Stable Metallic Enrichment in Conductive Filaments in TaOx–Based Resistive Switches Arising from Competing Diffusive Fluxes
Abstract
Oxide–based resistive–switching devices hold promise for solid–state memory technology. Information encoding is accomplished by electrically switching the device between two nonvolatile states with low and high resistance states (LRS/HRS). It is generally accepted that the change between these states is due to the motion of oxygen vacancies forming a continuous (LRS) or gapped (HRS) filament between the electrodes. Direct assessments of filaments are rare due to their small size and the difficulty of locating the filament. Electron microscopy experiments reveal the filament structure and chemistry in TaO2.0 ± 0.2–based 150 × 150 nm2 devices with cross–sectional geometry after forming with power dissipation lower than 1 mW. The filaments appear to be roughly hourglass–shaped with a diameter of less than 10 nm and are composed of Ta–rich and O–poor mostly amorphous material with local compositions as Ta–rich as TaO0.4. The as–formed HRS has a gap up to 10 nm wide located next to the anode and composed of nearly stoichiometric TaO2.5. The tantalum and oxygen distribution is consistent with filaments formed by the motion of both Ta and O driven by temperature gradients (Soret effect) and an electric field. As a result, this interpretation points towards a new compact model ofmore »
- Authors:
-
- Carnegie Mellon Univ., Pittsburgh, PA (United States)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1560388
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Advanced Electronic Materials
- Additional Journal Information:
- Journal Volume: 5; Journal Issue: 7; Journal ID: ISSN 2199-160X
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; electroformation; field‐driven diffusion; filaments; resistive switching; Soret effect
Citation Formats
Ma, Yuanzhi, Goodwill, Jonathan M., Li, Dasheng, Cullen, David A., Poplawsky, Jonathan D., More, Karren L., Bain, James A., and Skowronski, Marek. Stable Metallic Enrichment in Conductive Filaments in TaOx–Based Resistive Switches Arising from Competing Diffusive Fluxes. United States: N. p., 2019.
Web. doi:10.1002/aelm.201800954.
Ma, Yuanzhi, Goodwill, Jonathan M., Li, Dasheng, Cullen, David A., Poplawsky, Jonathan D., More, Karren L., Bain, James A., & Skowronski, Marek. Stable Metallic Enrichment in Conductive Filaments in TaOx–Based Resistive Switches Arising from Competing Diffusive Fluxes. United States. https://doi.org/10.1002/aelm.201800954
Ma, Yuanzhi, Goodwill, Jonathan M., Li, Dasheng, Cullen, David A., Poplawsky, Jonathan D., More, Karren L., Bain, James A., and Skowronski, Marek. Mon .
"Stable Metallic Enrichment in Conductive Filaments in TaOx–Based Resistive Switches Arising from Competing Diffusive Fluxes". United States. https://doi.org/10.1002/aelm.201800954. https://www.osti.gov/servlets/purl/1560388.
