Spin-sensitive multifunctional devices based on lateral graphene/MoS₂ heterostructures

Abstract

Using first-principles calculations and quantum transport simulations, we simulated multifunctional devices based on lateral graphene/MoS₂ heterostructures, including rectifiers, spin filters, and optoelectronic devices. We investigated the effects of doping, bias voltage, gate voltage, and interface configurations on the device performance. We considered two types of lateral graphene/MoS₂ heterostructures, with graphene connected to either the S edge (C-S) or Mo edge (C-Mo) of the MoS₂. Our calculations show magnetic coupling at the graphene/MoS₂ interfaces even though they are composed of non-magnetic materials, which is consistent with previous theoretical studies. The spin polarization effects degraded the rectification ratios of the graphene/MoS₂ rectifiers. However, n-type doping of MoS₂ could significantly enhance the rectification ratio of the C-S device to 10⁵ and increase the current by an order of magnitude. The C-Mo device was shown to be highly suitable for spin filter applications, with a spin current polarization ratio of almost 100% under bias and gate voltage modulation. For optoelectronic applications, both types of lateral graphene/MoS₂ heterostructures exhibited high photocurrent peaks across the infrared, visible, and/or ultraviolet light regions, with a maximum photocurrent of 13 μA/mm² and suitable bias and gate voltages. Our study reveals the magnetic multifunctional nature of lateral graphene/MoS₂ heterostructure devices, and can serve as a theoretical guide for the design and modulation of high-performance multifunctional devices based on two-dimensional lateral heterostructures.

Keywords

first-principles calculation / lateral heterostructure / optoelectronic device / rectifier / spin polarization

References

[1] Castro Neto AH, Guinea F, Peres NMR, Novoselov KS, Geim AK. The electronic properties of graphene. Rev Mod Phys. 2009; 81(1): 109.

[2] Churchill HO, Jarillo-Herrero P. Two-dimensional crystals: phosphorus joins the family. Nat Nanotechnol. 2014; 9(5): 330.

[3] Wang QH, Kalantar-Zadeh K, Kis A, Coleman JN, Strano MS. Electronics and optoelectronics of two-dimensional transition metal dichalcogenides. Nat Nanotechnol. 2012; 7(11): 699-712.

[4] Mannix AJ, Kiraly B, Hersam MC, Guisinger NP. Synthesis and chemistry of elemental 2D materials. Nat Rev Chem. 2017; 1(2):0014.

[5] Fei R, Kang W, Yang L. Ferroelectricity and phase transitions in monolayer group-IV monochalcogenides. Phys Rev Lett. 2016; 117(9):097601.

[6] Von Rohr FO, Ji H, Cevallos FA, Gao T, Ong NP, Cava RJ. High-pressure synthesis and characterization of β-GeSe-a six-membered-ring semiconductor in an uncommon boat conformation. J Am Chem Soc. 2017; 139(7): 2771.

[7] Guan S, Liu C, Lu Y, Yao Y, Yang SA. Tunable ferroelectricity and anisotropic electric transport in monolayer β-GeSe. Phys Rev B. 2018; 97(14):144104.

[8] Yin H, Liu C, Zheng G-P, Wang Y, Ren F. Ab initio simulation studies on the room-temperature ferroelectricity in two-dimensional β-phase GeS. Appl Phys Lett. 2019; 114(19):192903.

[9] Zhong M, Xia Q, Pan L, et al. Thickness-dependent carrier transport characteristics of a new 2D elemental semiconductor: black arsenic. Adv Funct Mater. 2018; 28(43):1802581.

[10] Yan S, Wang K, Guo Z, Wu Y-N, Chen S. Tunneling field-effect transistors with two-dimensional BiN as the channel semiconductor. Appl Phys Lett. 2024; 124(14):143502.

[11] Jiang J, Xu L, Qiu C, Peng L-M. Ballistic two-dimensional InSe transistors. Nature. 2023; 616(7957): 470-475.

[12] An Y, Wang K, Gong S, et al. Nanodevices engineering and spin transport properties of MnBi₂Te₄ monolayer. NPJ Comput Mater. 2021; 7(1): 45.

[13] Gao Y, Liao J, Wang H, et al. Electronic transport properties and nanodevice designs for monolayer MoSi₂P₄. Phys Rev Appl. 2022; 18(3):034033.

