赝弹性银硫系化合物阻变行为的透射电镜研究
熊雨薇,李京仓,谭治远,朱明芸,尹奎波*,商尚炀,魏 琦,夏奕东,孙立涛*
(1.东南大学-FEI 纳皮米中心,MEMS 教育部重点实验室,东南大学电子科学与工程学院,江苏南京210096;2.固体微结构国家实验室,南京大学材料科学与工程学院,江苏南京210093)
摘 要 银硫系化合物由于尺寸可缩减性好、擦写速度快、具有多值存储能力等优点,在阻变存储器介质材料研究中受到广泛关注。但随着介质材料尺寸的不断缩小,材料表/界面结构对器件的性能产生的影响尚不明确。因此从微观尺度上揭示阻变介质材料表/界面对性能影响的相关机理至关重要。本文利用脉冲激光沉积制备了Ag10Ge15Te75薄膜,并在透射电子显微镜中构建了以其为介质的阻变存储器,研究了其阻变过程中微观形貌与物相的演化。实验发现,尺寸在20 nm以下的Ag10Ge15Te75薄膜在被电压脉冲熔断后,能够用“冷焊”的方式重新连接并仍保持阻变特性。当给其施加正向电压时,薄膜中生成Ag2Te多晶颗粒。当挤压拉伸薄膜时,Ag2Te多晶颗粒不会消失。当施加反向电压时,Ag2Te多晶颗粒消失。分析认为,Ag10Ge15Te75薄膜的形变属于Coble赝弹性,Ag2Te多晶的生成与电场诱导沉积有关。实验的结果对于构建新型柔性阻变存储器结构具有一定的指导意义。
关键词 Ag10Ge15Te75;透射电子显微镜;阻变存储器;赝弹性行为
中图分类号:TB303;TN303;TN304;TN604;TG115.21+5.3
文献标识码:Adoi:10.3969/j.issn.1000-6281.2021.06.001
Investigation of the resistive switching behavior of pseudoelastic silver chalcogenides via TEM
XIONG Yu-wei1,LI Jing-cang1,TAN Zhi-yuan1,ZHU Ming-yun1,YIN Kui-bo1*,SHANG Shang-yang1,WEI Qi1,XIA Yi-dong1,SUN Li-tao1*
(1.SEU-FEI Nano-Pico Center, Key Laboratory of MEMS of Ministry of Education, Department of Electronic Science and Engineering, Southeast University, Nanjing Jiangsu 210096;National Laboratory of Solid State Microstructures, Department of Materials Science and Engineering, Nanjing University, Nanjing Jiangsu 210093, China)
Abstract Silver chalcogenide has been one of the most attractive dielectric materials in resistive random-access memory (RRAM) due to its excellent miniaturization potential, fast operation speed and multilevel data storage capacity. However, the influence of material surface/interface structure on device performance is ambiguous as the size of dielectric material decreases. Therefore, it is significant to reveal the corresponding mechanism of dielectric materials at atomic scale. In this paper, Ag10Ge15Te75 films were prepared by pulsed laser deposition, and a RRAM device based on the Ag10Ge15Te75 films was constructed in the transmission electron microscope (TEM). The evolution of morphology and phase during the resistive switching process was studied. It was found that the Ag10Ge15Te75 thin films with the sizebelow 20 nm could be reconnected by cold welding after being fused by voltage pulse and still retain resistive switching characteristics. When the forward voltage is applied, Ag2Te particles are formed in the film. Ag2Te particles will not disappear until the reverse voltage is applied, even though the film is compressed or stretched. It can be concluded that the deformation of Ag10Ge15Te75 film belongs to Coble pseudoelasticity, and the formation of Ag2Te is related to electrical field induced precipitation reaction. This work provides deep insights into mechanistic understanding of resistive switching in Ag10Ge15Te75 and a valuable strategy for producing flexible RRAM.
Keywords Ag10Ge15Te75; transmission electron microscope; RRAM; pseudoelastic behavior
“全文下载请到同方知网,万方数据库或重庆维普等数据库中下载!”
[1] WANG Z R, WU H Q, BURR G W, et al. Resistive switching materials for information processing[J]. Nature Reviews Materials,2020,5(3):173-195.
[2] 熊雨薇. 基于银硫系化合物阻变存储器的工作机理研究[D]. 南京:东南大学,2016.
[3] 许含霓. 银硫系化合物的相变行为与电运输特性研究[D]. 南京:南京大学,2012.
