Filament Formation in TaO x Thin Films for Memristor Device Application: Modeling Electron Energy Loss Spectra and Electron Transport

Jiang, Jie; Pachter, Ruth; Mahalingam, Krishnamurthy; Ciston, Jim; Dhall, Rohan; Bondi, Robert J.; Marinella, Matthew J.; Telesca, Donald A.; Ganguli, Sabyasachi

doi:10.1002/aelm.202200828

Title: Filament Formation in TaO _x Thin Films for Memristor Device Application: Modeling Electron Energy Loss Spectra and Electron Transport

Journal Article · Thu Oct 20 00:00:00 EDT 2022 · Advanced Electronic Materials

DOI:https://doi.org/10.1002/aelm.202200828· OSTI ID:1894172

Jiang, Jie ^[1];

^[1]; Mahalingam, Krishnamurthy ^[1]; Ciston, Jim ^[2]; Dhall, Rohan ^[2]; Bondi, Robert J. ^[3]; Marinella, Matthew J. ^[4]; Telesca, Donald A. ^[5]; Ganguli, Sabyasachi ^[1]

Air Force Research Laboratory Materials and Manufacturing Directorate Wright‐Patterson Air Force Base Dayton OH 45433 USA
National Center for Electron Microscopy Molecular Foundry Lawrence Berkeley National Laboratory Berkeley CA 94720 USA
Quantum Generative Materials LLC Cheyenne WY 82001 USA
School of Electrical Computer and Energy Engineering Arizona State University Tempe AZ 85281 USA
Air Force Research Laboratory Information Directorate Rome NY 13441 USA

Abstract Although understanding filament formation in oxide‐based memristive devices by theory has emerged, there are still fundamental unanswered questions. Importantly, for practical application of thin films the material in its amorphous state is to be considered, but mostly lacking so far, and details on sub‐stoichiometry are also scarce. To gain insight into the optical and electronic properties of sub‐stoichiometric amorphous tantalum oxide (TaO _x ), the electron energy loss spectrum (EELS) of model systems is characterized theoretically and electron transport characteristics are analyzed in detail. Calculated blue‐shifts by increasing sub‐stoichiometry explained the measurements, potentially suggesting estimation of oxygen vacancy concentrations through EEL spectra. Electron transport results based on TaO _x material models validated by EELS measurements show that oxygen vacancy filamentary paths are initiated at low bias upon increasing sub‐stoichiometry yet noting an interplay with the local amorphous structure. Contact resistances at interfaces of the TaO _x switching layer and a tantalum scavenging layer or titanium nitride electrode are quantified, indicating the possibility for either oxygen vacancy‐ or metal cluster‐based conduction mechanisms at the interface. The computational work, combined with experimental characterization for validation, provides a basis for investigating effects of sub‐stoichiometry on filament formation in TaO _x thin film memristive devices.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: DE‐AC02‐05CH11231; AC02-05CH11231

OSTI ID:: 1894172

Alternate ID(s):: OSTI ID: 1894173; OSTI ID: 1992472

Journal Information:: Advanced Electronic Materials, Journal Name: Advanced Electronic Materials Vol. 9 Journal Issue: 1; ISSN 2199-160X

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: United States

Language:: English

References (58)

Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Simulation of TaOx-based complementary resistive switches by a physics-based memristive model Siemon, A.; Menzel, S.; Marchewka, A. 2014 IEEE International Symposium on Circuits and Systems (ISCAS) https://doi.org/10.1109/ISCAS.2014.6865411	conference	June 2014
Hybrid functionals based on a screened Coulomb potential Heyd, Jochen; Scuseria, Gustavo E.; Ernzerhof, Matthias The Journal of Chemical Physics, Vol. 118, Issue 18 https://doi.org/10.1063/1.1564060	journal	May 2003
Memristor modeling: challenges in theories, simulations, and device variability Gao, Lili; Ren, Qingying; Sun, Jiawei Journal of Materials Chemistry C, Vol. 9, Issue 47 https://doi.org/10.1039/D1TC04201G	journal	January 2021
Synergistic Resistive Switching Mechanism of Oxygen Vacancies and Metal Interstitials in Ta ₂ O ₅ Zhu, Linggang; Zhou, Jian; Guo, Zhonglu The Journal of Physical Chemistry C, Vol. 120, Issue 4 https://doi.org/10.1021/acs.jpcc.5b11080	journal	January 2016
Electrical conductivity in oxygen-deficient phases of tantalum pentoxide from first-principles calculations Bondi, Robert J.; Desjarlais, Michael P.; Thompson, Aidan P. Journal of Applied Physics, Vol. 114, Issue 20 https://doi.org/10.1063/1.4829900	journal	November 2013
Oxidation state and interfacial effects on oxygen vacancies in tantalum pentoxide Bondi, Robert J.; Marinella, Matthew J. Journal of Applied Physics, Vol. 117, Issue 8 https://doi.org/10.1063/1.4913206	journal	February 2015
Density-functional study of bulk and surface properties of titanium nitride using different exchange-correlation functionals Marlo, M.; Milman, V. Physical Review B, Vol. 62, Issue 4 https://doi.org/10.1103/PhysRevB.62.2899	journal	July 2000
From ultrasoft pseudopotentials to the projector augmented-wave method Kresse, G.; Joubert, D. Physical Review B, Vol. 59, Issue 3, p. 1758-1775 https://doi.org/10.1103/PhysRevB.59.1758	journal	January 1999
Chemical Structure of Conductive Filaments in Tantalum Oxide Memristive Devices and Its Implications for the Formation Mechanism Heisig, Thomas; Lange, Kristof; Gutsche, Alexander Advanced Electronic Materials, Vol. 8, Issue 8 https://doi.org/10.1002/aelm.202100936	journal	February 2022
Ab initio reflectance difference spectra of the bare and adsorbate covered Cu(110) surfaces Harl, J.; Kresse, G.; Sun, L. D. Physical Review B, Vol. 76, Issue 3 https://doi.org/10.1103/PhysRevB.76.035436	journal	July 2007
Density functional theory study of TiO $_{2}$ /Ag interfaces and their role in memristor devices Prada, Stefano; Rosa, Massimo; Giordano, Livia Physical Review B, Vol. 83, Issue 24 https://doi.org/10.1103/PhysRevB.83.245314	journal	June 2011
Electron correlation in semiconductors and insulators: Band gaps and quasiparticle energies Hybertsen, Mark S.; Louie, Steven G. Physical Review B, Vol. 34, Issue 8, p. 5390-5413 https://doi.org/10.1103/PhysRevB.34.5390	journal	October 1986
Extrinsic Dopant Effects on Oxygen Vacancy Formation Energies in ZrO₂ with Implication for Memristive Device Performance Yildirim, Handan; Pachter, Ruth ACS Applied Electronic Materials, Vol. 1, Issue 4 https://doi.org/10.1021/acsaelm.8b00090	journal	March 2019
First principles study of oxygen vacancy defects in tantalum pentoxide Ramprasad, R. Journal of Applied Physics, Vol. 94, Issue 9 https://doi.org/10.1063/1.1615700	journal	November 2003
