关联电子体系新奇磁学性质的研究
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摘要
本论文报道了几种典型的关联电子体系材料的合成方法、晶体结构与磁学、电学性质。系统的研究了关联电子体系材料在低温下自旋的关联有序态,并在深入材料结构与性能关系的基础上对材料表现出丰富的磁学现象给出了科学的解释。
在第一章绪论中,介绍了Mott绝缘体的提出、内容以及Mott-Hubbard模型,对材料磁性的起源、磁性的分类、自旋间的交换相互作用等进行了总结。第二章中,对无机合成技术中三种常用的制备技术进行了介绍,并对一些相关测试原理、技术参数与指标进行归纳总结。第三章中,详细的研究了Li(Mn,Cr)O2材料的磁学性质。自旋轨道耦合效应在高温区对材料的磁化率曲线起着重要的影响,表明了该体系存在着传统凝聚态体系所不具备的自旋和轨道自由度间的耦合。该材料在低温呈现类自旋玻璃态行为;表明该体系存在较强的量子涨落(quantum fluctuation)。第四章中,系统的讨论了六方晶系的Li0.8V0.8O2的水热合成条件,并且通过XPS能谱表征发现体系中V离子的价态为+4价。材料呈现出的低温顺磁基态和典型的半导体导电行为都说明该体系基态是Anderson绝缘体。第五章中,具体地讨论了空穴掺杂对于低温自旋链系统材料LiCuVO4的影响。通过XPS能谱、Raman光谱与磁性方面的研究,我们发现空穴掺杂可以诱导体系出现部分低自旋态的Cu3+离子,材料的磁学性质的变化源于非磁性Cu3+离子的影响,而非普遍意义上的Zhang-Rice单重态。第六章主要围绕着对反尖晶石结构LiNiVO4材料磁学性质的研究展开,发现该材料在高温存在自旋轨道耦合效应,在低温呈现短程反铁磁有序的磁基态。
The free electron theory of metal and band theory of solids are based on the single-electron approximation. In solid state physics, atom is composed of the valence electrons and ion. When we study the electron motions, the Born-Oppenheimer approximation is an important assumption that the electronic motion and ion motion in molecules are independent of each other. In the theory of free electron, ion can be regarded as background with positive charge to maintain charge neutral. While in the single-electron approximation of band theory, the effect of ion is summed up as the periodic potential and the other electrons move in the mean field. The effects of electron-electron interaction are included in the exchange-correlated term by various methods, such as Hartree-Fork theory and Density-functional theory. As the correlated interaction becomes stronger, the single-electron approximation will be invalidated. Especially for the d-electron transition metal oxides, the correlated interaction among the electrons is so strong that the novel properties can not be well explained by the traditional condensed matter theories.
The correlated interaction among electrons induces a series of important physical phenomena, such as novel magnetic properties, giant magnetoresistance, superconductivity, and so on. In the correlated system, there also exist the correlated interaction among spins, between spins and orbits, and between spins and lattices. Such correlated interaction is the physical origin of novel magnetic properties in solids. The magnetic effect comes from the correlated interaction among electrons, rather than the effect of quantum relativism.
In this thesis, we explored some typical kinds of materials with correlated interaction and studied their synthesis processes, lattice structure, magnetic properties and electronic properties. We also offered our perspective on their novel and abundant magnetic phenomena.
(1)In most manganites, Mn3+ ion is in High-spin state with three 3d electrons in t2g orbits and the last in the eg orbits. Some interesting and important properties are concerned with the two eg orbits under the strong electron correlation. Our experimental and theoretical study find that rhombohedral Li(Mn,Cr)O2 displays abnormal spin state with four 3d electrons occupying all three t2g orbits, S=1. Furthermore, a magnetic transition from paramagnetism to paramagnetism is found in high-temperature region, which shows changes of magnetic moment. Spin-orbit coupling plays an important role in this transition. The materials shows spin-glass-like behavior in low-temperature region, which should comes from the effect of geometrical frustration and abnormal t2g properties.
(2)Rhombohedral Li0.8V0.8O2 was synthesized by hydrothermal method, and the influence of alkalinity on the hydrothermal treatment is also studied. The measurement of dc/ac susceptibility shows paramagentism in the whole temperature region between 2 K and 300 K. Typical semiconducting behaviors of resistivity is found, which can be explained by the variable-range-hopping mechanism. In Li0.8V0.8O2, Li+ and V4+ ion are disorderly distributed in the 3a and 3b sites. Disorder can induce the localization of electron state. Model of Anderson weak localization is employed to explain the low-temperature paramagnetism and semiconducting behavior.
(3)Low-temperature quantum magnets have attracted considerable attentions because of their rich and interesting quantum magnetic phenomena, which have no analogy in high dimensions due to the enhanced quantum fluctuations in the one-dimensional (1D) structure. We systemically study the effect of hole-doping on the structure, valence state and magnetic properties of one-dimensional spin chain material LiCuVO4. XPS results showed that the valence state of V and O ion maintain unchanged before and after hole- doping. But the valence of Cu ion changes and partly +3 Cu ion appear, which is in correspondence with results of magnetic moment calculation. Part nonmagnetic [Cu3+O4] units suppress the magnetic susceptibility and induce new magnetic ordering at low temperature.
(4)Despite the same chemical formula with that of LiCuVO4, LiNiVO4 has a totally different lattice structure, because of the John-Teller effect of Cu2+ ion. LiNiVO4 is of the inverse spinel structure with space group Fd 3 m, whose Li+ and Ni2+ ion disorderly occupy the space of octahedron, and V5+ ion is in the space of tetrahedron. The chemical formula can also be represented as V(LiNi)O4. There exists spin-orbit coupling in the high-temperature region, and LiNiVO4 displays short-range antiferromagnetic order.
