Bi_(2)O_(2)Se is highly competitive as a candidate of next-generation high-performance semiconductors.Though dubbed as semiconductor,Bi_(2)O_(2)Se films exhibited high conductance,i.e.,metallic behavior,due to spontan...Bi_(2)O_(2)Se is highly competitive as a candidate of next-generation high-performance semiconductors.Though dubbed as semiconductor,Bi_(2)O_(2)Se films exhibited high conductance,i.e.,metallic behavior,due to spontaneously ionized defects.Semiconducting/insulating films are of practical importance in broad applications based on low-power,high-performance electronics,the existence of which lacks firm evidence.Here,we synthesized highly insulating films in a controlled way,which exhibit semiconducting behavior with channel resistance up to 1 TΩ.The electron chemical potential lies within the band gap,in some cases,even below the charge neutrality level,signifying the trace of hole-type semiconducting.The performance of insulating devices remains high,comparable to high-quality devices previously.Especially,the threshold voltage(Vth)is positive,contrary to common negative values reported.Calculations indicate that our synthesis conditions suppress electron donors(Se vacancies(VSe))and promote the formation of compensating acceptors(Bi vacancies(VBi)),leading to insulating behaviors.Our work offers insights into electron dynamics of Bi_(2)O_(2)Se,moves one step further towards p-type transistors and provides a valuable playground for engineering ferroelectricity in high-performance semiconductors.展开更多
The on-demand modulation of defects in materials for the effective modulation of optical nonlinearity is desirable,while it remains a great challenge.In this work,we demonstrate that electrochemical activation is a fa...The on-demand modulation of defects in materials for the effective modulation of optical nonlinearity is desirable,while it remains a great challenge.In this work,we demonstrate that electrochemical activation is a facile and convenient approach to modulating the broadband third-order nonlinear absorption of nanoporous tungsten oxide(WO3-x)thin film.The film does not exhibit optical nonlinearity at the initial state,while shows a distinct saturable absorption under an applied voltage of-2.5 V with the excitation of 515,800,and 1,030 nm laser.The nonlinear absorption coefficient(β_(eff))is-766.38±6.67 cm·GW^(-1) for 1,030 nm laser,-624.24±17.15 cm·GW-1 for 800 nm laser,and-120.70±11.49 cm·GW^(-1) for 515 nm laser,and the performance is competitive among inorganic saturable absorbers.The activation is accomplished in 2 min.The performance enhancement is ascribed to the formation of abundant in-gap defect states because of the reduction of the tungsten atoms,and a Pauli-blocking effect occurs during the excitation of in-gap defect states.The small feature size of WO_(3-x)(-12 nm)enables the effective and fast introduction and removal of the defects in porous film,and accordingly the fast and broadband modulation of optical nonlinearity.Our results suggest a controllable,effective,and convenient approach to tuning the nonlinear absorption of materials.展开更多
基金supported by the National Natural Science Foundation of China(Nos.11904294 and 62004172)the foundation of Westlake Multidisciplinary Research Initiative Center(MRIC,Nos.MRIC20200402 and 20200101).
文摘Bi_(2)O_(2)Se is highly competitive as a candidate of next-generation high-performance semiconductors.Though dubbed as semiconductor,Bi_(2)O_(2)Se films exhibited high conductance,i.e.,metallic behavior,due to spontaneously ionized defects.Semiconducting/insulating films are of practical importance in broad applications based on low-power,high-performance electronics,the existence of which lacks firm evidence.Here,we synthesized highly insulating films in a controlled way,which exhibit semiconducting behavior with channel resistance up to 1 TΩ.The electron chemical potential lies within the band gap,in some cases,even below the charge neutrality level,signifying the trace of hole-type semiconducting.The performance of insulating devices remains high,comparable to high-quality devices previously.Especially,the threshold voltage(Vth)is positive,contrary to common negative values reported.Calculations indicate that our synthesis conditions suppress electron donors(Se vacancies(VSe))and promote the formation of compensating acceptors(Bi vacancies(VBi)),leading to insulating behaviors.Our work offers insights into electron dynamics of Bi_(2)O_(2)Se,moves one step further towards p-type transistors and provides a valuable playground for engineering ferroelectricity in high-performance semiconductors.
基金supported by the National Natural Science Foundation of China(Nos.51772214,51432006,and 51701170)the Ministry of Science and Technology of China(No.2011DFG52970)+2 种基金the Ministry of Education of China(IRT14R23),111 Project(No.B13025)the Innovation Program of Shanghai Municipal Education Commission,the national youth talent support program(No.W03070073)the project of science and technology plan of Fujian Province(No.2018J01520).
文摘The on-demand modulation of defects in materials for the effective modulation of optical nonlinearity is desirable,while it remains a great challenge.In this work,we demonstrate that electrochemical activation is a facile and convenient approach to modulating the broadband third-order nonlinear absorption of nanoporous tungsten oxide(WO3-x)thin film.The film does not exhibit optical nonlinearity at the initial state,while shows a distinct saturable absorption under an applied voltage of-2.5 V with the excitation of 515,800,and 1,030 nm laser.The nonlinear absorption coefficient(β_(eff))is-766.38±6.67 cm·GW^(-1) for 1,030 nm laser,-624.24±17.15 cm·GW-1 for 800 nm laser,and-120.70±11.49 cm·GW^(-1) for 515 nm laser,and the performance is competitive among inorganic saturable absorbers.The activation is accomplished in 2 min.The performance enhancement is ascribed to the formation of abundant in-gap defect states because of the reduction of the tungsten atoms,and a Pauli-blocking effect occurs during the excitation of in-gap defect states.The small feature size of WO_(3-x)(-12 nm)enables the effective and fast introduction and removal of the defects in porous film,and accordingly the fast and broadband modulation of optical nonlinearity.Our results suggest a controllable,effective,and convenient approach to tuning the nonlinear absorption of materials.