6710 wileyonlinelibrary.com simple structure, high density, low power consumption, and fast switching speed. [ 1 ] To date, versatile resistive switching phenomena have been reported in various insulating or semiconducting materials, including binary transition metal oxides (NiO, TiO 2 , Ta 2 O 5 , ZnO, and HfO 2 ), [2][3][4][5][6][7] perovskite oxides, [ 8 ] solid electrolytes, [ 9 ] organic materials, [ 10 ] and amorphous Si. [ 11 ] Recently, carbon-based materials such as carbon nanotubes, [ 12,13 ] graphene-like conductive carbon, [ 14 ] and amorphous carbon [ 15,16 ] have also been considered as a potential element for resistance-change materials. Among these, graphene oxide (GO), a graphene sheet decorated with oxygen groups (epoxide, hydroxyl, and carboxyl) on both sides, is one of the most promising candidates owing to its easy methods such as drop casting, spin coating, Langmuir-Blodgett (LB) deposition, and vacuum fi ltration required for the fabrication of uniform thin fi lms. [ 17 ] Besides, the switching properties of GO thin fi lms can be tuned by changing their chemical functionalities through a reduction process [ 18 ] or by mixing with other materials such as polymers, [ 19,20 ] nanoparticles, [ 21 ] and MoS 2 .[ 22 ] Although various GO-based memory devices have been suggested by research groups, [23][24][25][26][27][28] the exact mechanism of bistable resistive switching behavior in GO thin fi lms is still not fully understood.Previously, our group reported the development of a fl exible nonvolatile memory device based on spin-casted GO thin fi lms. [ 29 ] We presented the resistive switching mechanism as the formation and rupture of conducting nanofi laments formed at the amorphous top interface layer (TIL) between a GO thin fi lm and an Al top electrode. To verify a microscopic model of this mechanism, it is crucial to directly observe the existence of conducting fi laments.Herein, we report on the direct visualization of nanoscale metallic fi laments formed at the amorphous TIL during the set process. Using a spherical-aberration-corrected transmission electron microscope (TEM) operated at 80 kV, we obtained crosssectional TEM images of GO thin fi lms sandwiched between two Al electrodes. A quantitative calculation of the structural changes in the GO thin fi lms after top electrode deposition was achieved using the radial distribution function (RDF) of fast Fourier transform (FFT) patterns acquired from the atomicresolution TEM images. In addition, we used atomic-resolution TEM and energy-fi ltered TEM (EFTEM) elemental mapping to identify the origin of the nanoscale metallic fi laments induced
Direct Observation of Conducting Nanofi laments in Graphene-Oxide-Resistive Switching MemorySung Kyu Kim , Jong Yoon Kim , Sung-Yool Choi , * Jeong Yong Lee , * and Hu Young Jeong * Determining the presence of conducting fi laments in resistive random access memory with nanoscale thin fi lms is vital to unraveling resistive switching mechanisms. Bistable resistive switching within graphene-oxide (G...