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Materials with field-tunable polarization are of broad interest to condensed matter sciences and solid-state device technologies. Here, using hydrogen (H) donor doping, we modify the room temperature metallic phase of a perovskite nickelate NdNiO into an insulating phase with both metastable dipolar polarization and space-charge polarization. We then demonstrate transient negative differential capacitance in thin film capacitors. The space-charge polarization caused by long-range movement and trapping of protons dominates when the electric field exceeds the threshold value. First-principles calculations suggest the polarization originates from the polar structure created by H doping. We find that polarization decays within ~1 second which is an interesting temporal regime for neuromorphic computing hardware design, and we implement the transient characteristics in a neural network to demonstrate unsupervised learning. These discoveries open new avenues for designing ferroelectric materials and electrets using light-ion doping.
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http://dx.doi.org/10.1038/s41467-024-49213-0 | DOI Listing |
ACS Appl Electron Mater
August 2025
Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, United States.
Manipulating electronic orbital states in quantum materials provides a powerful means of controlling their physical properties and technological functionality. Here, we demonstrate that orbital populations in strongly correlated oxide thin films can be continuously and reversibly tuned through postsynthesis He ion implantation. Using LaNiO as a model system, we show that the orbital preference can be systematically adjusted from favoring in-plane occupation toward out-of-plane states through precise control of ion fluence.
View Article and Find Full Text PDFAdv Mater
August 2025
Beijing National Center for Electron Microscopy and Laboratory of Advanced Materials, Department of Materials Science and Engineering, Tsinghua University, Beijing, 100084, China.
Oxygen octahedra tilt, an important knob to tune properties of perovskite oxides and their derivatives, determines the coupling patterns and emergent states. Conventional methods, such as strain and doping, are primarily employed to modulate the magnitude of the octahedra tilt. The switching of the tilt, however, is challenging due to the intrinsic interlocked coupling.
View Article and Find Full Text PDFNano Lett
August 2025
Hefei National Research Center for Physical Sciences at Microscale and School of Emergent Technology, University of Science and Technology of China, Hefei 230026, China.
Epitaxial growth serves as a critical platform for tailoring electronic interactions. Here, we synthesized high-quality NdSrNiO thin films on (LaSr)(AlTa)O (LSAT) (001) and SrTiO (STO) (001) substrates and systematically investigated the effects of substrate strain and chemical doping on their low-energy electronic structures using angle-resolved photoemission spectroscopy (ARPES). Transport measurements reveal that Sr doping strongly suppresses the metal-insulator transition (MIT) temperature on both substrates, with accelerated suppression in STO (001)-grown samples.
View Article and Find Full Text PDFACS Nano
August 2025
Sandia National Laboratories, 7011 East Avenue, Livermore, California 94550, United States of America.
The insertion of electron-donating ions has emerged as a powerful technique to manipulate the electronic structure of correlated oxides. However, the resulting electronic structure remains poorly understood, with challenges in quantifying dopant concentration, unexplained differences with substitutionally doped films, and a poor understanding of how dopant atoms interact with insulator-metal transitions (IMTs). Here, these issues are addressed in the context of the rare earth nickelates, a prototypical correlated oxide family with widely tunable electronic behavior under the insertion of protons and alkali metals as interstitial dopants.
View Article and Find Full Text PDFInorg Chem
August 2025
Instituto de Ciencia de Materiales de Madrid, CSIC, Cantoblanco, 28049 Madrid, Spain.
Recently, a new class of high-temperature superconductors, NiO (where represents rare-earth elements) with infinite-layer (IL) structure, has been identified. They possess the same structural framework as the renowned high- cuprates but with nickel replacing copper as the central element. In this study, we successfully synthesized infinite-layer samples of PrNiAlO in the bulk polycrystalline form through topotactic reduction of the PrNiAlO orthorhombic perovskite, via treatment with CaH.
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