Grain boundaries in two-dimensional(2D)semiconductors generally induce distorted band alignment and interfacial charge,which impair their electronic properties for device applications.Here,we report the improvement of...Grain boundaries in two-dimensional(2D)semiconductors generally induce distorted band alignment and interfacial charge,which impair their electronic properties for device applications.Here,we report the improvement of band alignment at the grain boundaries of PtSe_(2),a 2D semiconductor,with selective adsorption of a presentative organic acceptor,tetracyanoquinodimethane(TCNQ).TCNQ molecules show selective adsorption at the PtSe_(2)grain boundary with strong interfacial charge.The adsorption of TCNQ distinctly improves the band alignment at the PtSe_(2)grain boundaries.With the charge transfer between the grain boundary and TCNQ,the local charge is inhibited,and the band bending at the grain boundary is suppressed,as revealed by the scanning tunneling microscopy and spectroscopy(STM/S)results.Our finding provides an effective method for the advancement of the band alignment at the grain boundary by functional molecules,improving the electronic properties of 2D semiconductors for their future applications.展开更多
Semiconducting heterojunctions(HJs),comprised of atomically thin transition metal dichalcogenides(TMDs),have shown great potentials in electronic and optoelectronic applications.Organic/TMD hybrid bilayers hold enhanc...Semiconducting heterojunctions(HJs),comprised of atomically thin transition metal dichalcogenides(TMDs),have shown great potentials in electronic and optoelectronic applications.Organic/TMD hybrid bilayers hold enhanced pumping efficiency of interfacial excitons,tunable electronic structures and optical properties,and other superior advantages to these inorganic HJs.Here,we report a direct probe of the interfacial electronic structures of a crystalline monolayer(ML)perylene-3,4,9,10-tetracarboxylic-dianhydride(PTCDA)/ML-WSe_(2) HJ using scanning tunneling microscopy,photoluminescence,and first-principle calculations.Strong PTCDAAA/Se_(2) interfacial interactions lead to appreciable hybridization of the WSe_(2) conduction band with PTCDA unoccupied states,accompanying with a significant amount of PTCDA-to-WSe_(2) charge transfer(by 0.06 e/PTCDA).A type-ll band alignment was directly determined with a valence band offset of-1.69 eV,and an apparent conduction band offset of-1.57 eV.Moreover,we found that the local stacking geometry at the HJ interface differentiates the hybridized interfacial states.展开更多
基金the National Key Research and Development Program of China(Nos.2021YFA1400100,2020YFA0308800,and 2019YFA0308000)the National Natural Science Foundation of China(Nos.92163206 and 62171035)+2 种基金the Beijing Nova Program from Beijing Municipal Science&Technology Commission(No.Z211100002121072)the Beijing Natural Science Foundation(Nos.Z190006 and 4192054)Calculations were performed at the Physics Lab of High-Performance Computing of Renmin University of China,and Beijing Super Cloud Computing Center.
文摘Grain boundaries in two-dimensional(2D)semiconductors generally induce distorted band alignment and interfacial charge,which impair their electronic properties for device applications.Here,we report the improvement of band alignment at the grain boundaries of PtSe_(2),a 2D semiconductor,with selective adsorption of a presentative organic acceptor,tetracyanoquinodimethane(TCNQ).TCNQ molecules show selective adsorption at the PtSe_(2)grain boundary with strong interfacial charge.The adsorption of TCNQ distinctly improves the band alignment at the PtSe_(2)grain boundaries.With the charge transfer between the grain boundary and TCNQ,the local charge is inhibited,and the band bending at the grain boundary is suppressed,as revealed by the scanning tunneling microscopy and spectroscopy(STM/S)results.Our finding provides an effective method for the advancement of the band alignment at the grain boundary by functional molecules,improving the electronic properties of 2D semiconductors for their future applications.
基金supported by the National Key R&D Program of China(Nos.2018FYA0305800 and 2018YFA0703700)the National Natural Science Foundation of China(Nos.11774268 and 11974012)+2 种基金the Strategic Priority Research Program of Chinese Academy of Sciences(No.XDB30000000)support from the Fundamental Research Funds for the Central Universities,Chinathe Research Funds of Renmin University of China(Nos.16XNLQ01 and 19XNQ025)。
文摘Semiconducting heterojunctions(HJs),comprised of atomically thin transition metal dichalcogenides(TMDs),have shown great potentials in electronic and optoelectronic applications.Organic/TMD hybrid bilayers hold enhanced pumping efficiency of interfacial excitons,tunable electronic structures and optical properties,and other superior advantages to these inorganic HJs.Here,we report a direct probe of the interfacial electronic structures of a crystalline monolayer(ML)perylene-3,4,9,10-tetracarboxylic-dianhydride(PTCDA)/ML-WSe_(2) HJ using scanning tunneling microscopy,photoluminescence,and first-principle calculations.Strong PTCDAAA/Se_(2) interfacial interactions lead to appreciable hybridization of the WSe_(2) conduction band with PTCDA unoccupied states,accompanying with a significant amount of PTCDA-to-WSe_(2) charge transfer(by 0.06 e/PTCDA).A type-ll band alignment was directly determined with a valence band offset of-1.69 eV,and an apparent conduction band offset of-1.57 eV.Moreover,we found that the local stacking geometry at the HJ interface differentiates the hybridized interfacial states.