@article{osti_1560388,
title = {Stable Metallic Enrichment in Conductive Filaments in TaOx–Based Resistive Switches Arising from Competing Diffusive Fluxes},
author = {Ma, Yuanzhi and Goodwill, Jonathan M. and Li, Dasheng and Cullen, David A. and Poplawsky, Jonathan D. and More, Karren L. and Bain, James A. and Skowronski, Marek},
abstractNote = {Oxide–based resistive–switching devices hold promise for solid–state memory technology. Information encoding is accomplished by electrically switching the device between two nonvolatile states with low and high resistance states (LRS/HRS). It is generally accepted that the change between these states is due to the motion of oxygen vacancies forming a continuous (LRS) or gapped (HRS) filament between the electrodes. Direct assessments of filaments are rare due to their small size and the difficulty of locating the filament. Electron microscopy experiments reveal the filament structure and chemistry in TaO2.0 ± 0.2–based 150 × 150 nm2 devices with cross–sectional geometry after forming with power dissipation lower than 1 mW. The filaments appear to be roughly hourglass–shaped with a diameter of less than 10 nm and are composed of Ta–rich and O–poor mostly amorphous material with local compositions as Ta–rich as TaO0.4. The as–formed HRS has a gap up to 10 nm wide located next to the anode and composed of nearly stoichiometric TaO2.5. The tantalum and oxygen distribution is consistent with filaments formed by the motion of both Ta and O driven by temperature gradients (Soret effect) and an electric field. As a result, this interpretation points towards a new compact model of resistive–switching devices.},
doi = {10.1002/aelm.201800954},
journal = {Advanced Electronic Materials},
number = 7,
volume = 5,
place = {United States},
year = {Mon Apr 29 00:00:00 EDT 2019},
month = {Mon Apr 29 00:00:00 EDT 2019}
}
Web of Science
Works referenced in this record:
Effective ionic radii in oxides and fluorides
journal, May 1969
- Shannon, R. D.; Prewitt, C. T.
- Acta Crystallographica Section B Structural Crystallography and Crystal Chemistry, Vol. 25, Issue 5
Electro-Thermal Model of Threshold Switching in TaO x -Based Devices
journal, March 2017
- Goodwill, Jonathan M.; Sharma, Abhishek A.; Li, Dasheng
- ACS Applied Materials & Interfaces, Vol. 9, Issue 13
Anatomy of a Nanoscale Conduction Channel Reveals the Mechanism of a High-Performance Memristor
journal, November 2011
- Miao, Feng; Strachan, John Paul; Yang, J. Joshua
- Advanced Materials, Vol. 23, Issue 47, p. 5633-5640
Spectromicroscopy of tantalum oxide memristors
journal, June 2011
- Strachan, John Paul; Medeiros-Ribeiro, Gilberto; Yang, J. Joshua
- Applied Physics Letters, Vol. 98, Issue 24, Article No. 242114
Electrical transport and thermometry of electroformed titanium dioxide memristive switches
journal, December 2009
- Borghetti, Julien; Strukov, Dmitri B.; Pickett, Matthew D.
- Journal of Applied Physics, Vol. 106, Issue 12
Thermochemical resistive switching: materials, mechanisms, and scaling projections
journal, July 2011
- Ielmini, Daniele; Bruchhaus, Rainer; Waser, Rainer
- Phase Transitions, Vol. 84, Issue 7
Erratum to: The O-Ta (Oxygen-Tantalum) system
journal, August 1997
- Garg, S. P.; Krishnamurthy, N.; Awasthi, A.
- Journal of Phase Equilibria, Vol. 18, Issue 4
Heat transport in thin dielectric films
journal, March 1997
- Lee, S. -M.; Cahill, David G.
- Journal of Applied Physics, Vol. 81, Issue 6
Imaging the Three-Dimensional Conductive Channel in Filamentary-Based Oxide Resistive Switching Memory
journal, November 2015
- Celano, Umberto; Goux, Ludovic; Degraeve, Robin
- Nano Letters, Vol. 15, Issue 12
Z-contrast stem for materials science
journal, June 1989
- Pennycook, S. J.
- Ultramicroscopy, Vol. 30, Issue 1-2
Experimental quantification of annular dark-field images in scanning transmission electron microscopy
journal, November 2008
- LeBeau, James M.; Stemmer, Susanne
- Ultramicroscopy, Vol. 108, Issue 12
Atomic Radii and Interatomic Distances in Metals
journal, March 1947
- Pauling, Linus
- Journal of the American Chemical Society, Vol. 69, Issue 3
Comprehensive Physical Model of Dynamic Resistive Switching in an Oxide Memristor
journal, February 2014
- Kim, Sungho; Choi, ShinHyun; Lu, Wei
- ACS Nano, Vol. 8, Issue 3
Conduction Channel Formation and Dissolution Due to Oxygen Thermophoresis/Diffusion in Hafnium Oxide Memristors
journal, November 2016
- Kumar, Suhas; Wang, Ziwen; Huang, Xiaopeng
- ACS Nano, Vol. 10, Issue 12
Impact of oxygen exchange reaction at the ohmic interface in Ta 2 O 5 -based ReRAM devices
journal, January 2016
- Kim, Wonjoo; Menzel, Stephan; Wouters, Dirk J.
