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Title: Quantitative Observation of Threshold Defect Behavior in Memristive Devices with Operando X-ray Microscopy

Memristive devices are an emerging technology that enables both rich interdisciplinary science and novel device functionalities, such as nonvolatile memories and nanoionics-based synaptic electronics. Recent work has shown that the reproducibility and variability of the devices depend sensitively on the defect structures created during electroforming as well as their continued evolution under dynamic electric fields. However, a fundamental principle guiding the material design of defect structures is still lacking due to the difficulty in understanding dynamic defect behavior under different resistance states. Here, we unravel the existence of threshold behavior by studying model, single-crystal devices: resistive switching requires that the pristine oxygen vacancy concentration reside near a critical value. Theoretical calculations show that the threshold oxygen vacancy concentration lies at the boundary for both electronic and atomic phase transitions. Through operando, multimodal X-ray imaging, we show that field tuning of the local oxygen vacancy concentration below or above the threshold value is responsible for switching between different electrical states. Lastly, these results provide a general strategy for designing functional defect structures around threshold concentrations to create dynamic, field-controlled phases for memristive devices.
Authors:
ORCiD logo [1] ;  [2] ;  [3] ;  [3] ;  [3] ;  [3] ;  [3] ;  [3] ;  [4] ; ORCiD logo [3] ;  [3] ;  [3] ;  [3]
  1. Argonne National Lab. (ANL), Argonne, IL (United States); A*STAR (Agency for Science, Technology and Research) (Singapore)
  2. Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Science and Technology of China, Anhui (China)
  3. Argonne National Lab. (ANL), Argonne, IL (United States)
  4. Argonne National Lab. (ANL), Argonne, IL (United States); KAIST, Daejeon (Korea)
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 12; Journal Issue: 5; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; WO3; memristive devices; operando X-ray imaging; quantitative oxygen vacancy profile; threshold defect behavior
OSTI Identifier:
1455044

Liu, Huajun, Dong, Yongqi, Cherukara, Mathew J., Sasikumar, Kiran, Narayanan, Badri, Cai, Zhonghou, Lai, Barry, Stan, Liliana, Hong, Seungbum, Chan, Maria K. Y., Sankaranarayanan, Subramanian K. R. S., Zhou, Hua, and Fong, Dillon D.. Quantitative Observation of Threshold Defect Behavior in Memristive Devices with Operando X-ray Microscopy. United States: N. p., Web. doi:10.1021/acsnano.8b02028.
Liu, Huajun, Dong, Yongqi, Cherukara, Mathew J., Sasikumar, Kiran, Narayanan, Badri, Cai, Zhonghou, Lai, Barry, Stan, Liliana, Hong, Seungbum, Chan, Maria K. Y., Sankaranarayanan, Subramanian K. R. S., Zhou, Hua, & Fong, Dillon D.. Quantitative Observation of Threshold Defect Behavior in Memristive Devices with Operando X-ray Microscopy. United States. doi:10.1021/acsnano.8b02028.
Liu, Huajun, Dong, Yongqi, Cherukara, Mathew J., Sasikumar, Kiran, Narayanan, Badri, Cai, Zhonghou, Lai, Barry, Stan, Liliana, Hong, Seungbum, Chan, Maria K. Y., Sankaranarayanan, Subramanian K. R. S., Zhou, Hua, and Fong, Dillon D.. 2018. "Quantitative Observation of Threshold Defect Behavior in Memristive Devices with Operando X-ray Microscopy". United States. doi:10.1021/acsnano.8b02028.
@article{osti_1455044,
title = {Quantitative Observation of Threshold Defect Behavior in Memristive Devices with Operando X-ray Microscopy},
author = {Liu, Huajun and Dong, Yongqi and Cherukara, Mathew J. and Sasikumar, Kiran and Narayanan, Badri and Cai, Zhonghou and Lai, Barry and Stan, Liliana and Hong, Seungbum and Chan, Maria K. Y. and Sankaranarayanan, Subramanian K. R. S. and Zhou, Hua and Fong, Dillon D.},
abstractNote = {Memristive devices are an emerging technology that enables both rich interdisciplinary science and novel device functionalities, such as nonvolatile memories and nanoionics-based synaptic electronics. Recent work has shown that the reproducibility and variability of the devices depend sensitively on the defect structures created during electroforming as well as their continued evolution under dynamic electric fields. However, a fundamental principle guiding the material design of defect structures is still lacking due to the difficulty in understanding dynamic defect behavior under different resistance states. Here, we unravel the existence of threshold behavior by studying model, single-crystal devices: resistive switching requires that the pristine oxygen vacancy concentration reside near a critical value. Theoretical calculations show that the threshold oxygen vacancy concentration lies at the boundary for both electronic and atomic phase transitions. Through operando, multimodal X-ray imaging, we show that field tuning of the local oxygen vacancy concentration below or above the threshold value is responsible for switching between different electrical states. Lastly, these results provide a general strategy for designing functional defect structures around threshold concentrations to create dynamic, field-controlled phases for memristive devices.},
doi = {10.1021/acsnano.8b02028},
journal = {ACS Nano},
number = 5,
volume = 12,
place = {United States},
year = {2018},
month = {5}
}