Mechanisms of Hysteresis and Reversibility across the Voltage-Driven Perovskite–Brownmillerite Transformation in Electrolyte-Gated Ultrathin La0.5Sr0.5CoO3−δ

Postiglione, William M.; Yu, Guichuan; Chaturvedi, Vipul; Zhou, Hua; Heltemes, Kei; Jacobson, Andrew; Greven, Martin; Leighton, Chris

doi:10.1021/acsami.4c01336

Mechanisms of Hysteresis and Reversibility across the Voltage-Driven Perovskite–Brownmillerite Transformation in Electrolyte-Gated Ultrathin La_0.5Sr_0.5CoO_3−δ

Journal Article · Tue Apr 02 00:00:00 UTC 2024 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.4c01336· OSTI ID:2569705

^[1]; Yu, Guichuan ^[1]; ^[1]; ^[2]; Heltemes, Kei ^[1]; Jacobson, Andrew ^[1]; Greven, Martin ^[1]; ^[1]

Univ. of Minnesota, Minneapolis, MN (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Perovskite cobaltites have emerged as archetypes for electrochemical control of materials properties in electrolyte-gate devices. Voltage-driven redox cycling can be performed between fully oxygenated perovskite and oxygen-vacancy-ordered brownmillerite phases, enabling exceptional modulation of the crystal structure, electronic transport, thermal transport, magnetism, and optical properties. The vast majority of studies, however, have focused heavily on the perovskite and brownmillerite end points. In contrast, here we focus on hysteresis and reversibility across the entire perovskite ↔ brownmillerite topotactic transformation, combining gate-voltage hysteresis loops, minor hysteresis loops, quantitative operando synchrotron X-ray diffraction, and temperature-dependent (magneto)transport, on ion-gel-gated ultrathin (10-unit-cell) epitaxial La_0.5Sr_0.5CoO_3-δ films. Further, gate-voltage hysteresis loops combined with operando diffraction reveal a wealth of new mechanistic findings, including asymmetric redox kinetics due to differing oxygen diffusivities in the two phases, nonmonotonic transformation rates due to the first-order nature of the transformation, and limits on reversibility due to first-cycle structural degradation. Minor loops additionally enable the first rational design of an optimal gate-voltage cycle. Combining this knowledge, we demonstrate state-of-the-art nonvolatile cycling of electronic and magnetic properties, encompassing >10⁵ transport ON/OFF ratios at room temperature, and reversible metal-insulator-metal and ferromagnet-nonferromagnet-ferromagnet cycling, all at 10-unit-cell thickness with high room-temperature stability. This paves the way for future work to establish the ultimate cycling frequency and endurance of such devices.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 2569705

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 15 Vol. 16; ISSN 1944-8244; ISSN 1944-8252

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Mechanisms of Hysteresis and Reversibility across the Voltage-Driven Perovskite–Brownmillerite Transformation in Electrolyte-Gated Ultrathin La0.5Sr0.5CoO3−δ

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Mechanisms of Hysteresis and Reversibility across the Voltage-Driven Perovskite–Brownmillerite Transformation in Electrolyte-Gated Ultrathin La_0.5Sr_0.5CoO_3−δ