Li iontronics in single-crystalline T-Nb2O5 thin films with vertical ionic transport channels

Han, Hyeon; Jacquet, Quentin; Jiang, Zhen; Sayed, Farheen N.; Jeon, Jae-Chun; Sharma, Arpit; Schankler, Aaron M.; Kakekhani, Arvin; Meyerheim, Holger L.; Park, Jucheol; Nam, Sang Yeol; Griffith, Kent J.; Simonelli, Laura; Rappe, Andrew M.; Grey, Clare P.; Parkin, Stuart S. P.

doi:10.1038/s41563-023-01612-2

Title: Li iontronics in single-crystalline T-Nb2O5 thin films with vertical ionic transport channels

Journal Article · 26 July 2023 · Nature Materials

DOI: https://doi.org/10.1038/s41563-023-01612-2 · OSTI ID:1992697

; Jacquet, Quentin;

; Sayed, Farheen N.; Jeon, Jae-Chun; Sharma, Arpit;

;

; Park, Jucheol; Nam, Sang Yeol;

;

Abstract The niobium oxide polymorph T -Nb ₂ O ₅ has been extensively investigated in its bulk form especially for applications in fast-charging batteries and electrochemical (pseudo)capacitors. Its crystal structure, which has two-dimensional (2D) layers with very low steric hindrance, allows for fast Li-ion migration. However, since its discovery in 1941, the growth of single-crystalline thin films and its electronic applications have not yet been realized, probably due to its large orthorhombic unit cell along with the existence of many polymorphs. Here we demonstrate the epitaxial growth of single-crystalline T -Nb ₂ O ₅ thin films, critically with the ionic transport channels oriented perpendicular to the film’s surface. These vertical 2D channels enable fast Li-ion migration, which we show gives rise to a colossal insulator–metal transition, where the resistivity drops by 11 orders of magnitude due to the population of the initially empty Nb 4 d ⁰ states by electrons. Moreover, we reveal multiple unexplored phase transitions with distinct crystal and electronic structures over a wide range of Li-ion concentrations by comprehensive in situ experiments and theoretical calculations, which allow for the reversible and repeatable manipulation of these phases and their distinct electronic properties. This work paves the way for the exploration of novel thin films with ionic channels and their potential applications.

View Journal Article

Cite

Export

Save

Sponsoring Organization:: USDOE

Grant/Contract Number:: SC0019281

OSTI ID:: 1992697

Journal Information:: Nature Materials, Journal Name: Nature Materials Journal Issue: 9 Vol. 22; ISSN 1476-1122

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

References (43)

