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Abstract Materials with tunable infrared refractive index changes have enabled active metasurfaces for novel control of optical circuits, thermal radiation, and more. Ion‐gel‐gated epitaxial films of the perovskite cobaltite La1−xSrxCoO3−δ(LSCO) with 0.00 ≤x≤ 0.70 offer a new route to significant, voltage‐tuned, nonvolatile refractive index modulation for infrared active metasurfaces, shown here through Kramers–Kronig‐consistent dispersion models, structural and electronic transport characterization, and electromagnetic simulations before and after electrochemical reduction. As‐grown perovskite films are high‐index insulators forx< 0.18 but lossy metals forx> 0.18, due to a percolation insulator‐metal transition. Positive‐voltage gating of LSCO transistors withx> 0.18 reveals a metal‐insulator transition from the metallic perovskite phase to a high‐index (n> 2.5), low‐loss insulating phase, accompanied by a perovskite to oxygen‐vacancy‐ordered brownmillerite transformation at highx. Atx< 0.18, despite nominally insulating character, the LSCO films undergo remarkable refractive index changes to another lower‐index, lower‐loss insulating perovskite state with Δn >0.6. In simulations of plasmonic metasurfaces, these metal‐insulator and insulator‐insulator transitions support significant, varied mid‐infrared reflectance modulation, thus framing electrochemically gated LSCO as a diverse library of room‐temperature phase‐change materials for applications including dynamic thermal imaging, camouflage, and optical memories.
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Versatile and Highly Efficient Controls of Reversible Topotactic Metal–Insulator Transitions through Proton Intercalation
Abstract The ability to tailor a new crystalline structure and associated functionalities with a variety of stimuli is one of the key issues in material design. Developing synthetic routes to functional materials with partially absorbed nonmetallic elements (i.e., hydrogen and nitrogen) can open up more possibilities for preparing novel families of electronically active oxide compounds. Fast and reversible uptake and release of hydrogen in epitaxial ABO3manganite films through an adapted low‐frequency inductively coupled plasma technology is introduced. Compared with traditional dopants of metallic cations, the plasma‐assisted hydrogen implantations not only produce reversibly structural transformations from pristine perovskite (PV) phase to a newly found protonation‐driven brownmillerite one but also regulate remarkably different electronic properties driving the material from a ferromagnetic metal to a weakly ferromagnetic insulator for a range of manganite (La1−xSrxMnO3) thin films. Moreover, a reversible perovskite‐brownmillerite‐perovskite transition is achieved at a relatively low temperature (T≤ 350 °C), enabling multifunctional modulations for integrated electronic systems. The fast, low‐temperature control of structural and electronic properties by the facile hydrogenation/dehydrogenation treatment substantially widens the space for exploring new possibilities of novel properties in proton‐based multifunctional materials.
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- Award ID(s):
- 1708615
- PAR ID:
- 10460759
- Author(s) / Creator(s):
- ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; more »
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Functional Materials
- Volume:
- 29
- Issue:
- 50
- ISSN:
- 1616-301X
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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