Engineering Nonvolatile Polarization in 2D α-InSe/α-GaSe Ferroelectric Junctions

Overview

Journal Nanomaterials (Basel)

Date 2025 Feb 13

PMID 39940138

Authors

Peipei Li

Delin Kong

Jin Yang

Shuyu Cui

Qi Chen

Yue Liu

Ziheng He

Feng Liu

Yingying Xu

Huiyun Wei

Xinhe Zheng

Mingzeng Peng

Affiliations

Soon will be listed here.

Abstract

The advent of two-dimensional (2D) ferroelectrics offers a new paradigm for device miniaturization and multifunctionality. Recently, 2D α-InSe and related III-VI compound ferroelectrics manifest room-temperature ferroelectricity and exhibit reversible spontaneous polarization even at the monolayer limit. Here, we employ first-principles calculations to investigate group-III selenide van der Waals (vdW) heterojunctions built up by 2D α-InSe and α-GaSe ferroelectric (FE) semiconductors, including structural stability, electrostatic potential, interfacial charge transfer, and electronic band structures. When the FE polarization directions of α-InSe and α-GaSe are parallel, both the α-InSe/α-GaSe P↑↑ (UU) and α-InSe/α-GaSe P↓↓ (NN) configurations possess strong built-in electric fields and hence induce electron-hole separation, resulting in carrier depletion at the α-InSe/α-GaSe heterointerfaces. Conversely, when they are antiparallel, the α-InSe/α-GaSe P↓↑ (NU) and α-InSe/α-GaSe P↑↓ (UN) configurations demonstrate the switchable electron and hole accumulation at the 2D ferroelectric interfaces, respectively. The nonvolatile characteristic of ferroelectric polarization presents an innovative approach to achieving tunable n-type and p-type conductive channels for ferroelectric field-effect transistors (FeFETs). In addition, in-plane biaxial strain modulation has successfully modulated the band alignments of the α-InSe/α-GaSe ferroelectric heterostructures, inducing a type III-II-III transition in UU and NN, and a type I-II-I transition in UN and NU, respectively. Our findings highlight the great potential of 2D group-III selenides and ferroelectric vdW heterostructures to harness nonvolatile spontaneous polarization for next-generation electronics, nonvolatile optoelectronic memories, sensors, and neuromorphic computing.

References

Xue F, Zhang J, Hu W, Hsu W, Han A, Leung S . Multidirection Piezoelectricity in Mono- and Multilayered Hexagonal α-InSe. ACS Nano. 2018; 12(5):4976-4983. DOI: 10.1021/acsnano.8b02152. View

Si M, Liao P, Qiu G, Duan Y, Ye P . Ferroelectric Field-Effect Transistors Based on MoS and CuInPS Two-Dimensional van der Waals Heterostructure. ACS Nano. 2018; 12(7):6700-6705. DOI: 10.1021/acsnano.8b01810. View

Fong D, Stephenson G, Streiffer S, Eastman J, Auciello O, Fuoss P . Ferroelectricity in ultrathin perovskite films. Science. 2004; 304(5677):1650-3. DOI: 10.1126/science.1098252. View

Zhou Y, Wu D, Zhu Y, Cho Y, He Q, Yang X . Out-of-Plane Piezoelectricity and Ferroelectricity in Layered α-InSe Nanoflakes. Nano Lett. 2017; 17(9):5508-5513. DOI: 10.1021/acs.nanolett.7b02198. View

Meng S, Wang J, Shi H, Sun X, Gao B . Distinct ultrafast carrier dynamics of α-InSe and β-InSe: contributions from band filling and bandgap renormalization. Phys Chem Chem Phys. 2021; 23(42):24313-24318. DOI: 10.1039/d1cp03874e. View

Sun J, Remsing R, Zhang Y, Sun Z, Ruzsinszky A, Peng H . Accurate first-principles structures and energies of diversely bonded systems from an efficient density functional. Nat Chem. 2016; 8(9):831-6. DOI: 10.1038/nchem.2535. View

