Van der Waals (vdWs) stacking of two-dimensional (2D) materials can effectively weaken the Fermi level pinning (FLP) effect in metal/semiconductor contacts due to dangling-bond-free surfaces. However, the inherent vdW...Van der Waals (vdWs) stacking of two-dimensional (2D) materials can effectively weaken the Fermi level pinning (FLP) effect in metal/semiconductor contacts due to dangling-bond-free surfaces. However, the inherent vdWs gap always induces a considerable tunneling barrier, significantly limiting carrier injection. Herein, by inducing a sp^(2) to sp^(3) hybridization transformation in 2D carbon-based metal via surface defect engineering, the large orbital overlap can form an efficient carrier channel, overcoming the tunneling barrier. Specifically, by selecting the 2D carbon-based X_(3)C_(2) (X = Cd, Hg, and Zn) metal and the 2D MSi_(2)N_(4) (M = Cr, Hf, Mo, Ti, V, and Zr) semiconductor, we constructed 36 metal/semiconductor contacts. For vdWs contacts, although Ohmic contacts can be formed at the interface, the highest tunneling probability (P TB) is only 3.11%. As expected, the P TB can be significantly improved, as high as 48.73%, when MSi_(2)N_(4), accompanied by surface nitrogen vacancies, forms an interface covalent bond with X_(3)C_(2). Simultaneously, weak FLP and Ohmic contact remain at the covalent-bond-based surface, attributing to the protection of the MSi_(2)N_(4) band-edge electronic states by the outlying Si-N sublayer. Our work provides a promising path for advancing the progress of 2D electronic and photoelectronic devices.展开更多
Discovery of materials using“bottom-up”or“top-down”approach is of great interest in materials science.Layered materials consisting of two-dimensional(2D)building blocks provide a good platform to explore new mater...Discovery of materials using“bottom-up”or“top-down”approach is of great interest in materials science.Layered materials consisting of two-dimensional(2D)building blocks provide a good platform to explore new materials in this respect.In van der Waals(vdW)layered materials,these building blocks are charge neutral and can be isolated from their bulk phase(top-down),but usually grow on substrate.In ionic layered materials,they are charged and usually cannot exist independently but can serve as motifs to construct new materials(bottom-up).In this paper,we introduce our recently constructed databases for 2D material-substrate interface(2DMSI),and 2D charged building blocks.For 2DMSI database,we systematically build a workflow to predict appropriate substrates and their geometries at substrates,and construct the 2DMSI database.For the 2D charged building block database,1208 entries from bulk material database are identified.Information of crystal structure,valence state,source,dimension and so on is provided for each entry with a json format.We also show its application in designing and searching for new functional layered materials.The 2DMSI database,building block database,and designed layered materials are available in Science Data Bank at https://doi.org/10.57760/sciencedb.j00113.00188.展开更多
基金supported by China Postdoctoral Science Foundation(No.2022M711691)the National Natural Science Foundation of China(Nos.12104130 and 12304085)+3 种基金Six talent peaks project in Jiangsu Province(No.XCL-104)the open research fund of Key Laboratory of Quantum Materials and Devices(Southeast University)Ministry of Education(No.3207022401C3)Natural Science Foundation of Nanjing University of Posts and Telecommunications(No.NY221102).
文摘Van der Waals (vdWs) stacking of two-dimensional (2D) materials can effectively weaken the Fermi level pinning (FLP) effect in metal/semiconductor contacts due to dangling-bond-free surfaces. However, the inherent vdWs gap always induces a considerable tunneling barrier, significantly limiting carrier injection. Herein, by inducing a sp^(2) to sp^(3) hybridization transformation in 2D carbon-based metal via surface defect engineering, the large orbital overlap can form an efficient carrier channel, overcoming the tunneling barrier. Specifically, by selecting the 2D carbon-based X_(3)C_(2) (X = Cd, Hg, and Zn) metal and the 2D MSi_(2)N_(4) (M = Cr, Hf, Mo, Ti, V, and Zr) semiconductor, we constructed 36 metal/semiconductor contacts. For vdWs contacts, although Ohmic contacts can be formed at the interface, the highest tunneling probability (P TB) is only 3.11%. As expected, the P TB can be significantly improved, as high as 48.73%, when MSi_(2)N_(4), accompanied by surface nitrogen vacancies, forms an interface covalent bond with X_(3)C_(2). Simultaneously, weak FLP and Ohmic contact remain at the covalent-bond-based surface, attributing to the protection of the MSi_(2)N_(4) band-edge electronic states by the outlying Si-N sublayer. Our work provides a promising path for advancing the progress of 2D electronic and photoelectronic devices.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.61888102,52272172,and 52102193)the Major Program of the National Natural Science Foundation of China(Grant No.92163206)+2 种基金the National Key Research and Development Program of China(Grant Nos.2021YFA1201501 and 2022YFA1204100)the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB30000000)the Fundamental Research Funds for the Central Universities.
文摘Discovery of materials using“bottom-up”or“top-down”approach is of great interest in materials science.Layered materials consisting of two-dimensional(2D)building blocks provide a good platform to explore new materials in this respect.In van der Waals(vdW)layered materials,these building blocks are charge neutral and can be isolated from their bulk phase(top-down),but usually grow on substrate.In ionic layered materials,they are charged and usually cannot exist independently but can serve as motifs to construct new materials(bottom-up).In this paper,we introduce our recently constructed databases for 2D material-substrate interface(2DMSI),and 2D charged building blocks.For 2DMSI database,we systematically build a workflow to predict appropriate substrates and their geometries at substrates,and construct the 2DMSI database.For the 2D charged building block database,1208 entries from bulk material database are identified.Information of crystal structure,valence state,source,dimension and so on is provided for each entry with a json format.We also show its application in designing and searching for new functional layered materials.The 2DMSI database,building block database,and designed layered materials are available in Science Data Bank at https://doi.org/10.57760/sciencedb.j00113.00188.