- Nanoscale, Vol. 8, Issue 41
Probing nanoscale oxygen ion motion in memristive systems
journal, May 2017
- Yang, Yuchao; Zhang, Xiaoxian; Qin, Liang
- Nature Communications, Vol. 8, Issue 1
Coexistence of Filamentary and Homogeneous Resistive Switching in Fe-Doped SrTiO3 Thin-Film Memristive Devices
journal, August 2010
- Muenstermann, Ruth; Menke, Tobias; Dittmann, Regina
- Advanced Materials, Vol. 22, Issue 43, p. 4819-4822
Direct Identification of the Conducting Channels in a Functioning Memristive Device
journal, June 2010
- Strachan, John Paul; Pickett, Matthew D.; Yang, J. Joshua
- Advanced Materials, Vol. 22, Issue 32, p. 3573-3577
Transient Thermometry and High-Resolution Transmission Electron Microscopy Analysis of Filamentary Resistive Switches
journal, July 2016
- Kwon, Jonghan; Sharma, Abhishek A.; Chen, Chao-Yang
- ACS Applied Materials & Interfaces, Vol. 8, Issue 31
The mechanism of electroforming of metal oxide memristive switches
journal, May 2009
- Joshua Yang, J.; Miao, Feng; Pickett, Matthew D.
- Nanotechnology, Vol. 20, Issue 21
Separation of current density and electric field domains caused by nonlinear electronic instabilities
journal, May 2018
- Kumar, Suhas; Williams, R. Stanley
- Nature Communications, Vol. 9, Issue 1
Nanoscale cation motion in TaOx, HfOx and TiOx memristive systems
journal, September 2015
- Wedig, Anja; Luebben, Michael; Cho, Deok-Yong
- Nature Nanotechnology, Vol. 11, Issue 1
Analytical Modeling of Oxide-Based Bipolar Resistive Memories and Complementary Resistive Switches
journal, July 2014
- Ambrogio, Stefano; Balatti, Simone; Gilmer, David C.
- IEEE Transactions on Electron Devices, Vol. 61, Issue 7
Avalanche-Discharge-Induced Electrical Forming in Tantalum Oxide-Based Metal-Insulator-Metal Structures
journal, October 2015
- Skaja, Katharina; Bäumer, Christoph; Peters, Oliver
- Advanced Functional Materials, Vol. 25, Issue 46
Effect of thermal insulation on the electrical characteristics of NbO x threshold switches
journal, February 2018
- Wang, Ziwen; Kumar, Suhas; Wong, H. -S. Philip
- Applied Physics Letters, Vol. 112, Issue 7
Nanoionic Resistive Switching Memories: On the Physical Nature of the Dynamic Reset Process
journal, November 2015
- Marchewka, Astrid; Roesgen, Bernd; Skaja, Katharina
- Advanced Electronic Materials, Vol. 2, Issue 1
Memristive devices for computing
journal, January 2013
- Yang, J. Joshua; Strukov, Dmitri B.; Stewart, Duncan R.
- Nature Nanotechnology, Vol. 8, Issue 1, p. 13-24
Physical electro-thermal model of resistive switching in bi-layered resistance-change memory
journal, April 2013
- Kim, Sungho; Kim, Sae-Jin; Kim, Kyung Min
- Scientific Reports, Vol. 3, Issue 1
Effect of voltage polarity and amplitude on electroforming of TiO2 based memristive devices
journal, January 2013
- Jiang, Hao; Xia, Qiangfei
- Nanoscale, Vol. 5, Issue 8
Multiple Memory States in Resistive Switching Devices Through Controlled Size and Orientation of the Conductive Filament
journal, January 2013
- Balatti, S.; Larentis, S.; Gilmer, D. C.
