Growth of bilayer MoTe2 single crystals with strong non-linear Hall effect

Teng Ma, Hao Chen, Kunihiro Yananose, Xin Zhou, Lin Wang, Runlai Li, Ziyu Zhu, Zhenyue Wu, Qing-Hua Xu, Jaejun Yu, Cheng Wei Qiu, Alessandro Stroppa () and Kian Ping Loh ()
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Teng Ma: National University of Singapore
Hao Chen: National University of Singapore
Kunihiro Yananose: Seoul National University
Xin Zhou: National University of Singapore
Lin Wang: National University of Singapore
Runlai Li: National University of Singapore
Ziyu Zhu: National University of Singapore
Zhenyue Wu: National University of Singapore
Qing-Hua Xu: National University of Singapore
Jaejun Yu: Seoul National University
Cheng Wei Qiu: National University of Singapore
Alessandro Stroppa: University of L’Aquila
Kian Ping Loh: National University of Singapore

Nature Communications, 2022, vol. 13, issue 1, 1-10

Abstract: Abstract The reduced symmetry in strong spin-orbit coupling materials such as transition metal ditellurides (TMDTs) gives rise to non-trivial topology, unique spin texture, and large charge-to-spin conversion efficiencies. Bilayer TMDTs are non-centrosymmetric and have unique topological properties compared to monolayer or trilayer, but a controllable way to prepare bilayer MoTe2 crystal has not been achieved to date. Herein, we achieve the layer-by-layer growth of large-area bilayer and trilayer 1T′ MoTe2 single crystals and centimetre-scale films by a two-stage chemical vapor deposition process. The as-grown bilayer MoTe2 shows out-of-plane ferroelectric polarization, whereas the monolayer and trilayer crystals are non-polar. In addition, we observed large in-plane nonlinear Hall (NLH) effect for the bilayer and trilayer Td phase MoTe2 under time reversal-symmetric conditions, while these vanish for thicker layers. For a fixed input current, bilayer Td MoTe2 produces the largest second harmonic output voltage among the thicker crystals tested. Our work therefore highlights the importance of thickness-dependent Berry curvature effects in TMDTs that are underscored by the ability to grow thickness-precise layers.

Date: 2022
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DOI: 10.1038/s41467-022-33201-3

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