High entropy oxides (HEOs), based on the incorporation of multiple‐principal cations into the crystal lattice, offer the possibility to explore previously inaccessible oxide compositions and unconventional properties. Here it is demonstrated that despite the chemical complexity of HEOs external stimuli, such as epitaxial strain, can selectively stabilize certain magneto‐electronic states. Epitaxial (Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)3O4‐HEO thin films are grown in three different strain states: tensile, compressive, and relaxed. A unique coexistence of rocksalt and spinel‐HEO phases, which are fully coherent with no detectable chemical segregation, is revealed by transmission electron microscopy. This dual‐phase coexistence appears as a universal phenomenon in (Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)3O4epitaxial films. Prominent changes in the magnetic anisotropy and domain structure highlight the strain‐induced bidirectional control of magnetic properties in HEOs. When the films are relaxed, their magnetization behavior is isotropic, similar to that of bulk materials. However, under tensile strain, the hardness of the out‐of‐plane (OOP) axis increases significantly. On the other hand, compressive straining results in an easy OOP magnetization and a maze‐like magnetic domain structure, indicating the perpendicular magnetic anisotropy. Generally, this study emphasizes the adaptability of the high entropy design strategy, which, when combined with coherent strain engineering, opens additional prospects for fine‐tuning properties in oxides.
As a new class of multi-principal component oxides with high chemical disorder, high-entropy oxides (HEOs) have attracted much attention. The stability and tunability of their structure and properties are of great interest and importance, but remain unclear. By using in situ synchrotron radiation X-ray diffraction, Raman spectroscopy, ultraviolet–visible absorption spectroscopy, and ex situ high-resolution transmission electron microscopy, here we show the existence of lattice distortion in the crystalline (Ce0.2La0.2Pr0.2Sm0.2Y0.2)O2−δHEO according to the deviation of bond angles from the ideal values, and discover a pressure-induced continuous tuning of lattice distortion (bond angles) and band gap. As continuous bending of bond angles, pressure eventually induces breakdown of the long-range connectivity of lattice and causes amorphization. The amorphous state can be partially recovered upon decompression, forming glass–nanoceramic composite HEO. These results reveal the unexpected flexibility of the structure and properties of HEOs, which could promote the fundamental understanding and applications of HEOs.
more » « less- PAR ID:
- 10154168
- Publisher / Repository:
- Nature Publishing Group
- Date Published:
- Journal Name:
- Communications Chemistry
- Volume:
- 2
- Issue:
- 1
- ISSN:
- 2399-3669
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract The enhanced compositional flexibility to incorporate multiple-principal cations in high entropy oxides (HEOs) offers the opportunity to expand boundaries for accessible compositions and unconventional properties in oxides. Attractive functionalities have been reported in some bulk HEOs, which are attributed to the long-range compositional homogeneity, lattice distortion, and local chemical bonding characteristics in materials. However, the intricate details of local composition fluctuation, metal-oxygen bond distortion and covalency are difficult to visualize experimentally, especially on the atomic scale. Here, we study the atomic structure-chemical bonding-property correlations in a series of perovskite-HEOs utilizing the recently developed four-dimensional scanning transmission electron microscopy techniques which enables to determine the structure, chemical bonding, electric field, and charge density on the atomic scale. The existence of compositional fluctuations along with significant composition-dependent distortion of metal-oxygen bonds is observed. Consequently, distinct variations of metal-oxygen bonding covalency are shown by the real-space charge-density distribution maps with sub-ångström resolution. The observed atomic features not only provide a realistic picture of the local physico-chemistry of chemically complex HEOs but can also be directly correlated to their distinctive magneto-electronic properties.more » « less
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High-entropy oxides (HEOs) containing five or more cations have garnered significant attention recently due to their vastly tunable compositional space, along with their remarkable physical and mechanical properties, exceptional thermal stability, and phase reversibility at elevated temperatures. These characteristics position HEOs as promising candidates for structural components and coatings in high-temperature applications. While much of the ongoing research on HEOs centers around understanding processing-structure relationships, there remains a dearth of knowledge concerning their mechanical properties, crucial for their prospective high-temperature applications. Whether in bulk form or as coatings, the efficacy of HEOs hinges on robust mechanical properties across a spectrum of temperatures, to ensure structural integrity, fracture resistance, and resilience to thermal stress. This review offers a succinct synthesis of recent advancements in HEO research, spanning from processing techniques to mechanical behaviors under extreme conditions. Emphasis is placed on three key aspects: (1) Investigating the influence of processing parameters on HEO crystal structures. (2) Analyzing the interplay between crystal structure and mechanical properties, elucidating deformation mechanisms. (3) Examining the mechanical behavior of HEOs under extreme temperatures and pressures. Through this review, we aim to illuminate the effective control of HEOs’ unique structures and mechanical properties, paving the way for their future applications in extreme environments.
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