Direct observation of delithiation as the origin of analog memristance in LixNbO2

Howard, Sebastian A.; Singh, Christopher N.; Paez, Galo J.; Wahila, Matthew J.; Wangoh, Linda W.; Sallis, Shawn; Tirpak, Keith; Liang, Yufeng; Prendergast, David; Zuba, Mateusz; Rana, Jatinkumar; Weidenbach, Alex; McCrone, Timothy M.; Yang, Wanli; Lee, Tien -Lin; Rodolakis, Fanny; Doolittle, William; Lee, Wei -Cheng; Piper, Louis F. J.

doi:10.1063/1.5108525

Title: Direct observation of delithiation as the origin of analog memristance in Li_xNbO₂

Journal Article · 09 July 2019 · APL Materials

DOI: https://doi.org/10.1063/1.5108525 · OSTI ID:1559938

Howard, Sebastian A. ^[1];

^[1]; Paez, Galo J. ^[1];

^[1]; Wangoh, Linda W. ^[1]; Sallis, Shawn ^[1];

^[1];

^[2];

^[2]; Zuba, Mateusz ^[1]; Rana, Jatinkumar ^[1]; Weidenbach, Alex ^[3]; McCrone, Timothy M. ^[3];

^[2]; Lee, Tien -Lin ^[4];

^[5]; Doolittle, William ^[3]; Lee, Wei -Cheng ^[1];

^[1]

Binghamton Univ., Binghamton, NY (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Georgia Inst. of Technology, Atlanta, GA (United States)
Diamond Light Source Ltd., Oxfordshire (United Kingdom)
Argonne National Lab. (ANL), Argonne, IL (United States)

The discovery of analog Li_xNbO₂ memristors revealed a promising new memristive mechanism wherein the diffusion of Li⁺ rather than O^2- ions enables precise control of the resistive states. However, directly correlating lithium concentration with changes to the electronic structure in active layers remains a challenge and is required to truly understand the underlying physics. Chemically delithiated single crystals of LiNbO₂ present a model system for correlating lithium variation with spectroscopic signatures from operando soft x-ray spectroscopy studies of device active layers. Using electronic structure modeling of the x-ray spectroscopy of Li_xNbO₂ single crystals, we demonstrate that the intrinsic memristive behavior in Li_xNbO₂ active layers results from field-induced degenerate p-type doping. We show that electrical operation of Li_xNbO₂-based memristors is viable even at marginal Li deficiency and that the analog memristive switching occurs well before the system is fully metallic. This study serves as a benchmark for material synthesis and characterization of future Li_xNbO₂-based memristor devices and suggests that valence change switching is a scalable alternative that circumvents the electroforming typically required for filamentary-based memristors.

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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Organization:: Air Force Research Laboratory (AFRL) - Air Force Office of Scientific Research (AFOSR); Fulbright Program; National Science Foundation (NSF); Diamond Light Source, UK; Brookhaven National Laboratory (BNL); Argonne National Laboratory - Advanced Photon Source; Brookhaven National Laboratory (BNL) - National Synchrotron Light Source II; Lawrence Berkeley National Laboratory (LBNL); USDOE

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1559938

Alternate ID(s):: OSTI ID: 1532798; OSTI ID: 1594923; OSTI ID: 1689690

Journal Information:: APL Materials, Journal Name: APL Materials Journal Issue: 7 Vol. 7; ISSN 2166-532X

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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