Resistive-switching tunability with size-dependent all-inorganic zero-dimensional tetrahedrite quantum dots  

具有尺寸依赖性的全无机Cu12Sb4S13量子点的阻变存储性能

作　　者：Zhiqing Wang Yueli Liu Jie Shen Wen Chen Jun Miao Ang Li Ke Liu Jing Zhou 王志青;刘曰利;沈杰;陈文;苗君;李昂;刘珂;周静(State Key Laboratory of Advanced Technology for Materials Synthesis and Processing,School of Materials Science and Engineering,Wuhan University of Technology,Wuhan 430070,China;State Key Laboratory of Silicate Materials for Architectures,School of Materials Science and Engineering,Wuhan University of Technology,Wuhan 430070,China;School of Materials Science and Engineering,University of Science and Technology Beijing,Beijing 100083,China)

机构地区：[1]State Key Laboratory of Advanced Technology for Materials Synthesis and Processing,School of Materials Science and Engineering,Wuhan University of Technology,Wuhan 430070,China [2]State Key Laboratory of Silicate Materials for Architectures,School of Materials Science and Engineering,Wuhan University of Technology,Wuhan 430070,China [3]School of Materials Science and Engineering,University of Science and Technology Beijing,Beijing 100083,China

出　　处：《Science China Materials》2020年第12期2497-2508,共12页中国科学（材料科学（英文版）

基　　金：supported by the National Natural Science Foundation of China(51572205,11674258 and 51802093);the Joint Fund of Ministry of Education for Equipment Pre-research the Fundamental Research(6141A02022262);the Excellent Dissertation Cultivation Funds of Wuhan University of Technology(2018-YS-001);the Fundamental Research Funds for the Central Universities(2019zy-007)。

摘　　要：All-inorganic zero-dimensional(0D)tetrahedrite(Cu12Sb4S13,CAS)quantum dots(QDs)have attracted extensive attention due to their excellent optical properties,bandgap tunability,and carrier mobility.In this paper,various sized CAS QDs(5.1,6.7,and 7.9 nm)are applied as a switching layer with the structure F:Sn O2(FTO)/CAS QDs/Au,and in doing so,the nonvolatile resistive-switching behavior of electronics based on CAS QDs is reported.The SET/RESET voltage tunability with size dependency is observed for memory devices based on CAS QDs for the first time.Results suggest that differently sized CAS QDs result in different band structures and the regulation of the SET/RESET voltage occurs simply and effectively due to the uniform size of the CAS QDs.Moreover,the presented memory devices have reliable bipolar resistive-switching properties,a resistance(ON/OFF)ratio larger than 104,high reproducibility,and good data retention ability.After 1.4×10^6s of stability testing and 104cycles of quick read tests,the change rate of the ON/OFF ratio is smaller than 0.1%.Furthermore,resistiveswitching stability can be improved by ensuring a uniform particle size for the CAS QDs.The theoretical calculations suggest that the space-charge-limited currents(SCLCs),which are functioned by Cu 3d,Cu 3p and S 3p to act as electron selftrapping centers due to their quantum confinement and form conduction pathways under an electric field,are responsible for the resistive-switching effect.This paper demonstrates that CAS QDs are promising as a novel resistive-switching material in memory devices and can be used to facilitate the application of next-generation nonvolatile memory.全无机零维Cu12Sb4S13量子点因其优异的光学性能、带隙可调性和载流子迁移率而受到广泛关注.本文首次报道了Cu12Sb4S13量子点的阻变存储特性,构建的FTO/Cu12Sb4S13QDs/Au阻变存储器具有良好的可再现性和可靠的双极性电阻开关特性.量子点的写入/擦除电压具有尺寸依赖性,通过控制Cu12Sb4S13量子点的尺寸调控其能带结构进而调控写入/擦除电压,实现了器件的写入/擦除电压的有效调控.同时,器件具有较大开/关比(大于104),优异的保持性和耐久性.在保持1.4×10^6s和经过104次快速读取后,阻变性能变化率小于0.1%.性能稳定性的提升也得益于更加均一的量子点尺寸,因此可通过制备尺寸均匀的量子点来提升器件稳定性.理论计算表明Cu12Sb4S13量子点的阻变机理由空间电荷限制电流机制占主导,在电场作用下,Cu 3d、Cu 3p和S 3p作为电子自俘获中心进行电子的俘获与去俘获,从而改变了Cu12Sb4S13量子点的阻值.结果表明,Cu12Sb4S13量子点可作为一种新型的阻性开关材料,在数据存储器件中具有巨大的应用潜力,有望促进下一代非易失性存储器的发展与应用.

关 键 词：memory device tetrahedrite quantum dots resistive-switching tunability resistance mechanism 

分 类 号：TP333[自动化与计算机技术—计算机系统结构] TB383.1[自动化与计算机技术—计算机科学与技术]