Orbital degree of freedom in high entropy oxides

Yan, Jiaqiang; Kumar, Abinash; Chi, Miaofang; Brahlek, Matthew; Ward, Thomas Z.; McGuire, Michael A.

doi:10.1103/physrevmaterials.8.024404

Phys. Rev. Materials

2024

DOI: 10.1103/physrevmaterials.8.024404

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Orbital degree of freedom in high entropy oxides

Jiaqiang Yan,

Abinash Kumar,

Miaofang Chi

et al.

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2024

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Cited by 3 publications

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Order within disorder: Unveiling the potential of high entropy materials in energy storage and electrocatalysis

Lokhande,

Malavekar,

Kim

et al. 2024

Energy Storage Materials

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Order within disorder: Unveiling the potential of high entropy materials in energy storage and electrocatalysis

Lokhande,

Malavekar,

Kim

et al. 2024

Energy Storage Materials

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Robust electronic phase transition against cation disorder in high-entropy pyrochlore iridates

Contant,

McNally,

Krajewska

et al. 2024

AIP Advances

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High-entropy pyrochlore iridates A2Ir2O7 with multiple trivalent A cations were synthesized. The parent ternary A2Ir2O7 displays a variety of electronic phases depending on the size of A cations; Pr2Ir2O7 with a large A cation shows semimetallic behavior down to low temperatures, whereas A2Ir2O7 with smaller A cations, such as Nd2Ir2O7 and Eu2Ir2O7, displays a (semi)metal to magnetic insulator transition as a function of temperature. By further reducing the A cation size, smaller than Y3+, A2Ir2O7 becomes a Mott insulator, and long-range magnetic order takes place below room temperature. The metal–insulator transition and magnetic ordering turned out to be robust against strong disorder induced by the mixing of more than five A-cations in the high-entropy A2Ir2O7. The transition temperatures were found to scale with the average ionic radius of multiple A-cations. In contrast, high-entropy A2Ir2O7 including Bi3+ exhibits metallic behavior down to 2 K, which is likely associated with the presence of oxygen vacancies as in the parent Bi2Ir2O7. Although these indicate that the overall electronic structure of A2Ir2O7 remains intact in the presence of high-entropy configuration at the A-site, the transport properties suggest that fine details of the band structure may be modulated by local distortion. Strong disorder at the A-site of complex oxides may be exploited as a tool to control electronic properties.

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Embracing disorder in quantum materials design

Mazza,

Yan,

Middey

et al. 2024

Applied Physics Letters

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Many of the most exciting materials discoveries in fundamental condensed matter physics are made in systems hosting some degree of intrinsic disorder. While disorder has historically been regarded as something to be avoided in materials design, it is often of central importance to correlated and quantum materials. This is largely driven by the conceptual and theoretical ease to handle, predict, and understand highly uniform systems that exhibit complex interactions, symmetries, and band structures. In this Perspective, we highlight how flipping this paradigm has enabled exciting possibilities in the emerging field of high entropy materials, focusing primarily on high entropy oxide and chalcogenide quantum materials. These materials host high levels of cation or anion compositional disorder while maintaining unexpectedly uniform single crystal lattices. The diversity of atomic scale interactions of spin, charge, orbital, and lattice degrees of freedom are found to emerge into coherent properties on much larger length scales. Thus, altering the variance and magnitudes of the atomic scale properties through elemental selection can open new routes to tune global correlated phases, such as magnetism, metal–insulator transitions, ferroelectricity, and even emergent topological responses. The strategy of embracing disorder in this way provides a much broader pallet from which functional states can be designed for next-generation microelectronic and quantum information systems.

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Orbital degree of freedom in high entropy oxides

Cited by 3 publications

References 55 publications

Order within disorder: Unveiling the potential of high entropy materials in energy storage and electrocatalysis

Order within disorder: Unveiling the potential of high entropy materials in energy storage and electrocatalysis

Robust electronic phase transition against cation disorder in high-entropy pyrochlore iridates

Embracing disorder in quantum materials design

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