Application of the Quantum-Point-Contact Formalism to Model the Filamentary Conduction in Ta 2 O 5 -Based Resistive Switching Devices Andrade, Jaime M. M.; Rosário, Carlos M. M.; Menzel, Stephan Physical Review Applied, Vol. 17, Issue 3 https://doi.org/10.1103/PhysRevApplied.17.034062	journal	March 2022
Memristor-The missing circuit element Chua, L. IEEE Transactions on Circuit Theory, Vol. 18, Issue 5 https://doi.org/10.1109/TCT.1971.1083337	journal	January 1971
Using Dopants to Tune Oxygen Vacancy Formation in Transition Metal Oxide Resistive Memory Jiang, Hao; Stewart, Derek A. ACS Applied Materials & Interfaces, Vol. 9, Issue 19 https://doi.org/10.1021/acsami.7b00139	journal	May 2017
Phase separation in amorphous tantalum oxide from first principles Pedersen, Christian Søndergaard; Chang, Jin Hyun; Li, Yang APL Materials, Vol. 8, Issue 7 https://doi.org/10.1063/5.0011390	journal	July 2020
Density-functional method for nonequilibrium electron transport Brandbyge, Mads; Mozos, José-Luis; Ordejón, Pablo Physical Review B, Vol. 65, Issue 16, Article No. 165401 https://doi.org/10.1103/PhysRevB.65.165401	journal	March 2002
Memristive switching mechanism for metal/oxide/metal nanodevices Yang, J. Joshua; Pickett, Matthew D.; Li, Xuema Nature Nanotechnology, Vol. 3, Issue 7 https://doi.org/10.1038/nnano.2008.160	journal	June 2008
Quantitative, Dynamic TaO _x Memristor/Resistive Random Access Memory Model Lee, Seung Hwan; Moon, John; Jeong, YeonJoo ACS Applied Electronic Materials, Vol. 2, Issue 3 https://doi.org/10.1021/acsaelm.9b00792	journal	February 2020
Exploring local currents in molecular junctions Solomon, Gemma C.; Herrmann, Carmen; Hansen, Thorsten Nature Chemistry, Vol. 2, Issue 3 https://doi.org/10.1038/nchem.546	journal	February 2010
In situ observation of filamentary conducting channels in an asymmetric Ta2O5−x/TaO2−x bilayer structure Park, Gyeong-Su; Kim, Young Bae; Park, Seong Yong Nature Communications, Vol. 4, Issue 1 https://doi.org/10.1038/ncomms3382	journal	September 2013
The missing memristor found Strukov, Dmitri B.; Snider, Gregory S.; Stewart, Duncan R. Nature, Vol. 453, Issue 7191 https://doi.org/10.1038/nature06932	journal	May 2008
Role of atomistic structure in the stochastic nature of conductivity in substoichiometric tantalum pentoxide Bondi, Robert J.; Fox, Brian P.; Marinella, Matthew J. Journal of Applied Physics, Vol. 119, Issue 12 https://doi.org/10.1063/1.4943163	journal	March 2016
Controlling the TiN Electrode Work Function at the Atomistic Level: A First Principles Investigation Calzolari, Arrigo; Catellani, Alessandra IEEE Access, Vol. 8 https://doi.org/10.1109/ACCESS.2020.3017726	journal	January 2020
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set Kresse, G.; Furthmüller, J. Computational Materials Science, Vol. 6, Issue 1, p. 15-50 https://doi.org/10.1016/0927-0256(96)00008-0	journal	July 1996
Sub-nanosecond switching of a tantalum oxide memristor Torrezan, Antonio C.; Strachan, John Paul; Medeiros-Ribeiro, Gilberto Nanotechnology, Vol. 22, Issue 48 https://doi.org/10.1088/0957-4484/22/48/485203	journal	November 2011
Reactive sputtering of substoichiometric Ta₂O_x for resistive memory applications Stevens, James E.; Lohn, Andrew J.; Decker, Seth A. Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 32, Issue 2, Article No. 021501 https://doi.org/10.1116/1.4828701	journal	March 2014
Influence of the exchange screening parameter on the performance of screened hybrid functionals Krukau, Aliaksandr V.; Vydrov, Oleg A.; Izmaylov, Artur F. The Journal of Chemical Physics, Vol. 125, Issue 22 https://doi.org/10.1063/1.2404663	journal	December 2006
