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 · Wed Jul 10 00:00:00 EDT 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.

View Accepted Manuscript (DOE)

View Accepted Manuscript (Publisher)

Cite

Export

Save

Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (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 Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357; SC0012704; AC02-05CH11231

OSTI ID:: 1559938

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

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

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

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 9 works

Citation information provided by
Web of Science

References (39)

Electronic structure and electron-phonon interactions in layered ${Li}_{x}$ ${NbO}_{2}$ and ${Na}_{x}$ ${NbO}_{2}$ Novikov, D. L.; Gubanov, V. A.; Zubkov, V. G. Physical Review B, Vol. 49, Issue 22 https://doi.org/10.1103/physrevb.49.15830	journal	June 1994
Two centuries of memristors Prodromakis, Themistoklis; Toumazou, Christofer; Chua, Leon Nature Materials, Vol. 11, Issue 6 https://doi.org/10.1038/nmat3338	journal	May 2012
A New Potassium Intercalation Compound of 3 R -Nb _1.1 S ₂ and its Superconducting Hydrated Derivative Synthesized via Soft Chemistry Strategy Hao, Qiao-Yan; Zhu, Bai-Chuan; Wang, Da-Ke ChemistrySelect, Vol. 1, Issue 11 https://doi.org/10.1002/slct.201600324	journal	July 2016
Quantifying redox-induced Schottky barrier variations in memristive devices via in operando spectromicroscopy with graphene electrodes Baeumer, Christoph; Schmitz, Christoph; Marchewka, Astrid Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms12398	journal	August 2016
Halide based MBE of crystalline metals and oxides Greenlee, Jordan D.; Calley, W. Laws; Henderson, Walter physica status solidi (c), Vol. 9, Issue 2 https://doi.org/10.1002/pssc.201100468	journal	December 2011
The crystallization and properties of sputter deposited lithium niobite Shank, Joshua C.; Brooks Tellekamp, M.; Alan Doolittle, W. Thin Solid Films, Vol. 609 https://doi.org/10.1016/j.tsf.2016.01.030	journal	June 2016
Superconductivity in the layered compound LixNbO2 Geselbracht, Margret J.; Richardson, Thomas J.; Stacy, Angelica M. Nature, Vol. 345, Issue 6273 https://doi.org/10.1038/345324a0	journal	May 1990
Surface reconstruction and chemical evolution of stoichiometric layered cathode materials for lithium-ion batteries Lin, Feng; Markus, Isaac M.; Nordlund, Dennis Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms4529	journal	March 2014
In situ grown Nb ₄ N ₅ nanocrystal on nitrogen-doped graphene as a novel anode for lithium ion battery Dong, Chenlong; Wang, Xin; Liu, Xiangye RSC Advances, Vol. 6, Issue 84 https://doi.org/10.1039/c6ra13647h	journal	January 2016
QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials Giannozzi, Paolo; Baroni, Stefano; Bonini, Nicola Journal of Physics: Condensed Matter, Vol. 21, Issue 39, Article No. 395502 https://doi.org/10.1088/0953-8984/21/39/395502	journal	September 2009
Band offsets in transition-metal oxide heterostructures Goldfarb, I.; Ohlberg, D. A. A.; Strachan, J. P. Journal of Physics D: Applied Physics, Vol. 46, Issue 29 https://doi.org/10.1088/0022-3727/46/29/295303	journal	June 2013
First-principles study of the electronic and vibrational properties of $Li Nb O_{2}$ Ylvisaker, Erik R.; Pickett, Warren E. Physical Review B, Vol. 74, Issue 7 https://doi.org/10.1103/physrevb.74.075104	journal	August 2006
