DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Highly Uniform Resistive Switching in HfO2 Films Embedded with Ordered Metal Nanoisland Arrays

Abstract

Abstract Memristors enter a critical developmental stage where emerging large‐scale integration methods face major challenges with severe switching instabilities in the oxide layer. Here, the superior uniformity is achieved within HfO 2 films by embedding highly ordered metal nanoisland (NI) arrays. Embedded films exhibit a significant reduction in both SET and RESET while displaying enhanced uniformity in operating voltages and resistance states. This behavior is attributed to the concentration of electric fields along Pt and Ti NIs and their interactions with the surrounding oxide film matrix environment, which induce separate and distinct filamentary formation mechanisms that affect the stability. A method is reported to further optimize the uniformity of the SET voltage by translating the NI array position down the film‐thickness dimension towards the bottom electrode. A comparison of the density and distribution of the oxygen vacancies responsible for the formation/dissolution of conducting filaments is made via combined electrostatic force microscopy and conductive atomic force microscopy (c‐AFM) studies. Finally, complete observation of the morphological evolution of conducting filaments produced by Pt and Ti is enabled by 3D c‐AFM nanotomography and cross‐sectional scanning transmission electron microscopy–energy dispersive spectroscopy to provide direct correlations between NI‐oxide interactions and overall switching performance.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [1]
  1. Univ. of Massachusetts, Amherst, MA (United States)
  2. Univ. of California, Irvine, CA (United States)
Publication Date:
Research Org.:
Univ. of California, Irvine, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; National Science Foundation (NSF); USDOE
OSTI Identifier:
1612194
Alternate Identifier(s):
OSTI ID: 1507442
Grant/Contract Number:  
SC0014430; CMMI-1025020; CBET-1706113; DMR-1629270; DMR-1506535; DE‐SC0014430
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Functional Materials
Additional Journal Information:
Journal Volume: 29; Journal Issue: 25; Journal ID: ISSN 1616-301X
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; chemistry; science & technology; materials science; physics; filamentary conduction; memristor; nanotomography; oxygen vacancies; resistive switching

Citation Formats

Wang, Jiaying, Li, Linze, Huyan, Huaixun, Pan, Xiaoqing, and Nonnenmann, Stephen S. Highly Uniform Resistive Switching in HfO2 Films Embedded with Ordered Metal Nanoisland Arrays. United States: N. p., 2019. Web. doi:10.1002/adfm.201808430.
Wang, Jiaying, Li, Linze, Huyan, Huaixun, Pan, Xiaoqing, & Nonnenmann, Stephen S. Highly Uniform Resistive Switching in HfO2 Films Embedded with Ordered Metal Nanoisland Arrays. United States. https://doi.org/10.1002/adfm.201808430
Wang, Jiaying, Li, Linze, Huyan, Huaixun, Pan, Xiaoqing, and Nonnenmann, Stephen S. Tue . "Highly Uniform Resistive Switching in HfO2 Films Embedded with Ordered Metal Nanoisland Arrays". United States. https://doi.org/10.1002/adfm.201808430. https://www.osti.gov/servlets/purl/1612194.
@article{osti_1612194,
title = {Highly Uniform Resistive Switching in HfO2 Films Embedded with Ordered Metal Nanoisland Arrays},
author = {Wang, Jiaying and Li, Linze and Huyan, Huaixun and Pan, Xiaoqing and Nonnenmann, Stephen S.},
abstractNote = {Abstract Memristors enter a critical developmental stage where emerging large‐scale integration methods face major challenges with severe switching instabilities in the oxide layer. Here, the superior uniformity is achieved within HfO 2 films by embedding highly ordered metal nanoisland (NI) arrays. Embedded films exhibit a significant reduction in both SET and RESET while displaying enhanced uniformity in operating voltages and resistance states. This behavior is attributed to the concentration of electric fields along Pt and Ti NIs and their interactions with the surrounding oxide film matrix environment, which induce separate and distinct filamentary formation mechanisms that affect the stability. A method is reported to further optimize the uniformity of the SET voltage by translating the NI array position down the film‐thickness dimension towards the bottom electrode. A comparison of the density and distribution of the oxygen vacancies responsible for the formation/dissolution of conducting filaments is made via combined electrostatic force microscopy and conductive atomic force microscopy (c‐AFM) studies. Finally, complete observation of the morphological evolution of conducting filaments produced by Pt and Ti is enabled by 3D c‐AFM nanotomography and cross‐sectional scanning transmission electron microscopy–energy dispersive spectroscopy to provide direct correlations between NI‐oxide interactions and overall switching performance.},
doi = {10.1002/adfm.201808430},
journal = {Advanced Functional Materials},
number = 25,
volume = 29,
place = {United States},
year = {Tue Apr 16 00:00:00 EDT 2019},
month = {Tue Apr 16 00:00:00 EDT 2019}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 30 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Role of Ti Electrode on the Electrical Characterization of Filament within Al 2 O 3 Based Antifuse
journal, January 2018