在第一章绪论中,介绍了Mott绝缘体的提出、内容以及Mott-Hubbard模型,对材料磁性的起源、磁性的分类、自旋间的交换相互作用等进行了总结。第二章中,对无机合成技术中三种常用的制备技术进行了介绍,并对一些相关测试原理、技术参数与指标进行归纳总结。第三章中,详细的研究了Li(Mn,Cr)O2材料的磁学性质。自旋轨道耦合效应在高温区对材料的磁化率曲线起着重要的影响,表明了该体系存在着传统凝聚态体系所不具备的自旋和轨道自由度间的耦合。该材料在低温呈现类自旋玻璃态行为;表明该体系存在较强的量子涨落(quantum fluctuation)。第四章中,系统的讨论了六方晶系的Li0.8V0.8O2的水热合成条件,并且通过XPS能谱表征发现体系中V离子的价态为+4价。材料呈现出的低温顺磁基态和典型的半导体导电行为都说明该体系基态是Anderson绝缘体。第五章中,具体地讨论了空穴掺杂对于低温自旋链系统材料LiCuVO4的影响。通过XPS能谱、Raman光谱与磁性方面的研究,我们发现空穴掺杂可以诱导体系出现部分低自旋态的Cu3+离子,材料的磁学性质的变化源于非磁性Cu3+离子的影响,而非普遍意义上的Zhang-Rice单重态。第六章主要围绕着对反尖晶石结构LiNiVO4材料磁学性质的研究展开,发现该材料在高温存在自旋轨道耦合效应,在低温呈现短程反铁磁有序的磁基态。
The free electron theory of metal and band theory of solids are based on the single-electron approximation. In solid state physics, atom is composed of the valence electrons and ion. When we study the electron motions, the Born-Oppenheimer approximation is an important assumption that the electronic motion and ion motion in molecules are independent of each other. In the theory of free electron, ion can be regarded as background with positive charge to maintain charge neutral. While in the single-electron approximation of band theory, the effect of ion is summed up as the periodic potential and the other electrons move in the mean field. The effects of electron-electron interaction are included in the exchange-correlated term by various methods, such as Hartree-Fork theory and Density-functional theory. As the correlated interaction becomes stronger, the single-electron approximation will be invalidated. Especially for the d-electron transition metal oxides, the correlated interaction among the electrons is so strong that the novel properties can not be well explained by the traditional condensed matter theories.
The correlated interaction among electrons induces a series of important physical phenomena, such as novel magnetic properties, giant magnetoresistance, superconductivity, and so on. In the correlated system, there also exist the correlated interaction among spins, between spins and orbits, and between spins and lattices. Such correlated interaction is the physical origin of novel magnetic properties in solids. The magnetic effect comes from the correlated interaction among electrons, rather than the effect of quantum relativism.
In this thesis, we explored some typical kinds of materials with correlated interaction and studied their synthesis processes, lattice structure, magnetic properties and electronic properties. We also offered our perspective on their novel and abundant magnetic phenomena.
(1)In most manganites, Mn3+ ion is in High-spin state with three 3d electrons in t2g orbits and the last in the eg orbits. Some interesting and important properties are concerned with the two eg orbits under the strong electron correlation. Our experimental and theoretical study find that rhombohedral Li(Mn,Cr)O2 displays abnormal spin state with four 3d electrons occupying all three t2g orbits, S=1. Furthermore, a magnetic transition from paramagnetism to paramagnetism is found in high-temperature region, which shows changes of magnetic moment. Spin-orbit coupling plays an important role in this transition. The materials shows spin-glass-like behavior in low-temperature region, which should comes from the effect of geometrical frustration and abnormal t2g properties.
(2)Rhombohedral Li0.8V0.8O2 was synthesized by hydrothermal method, and the influence of alkalinity on the hydrothermal treatment is also studied. The measurement of dc/ac susceptibility shows paramagentism in the whole temperature region between 2 K and 300 K. Typical semiconducting behaviors of resistivity is found, which can be explained by the variable-range-hopping mechanism. In Li0.8V0.8O2, Li+ and V4+ ion are disorderly distributed in the 3a and 3b sites. Disorder can induce the localization of electron state. Model of Anderson weak localization is employed to explain the low-temperature paramagnetism and semiconducting behavior.
(3)Low-temperature quantum magnets have attracted considerable attentions because of their rich and interesting quantum magnetic phenomena, which have no analogy in high dimensions due to the enhanced quantum fluctuations in the one-dimensional (1D) structure. We systemically study the effect of hole-doping on the structure, valence state and magnetic properties of one-dimensional spin chain material LiCuVO4. XPS results showed that the valence state of V and O ion maintain unchanged before and after hole- doping. But the valence of Cu ion changes and partly +3 Cu ion appear, which is in correspondence with results of magnetic moment calculation. Part nonmagnetic [Cu3+O4] units suppress the magnetic susceptibility and induce new magnetic ordering at low temperature.
(4)Despite the same chemical formula with that of LiCuVO4, LiNiVO4 has a totally different lattice structure, because of the John-Teller effect of Cu2+ ion. LiNiVO4 is of the inverse spinel structure with space group Fd 3 m, whose Li+ and Ni2+ ion disorderly occupy the space of octahedron, and V5+ ion is in the space of tetrahedron. The chemical formula can also be represented as V(LiNi)O4. There exists spin-orbit coupling in the high-temperature region, and LiNiVO4 displays short-range antiferromagnetic order.
引文
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