[14] Dang J, Wu T, Yan S, et al. Electrical switching of spin-polarized light-emitting diodes based on a 2D CrI₃/hBN/WSe₂ heterostructure. Nat Commun. 2024; 15(1): 6799.

[15] Hu J, Li H, Chen A, et al. All-2D-materials subthreshold-free field-effect transistor with near-ideal switching slope. ACS Nano. 2024; 18(31): 20236-20246.

[16] Li M, Chen C, Shi Y, Li L. Heterostructures based on two-dimensional layered materials and their potential applications. Mater Today. 2016; 19(6): 322.

[17] Hong W, Shim GW, Yang SY, Jung DY, Choi S-Y. Improved electrical contact properties of MoS₂-graphene lateral heterostructure. Adv Funct Mater. 2018; 29(6):1807550.

[18] An Y, Hou Y, Wang K, et al. Multifunctional lateral transition-metal disulfides heterojunctions. Adv Funct Mater. 2020; 30(32):2002939.

[19] Aslam MA, Leitner S, Tyagi S, et al. All van der Waals semiconducting PtSe₂ field effect transistors with low contact resistance graphite electrodes. Nano Lett. 2024; 24(22): 6529.

[20] Song S, Lyu J, Qin L, Wang Z, Gong J, Yang S. Lateral graphene/MoS₂ heterostructures for steep-slope Dirac-source field-effect transistors. Phys Rev B. 2024; 110(12):125407.

[21] Che M, Wang B, Zhao X, et al. PdSe₂/2H-MoTe₂ heterojunction self-powered photodetector: broadband photodetection and linear/circular polarization capability. ACS Nano. 2024; 18(44): 30884-30895.

[22] Geim AK, Grigorieva IV. Van der Waals heterostructures. Nature. 2013; 499(7459): 419-425.

[23] Zhang F, Shi H, Yu Y, et al. Dynamic band-alignment modulation in MoTe₂/SnSe₂ heterostructure for high performance photodetector. Adv Opt Mater. 2024; 12(16):2303088.

[24] Pan Y, Zhu L, Lu L, et al. Polarized photodetectors based on 2D 2H-MoTe₂/1T'-MoTe₂/MoSe₂ van der Waals heterojunction. Adv Funct Mater. 2024; 34:2407931.

[25] Wang J, Liu C, Zhang L, et al. Selective enhancement of photoresponse with ferroelectric-controlled BP/In₂Se₃ vdW heterojunction. Adv Sci. 2023; 10(11):e2205813.

[26] Allain A, Kang J, Banerjee K, Kis A. Electrical contacts to two-dimensional semiconductors. Nat Mater. 2015; 14(12): 1195-1205.

[27] Kang J, Liu W, Sarkar D, Jena D, Banerjee K. Computational study of metal contacts to monolayer transition-metal dichalcogenide semiconductors. Phys Rev X. 2014; 4(3):031005.

[28] Avalos-Ovando O, Mastrogiuseppe D, Ulloa SE. Lateral heterostructures and one-dimensional interfaces in 2D transition metal dichalcogenides. J Phys Condens Matter. 2019; 31(21):213001.

[29] Zheng C, Zhang Q, Weber B, et al. Direct observation of 2D electrostatics and ohmic contacts in template-grown graphene/WS₂ heterostructures. ACS Nano. 2017; 11(3): 2785.

[30] Tang H-L, Chiu M-H, Tseng C-C, et al. Multilayer graphene-WSe₂ heterostructures for WSe₂ transistors. ACS Nano. 2017; 11(12): 12817.

[31] Ling X, Lin Y, Ma Q, et al. Parallel stitching of 2D materials. Adv Mater. 2016; 28(12): 2322-2329.

[32] GuimarãEs MHD, Gao H, Han Y, et al. Atomically thin ohmic edge contacts between two-dimensional materials. ACS Nano. 2016; 10(6): 6392-6399.

[33] Chen W, Yang Y, Zhang Z, Kaxiras E. Properties of in-plane graphene/MoS₂ heterojunctions. 2D Mater. 2017; 4(4):045001.

[34] Souza ES, Scopel WL, Miwa RH. Probing the local interface properties at a graphene-MoSe₂ in-plane lateral heterostructure: an ab initio study. Phys Chem Chem Phys. 2018; 20(26): 17952.