  • Tian, Min; Xu, Jing; Zhong, Huicai
  • ECS Journal of Solid State Science and Technology, Vol. 7, Issue 4
  • DOI: 10.1149/2.0051804jss

Tip loading effects on AFM-based transport measurements of metal–oxide interfaces
journal, September 2013


Interfacial Metal–Oxide Interactions in Resistive Switching Memories
journal, May 2017

  • Cho, Deok-Yong; Luebben, Michael; Wiefels, Stefan
  • ACS Applied Materials & Interfaces, Vol. 9, Issue 22
  • DOI: 10.1021/acsami.7b02921

Interfacial interactions and their impact on redox-based resistive switching memories (ReRAMs)
journal, August 2017


Imaging the Three-Dimensional Conductive Channel in Filamentary-Based Oxide Resistive Switching Memory
journal, November 2015


Controlled synthesis of Ni/CuOx/Ni nanowires by electrochemical deposition with self-compliance bipolar resistive switching
journal, March 2016

  • Park, Kyuhyun; Lee, Jang-Sik
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep23069

On the Switching Parameter Variation of Metal-Oxide RRAM—Part I: Physical Modeling and Simulation Methodology
journal, April 2012

  • Guan, Ximeng; Yu, Shimeng; Wong, H. -S. Philip
  • IEEE Transactions on Electron Devices, Vol. 59, Issue 4
  • DOI: 10.1109/TED.2012.2184545

Nonvolatile Memristive Switching Characteristics of TiO$_{\bm 2}$ Films Embedded With Nickel Nanocrystals
journal, January 2012

  • Panda, Debashis; Dhar, Achintya; Ray, Samit K.
  • IEEE Transactions on Nanotechnology, Vol. 11, Issue 1
  • DOI: 10.1109/TNANO.2011.2132142

Probing nanoscale oxygen ion motion in memristive systems
journal, May 2017

  • Yang, Yuchao; Zhang, Xiaoxian; Qin, Liang
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/ncomms15173

Enhancement of resistive switching properties in Al 2 O 3 bilayer-based atomic switches: multilevel resistive switching
journal, April 2018


Resistive Switching Mechanism in $\hbox{Zn}_{x}\hbox{Cd}_{1 - x}\hbox{S}$ Nonvolatile Memory Devices
journal, January 2007

  • Wang, Zheng; Griffin, Peter B.; McVittie, Jim
  • IEEE Electron Device Letters, Vol. 28, Issue 1
  • DOI: 10.1109/LED.2006.887640

Nonvolatile resistive switching memory utilizing gold nanocrystals embedded in zirconium oxide
journal, August 2007

  • Guan, Weihua; Long, Shibing; Jia, Rui
  • Applied Physics Letters, Vol. 91, Issue 6
  • DOI: 10.1063/1.2760156

Enhanced resistive switching characteristics in Al 2 O 3 memory devices by embedded Ag nanoparticles
journal, May 2017


Robust unipolar resistive switching of Co nano-dots embedded ZrO 2 thin film memories and their switching mechanism
journal, January 2012

  • Wu, Ming-Chi; Wu, Tsung-Han; Tseng, Tseung-Yuen
  • Journal of Applied Physics, Vol. 111, Issue 1
  • DOI: 10.1063/1.3674322

Growth of TiO x overlayers by chemical vapour deposition on a single-crystal copper substrate
journal, January 1994

  • Wu, Yuan Min; Nix, Roger M.
  • Journal of Materials Chemistry, Vol. 4, Issue 9
  • DOI: 10.1039/jm9940401403

Ag-NPs doping enhanced resistive switching performance and induced changes in magnetic properties of NiFe 2 O 4 thin films
journal, January 2017

  • Hao, Aize; Ismail, Muhammad; He, Shuai
  • RSC Adv., Vol. 7, Issue 74
  • DOI: 10.1039/C7RA08756J

Enhanced resistive switching in forming-free graphene oxide films embedded with gold nanoparticles deposited by electrophoresis
journal, November 2015


In depth nano spectroscopic analysis on homogeneously switching double barrier memristive devices
journal, June 2017