Electronic structure of β-Ta films from X-ray photoelectron spectroscopy and first-principles calculations Magnuson, Martin; Greczynski, Grzegorz; Eriksson, Fredrik Applied Surface Science, Vol. 470 https://doi.org/10.1016/j.apsusc.2018.11.096	journal	March 2019
On the Theory of Dispersion of X-Rays de L. Kronig, R. Journal of the Optical Society of America, Vol. 12, Issue 6 https://doi.org/10.1364/JOSA.12.000547	journal	January 1926
Ab initio pseudopotentials for electronic structure calculations of poly-atomic systems using density-functional theory Fuchs, Martin; Scheffler, Matthias Computer Physics Communications, Vol. 119, Issue 1 https://doi.org/10.1016/S0010-4655(98)00201-X	journal	June 1999
Non-metallic dopant modulation of conductivity in substoichiometric tantalum pentoxide: A first-principles study Bondi, Robert J.; Fox, Brian P.; Marinella, Matthew J. Journal of Applied Physics, Vol. 121, Issue 21 https://doi.org/10.1063/1.4983850	journal	June 2017
Materials selection for oxide-based resistive random access memories Guo, Yuzheng; Robertson, John Applied Physics Letters, Vol. 105, Issue 22 https://doi.org/10.1063/1.4903470	journal	December 2014
Oxygen vacancy effects in HfO₂-based resistive switching memory: First principle study Dai, Yuehua; Pan, Zhiyong; Wang, Feifei AIP Advances, Vol. 6, Issue 8 https://doi.org/10.1063/1.4961229	journal	August 2016
New Method for Calculating the One-Particle Green's Function with Application to the Electron-Gas Problem Hedin, Lars Physical Review, Vol. 139, Issue 3A https://doi.org/10.1103/PhysRev.139.A796	journal	August 1965
Smooth Interfacial Scavenging for Resistive Switching Oxide via the Formation of Highly Uniform Layers of Amorphous TaO_x Tsurumaki-Fukuchi, Atsushi; Nakagawa, Ryosuke; Arita, Masashi ACS Applied Materials & Interfaces, Vol. 10, Issue 6 https://doi.org/10.1021/acsami.7b15384	journal	February 2018
Evaluating tantalum oxide stoichiometry and oxidation states for optimal memristor performance Brumbach, Michael T.; Mickel, Patrick R.; Lohn, Andrew J. Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 32, Issue 5 https://doi.org/10.1116/1.4893929	journal	September 2014
An empirical model for silver tantalate Gao, H.; Otero-de-la-Roza, A.; Aouadi, S. M. Modelling and Simulation in Materials Science and Engineering, Vol. 21, Issue 5 https://doi.org/10.1088/0965-0393/21/5/055002	journal	May 2013
Band alignment between Ta₂O₅ and metals for resistive random access memory electrodes engineering Zhuo, V. Y. -Q.; Jiang, Y.; Li, M. H. Applied Physics Letters, Vol. 102, Issue 6 https://doi.org/10.1063/1.4792274	journal	February 2013
A high-energy electron scattering study of the electronic structure and elemental composition of O-implanted Ta films used for the fabrication of memristor devices Vos, M.; Grande, P. L.; Nandi, S. K. Journal of Applied Physics, Vol. 114, Issue 7 https://doi.org/10.1063/1.4818524	journal	August 2013
Mechanistic Analysis of Oxygen Vacancy-Driven Conductive Filament Formation in Resistive Random Access Memory Metal/NiO/Metal Structures Yildirim, Handan; Pachter, Ruth ACS Applied Materials & Interfaces, Vol. 10, Issue 11 https://doi.org/10.1021/acsami.7b17645	journal	February 2018
Redox-Based Resistive Switching Memories - Nanoionic Mechanisms, Prospects, and Challenges Waser, Rainer; Dittmann, Regina; Staikov, Georgi Advanced Materials, Vol. 21, Issue 25-26, p. 2632-2663 https://doi.org/10.1002/adma.200900375	journal	July 2009