[4] CAI F X, CORRELL J M, LEE S H, et al. A fully integrated reprogrammable memristor-CMOS system for efficient multiply–accumulate operations[J]. Nature Electronics. 2019,2(7):290-299.
[5] FENG Y L, HUANG P, ZHOU Z, et al. Negative differential resistance effect in Ru-based RRAM device fabricated by atomic layer deposition[J]. Nanoscale Research Letters, 2019, 14(1):86-90.
[6] MIKHAYLOV A N, BELOV A I, GUSEINOV D V, et al. Bipolar resistive switching and charge transport in silicon oxide memristor[J]. Materials Science & Engineering B, 2015, 194:48-54.
[7] ZHOU F, CHANG Y F, FOWLER B, et al. Stabilization of multiple resistance levels by current-sweep in SiOx-based resistive switching memory [J]. Applied Physics Letters, 2015, 106(6):629.
[8] BOUSOULAS P, ASENOV P, KARAGEORGIOU I, et al. Engineering amorphous-crystalline interfaces in TiO2-x/TiO2-y-based bilayer structures for enhanced resistive switching and synaptic properties [J]. Journal of Applied Physics, 2016, 120(15):625-630.
[9] HUANG X Y, WU H Q, GAO B, et al. HfO2/Al2O3 multilayer for RRAM arrays: a technique to improve tail-bit retention[J]. Nanotechnology, 2016, 27(39):395201.
[10] LUO Q, XU X X, LIU H T, et al. Super non-linear RRAM with ultra-low power for 3D vertical nano-crossbar arrays[J]. Nanoscale, 2016, 8(34):15629.
[11] TAMURA T, HASEGAWA T, TERABE K, et al. Switching property of atomic switch controlled by solid electrochemical reaction[J]. Japanese Journal of Applied,2006,45(12/13/14/15/16):364-366.
[12] MORALES-MASIS M, VAN DER MOLEN S J, FU W T, et al. Conductance switching in Ag2S devices fabricated by in situ sulfurization[J]. Nanotechnology, 2009, 20(9): 095710.
[13] KUND M, BEITEL G, PINNOW C U, et al. Conductive bridging RAM (CBRAM): an emerging non-volatile memory technology scalable to sub 20nm[C]. IEEE International electron Devices Meeting 2005,Washington, DC, 2005:773-776.
[14] JEON Y R, ABBAS Y, SOKOLOV A S, et al. Study of in situ silver migration in amorphous boron nitride CBRAM device[J]. ACS Applied Materials & Interfaces, 2019, 11(26):23329-23336.
[15] SAKAMOTO T, SUNAMURA H, KAWAURA H, et al. Nanometer-scale switches using copper sulfide[J]. Applied Physics Letters, 2003, 82(18):3032-3034.
[16] CHEN C, YANG Y C, ZENG F, et al. Bipolar resistive switching in Cu/AlN/Pt nonvolatile memory device[J]. Applied Physics Letters, 2010, 97(8):1625.
[17] CIOCCHINI N, LAUDATO M, BONIARDI M, et al. Bipolar switching in chalcogenide phase change memory[J]. Scientific Reports, 2016, 6:29162.
[18] TERABE K, HASEGAWA T, NAKAYAMA T, et al. Quantized conductance atomic switch. [J]. Nature, 2005, 433(7021):47-50.
[19] XU L, LI Y, YU N N, et al. Local order origin of thermal stability enhancement in amorphous Ag doping GeTe[J]. Applied Physics Letters, 2015, 106(3):031904.
[20] LI Y, ZHOU Y X, XU L, et al. Realization of functional complete stateful boolean logic in memristive crossbar[J]. Applied Materials and Interfacts.2016,8:34559-54567.
[21] SUN J, HE L B, LO Y C, et al. Liquid-like pseudoelasticity of sub-10-nm crystalline silver particles[J]. Nature Materials,2014,13(11):1007-1012.
[22] ZHANG Q B, SHI Z, YIN K B, et al. Spring-like pseudoelectroelasticity of monocrystalline Cu2S nanowire[J]. Nano Letters, 2018, 18:5070-5077.
[23] 翁素婷,张庆华,谷林. 原位电子显微学方法在材料研究中的应用[J]. 电子显微学报,2019,38(5):556-568.
[24] 董自麒,丁科元,王旭. 相变异质结存储材料相变行为的原位观测[J]. 电子显微学报,2021,40(1):1-6.
[25] CHEN L, LIU Z G, XIA Y D, et al. Electrical field induced precipitation reaction and percolation in Ag30Ge17Se53 amorphous electrolyte films [J]. Applied Physics Letters, 2009, 94(16): 162112.