Buda I, Lane C, Barbiellini B, Ruzsinszky A, Sun J, Bansil A . Characterization of Thin Film Materials using SCAN meta-GGA, an Accurate Nonempirical Density Functional. Sci Rep. 2017; 7:44766. PMC: 5363068. DOI: 10.1038/srep44766. View

Grimme S, Antony J, Ehrlich S, Krieg H . A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu. J Chem Phys. 2010; 132(15):154104. DOI: 10.1063/1.3382344. View

Han G, Chen Z, Drennan J, Zou J . Indium selenides: structural characteristics, synthesis and their thermoelectric performances. Small. 2014; 10(14):2747-65. DOI: 10.1002/smll.201400104. View

10.

Borlido P, Aull T, Huran A, Tran F, Marques M, Botti S . Large-Scale Benchmark of Exchange-Correlation Functionals for the Determination of Electronic Band Gaps of Solids. J Chem Theory Comput. 2019; 15(9):5069-5079. PMC: 6739738. DOI: 10.1021/acs.jctc.9b00322. View

11.

Nukala P, Ahmadi M, Wei Y, de Graaf S, Stylianidis E, Chakrabortty T . Reversible oxygen migration and phase transitions in hafnia-based ferroelectric devices. Science. 2021; 372(6542):630-635. DOI: 10.1126/science.abf3789. View

12.

Liu F, You L, Seyler K, Li X, Yu P, Lin J . Room-temperature ferroelectricity in CuInP2S6 ultrathin flakes. Nat Commun. 2016; 7:12357. PMC: 4987531. DOI: 10.1038/ncomms12357. View

13.

Zhu H, Wang Y, Xiao J, Liu M, Xiong S, Wong Z . Observation of piezoelectricity in free-standing monolayer MoS₂. Nat Nanotechnol. 2014; 10(2):151-5. DOI: 10.1038/nnano.2014.309. View

14.

Feng W, Gao F, Hu Y, Dai M, Li H, Wang L . High-performance and flexible photodetectors based on chemical vapor deposition grown two-dimensional InSe nanosheets. Nanotechnology. 2018; 29(44):445205. DOI: 10.1088/1361-6528/aadc73. View

15.

Xue W, Jiang Q, Wang F, He R, Pang R, Yang H . Discovery of Robust Ferroelectricity in 2D Defective Semiconductor α-Ga Se. Small. 2021; 18(8):e2105599. DOI: 10.1002/smll.202105599. View

16.

Lu H, Lipatov A, Ryu S, Kim D, Lee H, Zhuravlev M . Ferroelectric tunnel junctions with graphene electrodes. Nat Commun. 2014; 5:5518. DOI: 10.1038/ncomms6518. View

17.

Shi H, Li M, Nia A, Wang M, Park S, Zhang Z . Ultrafast Electrochemical Synthesis of Defect-Free In Se Flakes for Large-Area Optoelectronics. Adv Mater. 2020; 32(8):e1907244. DOI: 10.1002/adma.201907244. View

18.

Li L, Wu M . Binary Compound Bilayer and Multilayer with Vertical Polarizations: Two-Dimensional Ferroelectrics, Multiferroics, and Nanogenerators. ACS Nano. 2017; 11(6):6382-6388. DOI: 10.1021/acsnano.7b02756. View

19.

Pang K, Xu X, Wei Y, Ying T, Li W, Yang J . Integrating ferromagnetism and ferroelectricity in an iron chalcogenide monolayer: a first-principles study. Nanoscale. 2022; 14(38):14231-14239. DOI: 10.1039/d2nr04234g. View

20.

Kresse , Furthmuller . Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set. Phys Rev B Condens Matter. 1996; 54(16):11169-11186. DOI: 10.1103/physrevb.54.11169. View