Facet-Independent Electric-Field-Induced Volume Metallization of Tungsten Trioxide Films Altendorf, Simone G.; Jeong, Jaewoo; Passarello, Donata Advanced Materials, Vol. 28, Issue 26 https://doi.org/10.1002/adma.201505631	journal	May 2016
Li-Ion Synaptic Transistor for Low Power Analog Computing Fuller, Elliot J.; Gabaly, Farid El; Léonard, François Advanced Materials, Vol. 29, Issue 4 https://doi.org/10.1002/adma.201604310	journal	November 2016
Electric‐Field‐Controlled Phase Transformation in WO ₃ Thin Films through Hydrogen Evolution Wang, Meng; Shen, Shengchun; Ni, Jinyang Advanced Materials, Vol. 29, Issue 46 https://doi.org/10.1002/adma.201703628	journal	October 2017
Highly Efficient Uniaxial In‐Plane Stretching of a 2D Material via Ion Insertion Muscher, Philipp K.; Rehn, Daniel A.; Sood, Aditya Advanced Materials, Vol. 33, Issue 37 https://doi.org/10.1002/adma.202101875	journal	July 2021
The Effect of Crystallinity on the Rapid Pseudocapacitive Response of Nb2O5 Kim, Jong Woung; Augustyn, Veronica; Dunn, Bruce Advanced Energy Materials, Vol. 2, Issue 1 https://doi.org/10.1002/aenm.201100494	journal	December 2011
Atomistic Conversion Reaction Mechanism of WO ₃ in Secondary Ion Batteries of Li, Na, and Ca He, Yang; Gu, Meng; Xiao, Haiyan Angewandte Chemie International Edition, Vol. 55, Issue 21 https://doi.org/10.1002/anie.201601542	journal	April 2016
Die Oxyde des Niobs Brauer, Georg Zeitschrift f�r anorganische und allgemeine Chemie, Vol. 248, Issue 1 https://doi.org/10.1002/zaac.19412480101	journal	September 1941
Electrochromic oxides: a bandstructure approach Granqvist, C. Solar Energy Materials and Solar Cells, Vol. 32, Issue 4 https://doi.org/10.1016/0927-0248(94)90100-7	journal	April 1994
High power nano-Nb2O5 negative electrodes for lithium-ion batteries Lübke, Mechthild; Sumboja, Afriyanti; Johnson, Ian D. Electrochimica Acta, Vol. 192 https://doi.org/10.1016/j.electacta.2016.01.226	journal	February 2016
Understanding electrochemical potentials of cathode materials in rechargeable batteries Liu, Chaofeng; Neale, Zachary G.; Cao, Guozhong Materials Today, Vol. 19, Issue 2 https://doi.org/10.1016/j.mattod.2015.10.009	journal	March 2016
Niobium oxides and niobates physical properties: Review and prospects Nico, C.; Monteiro, T.; Graça, M. P. F. Progress in Materials Science, Vol. 80 https://doi.org/10.1016/j.pmatsci.2016.02.001	journal	July 2016
Evidence for Ionic Liquid Gate-Induced Metallization of Vanadium Dioxide Bars over Micron Length Scales Passarello, Donata; Altendorf, Simone G.; Jeong, Jaewoo Nano Letters, Vol. 17, Issue 5 https://doi.org/10.1021/acs.nanolett.6b05029	journal	April 2017
Low-Voltage, CMOS-Free Synaptic Memory Based on Li _X TiO ₂ Redox Transistors Li, Yiyang; Fuller, Elliot J.; Asapu, Shiva ACS Applied Materials & Interfaces, Vol. 11, Issue 42 https://doi.org/10.1021/acsami.9b14338	journal	September 2019
Synthesis and Dual-Mode Electrochromism of Anisotropic Monoclinic Nb₁₂O₂₉ Colloidal Nanoplatelets Lu, Hsin-Che; Ghosh, Sandeep; Katyal, Naman ACS Nano, Vol. 14, Issue 8 https://doi.org/10.1021/acsnano.0c03283	journal	July 2020
Control of Oxygen Vacancy Ordering in Brownmillerite Thin Films via Ionic Liquid Gating Han, Hyeon; Sharma, Arpit; Meyerheim, Holger L. ACS Nano, Vol. 16, Issue 4 https://doi.org/10.1021/acsnano.2c00012	journal	April 2022
Electrolytes and Interphases in Li-Ion Batteries and Beyond Xu, Kang Chemical Reviews, Vol. 114, Issue 23 https://doi.org/10.1021/cr500003w	journal	October 2014