- Advanced Materials, Vol. 25, Issue 10, p. 1474-1478
Direct Observations of Nanofilament Evolution in Switching Processes in HfO 2 -Based Resistive Random Access Memory by In Situ TEM Studies
journal, January 2017
- Li, Chao; Gao, Bin; Yao, Yuan
- Advanced Materials, Vol. 29, Issue 10
Electron energy-loss spectroscopy in the TEM
journal, December 2008
- Egerton, R. F.
- Reports on Progress in Physics, Vol. 72, Issue 1
Complementary Switching in Oxide-Based Bipolar Resistive-Switching Random Memory
journal, January 2013
- Nardi, Federico; Balatti, Simone; Larentis, Stefano
- IEEE Transactions on Electron Devices, Vol. 60, Issue 1
Physical origins of current and temperature controlled negative differential resistances in NbO2
journal, September 2017
- Kumar, Suhas; Wang, Ziwen; Davila, Noraica
- Nature Communications, Vol. 8, Issue 1
Subfilamentary Networks Cause Cycle-to-Cycle Variability in Memristive Devices
journal, July 2017
- Baeumer, Christoph; Valenta, Richard; Schmitz, Christoph
- ACS Nano, Vol. 11, Issue 7
Three-Dimensional Observation of the Conductive Filament in Nanoscaled Resistive Memory Devices
journal, April 2014
- Celano, Umberto; Goux, Ludovic; Belmonte, Attilio
- Nano Letters, Vol. 14, Issue 5
Direct Observation of Localized Radial Oxygen Migration in Functioning Tantalum Oxide Memristors
journal, February 2016
- Kumar, Suhas; Graves, Catherine E.; Strachan, John Paul
- Advanced Materials, Vol. 28, Issue 14
Controlling Conductive Filament and Tributyrin Sensing Using an Optimized Porous Iridium Interfacial Layer in Cu/Ir/TiN x O y /TiN
journal, December 2018
- Dutta, Mrinmoy; Maikap, Siddheswar; Qiu, Jiantai Timothy
- Advanced Electronic Materials
Redox-Based Resistive Switching Memories - Nanoionic Mechanisms, Prospects, and Challenges
journal, July 2009
- Waser, Rainer; Dittmann, Regina; Staikov, Georgi
- Advanced Materials, Vol. 21, Issue 25-26, p. 2632-2663
Modeling the Universal Set/Reset Characteristics of Bipolar RRAM by Field- and Temperature-Driven Filament Growth
journal, December 2011
- Ielmini, Daniele
- IEEE Transactions on Electron Devices, Vol. 58, Issue 12
Resistive Switching by Voltage-Driven Ion Migration in Bipolar RRAM—Part II: Modeling
journal, September 2012
- Larentis, Stefano; Nardi, Federico; Balatti, Simone
- IEEE Transactions on Electron Devices, Vol. 59, Issue 9
A Physics-Based Compact Model of Metal-Oxide-Based RRAM DC and AC Operations
journal, December 2013
- Huang, Peng; Liu, Xiao Yan; Chen, Bing
- IEEE Transactions on Electron Devices, Vol. 60, Issue 12
Characteristic electroforming behavior in Pt/TiO2/Pt resistive switching cells depending on atmosphere
journal, December 2008
- Jeong, Doo Seok; Schroeder, Herbert; Breuer, Uwe
- Journal of Applied Physics, Vol. 104, Issue 12
Physical modeling of the electroforming process in resistive-switching devices
conference, September 2017
- Marchewka, A.; Waser, R.; Menzel, S.
