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Title: Charge‐Density‐Wave Resistive Switching and Voltage Oscillations in Ternary Chalcogenide BaTiS 3
Abstract

Phase change materials, which show different electrical characteristics across the phase transitions, have attracted considerable research attention for their potential electronic device applications. Materials with metal‐to‐insulator or charge density wave (CDW) transitions such as VO2and 1T‐TaS2have demonstrated voltage oscillations due to their robust bi‐state resistive switching behavior with some basic neuronal characteristics. BaTiS3is a small bandgap ternary chalcogenide that has recently reported the emergence of CDW order below 245 K. Here, the discovery of DC voltage / current‐induced reversible threshold switching in BaTiS3devices between a CDW phase and a room temperature semiconducting phase is reported. The resistive switching behavior is consistent with a Joule heating scheme and sustained voltage oscillations with a frequency of up to 1 kHz are demonstrated by leveraging the CDW phase transition and the associated negative differential resistance. Strategies of reducing channel sizes and improving thermal management may further improve the device's performance. The findings establish BaTiS3as a promising CDW material for future electronic device applications, especially for energy‐efficient neuromorphic computing.

 
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Award ID(s):
2122071
NSF-PAR ID:
10473561
Author(s) / Creator(s):
 ;  ;  ;  ;  
Publisher / Repository:
Wiley Blackwell (John Wiley & Sons)
Date Published:
Journal Name:
Advanced Electronic Materials
Volume:
9
Issue:
11
ISSN:
2199-160X
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
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    Acknowledgement

    This work was supported by the U.S. National Science Foundation (NSF) Award No. ECCS-1931088. S.L. and H.W.S. acknowledge the support from the Improvement of Measurement Standards and Technology for Mechanical Metrology (Grant No. 22011044) by KRISS.

    References

    [1] Younget al.,IEEE Computational Intelligence Magazine,vol. 13, no. 3, pp. 55-75, 2018.

    [2] Hadsellet al.,Journal of Field Robotics,vol. 26, no. 2, pp. 120-144, 2009.

    [3] Najafabadiet al.,Journal of Big Data,vol. 2, no. 1, p. 1, 2015.

    [4] Zhaoet al.,Applied Physics Reviews,vol. 7, no. 1, 2020.

    [5] Zidanet al.,Nature Electronics,vol. 1, no. 1, pp. 22-29, 2018.

    [6] Wulfet al.,SIGARCH Comput. Archit. News,vol. 23, no. 1, pp. 20–24, 1995.

    [7] Wilkes,SIGARCH Comput. Archit. News,vol. 23, no. 4, pp. 4–6, 1995.

    [8] Ielminiet al.,Nature Electronics,vol. 1, no. 6, pp. 333-343, 2018.

    [9] Changet al.,Nano Letters,vol. 10, no. 4, pp. 1297-1301, 2010.

    [10] Qinet al., Physica Status Solidi (RRL) - Rapid Research Letters, pssr.202200075R1, In press, 2022.

     
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