  • Strobel, Julian; Hansen, Mirko; Dirkmann, Sven
  • Journal of Applied Physics, Vol. 121, Issue 24
  • DOI: 10.1063/1.4990145

Enhancement of Resistive Switching Characteristics in $ \hbox{Al}_{2}\hbox{O}_{3}$-Based RRAM With Embedded Ruthenium Nanocrystals
journal, June 2011


Effects of Titanium Layer Oxygen Scavenging on the High- k /InGaAs Interface
journal, June 2016

  • Winter, Roy; Shekhter, Pini; Tang, Kechao
  • ACS Applied Materials & Interfaces, Vol. 8, Issue 26
  • DOI: 10.1021/acsami.6b02957

Dynamic ‘hour glass’ model for SET and RESET in HfO2 RRAM
conference, June 2012

  • Degraeve, R.; Fantini, A.; Clima, S.
  • 2012 IEEE Symposium on VLSI Technology, 2012 Symposium on VLSI Technology (VLSIT)
  • DOI: 10.1109/VLSIT.2012.6242468

Highly Improved Uniformity in the Resistive Switching Parameters of TiO 2 Thin Films by Inserting Ru Nanodots
journal, February 2013

  • Yoon, Jung Ho; Han, Jeong Hwan; Jung, Ji Sim
  • Advanced Materials, Vol. 25, Issue 14
  • DOI: 10.1002/adma.201204572

Reliable Control of Filament Formation in Resistive Memories by Self-Assembled Nanoinsulators Derived from a Block Copolymer
journal, August 2014

  • You, Byoung Kuk; Park, Woon Ik; Kim, Jong Min
  • ACS Nano, Vol. 8, Issue 9
  • DOI: 10.1021/nn503713f

Filament observation in metal-oxide resistive switching devices
journal, March 2013

  • Celano, Umberto; Yin Chen, Yang; Wouters, Dirk J.
  • Applied Physics Letters, Vol. 102, Issue 12
  • DOI: 10.1063/1.4798525

Current rectifying and resistive switching in high density BiFeO3 nanocapacitor arrays on Nb-SrTiO3 substrates
journal, April 2015

  • Zhao, Lina; Lu, Zengxing; Zhang, Fengyuan
  • Scientific Reports, Vol. 5, Issue 1
  • DOI: 10.1038/srep09680

Statistical Fluctuations in HfO<sub><italic><bold>x</bold></italic></sub> Resistive-Switching Memory: Part I - Set/Reset Variability
journal, August 2014

  • Ambrogio, Stefano; Balatti, Simone; Cubeta, Antonio
  • IEEE Transactions on Electron Devices, Vol. 61, Issue 8
  • DOI: 10.1109/TED.2014.2330200

Resistive switching and its suppression in Pt/Nb:SrTiO3 junctions
journal, June 2014

  • Mikheev, Evgeny; Hoskins, Brian D.; Strukov, Dmitri B.
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms4990

Unipolar resistive switching of ZnO-single-wire memristors
journal, January 2014


Memristive switching mechanism for metal/oxide/metal nanodevices
journal, June 2008

  • Yang, J. Joshua; Pickett, Matthew D.; Li, Xuema
  • Nature Nanotechnology, Vol. 3, Issue 7
  • DOI: 10.1038/nnano.2008.160

Resistive switching characteristics of a Pt nanoparticle-embedded SiO2-based memory
journal, February 2013


Ferroelectric properties and switching endurance of Hf 0.5 Zr 0.5 O 2 films on TiN bottom and TiN or RuO 2 top electrodes : Ferroelectric properties and switching endurance of Hf
journal, February 2014

  • Park, Min Hyuk; Kim, Han Joon; Kim, Yu Jin
  • physica status solidi (RRL) - Rapid Research Letters, Vol. 8, Issue 6
  • DOI: 10.1002/pssr.201409017

Nanoionics-based resistive switching memories
journal, November 2007

  • Waser, Rainer; Aono, Masakazu
  • Nature Materials, Vol. 6, Issue 11, p. 833-840
  • DOI: 10.1038/nmat2023

Multifilamentary Conduction Modeling in Transition Metal Oxide-Based RRAM
journal, August 2017


Nitrogen-induced improvement of resistive switching uniformity in a HfO 2 -based RRAM device
journal, October 2012


Subfilamentary Networks Cause Cycle-to-Cycle Variability in Memristive Devices
journal, July 2017


Detailed leakage current analysis of metal–insulator–metal capacitors with ZrO 2 , ZrO 2 /SiO 2 /ZrO 2 , and ZrO 2 /Al 2 O 3 /ZrO 2 as dielectric and TiN electrodes
journal, January 2013

