visible-Light Harvesting in Cr₃(CN₃)₂

Xiaofeng Liu, Haidi Wang, Zhao Chen, Weiduo Zhu, Zhongjun Li^*, Wei Hu^*, Haixiao Xiao, Xiao Cheng Zeng^*

^*Corresponding author for this work

Department of Materials Science and Engineering

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

6 Citations (Scopus)

Abstract

Designing two-dimensional (2D) ferromagnetic (FM) semiconductors with elevated Curie temperature, high carrier mobility, and strong light harvesting is challenging but crucial to the development of spintronics with multifunctionalities. Herein, we show first-principles computation evidence of the 2D metal-organic framework Kagome ferromagnet Cr₃(CN₃)₂. Monolayer Cr₃(CN₃)₂ is predicted to be an FM semiconductor with a record-high Curie temperature of 943 K owing to the use of a single-atom linker (N), which results in strong direct d-p exchange interaction and hybridization between d_yz/xz and p_z of Cr and N, as well as excellent matching characteristics in energy and symmetry. The single-atom linker structural feature also leads to notable band dispersion and a relatively high carrier mobility of 420 cm² V^-1 s^-1. Moreover, under the in-plane strain, 2D Cr₃(CN₃)₂ can be tuned to possess a strong visible-light-harvesting functionality. These novel properties render monolayer Cr₃(CN₃)₂ a distinct 2D ferromagnet with high potential for the development of multifunctional spintronics. © 2023 American Chemical Society

Original language	English
Pages (from-to)	35-42
Number of pages	8
Journal	Nano Letters
Volume	24
Issue number	1
Online published	20 Dec 2023
DOIs	https://doi.org/10.1021/acs.nanolett.3c03044
Publication status	Published - 10 Jan 2024

Funding

Z. Li, W.H., and H.W. were financially supported by the National Key R&D Program of China (2022YFA1602601, 2022YFA1602600, 2016YFA0200604 and 2021YFB0300600), the National Natural Science Foundation of China (Grant Nos. 12174080, 22173093, 22103020, 22203026, and 22288201), the Anhui Provincial Key Research and Development Program (2022a05020052), the Program of State Key Laboratory of Quantum Optics and Quantum Optics Devices (Grant No. KF202005), the Network Information Project of Chinese Academy of Sciences (CASWX2021SF-0103), the Hefei National Laboratory for Physical Sciences at the Microscale (KF2020003), the Chinese Academy of Sciences Pioneer Hundred Talents Program (KJ2340000031), the Fundamental Research Funds for Central Universities (JZ2022HGTA0313 and JZ2022HGQA0198), the HPC Platform of Hefei University of Technology, the National Supercomputing Center in Wuxi, the Supercomputing Center of Chinese Academy of Sciences, the Supercomputing Center of USTC, and Tianjin, Shanghai, and Guangzhou Supercomputing Centers for the computational resources. X.C.Z. acknowledges support from the Hong Kong Global STEM Professorship Scheme.

Research Keywords

carrier mobility
Curie temperature
direct d−p exchange interaction
light harvesting
two-dimensional ferromagnetic semiconductor

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title = "Enhanced Direct Exchange Interaction and Hybridization by Single-Atom Linkers for High Curie Temperature and Superior Visible-Light Harvesting in Cr3(CN3)2",

abstract = "Designing two-dimensional (2D) ferromagnetic (FM) semiconductors with elevated Curie temperature, high carrier mobility, and strong light harvesting is challenging but crucial to the development of spintronics with multifunctionalities. Herein, we show first-principles computation evidence of the 2D metal-organic framework Kagome ferromagnet Cr3(CN3)2. Monolayer Cr3(CN3)2 is predicted to be an FM semiconductor with a record-high Curie temperature of 943 K owing to the use of a single-atom linker (N), which results in strong direct d-p exchange interaction and hybridization between dyz/xz and pz of Cr and N, as well as excellent matching characteristics in energy and symmetry. The single-atom linker structural feature also leads to notable band dispersion and a relatively high carrier mobility of 420 cm2 V-1 s-1. Moreover, under the in-plane strain, 2D Cr3(CN3)2 can be tuned to possess a strong visible-light-harvesting functionality. These novel properties render monolayer Cr3(CN3)2 a distinct 2D ferromagnet with high potential for the development of multifunctional spintronics. {\textcopyright} 2023 American Chemical Society",

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author = "Xiaofeng Liu and Haidi Wang and Zhao Chen and Weiduo Zhu and Zhongjun Li and Wei Hu and Haixiao Xiao and Zeng, {Xiao Cheng}",

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Enhanced Direct Exchange Interaction and Hybridization by Single-Atom Linkers for High Curie Temperature and Superior Visible-Light Harvesting in Cr₃(CN₃)₂. / Liu, Xiaofeng; Wang, Haidi; Chen, Zhao et al.
In: Nano Letters, Vol. 24, No. 1, 10.01.2024, p. 35-42.

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

TY - JOUR

T1 - Enhanced Direct Exchange Interaction and Hybridization by Single-Atom Linkers for High Curie Temperature and Superior Visible-Light Harvesting in Cr3(CN3)2

AU - Liu, Xiaofeng

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AU - Chen, Zhao

AU - Zhu, Weiduo

AU - Li, Zhongjun

AU - Hu, Wei

AU - Xiao, Haixiao

AU - Zeng, Xiao Cheng

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Y1 - 2024/1/10

N2 - Designing two-dimensional (2D) ferromagnetic (FM) semiconductors with elevated Curie temperature, high carrier mobility, and strong light harvesting is challenging but crucial to the development of spintronics with multifunctionalities. Herein, we show first-principles computation evidence of the 2D metal-organic framework Kagome ferromagnet Cr3(CN3)2. Monolayer Cr3(CN3)2 is predicted to be an FM semiconductor with a record-high Curie temperature of 943 K owing to the use of a single-atom linker (N), which results in strong direct d-p exchange interaction and hybridization between dyz/xz and pz of Cr and N, as well as excellent matching characteristics in energy and symmetry. The single-atom linker structural feature also leads to notable band dispersion and a relatively high carrier mobility of 420 cm2 V-1 s-1. Moreover, under the in-plane strain, 2D Cr3(CN3)2 can be tuned to possess a strong visible-light-harvesting functionality. These novel properties render monolayer Cr3(CN3)2 a distinct 2D ferromagnet with high potential for the development of multifunctional spintronics. © 2023 American Chemical Society

AB - Designing two-dimensional (2D) ferromagnetic (FM) semiconductors with elevated Curie temperature, high carrier mobility, and strong light harvesting is challenging but crucial to the development of spintronics with multifunctionalities. Herein, we show first-principles computation evidence of the 2D metal-organic framework Kagome ferromagnet Cr3(CN3)2. Monolayer Cr3(CN3)2 is predicted to be an FM semiconductor with a record-high Curie temperature of 943 K owing to the use of a single-atom linker (N), which results in strong direct d-p exchange interaction and hybridization between dyz/xz and pz of Cr and N, as well as excellent matching characteristics in energy and symmetry. The single-atom linker structural feature also leads to notable band dispersion and a relatively high carrier mobility of 420 cm2 V-1 s-1. Moreover, under the in-plane strain, 2D Cr3(CN3)2 can be tuned to possess a strong visible-light-harvesting functionality. These novel properties render monolayer Cr3(CN3)2 a distinct 2D ferromagnet with high potential for the development of multifunctional spintronics. © 2023 American Chemical Society

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