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外场激励通过调控强关联氧化物中自由度间的关联耦合作用, 触发其发生多重莫特电子相变和轨道重构, 在强关联电子相变氧化物体系中发现了丰富的新奇物性和量子转变, 为构筑新型类脑神经元逻辑器件、磁电耦合器件及能量转换器件奠定基础, 引起了凝聚态物理领域的广泛关注. 本工作系统地回顾了国内外科研团队在强关联氧化物电子相变特性多场调控领域的研究进展, 旨在凸显离子、应力场和栅极电场等新型功能调控自由度在强关联氧化物电子相变特性调控和新型功能特性设计中的关键作用, 阐明强关联氧化物中微观自由度的关联耦合作用对其宏观关联电子相变特性的基础调控规律, 为实现强关联氧化物电子相变特性的可控设计与精准调控提供理论依据, 期望利用多物理场的调控作用在强关联电子相变氧化物材料体系中发现更多的新物理、新物性、新器件和新应用.External-field-triggered multiple electronic phase transitions within correlated oxides open up a new paradigm to explore exotic physical functionalities and new quantum transitions via regulating the electron correlations and the interplay in the degrees of freedom, which makes the multidisciplinary fields have the promising application prospects, such as neuromorphic computing, magnetoelectric coupling, smart windows, bio-sensing, and energy conversion. This review presents a comprehensive picture of regulating the electronic phase transitions for correlated oxides via multi-field covering the VO2 and ReNiO3, thus highlighting the critical role of external field in exploring the exotic physical property and designing new quantum states. Beyond conventional semiconductors, the complex interplay in the charge, lattice, orbital and spin degrees of freedom within correlated oxides triggers abundant correlated physical functionalities that are rather susceptible to the external field. For example, hydrogen-related electron-doping Mottronics makes it possible to discover new electronic phase and magnetic ground states in the hydrogen-related phase diagram of correlated oxides. In addition, filling-controlled Mottronics by using hydrogenation triggers multiple orbital reconfigurations for correlated oxides away from the correlated electronic ground state that results in new quantum transitions via directly manipulating the d-orbital configuration and occupation, such as unconventional Ni-based superconductivity. The transition metals of correlated oxides are generally substituted by dopants to effectively adjust the electronic phase transitions via introducing the carrier doping and/or lattice strain. Imparting an interfacial strain to correlated oxides introduces an additional freedom to manipulate the electronic phase transition via distorting the lattice framework, owing to the interplay between charge and lattice degrees of freedom. In recent years, the polarization field associated with BiFeO3 or PMN-PT material triggered by a cross-plane electric field has been used to adjust the electronic phase transition of correlated oxides that enriches the promising correlated electronic devices. The exotic physical phenomenon as discovered in the correlated oxides originates from the non-equilibrium states that are triggered by imparting external fields. Nevertheless, the underneath mechanism as associated with the regulation in the electronic phase transitions of correlated oxides is still in a long-standing puzzle, owing to the strong correlation effect. As a representative case, hydrogen-associated Mottronic transition introduces an additional ion degree of freedom into the correlated oxides that is rather difficult to decouple from the correlated system. In addition, from the perspective of material synthesis, the above-mentioned correlated oxides are expected to be compatible with conventional semiconducting process, by which the prototypical correlated electronic devices can be largely developed. The key point that accurately adjusts and designs the electronic phase transitions for correlated oxides via external fields is presented to clarify the basic relationship between the microscopic degrees of freedom and macroscopic correlated physical properties. On the basis, the multiple electronic phase transitions as triggered by external field within correlated oxides provide new guidance for designing new functionality and interdisciplinary device applications.
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Keywords:
- strongly correlated oxides /
- electronic phase transition /
- correlated physical property regulation /
- metal-to-insulator transition
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图 3 化学掺杂调控强关联氧化物的电子相变特性 (a) 放电等离子体辅助的反应掺杂策略示意图[42]; (b) 掺杂VO2的相变温度随掺杂量的变化关系图[42]; (c) 掺杂VO2的相变尖锐度随相变温度的变化关系图[43]
Fig. 3. Regulating the electronic phase transition for correlated oxides via chemical doping: (a) Schematic of spark plasma assisted reactive doping strategy[42]; (b) the transition temperature for doped VO2 plotted as a function of doping concentration[42]; (c) the transition sharpness for doped VO2 plotted as a function of doping concentration[43].
图 4 质子化调控强关联氧化物的电子相变特性 (a) 质子化触发VO2发生多重轨道重构的示意图[5]; (b) 氢化VO2的氢含量深度分布图及其阻温特性[5]; (c) VO2中氢含量随W6+掺杂含量的变化关系图[57]
Fig. 4. Regulating the electronic phase transition for correlated oxides via protonation: (a) Schematic of hydrogen-induced multiple orbital reconfigurations within VO2[5]; (b) the depth profile of the hydrogen concentration and the temperature dependence of the resistivity for hydrogenated VO2[5]; (c) the hydrogen content for W6+-substituted VO2 plotted as a function of W6+ doping concentration[57].
图 5 界面应力调控强关联氧化物的电子相变特性 (a) 质子化触发NiO发生多重电子相变示意图[53]; (b) NiO/PMN-PT异质结的阻态翻转[53]; (c) 界面应力调控NiO的载流子跃迁激活能[53]
Fig. 5. Regulating the electronic phase transition for correlated oxides via interfacial strain: (a) Schematic of hydrogen-triggered multiple electronic phase transitions[53]; (b) the resistive switching of NiO/PMN-PT heterostructure[53]; (c) manipulating the carrier hooping energy of NiO by using interfacial strain[53].
图 6 特征电场调控氢化强关联氧化物的电子相变特性 (a) 特征电场触发VO2 可逆的氢致电子相变[5]; (b) 特征电场诱导氢化SmNiO3中类二极管的奇异输运行为[70]; (c) SmNiO3基海洋电场传感器原理图[71]; (d) SmNiO3海洋电场传感的晶体学各向异性[71]
Fig. 6. Regulating the electronic phase transition for hydrogenated correlated oxides via imparting a critical electric field: (a) Voltage-actuated reversible hydrogen-associated electronic phase transition of VO2 [5]; (b) electrically tunable diode-like transport behavior of hydrogenated SmNiO3 [70]; (c) schematic of SmNiO3-based ocean electric field sensor[71]; (d) the crystallographic anisotropy in the ocean electric field sensing of SmNiO3[71].
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