  • Weinreich, Wenke; Shariq, Ahmed; Seidel, Konrad
  • Journal of Vacuum Science & Technology B, Nanotechnology and Microelectronics: Materials, Processing, Measurement, and Phenomena, Vol. 31, Issue 1
  • DOI: 10.1116/1.4768791

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
  • DOI: 10.1021/nl500049g

Resistive Random Access Memory (ReRAM) Based on Metal Oxides
journal, December 2010


Nanosized Conducting Filaments Formed by Atomic-Scale Defects in Redox-Based Resistive Switching Memories
journal, March 2017


Fully Room-Temperature-Fabricated Nonvolatile Resistive Memory for Ultrafast and High-Density Memory Application
journal, April 2009

  • Yang, Yu Chao; Pan, Feng; Liu, Qi
  • Nano Letters, Vol. 9, Issue 4
  • DOI: 10.1021/nl900006g

Nanoscopic structural rearrangements of the Cu-filament in conductive-bridge memories
journal, January 2016


Metallization-induced damage in III–V semiconductors
journal, November 1998

  • Chen, Ching-Hui
  • Journal of Vacuum Science & Technology B: Microelectronics and Nanometer Structures, Vol. 16, Issue 6
  • DOI: 10.1116/1.590381

Electrochemical dynamics of nanoscale metallic inclusions in dielectrics
journal, June 2014

  • Yang, Yuchao; Gao, Peng; Li, Linze
  • Nature Communications, Vol. 5, Article No. 4232
  • DOI: 10.1038/ncomms5232

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
  • DOI: 10.1002/adma.200900375

Ferroelectric Resistive Switching in High-Density Nanocapacitor Arrays Based on BiFeO 3 Ultrathin Films and Ordered Pt Nanoelectrodes
journal, August 2016

  • Lu, Zengxing; Fan, Zhen; Li, Peilian
  • ACS Applied Materials & Interfaces, Vol. 8, Issue 36
  • DOI: 10.1021/acsami.6b07792

Field-driven migration of bipolar metal particles on solid electrolytes
journal, August 2008

  • Peppler, Klaus; Reitz, Christian; Janek, Jürgen
  • Applied Physics Letters, Vol. 93, Issue 7
  • DOI: 10.1063/1.2973042

Conductance tomography of conductive filaments in intrinsic silicon-rich silica RRAM
journal, January 2015

  • Buckwell, Mark; Montesi, Luca; Hudziak, Stephen
  • Nanoscale, Vol. 7, Issue 43
  • DOI: 10.1039/C5NR04982B

Metal–Oxide RRAM
journal, June 2012

  • Wong, H.-S. Philip; Lee, Heng-Yuan; Yu, Shimeng
  • Proceedings of the IEEE, Vol. 100, Issue 6, p. 1951-1970
  • DOI: 10.1109/JPROC.2012.2190369

Resistive Switching and Synaptic Behaviors of TaN/Al 2 O 3 /ZnO/ITO Flexible Devices With Embedded Ag Nanoparticles
journal, July 2016


Coexistence of bipolar and threshold resistive switching in TiO 2 based structure with embedded hafnium nanoparticles
journal, December 2016

  • Michelakaki, Irini; Bousoulas, Panagiotis; Stathopoulos, Spyros
  • Journal of Physics D: Applied Physics, Vol. 50, Issue 4
  • DOI: 10.1088/1361-6463/aa5161

Large Resistive Switching in Ferroelectric BiFeO 3 Nano-Island Based Switchable Diodes
journal, February 2013

  • Hong, Sahwan; Choi, Taekjib; Jeon, Ji Hoon
  • Advanced Materials, Vol. 25, Issue 16
  • DOI: 10.1002/adma.201204839

Photochemical Reduction of Oxygen Adsorbed to Nanocrystalline TiO 2 Films:  A Transient Absorption and Oxygen Scavenging Study of Different TiO 2 Preparations
journal, November 2006

  • Peiró, Ana M.; Colombo, Claudia; Doyle, Gerry
  • The Journal of Physical Chemistry B, Vol. 110, Issue 46
  • DOI: 10.1021/jp064591c

Effect of embedded metal nanocrystals on the resistive switching characteristics in NiN-based resistive random access memory cells
journal, March 2014

  • Yun, Min Ju; Kim, Hee-Dong; Man Hong, Seok
  • Journal of Applied Physics, Vol. 115, Issue 9
  • DOI: 10.1063/1.4867639

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
  • DOI: 10.1002/adfm.201500444

Resistive switching memories based on metal oxides: mechanisms, reliability and scaling
journal, May 2016