Linear optical properties in the projector-augmented wave methodology Gajdoš, M.; Hummer, K.; Kresse, G. Physical Review B, Vol. 73, Issue 4 https://doi.org/10.1103/PhysRevB.73.045112	journal	January 2006
Photoelectron diffraction determination of the geometry of a clean metal surface: Ta(100) Bartynski, R. A.; Heskett, D.; Garrison, K. Physical Review B, Vol. 40, Issue 8 https://doi.org/10.1103/PhysRevB.40.5340	journal	September 1989
Origin of the Ultra-nonlinear Switching Kinetics in Oxide-Based Resistive Switches Menzel, Stephan; Waters, Matthias; Marchewka, Astrid Advanced Functional Materials, Vol. 21, Issue 23 https://doi.org/10.1002/adfm.201101117	journal	September 2011
A physical model of switching dynamics in tantalum oxide memristive devices Mickel, Patrick R.; Lohn, Andrew J.; Joon Choi, Byung Applied Physics Letters, Vol. 102, Issue 22, Article No. 223502 https://doi.org/10.1063/1.4809530	journal	June 2013
Reduction of the forming voltage through tailored oxygen non-stoichiometry in tantalum oxide ReRAM devices Skaja, Katharina; Andrä, Michael; Rana, Vikas Scientific Reports, Vol. 8, Issue 1 https://doi.org/10.1038/s41598-018-28992-9	journal	July 2018
Diffusion of oxygen in amorphous tantalum oxide Stewart, Derek A. Physical Review Materials, Vol. 3, Issue 5 https://doi.org/10.1103/PhysRevMaterials.3.055605	journal	May 2019
Spatial Variation of Currents and Fields Due to Localized Scatterers in Metallic Conduction Landauer, R. IBM Journal of Research and Development, Vol. 1, Issue 3 https://doi.org/10.1147/rd.13.0223	journal	July 1957
A fast, high-endurance and scalable non-volatile memory device made from asymmetric Ta₂O_5−x/TaO_2−x bilayer structures Lee, Myoung-Jae; Lee, Chang Bum; Lee, Dongsoo Nature Materials, Vol. 10, Issue 8, p. 625-630 https://doi.org/10.1038/nmat3070	journal	July 2011
Review of memristor devices in neuromorphic computing: materials sciences and device challenges Li, Yibo; Wang, Zhongrui; Midya, Rivu Journal of Physics D: Applied Physics, Vol. 51, Issue 50 https://doi.org/10.1088/1361-6463/aade3f	journal	September 2018
Characteristics and transport mechanisms of triple switching regimes of TaO_x memristor Lian, Xiaojuan; Wang, Miao; Rao, Mingyi Applied Physics Letters, Vol. 110, Issue 17 https://doi.org/10.1063/1.4982593	journal	April 2017
QuantumATK: an integrated platform of electronic and atomic-scale modelling tools Smidstrup, Søren; Markussen, Troels; Vancraeyveld, Pieter Journal of Physics: Condensed Matter, Vol. 32, Issue 1 https://doi.org/10.1088/1361-648X/ab4007	journal	October 2019
Resistive switching memories based on metal oxides: mechanisms, reliability and scaling Ielmini, Daniele Semiconductor Science and Technology, Vol. 31, Issue 6 https://doi.org/10.1088/0268-1242/31/6/063002	journal	May 2016
Resistive switching materials for information processing Wang, Zhongrui; Wu, Huaqiang; Burr, Geoffrey W. Nature Reviews Materials, Vol. 5, Issue 3 https://doi.org/10.1038/s41578-019-0159-3	journal	January 2020

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36 MATERIALS SCIENCE
conducting filaments
density functional theory
electron energy loss spectrum
electron transport
memristors
thin film TaOx

Title: Filament Formation in TaO x Thin Films for Memristor Device Application: Modeling Electron Energy Loss Spectra and Electron Transport

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Title: Filament Formation in TaO _x Thin Films for Memristor Device Application: Modeling Electron Energy Loss Spectra and Electron Transport