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Title: Layered Semiconductor Cr0.32Ga0.68Te2.33 with Concurrent Broken Inversion Symmetry and Ferromagnetism: A Bulk Ferrovalley Material Candidate

Abstract

The valleytronic state found in group-VI transition-metal dichalcogenides such as MoS2 has attracted immense interest since its valley degree of freedom could be used as an information carrier. However, valleytronic applications require spontaneous valley polarization. Such an electronic state is predicted to be accessible in a new ferroic family of materials, i.e., ferrovalley materials, which features the coexistence of spontaneous spin and valley polarization. Although many atomic monolayer materials with hexagonal lattices have been predicted to be ferrovalley materials, no bulk ferrovalley material candidates have been reported or proposed. Here, in this work, we show that a new non-centrosymmetric van der Waals (vdW) semiconductor Cr0.32Ga0.68Te2.33, with intrinsic ferromagnetism, is a possible candidate for bulk ferrovalley material. This material exhibits several remarkable characteristics: (i) it forms a natural heterostructure between vdW gaps, a quasi-two-dimensional (2D) semiconducting Te layer with a honeycomb lattice stacked on the 2D ferromagnetic slab comprised of the (Cr, Ga)-Te layers, and (ii) the 2D Te honeycomb lattice yields a valley-like electronic structure near the Fermi level, which, in combination with inversion symmetry breaking, ferromagnetism, and strong spin-orbit coupling contributed by heavy Te element, creates a possible bulk spin-valley locked electronic state with valley polarization as suggested bymore » our DFT calculations. Further, this material can also be easily exfoliated to 2D atomically thin layers. Therefore, this material offers a unique platform to explore the physics of valleytronic states with spontaneous spin and valley polarization in both bulk and 2D atomic crystals.« less

Authors:
ORCiD logo [1];  [1]; ORCiD logo [1];  [2];  [1];  [3]; ORCiD logo [2];  [1]; ORCiD logo [1]; ORCiD logo [4]; ORCiD logo [1]; ORCiD logo [4];  [1]
  1. Pennsylvania State Univ., University Park, PA (United States)
  2. Tulane Univ., New Orleans, LA (United States)
  3. Michigan State Univ., East Lansing, MI (United States)
  4. Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
OSTI Identifier:
2000321
Grant/Contract Number:  
AC05-00OR22725; SC0019068; SC0014208
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 145; Journal Issue: 8; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; crystal structure; layers; magnetic properties; polarization; two dimensional materials

Citation Formats

Guan, Yingdong, Miao, Leixin, He, Jingyang, Ning, Jinliang, Chen, Yangyang, Xie, Weiwei, Sun, Jianwei, Gopalan, Venkatraman, Zhu, Jun, Wang, Xiaoping, Alem, Nasim, Zhang, Qiang, and Mao, Zhiqiang. Layered Semiconductor Cr0.32Ga0.68Te2.33 with Concurrent Broken Inversion Symmetry and Ferromagnetism: A Bulk Ferrovalley Material Candidate. United States: N. p., 2023. Web. doi:10.1021/jacs.2c12848.
Guan, Yingdong, Miao, Leixin, He, Jingyang, Ning, Jinliang, Chen, Yangyang, Xie, Weiwei, Sun, Jianwei, Gopalan, Venkatraman, Zhu, Jun, Wang, Xiaoping, Alem, Nasim, Zhang, Qiang, & Mao, Zhiqiang. Layered Semiconductor Cr0.32Ga0.68Te2.33 with Concurrent Broken Inversion Symmetry and Ferromagnetism: A Bulk Ferrovalley Material Candidate. United States. https://doi.org/10.1021/jacs.2c12848
Guan, Yingdong, Miao, Leixin, He, Jingyang, Ning, Jinliang, Chen, Yangyang, Xie, Weiwei, Sun, Jianwei, Gopalan, Venkatraman, Zhu, Jun, Wang, Xiaoping, Alem, Nasim, Zhang, Qiang, and Mao, Zhiqiang. Thu . "Layered Semiconductor Cr0.32Ga0.68Te2.33 with Concurrent Broken Inversion Symmetry and Ferromagnetism: A Bulk Ferrovalley Material Candidate". United States. https://doi.org/10.1021/jacs.2c12848. https://www.osti.gov/servlets/purl/2000321.
@article{osti_2000321,
title = {Layered Semiconductor Cr0.32Ga0.68Te2.33 with Concurrent Broken Inversion Symmetry and Ferromagnetism: A Bulk Ferrovalley Material Candidate},
author = {Guan, Yingdong and Miao, Leixin and He, Jingyang and Ning, Jinliang and Chen, Yangyang and Xie, Weiwei and Sun, Jianwei and Gopalan, Venkatraman and Zhu, Jun and Wang, Xiaoping and Alem, Nasim and Zhang, Qiang and Mao, Zhiqiang},
abstractNote = {The valleytronic state found in group-VI transition-metal dichalcogenides such as MoS2 has attracted immense interest since its valley degree of freedom could be used as an information carrier. However, valleytronic applications require spontaneous valley polarization. Such an electronic state is predicted to be accessible in a new ferroic family of materials, i.e., ferrovalley materials, which features the coexistence of spontaneous spin and valley polarization. Although many atomic monolayer materials with hexagonal lattices have been predicted to be ferrovalley materials, no bulk ferrovalley material candidates have been reported or proposed. Here, in this work, we show that a new non-centrosymmetric van der Waals (vdW) semiconductor Cr0.32Ga0.68Te2.33, with intrinsic ferromagnetism, is a possible candidate for bulk ferrovalley material. This material exhibits several remarkable characteristics: (i) it forms a natural heterostructure between vdW gaps, a quasi-two-dimensional (2D) semiconducting Te layer with a honeycomb lattice stacked on the 2D ferromagnetic slab comprised of the (Cr, Ga)-Te layers, and (ii) the 2D Te honeycomb lattice yields a valley-like electronic structure near the Fermi level, which, in combination with inversion symmetry breaking, ferromagnetism, and strong spin-orbit coupling contributed by heavy Te element, creates a possible bulk spin-valley locked electronic state with valley polarization as suggested by our DFT calculations. Further, this material can also be easily exfoliated to 2D atomically thin layers. Therefore, this material offers a unique platform to explore the physics of valleytronic states with spontaneous spin and valley polarization in both bulk and 2D atomic crystals.},
doi = {10.1021/jacs.2c12848},
journal = {Journal of the American Chemical Society},
number = 8,
volume = 145,
place = {United States},
year = {Thu Feb 16 00:00:00 EST 2023},
month = {Thu Feb 16 00:00:00 EST 2023}
}

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