[35] Wang X, Long R. Photoinduced anomalous electron transfer dynamics at a lateral MoS₂-graphene covalent junction. J Phys Chem Lett. 2021; 12(31): 7553-7559.

[36] Liu X, Gao J, Zhang G, Zhang Y-W. MoS₂-graphene in-plane contact for high interfacial thermal conduction. Nano Res. 2017; 10(9): 2944-2953.

[37] Zhou Y, Yang Y, Guo Y, Wang Q, Yan X. Influence of length and interface structure on electron transport properties of graphene-MoS₂ in-plane heterojunction. Appl Surf Sci. 2019; 497:143764.

[38] Li W, Wei J, Bian B, Liao B, Wang G. The effect of different covalent bond connections and doping on transport properties of planar graphene/MoS₂/graphene heterojunctions. Phys Chem Chem Phys. 2021; 23(11): 6871-6879.

[39] Ghayyem F, Kiakojouri A, Frank I, Nadimi E. Gas sensing properties of graphene/MoS₂/graphene lateral heterostructure: a first principles investigation. IEEE Sensors J. 2024; 24(22): 36334.

[40] Song S, Gong J, Jiang X, Yang S. Influence of the interface structure and strain on the rectification performance of lateral MoS₂/graphene heterostructure devices. Phys Chem Chem Phys. 2022; 24(4): 2265-2274.

[41] Chen J, Guo Y, Fan X, et al. Nanodevices from and electronic transport properties of ZrI₂ monolayers. Phys Rev Appl. 2023; 20(6):064048.

[42] Chen J, Guo Y, Ma C, et al. Magnetic nanodevices and spin-transport properties of a two-dimensional CrSCl monolayer. Phys Rev Appl. 2023; 19(5):054013.

[43] Chen J, Fan X, Li J, et al. Exploring the applications of ScXI (X = S, Se, Te) monolayers for microelectronic nanodevices and photoelectric sensors. Phys Rev Appl. 2024; 21(5):054053.

[44] Lü X-L, Xie H. Bipolar and unipolar valley filter effects in graphene-based P/N junction. New J Phys. 2020; 22(7):073003.

[45] Li N, He C, Wang Q, et al. Gate-tunable large-scale flexible monolayer MoS₂ devices for photodetectors and optoelectronic synapses. Nano Res. 2022; 15(6): 5418-5424.

[46] Jia W, Cao Z, Wang L, et al. The analysis of a plane wave pseudopotential density functional theory code on a GPU machine. Comput Phys Commun. 2013; 184(1): 9-18.

[47] Jia W, Fu J, Cao Z, et al. Fast plane wave density functional theory molecular dynamics calculations on multi-GPU machines. J Comput Phys. 2013; 251: 102-115.

[48] Li W, Guo Y, Luo Z, et al. A gate programmable van der Waals metal-ferroelectric-semiconductor vertical heterojunction memory. Adv Mater. 2022; 35(5):2208266.

[49] Li J, Lin C, Weng M, et al. Structural origin of the high-voltage instability of lithium cobalt oxide. Nat Nanotechnol. 2021; 16(5): 599-605.

[50] Ren X, Wang J, Zhu D, et al. Sn-C bonding riveted SnSe nanoplates vertically grown on nitrogen-doped carbon nanobelts for high-performance sodium-ion battery anodes. Nano Energy. 2018; 54: 322-330.

[51] Wu S, Yang X, Zhang H, et al. Unambiguous identification of carbon location on the N site in semi-insulating GaN. Phys Rev Lett. 2018; 121(14):145505.

[52] Perdew JP, Burke K, Ernzerhof M. Generalized gradient approximation made simple. Phys Rev Lett. 1996; 77(18): 3865-3868.

[53] Li Q, Yang C, Xu L, et al. Symmetric and excellent scaling behavior in ultrathin n- and p-type gate-all-around InAs nanowire transistors. Adv Funct Mater. 2023; 33(23):2214653.

[54] Liu S, Li Q, Yang C, et al. Performance limit of gate-all-around Si nanowire field-effect transistors: an ab initio quantum transport simulation. Phys Rev Appl. 2022; 18(5):054089.

[55] Pan Y, Dai J, Xu L, et al. Sub-5-nm monolayer silicane transistor: a first-principles quantum transport simulation. Phys Rev Appl. 2020; 14:024016.