Dynamics of Lithium Insertion in Electrochromic Titanium Dioxide Nanocrystal Ensembles Dahlman, Clayton J.; Heo, Sungyeon; Zhang, Youtian Journal of the American Chemical Society, Vol. 143, Issue 22 https://doi.org/10.1021/jacs.0c10628	journal	May 2021
High-Rate Intercalation without Nanostructuring in Metastable Nb ₂ O ₅ Bronze Phases Griffith, Kent J.; Forse, Alexander C.; Griffin, John M. Journal of the American Chemical Society, Vol. 138, Issue 28 https://doi.org/10.1021/jacs.6b04345	journal	July 2016
Unraveling the Nature of Anomalously Fast Energy Storage in T-Nb ₂ O ₅ Chen, Dongchang; Wang, Jeng-Han; Chou, Tsung-Fu Journal of the American Chemical Society, Vol. 139, Issue 20 https://doi.org/10.1021/jacs.7b03141	journal	May 2017
The Role of Ionic Liquid Breakdown in the Electrochemical Metallization of VO ₂ : An NMR Study of Gating Mechanisms and VO ₂ Reduction Hope, Michael A.; Griffith, Kent J.; Cui, Bin Journal of the American Chemical Society, Vol. 140, Issue 48 https://doi.org/10.1021/jacs.8b09513	journal	November 2018
Ionic and Electronic Conduction in TiNb ₂ O ₇ Griffith, Kent J.; Seymour, Ieuan D.; Hope, Michael A. Journal of the American Chemical Society, Vol. 141, Issue 42 https://doi.org/10.1021/jacs.9b06669	journal	September 2019
Issues and challenges facing rechargeable lithium batteries Tarascon, J.-M.; Armand, M. Nature, Vol. 414, Issue 6861, p. 359-367 https://doi.org/10.1038/35104644	journal	November 2001
Battery materials for ultrafast charging and discharging Kang, Byoungwoo; Ceder, Gerbrand Nature, Vol. 458, Issue 7235, p. 190-193 https://doi.org/10.1038/nature07853	journal	March 2009
Electric-field control of tri-state phase transformation with a selective dual-ion switch Lu, Nianpeng; Zhang, Pengfei; Zhang, Qinghua Nature, Vol. 546, Issue 7656 https://doi.org/10.1038/nature22389	journal	May 2017
A first-order Mott transition in LixCoO2 Marianetti, C. A.; Kotliar, G.; Ceder, G. Nature Materials, Vol. 3, Issue 9 https://doi.org/10.1038/nmat1178	journal	August 2004
High-rate electrochemical energy storage through Li+ intercalation pseudocapacitance Augustyn, Veronica; Come, Jérémy; Lowe, Michael A. Nature Materials, Vol. 12, Issue 6 https://doi.org/10.1038/nmat3601	journal	April 2013
Insulator to metal transition in WO3 induced by electrolyte gating Leng, X.; Pereiro, J.; Strle, J. npj Quantum Materials, Vol. 2, Issue 1 https://doi.org/10.1038/s41535-017-0039-2	journal	July 2017
Electrochemically induced amorphous-to-rock-salt phase transformation in niobium oxide electrode for Li-ion batteries Barnes, Pete; Zuo, Yunxing; Dixon, Kiev Nature Materials, Vol. 21, Issue 7 https://doi.org/10.1038/s41563-022-01242-0	journal	May 2022
Lithium-film ceramics for solid-state lithionic devices Zhu, Yuntong; Gonzalez-Rosillo, Juan Carlos; Balaish, Moran Nature Reviews Materials, Vol. 6, Issue 4 https://doi.org/10.1038/s41578-020-00261-0	journal	November 2020
Electrochemical ion insertion from the atomic to the device scale Sood, Aditya; Poletayev, Andrey D.; Cogswell, Daniel A. Nature Reviews Materials, Vol. 6, Issue 9 https://doi.org/10.1038/s41578-021-00314-y	journal	May 2021
Niobium tungsten oxides for high-rate lithium-ion energy storage Griffith, Kent J.; Wiaderek, Kamila M.; Cibin, Giannantonio Nature, Vol. 559, Issue 7715 https://doi.org/10.1038/s41586-018-0347-0	journal	July 2018
Giant reversible, facet-dependent, structural changes in a correlated-electron insulator induced by ionic liquid gating Jeong, Jaewoo; Aetukuri, Nagaphani B.; Passarello, Donata Proceedings of the National Academy of Sciences, Vol. 112, Issue 4 https://doi.org/10.1073/pnas.1419051112	journal	January 2015