Accurate X-Ray Spectral Predictions: An Advanced Self-Consistent-Field Approach Inspired by Many-Body Perturbation Theory Liang, Yufeng; Vinson, John; Pemmaraju, Sri Physical Review Letters, Vol. 118, Issue 9 https://doi.org/10.1103/physrevlett.118.096402	journal	March 2017
Radiation Effects on LiNbO$_2$ Memristors for Neuromorphic Computing Applications Greenlee, Jordan D.; Shank, Joshua C.; Tellekamp, M. Brooks IEEE Transactions on Nuclear Science, Vol. 60, Issue 6 https://doi.org/10.1109/tns.2013.2288218	journal	December 2013
Synaptic electronics: materials, devices and applications Kuzum, Duygu; Yu, Shimeng; Philip Wong, H-S Nanotechnology, Vol. 24, Issue 38 https://doi.org/10.1088/0957-4484/24/38/382001	journal	September 2013
Commentary: The Materials Project: A materials genome approach to accelerating materials innovation Jain, Anubhav; Ong, Shyue Ping; Hautier, Geoffroy APL Materials, Vol. 1, Issue 1 https://doi.org/10.1063/1.4812323	journal	July 2013
1.1 Moore's law: A path going forward Holt, William M. 2016 IEEE International Solid-State Circuits Conference (ISSCC) https://doi.org/10.1109/ISSCC.2016.7417888	conference	January 2016
Evidence of ion intercalation mediated band structure modification and opto-ionic coupling in lithium niobite Shank, Joshua C.; Tellekamp, M. Brooks; Doolittle, W. Alan Journal of Applied Physics, Vol. 117, Issue 3 https://doi.org/10.1063/1.4906125	journal	January 2015
In-situ oxygen x-ray absorption spectroscopy investigation of the resistance modulation mechanism in LiNbO ₂ memristors Greenlee, Jordan D.; Petersburg, Cole F.; Laws Calley, W. Applied Physics Letters, Vol. 100, Issue 18 https://doi.org/10.1063/1.4709422	journal	April 2012
Comparison of Interfacial and Bulk Ionic Motion in Analog Memristors Greenlee, Jordan D.; Calley, W. Laws; Moseley, Michael W. IEEE Transactions on Electron Devices, Vol. 60, Issue 1 https://doi.org/10.1109/ted.2012.2225145	journal	January 2013
Oxygen migration during resistance switching and failure of hafnium oxide memristors Kumar, Suhas; Wang, Ziwen; Huang, Xiaopeng Applied Physics Letters, Vol. 110, Issue 10 https://doi.org/10.1063/1.4974535	journal	March 2017
Superstructure and superconductivity in ${Li}_{1 - x} {NbO}_{2} (x \approx 0.7)$ single crystals Moshopoulou, E. G.; Bordet, P.; Capponi, J. J. Physical Review B, Vol. 59, Issue 14 https://doi.org/10.1103/physrevb.59.9590	journal	April 1999
A review on memristive devices and applications Prodromakis, T.; Toumazou, C. 2010 17th IEEE International Conference on Electronics, Circuits and Systems - (ICECS 2010) https://doi.org/10.1109/ICECS.2010.5724666	conference	December 2010
Quantum many-body effects in x-ray spectra efficiently computed using a basic graph algorithm Liang, Yufeng; Prendergast, David Physical Review B, Vol. 97, Issue 20 https://doi.org/10.1103/physrevb.97.205127	journal	May 2018
Scalable Memdiodes Exhibiting Rectification and Hysteresis for Neuromorphic Computing Shank, Joshua C.; Tellekamp, M. Brooks; Wahila, Matthew J. Scientific Reports, Vol. 8, Issue 1 https://doi.org/10.1038/s41598-018-30727-9	journal	August 2018
Liquid Phase Electro-Epitaxy of Memristive LiNbO ₂ Crystals Greenlee, Jordan D.; Shank, Joshua C.; Tellekamp, M. Brooks Crystal Growth & Design, Vol. 14, Issue 5 https://doi.org/10.1021/cg401775p	journal	April 2014
Review of memristor devices in neuromorphic computing: materials sciences and device challenges Li, Yibo; Wang, Zhongrui; Midya, Rivu Journal of Physics D: Applied Physics, Vol. 51, Issue 50 https://doi.org/10.1088/1361-6463/aade3f	journal	September 2018
Perspective: A review on memristive hardware for neuromorphic computation Sung, Changhyuck; Hwang, Hyunsang; Yoo, In Kyeong Journal of Applied Physics, Vol. 124, Issue 15 https://doi.org/10.1063/1.5037835	journal	October 2018