[56] Yu Q, Jauregui LA, Wu W, et al. Control and characterization of individual grains and grain boundaries in graphene grown by chemical vapour deposition. Nat Mater. 2011; 10(6): 443-449.

[57] Lauritsen JV, Kibsgaard J, Helveg S, et al. Size-dependent structure of MoS₂ nanocrystals. Nat Nanotechnol. 2007; 2(1): 53-58.

[58] Yazyev OV, Chen YP. Polycrystalline graphene and other two-dimensional materials. Nat Nanotechnol. 2014; 9(10): 755-767.

[59] Cao D, Shen T, Liang P, Chen X, Shu H. Role of chemical potential in flake shape and edge properties of monolayer MoS₂. J Phys Chem C. 2015; 119(8): 4294-4301.

[60] Brandbyge M, Mozos J-L, Ordejón P, Taylor J, Stokbro K. Density-functional method for nonequilibrium electron transport. Phys Rev B. 2002; 65(16):165401.

[61] Buttiker M, Imry Y, Landauer R, Pinhas S. Generalized many-channel conductance formula with application to small rings. Phys Rev B. 1985; 31(10): 6207-6215.

[62] Quantum ATK Package. Accessed October 28, 2025.

[63] Palsgaard M, Markussen T, Gunst T, Brandbyge M, Stokbro K. Efficient first-principles calculation of phonon-assisted photocurrent in large-scale solar-cell devices. Phys Rev Appl. 2018; 10(1):014026.

[64] Zhang L, Gong K, Chen J, et al. Generation and transport of valley-polarized current in transition-metal dichalcogenides. Phys Rev B. 2014; 90(19):195428.

[65] Li Y, Zhou Z, Zhang S, Chen Z. MoS₂ nanoribbons: high stability and unusual electronic and magnetic properties. J Am Chem Soc. 2008; 130(49): 16739-16744.

[66] Son YW, Cohen ML, Louie SG. Energy gaps in graphene nanoribbons. Phys Rev Lett. 2006; 97(21):216803.

[67] Quantum ATK Software. Accessed October 5, 2025.

[68] An Y, Zhang M, Wu D, et al. The rectifying and negative differential resistance effects in graphene/h-BN nanoribbon heterojunctions. Phys Chem Chem Phys. 2016; 18(40):27976.

[69] Su S, Gong J, Fan Z-Q. Tunnable rectifying performance of in-plane metal-semiconductor junctions based on passivated zigzag phosphorene nanoribbons. RSC Adv. 2018; 8(55): 31255-31260.

[70] Qiu C, Liu F, Xu L, et al. Dirac-source field-effect transistors as energy-efficient, high-performance electronic switches. Science. 2018; 361(6400): 387-392.

[71] Gong Y, Liu Z, Lupini AR, et al. Band gap engineering and layer-by-layer mapping of selenium-doped molybdenum disulfide. Nano Lett. 2013; 14(2):442.

[72] Duan X, Wang C, Fan Z, et al. Synthesis of WS_2xSe_2−2x alloy nanosheets with composition-tunable electronic properties. Nano Lett. 2015; 16(1):264.

[73] He Q, Liu Y, Tan C, Zhai W, Nam G-H, Zhang H. Quest for p-type two-dimensional semiconductors. ACS Nano. 2019; 13(11): 12294-12300.

[74] Cho B, Hahm MG, Choi M, et al. Charge-transfer-based gas sensing using atomic-layer MoS₂. Sci Rep. 2015; 5(1): 8052.

[75] G. ASTM. 173-03, Terrestrial Reference Spectra for Photovoltaic Performance Evaluation. American Society for Testing Materials (ASTM) International; 2012.

[76] Wang Q, Zhang Q, Zhao X, et al. High-energy gain upconversion in monolayer tungsten disulfide photodetectors. Nano Lett. 2019; 19(8): 5595-5603.

[77] Pan Y, Wang QZ, Yeats AL, et al. Helicity dependent photocurrent in electrically gated (Bi_1−xSb_x)₂Te₃ thin films. Nat Commun. 2017; 8(1):1037.

[78] Gunst T, Markussen T, Palsgaard MLN, Stokbro K, Brandbyge M. First-principles electron transport with phonon coupling: large scale at low cost. Phys Rev B. 2017; 96(16):161404.

RIGHTS & PERMISSIONS

2026 The Author(s). InfoMat published by UESTC and John Wiley & Sons Australia, Ltd.