Nanosized Conducting Filaments Formed by Atomic-Scale Defects in Redox-Based Resistive Switching Memories

被引:70
作者
Du, Hongchu [1 ,2 ]
Jia, Chun-Lin [1 ,3 ,4 ]
Koehl, Annemarie [3 ]
Barthel, Jun [1 ,2 ]
Dittmann, Regina [3 ]
Waser, Rainer [3 ,5 ,6 ]
Mayer, Joachim [1 ,2 ,6 ]
机构
[1] Forschungszentrum Julich, Ernst Ruska Ctr Microscopy & Spect Electrons, D-52425 Julich, Germany
[2] Rhein Westfal TH Aachen, Cent Facil Electron Microscopy GFE, D-52074 Aachen, Germany
[3] Forschungszentrum Julich, Peter Grunberg Inst, D-52425 Julich, Germany
[4] Xi An Jiao Tong Univ, Sch Elect & Informat Engn, Xian 710049, Peoples R China
[5] Rhein Westfal TH Aachen, IWE 2, D-52074 Aachen, Germany
[6] Julich Aachen Res Alliance, Sect Fundamentals Future Informat Technol JARA FI, Julich, Germany
关键词
X-RAY-ABSORPTION; DOPED SRTIO3; OXYGEN VACANCIES; OXIDE; RESISTANCE; DISLOCATIONS; MECHANISMS; RESOLUTION; DEVICES; GROWTH;
D O I
10.1021/acs.chemmater.7b00220
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Redox-based resistive switching phenomena are found in many metal oxides and hold great promise for applications in next-generation memories and neuromorphic computing systems. Resistive switching involves the formation and disruption of electrically conducting filaments through ion migration accompanied by local electrochemical redox reactions. These structural changes are often explained by point defects, but so far clear experimental evidence of such defects is missing. Here, nanosized conducting filaments in Fe doped SrTiO3 thin-film memories are visualized, for the first time, by scanning transmission electron microscopy and core-loss spectroscopy. Conducting filaments are identified by a high local concentration of trivalent titanium ions correlating to oxygen vacancies. Strontium vacancies and lattice distortions also exist in the filaments. Despite a high concentration of defects in the filaments, their general SrTiO3 perovskite structure is essentially preserved. First insights into the switching mechanism are deduced from a snapshot simultaneously showing multiple nanosized filaments in different evolutionary stages. The coexistence of a high Ti3+ concentration along with Sr- and O-vacancies in the conducting filaments provides atomic scale explanations for the resistive switching mechanisms. The results shed unique light on the complexity of the conducting filament formation that cation and anion defects need to be considered jointly.
引用
收藏
页码:3164 / 3173
页数:10
相关论文
共 56 条
[1]   SOFT-X-RAY-ABSORPTION STUDIES OF THE LOCATION OF EXTRA CHARGES INDUCED BY SUBSTITUTION IN CONTROLLED-VALENCE MATERIALS [J].
ABBATE, M ;
DEGROOT, FMF ;
FUGGLE, JC ;
FUJIMORI, A ;
TOKURA, Y ;
FUJISHIMA, Y ;
STREBEL, O ;
DOMKE, M ;
KAINDL, G ;
VANELP, J ;
THOLE, BT ;
SAWATZKY, GA ;
SACCHI, M ;
TSUDA, N .
PHYSICAL REVIEW B, 1991, 44 (11) :5419-5422
[2]   Verification of redox-processes as switching and retention failure mechanisms in Nb:SrTiO3/metal devices [J].
Baeumer, C. ;
Raab, N. ;
Menke, T. ;
Schmitz, C. ;
Rosezin, R. ;
Mueller, P. ;
Andre, M. ;
Feyer, V. ;
Bruchhaus, R. ;
Gunkel, F. ;
Schneider, C. M. ;
Waser, R. ;
Dittmann, R. .
NANOSCALE, 2016, 8 (29) :13967-13975
[3]   Quantifying redox-induced Schottky barrier variations in memristive devices via in operando spectromicroscopy with graphene electrodes [J].
Baeumer, Christoph ;
Schmitz, Christoph ;
Marchewka, Astrid ;
Mueller, David N. ;
Valenta, Richard ;
Hackl, Johanna ;
Raab, Nicolas ;
Rogers, Steven P. ;
Khan, M. Imtiaz ;
Nemsak, Slavomir ;
Shim, Moonsub ;
Menzel, Stephan ;
Schneider, Claus Michael ;
Waser, Rainer ;
Dittmann, Regina .
NATURE COMMUNICATIONS, 2016, 7
[4]  
Barthel J., 2015, J LARGE SCALE RES FA, V1, pA34, DOI [10.17815/jlsrf-1-57, DOI 10.17815/JLSRF-1-57, DOI 10.17815/J1SRF-1-57]
[5]  
Barthel J., 2016, PROBE STEM SIMULATIO
[6]   Probing bonding and electronic structure at atomic resolution with spectroscopic imaging [J].
Botton, Gianluigi A. .
MRS BULLETIN, 2012, 37 (01) :21-28
[7]   Assessment of Strain-Generated Oxygen Vacancies Using SrTiO3 Bicrystals [J].
Choi, Si-Young ;
Kim, Sung-Dae ;
Choi, Minseok ;
Lee, Hak-Sung ;
Ryu, Jungho ;
Shibata, Naoya ;
Mizoguchi, Teruyasu ;
Tochigi, Eita ;
Yamamoto, Takahisa ;
Kang, Suk-Joong L. ;
Ikuhara, Yuichi .
NANO LETTERS, 2015, 15 (06) :4129-4134
[8]   THE SCATTERING OF ELECTRONS BY ATOMS AND CRYSTALS .1. A NEW THEORETICAL APPROACH [J].
COWLEY, JM ;
MOODIE, AF .
ACTA CRYSTALLOGRAPHICA, 1957, 10 (10) :609-619
[9]   OXYGEN 1S X-RAY-ABSORPTION OF TETRAVALENT TITANIUM-OXIDES - A COMPARISON WITH SINGLE-PARTICLE CALCULATIONS [J].
DEGROOT, FMF ;
FABER, J ;
MICHIELS, JJM ;
CZYZYK, MT ;
ABBATE, M ;
FUGGLE, JC .
PHYSICAL REVIEW B, 1993, 48 (04) :2074-2080
[10]   OXYGEN 1S X-RAY-ABSORPTION EDGES OF TRANSITION-METAL OXIDES [J].
DEGROOT, FMF ;
GRIONI, M ;
FUGGLE, JC ;
GHIJSEN, J ;
SAWATZKY, GA ;
PETERSEN, H .
PHYSICAL REVIEW B, 1989, 40 (08) :5715-5723