Synergistic Effect of Singly Charged Oxygen Vacancies and Ligand Field for Regulating Transport Properties of Resistive Switching Memories

  • D. Das
    D. Das
    Department of Physics, School of Natural Sciences, Shiv Nadar University, NH-91, Dadri, Gautam Buddha Nagar, Uttar Pradesh 201314, India
    More by D. Das
  • A. Barman
    A. Barman
    Department of Physics, School of Natural Sciences, Shiv Nadar University, NH-91, Dadri, Gautam Buddha Nagar, Uttar Pradesh 201314, India
    More by A. Barman
  • S. Kumar
    S. Kumar
    Department of Physics, School of Natural Sciences, Shiv Nadar University, NH-91, Dadri, Gautam Buddha Nagar, Uttar Pradesh 201314, India
    More by S. Kumar
  • A. K. Sinha
    A. K. Sinha
    Synchrotron Utilization Section, Raja Ramanna Center for Advanced Technology (RRCAT), Indore, Madhya Pradesh 452013, India
    Homi Bhabha National Institute, Anishaktinagar, Mumbai 400094, India
    More by A. K. Sinha
  • M. Gupta
    M. Gupta
    UGC-DAE Consortium for Scientific Research, Khandwa Road, Indore, Madhya Pradesh 452001, India
    More by M. Gupta
  • R. Singhal
    R. Singhal
    Department of physics, Malaviya National Institute of Technology Jaipur, JLN Marg, Malaviya Nagar, Jaipur 302017, India
    More by R. Singhal
  • P. Johari*
    P. Johari
    Department of Physics, School of Natural Sciences, Shiv Nadar University, NH-91, Dadri, Gautam Buddha Nagar, Uttar Pradesh 201314, India
    *P.J.: e-mail, [email protected]
    More by P. Johari
  • , and 
  • A. Kanjilal*
    A. Kanjilal
    Department of Physics, School of Natural Sciences, Shiv Nadar University, NH-91, Dadri, Gautam Buddha Nagar, Uttar Pradesh 201314, India
    *A.K.: e-mail, [email protected]
    More by A. Kanjilal
Cite this: J. Phys. Chem. C 2019, 123, 44, 26812–26822
Publication Date (Web):October 15, 2019
https://doi.org/10.1021/acs.jpcc.9b08078
Copyright © 2019 American Chemical Society
Article Views
659
Altmetric
-
Citations
LEARN ABOUT THESE METRICS
Read OnlinePDF (9 MB)
Supporting Info (1)»

Abstract

The controlled incorporation of defect species in amorphous oxide (AO) for regulating charge transport properties is highly demanding and challenging, especially for resistive switching (RS) memories. Here, we use pulsed electron beam deposition technique to engineer the growth of AO films, which show a large decrease (∼33%) in the t2g–eg gap. Our collective experiments and density functional theory (DFT) based ab initio simulations reveal the presence of undercoordinated TiO5 units, causing a decrease in the t2g–eg gap. Further, the importance of TiO5 in facilitating excess electron localization is demonstrated, showing an evolution of a broad defect band within the energy gap. The origin of this band (singly charged oxygen vacancy) is resolutely established by X-ray photoelectron spectroscopy and electron paramagnetic resonance measurements and is also supported by calculated partial charge density and Bader charge analysis. The preeminence of singly charged oxygen vacancies cause a low-current level (up to 1–5 nA) RS operation with a gradual change of resistance states, which could set their path for the energy-efficient neuromorphic computing application. Finally, a new model based on probabilistic Markov chain algorithm is also developed to unfold the gradual change of resistance states from the fundamental defect interaction perspective.

Supporting Information

ARTICLE SECTIONS
Jump To

The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.jpcc.9b08078.

  • Ti K-edge XANES spectra, structures of a-TiO2 at various temperatures during molecular dynamics simulation, average Ti–O bond length in a-TiO2 and their distortion index, DOS of different charge state of oxygen vacancies, and details of the Monte Carlo simulations (PDF)

Terms & Conditions

Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html.

Cited By


This article is cited by 4 publications.

  1. Dnyanesh Vernekar, Mohammad Dayyan, Satyajit Ratha, Chandrashekhar V. Rode, M.Ali Haider, Tuhin Suvra Khan, Dinesh Jagadeesan. Direct Oxidation of Cyclohexane to Adipic Acid by a WFeCoO(OH) Catalyst: Role of Brønsted Acidity and Oxygen Vacancies. ACS Catalysis 2021, 11 (17) , 10754-10766. https://doi.org/10.1021/acscatal.1c01464
  2. Chia-Hsun Hsu, Xin-Peng Geng, Wan-Yu Wu, Ming-Jie Zhao, Pao-Hsun Huang, Xiao-Ying Zhang, Zhan-Bo Su, Zi-Rong Chen, Shui-Yang Lien. Effect of oxygen annealing temperature on properties of spatial atomic layer deposited aluminum-doped zinc oxide films. Materials Science in Semiconductor Processing 2021, 133 , 105929. https://doi.org/10.1016/j.mssp.2021.105929
  3. Tingting Qin, Dong Wang, Xiaoyu Zhang, Yan Wang, Nicholas E. Drewett, Wei Zhang, Taowen Dong, Tian Li, Zizhun Wang, Ting Deng, Zhongyu Pan, Nailin Yue, Rongrong Yang, Keke Huang, Shouhua Feng, Renzhong Huang, Weitao Zheng. Unlocking the Optimal Aqueous δ-Bi2O3 Anode via Unifying Octahedrally Liberated Bi-Atoms and Spilled Nano-Bi Exsolution. Energy Storage Materials 2021, 36 , 376-386. https://doi.org/10.1016/j.ensm.2021.01.013
  4. D. Das, A. Barman, P. K. Sarkar, P. Rajput, S. N. Jha, R. Hübner, D. Kanjilal, P. Johari, A. Kanjilal. Metal-induced progressive alteration of conducting states in memristors for implementing an efficient analog memory: a DFT-supported experimental approach. Journal of Materials Chemistry C 2021, 9 (9) , 3136-3144. https://doi.org/10.1039/D0TC04918B