In operando evidence of deoxygenation in ionic liquid gating of YBa ₂ Cu ₃ O _7-X Perez-Muñoz, Ana M.; Schio, Pedro; Poloni, Roberta Proceedings of the National Academy of Sciences, Vol. 114, Issue 2 https://doi.org/10.1073/pnas.1613006114	journal	December 2016
Strongly correlated perovskite lithium ion shuttles Sun, Yifei; Kotiuga, Michele; Lim, Dawgen Proceedings of the National Academy of Sciences, Vol. 115, Issue 39 https://doi.org/10.1073/pnas.1805029115	journal	August 2018
Strain-driven formation of epitaxial nanostructures in brownmillerite strontium cobaltite thin films Han, Hyeon; Deniz, Hakan; Parkin, Stuart S. P. Proceedings of the National Academy of Sciences, Vol. 120, Issue 12 https://doi.org/10.1073/pnas.2221651120	journal	March 2023
CL��SS: The hard X-ray absorption beamline of the ALBA CELLS synchrotron Simonelli, L.; Marini, C.; Olszewski, W. Cogent Physics, Vol. 3, Issue 1 https://doi.org/10.1080/23311940.2016.1231987	journal	September 2016
Die Kristallstruktur von T -Nb ₂ O ₅ Kato, K.; Tamura, S. Acta Crystallographica Section B Structural Crystallography and Crystal Chemistry, Vol. 31, Issue 3 https://doi.org/10.1107/S0567740875003603	journal	March 1975
Suppression of Metal-Insulator Transition in VO2 by Electric Field-Induced Oxygen Vacancy Formation Jeong, J.; Aetukuri, N.; Graf, T. Science, Vol. 339, Issue 6126 https://doi.org/10.1126/science.1230512	journal	March 2013
Ionic Gating for Tuning Electronic and Magnetic Properties Guan, Yicheng; Han, Hyeon; Li, Fan Annual Review of Materials Research, Vol. 53, Issue 1 https://doi.org/10.1146/annurev-matsci-080619-012219	journal	July 2023
Electrochemical and In Situ XAFS-XRD Investigation of Nb[sub 2]O[sub 5] for Rechargeable Lithium Batteries Kodama, Ryoji; Terada, Yasuko; Nakai, Izumi Journal of The Electrochemical Society, Vol. 153, Issue 3 https://doi.org/10.1149/1.2163788	journal	January 2006
Characterization of Amorphous Anodic Nb2O5 Nanofilm for Gas Sensing Kowalski, Damian; Aoki, Yoshitaka; Habazaki, Hiroki ECS Transactions, Vol. 16, Issue 48 https://doi.org/10.1149/1.3149569	journal	August 2009
An Electrochemical Cell for Operando Study of Lithium Batteries Using Synchrotron Radiation Leriche, J. B.; Hamelet, S.; Shu, J. Journal of The Electrochemical Society, Vol. 157, Issue 5 https://doi.org/10.1149/1.3355977	journal	January 2010
Heteroepitaxial Growth of T-Nb2O5 on SrTiO3 Boschker, Jos; Markurt, Toni; Albrecht, Martin Nanomaterials, Vol. 8, Issue 11 https://doi.org/10.3390/nano8110895	journal	November 2018

Similar Records

Li iontronics in single-crystalline T-Nb2O5 thin films with vertical ionic transport channels

Journal Article · 2023 · Nature Materials · OSTI ID:2421101

Han, Hyeon; Jacquet, Quentin; Jiang, Zhen; +13 more

Simultaneous Solid Electrolyte Deposition and Cathode Lithiation for Thin Film Batteries and Lithium Iontronic Devices

Journal Article · 2024 · ACS Energy Letters · OSTI ID:2351014

Warecki, Zoey; Ferrari, Victoria Castagna; Robinson, Donald Arlington; +9 more

Redox Gating for Colossal Carrier Modulation and Unique Phase Control

Journal Article · 2024 · Advanced Materials · OSTI ID:2281256

Zhang, Le; Liu, Changjiang; Cao, Hui; +9 more

Title: Li iontronics in single-crystalline T-Nb2O5 thin films with vertical ionic transport channels

Citation Formats

References (43)

Similar Records

Related Subjects