Reversible doping polarity and ultrahigh carrier density in two-dimensional van der Waals ferroelectric heterostructures

doi:10.1007/s11467-022-1244-4

Front. Phys.

2023, Vol. 18

Issue (3) : 33307 https://doi.org/10.1007/s11467-022-1244-4

RESEARCH ARTICLE

Reversible doping polarity and ultrahigh carrier density in two-dimensional van der Waals ferroelectric heterostructures

Yanyan Li¹, Mingjun Yang¹, Yanan Lu¹, Dan Cao², Xiaoshuang Chen³, Haibo Shu¹(

)

¹. College of Optical and Electronic Technology, China Jiliang University, Hangzhou 310018, China
². College of Science, China Jiliang University, Hangzhou 310018, China
³. National Laboratory for Infrared Physics, Shanghai Institute of Technical Physics, Chinese Academy of Science, Shanghai 200083, China

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Abstract

Van der Waals semiconductor heterostructures (VSHs) composed of two or more two-dimensional (2D) materials with different band gaps exhibit huge potential for exploiting high-performance multifunctional devices. The application of 2D VSHs in atomically thin devices highly depends on the control of their carrier type and density. Herein, on the basis of comprehensive first-principles calculations, we report a new strategy to manipulate the doping polarity and carrier density in a class of 2D VSHs consisting of atomically thin transition metal dichalcogenides (TMDs) and α-In₂X₃ (X = S, Se) ferroelectrics via switchable polarization field. Our calculated results indicate that the band bending of In₂X₃ layer driven by the FE polarization can be utilized for engineering the band alignment and doping polarity of TMD/In₂X₃ VSHs, which enables us to control their carrier density and type of the VSHs by the orientation and magnitude of local FE polarization field. Inspired by these findings, we demonstrate that doping-free p−n junctions achieved in MoTe₂/In₂Se₃ VSHs exhibit high carrier density (10¹³−10¹⁴ cm⁻²), and the inversion of the VHSs from n−p junctions to p−i−n junctions has been realized by the polarization switching from upward to downward states. This work provides a nonvolatile and nondestructive doping strategy for obtaining programmable p−n van der Waals (vdW) junctions and opens the possibilities for self-powered and multifunctional device applications.

Keywords van der Waals heterostructures ferroelectric polarization carrier type band alignment density-functional theory

Corresponding Author(s): Haibo Shu

Issue Date: 11 January 2023

Cite this article:

Yanyan Li,Mingjun Yang,Yanan Lu, et al. Reversible doping polarity and ultrahigh carrier density in two-dimensional van der Waals ferroelectric heterostructures[J]. Front. Phys. , 2023, 18(3): 33307.

URL:

https://academic.hep.com.cn/fop/EN/10.1007/s11467-022-1244-4
https://academic.hep.com.cn/fop/EN/Y2023/V18/I3/33307

Fig.1 Atomic structures and intrinsic polarization of 2D α-In₂X₃ ferroelectrics. (a) Top and side views of the atomic structure of trilayer In₂X₃ nanosheets in FE and PE phases. The arrows ↓ and ↑ denote the ferroelectric α-In₂X₃ nanosheet in P_down and P_up states, respectively. The rhombic frames represent the range of a unit cell. The blue and orange balls denote In and X atoms, respectively. (b) The average EPD (Φ) of a trilayer α-In₂Se₃ along the out-of-plane direction. Here ΔΦ denotes the electrostatic potential difference between two surface terminations. (c) The μ of 2D α-In₂X₃ ferroelectrics as a function of ΔΦ.

Fig.2 Polarization effect on electronic properties of 2D α-In₂X₃ nanosheets. (a) Projected band structure and DOS of a trilayer α-In₂Se₃ nanosheet obtained by the HSE06 functional. The Fermi level is set to the energy zero point. (b) Charge density isosurfaces of CBM and VBM states in the trilayer α-In₂Se₃ nanosheet. (c) Schematic of the polarization-induced layer-by-layer band shift in a trilayer α-In₂X₃ nanosheet. (d) Band-edge energies of eight 2D α-In₂X₃ structures relative to the vacuum level. E_C and E_V correspond to the energy of CBM and VBM, respectively. The arrows indicate the polarization direction.

Fig.3 Top and side views of the atomic structure of 2D MoTe₂/In₂Se₃ VSHs in P_down and P_up states. The solid frames denote the supercells of α-In₂Se₃ and MoTe₂ used for the construction of VSHs, and the dash frames denote the primitive cell of α-In₂Se₃ and MoTe₂. T-In₂Se₃ and B-In₂Se₃ denote the top-layer and bottom-layer In₂Se₃, respectively.

Fig.4 Band alignments of 2D MoTe₂/In₂Se₃(↑) VSHs with the thickness range of In₂Se₃ layer from 1L to 3L. (a?c) Projected band structure and DOS of VSH with (a) 1L-In₂Se₃, (b) 2L-In₂Se₃, and (c) 3L-In₂Se₃. The red and blue bands denote the contribution from In₂Se₃ and MoTe₂ layers, respectively. The horizontal dash lines denote the position of Fermi level. T-In₂Se₃, M-In₂Se₃, and B-In₂Se₃ represent the top-layer, middle-layer, and bottom-layer In₂Se₃ in the VSHs, respectively. (d) Schematic of band alignments of MoTe₂/In₂Se₃(↑) VSHs. The black and gray arrows denote the carrier transport direction and polarization direction, respectively.

Fig.5 Band alignments of 2D MoTe₂/In₂Se₃(↓) VSHs with the thickness range of In₂Se₃ layer from 1L to 3L. (a?c) Projected band structure and DOS of VSH with (a) 1L-In₂Se₃, (b) 2L-In₂Se₃, and (c) 3L-In₂Se₃. The red and blue bands represent the contribution of In₂Se₃ and MoTe₂ layers, respectively. The horizontal dash lines denote the position of Fermi level. T-In₂Se₃, M-In₂Se₃, and B-In₂Se₃ represent the top-layer, middle-layer, and bottom-layer In₂Se₃ in the VSHs, respectively. (d) Schematic of band alignments of MoTe₂/In₂Se₃(↓) VSHs. The arrows indicate the polarization direction.

Fig.6 Average electrostatic potential (Φ) and interfacial charge transfer of MoTe₂/In₂Se₃ VSHs. (a) Electrostatic potential distribution of MoTe₂/3L-In₂Se₃ VSH in P_up (red line) and P_down (blue line) states. (b) Electrostatic potential differences (ΔΦ) of MoTe₂/In₂Se₃ VSHs and isolated In₂Se₃ nanosheets as a function of In₂Se₃ layer thickness. (c) The charge-density difference and interfacial charge transfer (Q) of MoTe₂/3L-In₂Se₃ VSH in P_down (left) and P_up (right) state.

Fig.7 Polarization-dependent carrier density in 2D MoTe₂/In₂Se₃ VSHs. The σ_n (solid lines) and σ_p (dash lines) of MoTe₂/In₂Se₃ VSHs in (a) P_up state and (b) P_down state. The VSH-nL (n = 1?3) denote the MoTe₂/In₂Se₃ VSH with nL-In₂Se₃ layer. The spatial distribution of (c) σ_n and (d) σ_p in MoTe₂/3L-In₂Se₃ VSH along the FE switching pathway from the P_up state, PE phase, to P_down state.

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