Memristive devices for computing Yang, J. Joshua; Strukov, Dmitri B.; Stewart, Duncan R. Nature Nanotechnology, Vol. 8, Issue 1, p. 13-24 https://doi.org/10.1038/nnano.2012.240	journal	January 2013
Memristive switching mechanism for metal/oxide/metal nanodevices Yang, J. Joshua; Pickett, Matthew D.; Li, Xuema Nature Nanotechnology, Vol. 3, Issue 7 https://doi.org/10.1038/nnano.2008.160	journal	June 2008
High Performance Ultra-Thin Niobium Films for Superconducting Hot-Electron Devices Jia, X. Q.; Kang, L.; Liu, X. Y. IEEE Transactions on Applied Superconductivity, Vol. 23, Issue 3 https://doi.org/10.1109/tasc.2012.2235508	journal	June 2013
Comparison of thermal and plasma-enhanced atomic layer deposition of niobium oxide thin films Basuvalingam, Saravana Balaji; Macco, Bart; Knoops, Harm C. M. Journal of Vacuum Science & Technology A, Vol. 36, Issue 4 https://doi.org/10.1116/1.5034097	journal	July 2018
Epitaxial niobium dioxide thin films by reactive-biased target ion beam deposition Wang, Yuhan; Comes, Ryan B.; Kittiwatanakul, Salinporn Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 33, Issue 2 https://doi.org/10.1116/1.4906143	journal	March 2015
Quantifying redox-induced Schottky barrier variations in memristive devices via in operando spectromicroscopy with graphene electrodes Bäumer, Christoph; Schmitz, Christoph; Marchewka, Astrid RWTH Aachen University https://doi.org/10.18154/rwth-2017-00575	text	January 2016
Advanced capabilities for materials modelling with Quantum ESPRESSO Unknown, (:Unkn) My University https://doi.org/10.34944/dspace/4844	text	January 2017
Oxygen migration during resistance switching and failure of hafnium oxide memristors Kumar, Suhas; Wang, Ziwen; Huang, Xiaopeng arXiv https://doi.org/10.48550/arxiv.1703.03106	text	January 2017
Advanced capabilities for materials modelling with Quantum ESPRESSO Giannozzi, P.; Andreussi, O.; Brumme, T. arXiv https://doi.org/10.48550/arxiv.1709.10010	text	January 2017
Quantum Many-Body Effects in X-Ray Spectra Efficiently Computed using a Basic Graph Algorithm Liang, Yufeng; Prendergast, David arXiv https://doi.org/10.48550/arxiv.1801.04073	text	January 2018
Scalable Memdiodes Exhibiting Rectification and Hysteresis for Neuromorphic Computing Shank, Joshua C.; Tellekamp, M. Brooks; Wahila, Matthew J. arXiv https://doi.org/10.48550/arxiv.1910.03700	text	January 2019

Cited By (1)

Emerging materials in neuromorphic computing: Guest editorial Burr, Geoffrey W.; Sebastian, Abu; Vianello, Elisa APL Materials, Vol. 8, Issue 1 https://doi.org/10.1063/1.5143659	journal	January 2020

Similar Records

Understanding the electrochemical lithiation/delithiation process in the anode material for lithium ion batteries NiFeOPO₄/C using ex-situ X-ray absorption near edge spectroscopy and in-situ synchrotron X-ray

Journal Article · Thu Jul 12 00:00:00 EDT 2018 · Electrochimica Acta · OSTI ID:1559938

Aziam, H.; Garhi, G.; Tamraoui, Y.; +7 more

Superconductivity in the layered compounds M[sub x]NbO[sub 2] (M = Li, Na)

Miscellaneous · Tue Jan 01 00:00:00 EST 1991 · OSTI ID:1559938

Geselbracht, M J

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

Journal Article · Tue May 01 00:00:00 EDT 2018 · ACS Nano · OSTI ID:1559938

Liu, Huajun; Dong, Yongqi; Cherukara, Mathew J.; +10 more

Related Subjects

36 MATERIALS SCIENCE

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

Citation Formats

References (39)

Cited By (1)

Similar Records

Related Subjects

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