- 2017 International Conference on Simulation of Semiconductor Processes and Devices (SISPAD)
Impact of Joule heating on the microstructure of nanoscale TiO 2 resistive switching devices
journal, April 2013
- Meng Lu, Yi; Noman, Mohammad; Picard, Yoosuf N.
- Journal of Applied Physics, Vol. 113, Issue 16
Oxygen Vacancy Creation, Drift, and Aggregation in TiO 2 -Based Resistive Switches at Low Temperature and Voltage
journal, March 2015
- Kwon, Jonghan; Sharma, Abhishek A.; Bain, James A.
- Advanced Functional Materials, Vol. 25, Issue 19
Thermophoresis/diffusion as a plausible mechanism for unipolar resistive switching in metal–oxide–metal memristors
journal, March 2012
- Strukov, Dmitri B.; Alibart, Fabien; Stanley Williams, R.
- Applied Physics A, Vol. 107, Issue 3
Reduction in the reset current in a resistive random access memory consisting of NiOx brought about by reducing a parasitic capacitance
journal, July 2008
- Kinoshita, K.; Tsunoda, K.; Sato, Y.
- Applied Physics Letters, Vol. 93, Issue 3
Pulse-Programming Instabilities of Unipolar-Type NiOx
journal, June 2010
- Deok-Kee Kim,
- IEEE Electron Device Letters, Vol. 31, Issue 6
Atomic structure of conducting nanofilaments in TiO2 resistive switching memory
journal, January 2010
- Kwon, Deok-Hwang; Kim, Kyung Min; Jang, Jae Hyuck
- Nature Nanotechnology, Vol. 5, Issue 2
Direct Evidence of the Overshoot Suppression in Ta<sub>2</sub>O<sub>5</sub>-Based Resistive Switching Memory With an Integrated Access Resistor
journal, October 2015
- Fan, Yang-Shun; Zhang, Leqi; Crotti, Davide
- IEEE Electron Device Letters, Vol. 36, Issue 10
Sub-10 nm Ta Channel Responsible for Superior Performance of a HfO2 Memristor
journal, June 2016
- Jiang, Hao; Han, Lili; Lin, Peng
- Scientific Reports, Vol. 6, Issue 1
Formation of the Conducting Filament in TaO x -Resistive Switching Devices by Thermal-Gradient-Induced Cation Accumulation
journal, June 2018
- Ma, Yuanzhi; Li, Dasheng; Herzing, Andrew A.
- ACS Applied Materials & Interfaces, Vol. 10, Issue 27
Impact of oxygen exchange reaction at the ohmic interface in Ta2O5-based ReRAM devices.
text, January 2016
- Kim, W.; Menzel, S.; Wouters, Dj
- Apollo - University of Cambridge Repository
Direct Observation of Localized Radial Oxygen Migration in Functioning Tantalum Oxide Memristors
text, January 2016
- Kumar, Suhas; Graves, Catherine E.; Strachan, John Paul
- arXiv
Works referencing / citing this record:
Influence of Nitrogen Adsorption of Doped Ta on Characteristics of SiN x ‐Based Resistive Random Access Memory
journal, September 2019
- Guo, Jingshu; Gao, Haixia; Jiang, Pengfei
- physica status solidi (a), Vol. 216, Issue 22
Metallic filamentary conduction in valence change-based resistive switching devices: the case of TaO x thin film with x ∼ 1
journal, January 2019
- Rosário, Carlos M. M.; Thöner, Bo; Schönhals, Alexander
- Nanoscale, Vol. 11, Issue 36
Intrinsic current overshoot during thermal-runaway threshold switching events in TaO x devices
journal, July 2019
- Goodwill, Jonathan M.; Skowronski, Marek
- Journal of Applied Physics, Vol. 126, Issue 3
Nanoscale density variations in sputtered amorphous TaO x functional layers in resistive switching devices
journal, February 2020
- Xu, Qiyun; Ma, Yuanzhi; Skowronski, Marek
- Journal of Applied Physics, Vol. 127, Issue 5