凝態物質的物理性質決定於其價電子的電子結構。電子與電子間關聯性效應而產生之新奇現象，是當代凝態物理研究中非常熱門的主題之一。例如高溫超導、龐磁阻及導體絕緣相變……等奇特現象，已吸引許多科學家投入研究。先進的實驗設備如同步輻射光源、電子能譜儀及薄膜磊晶成長技術等，為加速研究前述奇特現象的強大工具。本論文研究係結合電子能譜技術及臨場磁性薄膜成長技術，探討電子與電子間關聯性效應對物質的新穎磁性性質之影響。我們提出別於傳統能帶理論的觀點，來解釋四氧化三鐵(Fe3O4)與二氧化鉻(CrO2)的奇異半金屬特性。
首先我們應用電子自旋解析光電子發射實驗，來探討Fe3O4的半金屬性及其電子結構。在費米能階附近的自旋極化測量顯示，能帶理論所預測之半金屬性需要重新考慮，而運用一個相對於能帶理論而言較為侷化的電子結構模型，則可以成功地詮釋自旋極化測量結果。我們亦應用共振式光電子發射實驗的磁圓二向性，研究Fe3O4電子結構的相關物理量。電子自旋解析能譜實驗結果顯示，Fe3O4是一個強關聯電子系統，傳統能帶理論不能完整地描述Fe3O4的磁性與電子結構。
在CrO2方面，我們發展一套全新的自旋解析軟X光吸收能譜實驗技術，來探討CrO2非佔有態的自旋解析電子結構。實驗結果顯示，在費米能階附近的電子自旋極化接近100%，直接證明CrO2具有半金屬的特性。我們亦發現CrO2 的3d電子呈現出Mott-Hubbard系統的特徵。因此CrO2不但具有電子強關聯系統的特性，另一方面也具有能帶特性，即是CrO2價電子展現了侷化與非侷化的雙重性質。
對於強關聯電子系統的電子結構與磁性性質而言，電子與電子間關聯性扮演決定性的角色。藉由尖端電子能譜實驗，我們深入地研究未來自旋電子學應用上具有潛力的磁性材料之電子結構。現有的理論並不能完整地描述我們的新發現。期許本論文能成為未來半金屬材料電子結構之理論發展契機。

Physical properties of condensed matter are mainly determined by valence electrons. Fascinating phenomena related to electron-electron correlations, such as high temperature superconductivity, colossal magnetoresistance, and metal-to-insulator transition, are important topics in modern condensed
physics. The advances in experimental techniques, such as synchrotron radiation, electron spectroscopies, and epitaxial growth of thin films, provide us with great opportunities to unravel the underling physics of these novel phenomena. In this thesis, we performed advanced electron spectroscopic measurements to study magnetic materials in which electron-electron correlations are important. Particularly, we present a viewpoint different from the conventional band theory to describe the half-metallic behavior of
Fe$_3$O$_4$ and CrO$_2$.
First we studied the half-metallic feature and the electronic structure of Fe$_3$O$_4$ using spin-polarized photoemission. The measured spin polarization in the vicinity of the Fermi level shows that Fe$_3$O$_4$ is not half-metallic as predicted by band theory. We can successfully interpret the experimental
results using a cluster model. With the measurements of magnetic circular dichroism in Fe $2p$ resonant photoemission and cluster model calculations, we obtained the parameters of the electronic structure of Fe$_3$O$_4$. These results indicate that Fe$_3$O$_4$ is a system with strong electron-electron
interactions. Furthermore, we developed a spin-resolved soft x-ray absorption technique to explore the unoccupied electronic structure of CrO$_2$. The spin-polarization in the vicinity of the Fermi level is close to 100\%, providing direct evidence of half-metallicity. The measurements also show the
existence of an atomic-like Cr $3d$ state not far away from the Fermi level with a spin polarization of only 50\%, establishing its Mott-Hubbard character. We conclude that CrO$_2$ has a dualistic electronic nature.
In a strongly correlated system, electron correlations play an important role in its magnetic properties. With advanced electron spectroscopic measurements, we studied the electronic structure of important magnetic materials for spintronics. However none of the present theory can fully describe our new
findings; the results presented in this thesis might shed some light on the physics of half-metallic oxides.

{1}Introduction
{1.1}Overview
{1.2}Strongly Correlated Electron System}
A. Interacting electrons in transition-metal oxide}
B. Hubbard model
C. Anderson impurity model
D. Zaanen-Sawatzky-Allen classification scheme
E. Ground state configuration}
{2}Electron Spectroscopies
{2.1}Photoemission
{2.1.1}Single-particle excitation}
A. Spectral function
B. Coherent and incoherent excitation
{2.1.2}Resonant photoemission (RESPES)
{2.1.3}Photoemission set-up
{2.1.4}Attenuation lengths of photoelectron
{2.1.5}Spin-resolved photoemission
A. Spin polarimetry
B. Performance test
{2.2}Soft X-ray Absorption (XAS)
{2.2.1}$L-$edge Absorption}
{2.2.2}X-ray magnetic circular dichroism}
{2.2.3}Oxygen $1s$ XAS
{2.2.4}Spin-resolved O $1s$ XAS
{3}Epitaxial Growth of Oxide Thin Films
{3.1}In-Situ Structure Characterizations
{3.1.1}LEED
{3.1.2}RHEED
A. RHEED oscillations
B. Damping in RHEED oscillation - step flow
{3.2}Experimental Setup
{3.3}Epitaxial Growth of Iron Oxide
{3.3.1}Thin film epitaxy
A. Preparation
B. X-ray diffraction
{3.3.2}Surface reconstruction
A. Surface termination
B. Aging effect
{3.3.3}Multi-layer growth
{3.4}Iron Oxide Grown on Pt(111)
{3.4.1}Growth}
{3.4.2}Moir\'{e} pattern
{3.4.3}Fe$_3$O$_4$(111)
{3.5}Electronic Structure of ML FeO/Pt(111)
{4}Electronic Structure of Magnetite}
{4.1}Fundamental Issues about Magnetite
{4.1.1}Verwey transition
{4.1.2}Half metals predicted by band theory
{4.2}Overview
{4.2.1}Band picture
{4.2.2}Localized picture
{4.3}Spin Polarized Measurements
{4.3.1}Spin polarized photoemission
A. Experiments
B. Results
C. Fractional parentage: the upper limit of SP
D.Reduction in measured SP
E. Conclusions
{4.4}Magnetic Circular Dichroism in Fe $2p$ Resonant Photoemission
{4.4.1}XAS of Fe $L-$edge absorption
{4.4.2}MCD in Fe $2p$ resonant photoemission
{4.4.3}Comparison with calculations
{4.4.4}Partial density of states of Fe 3$d$
{4.4.5}MCD in Fe $L-$edge absorption
{4.4.6}Conclusions
{5}Dualistic Electronic Nature of CrO$_2$
{5.1}Introduction
{5.1.1}Crystal structure
{5.1.2}Double exchange
{5.1.3}Self-doping
{5.2}Epitaxial CrO$_2$ Thin Film
{5.2.1}Surface treatment
A. Cr $2p$ PES results
B. Spin resolved photoemission
C. O $1s$ XAS results
{5.2.2}Polarization dependent O $K-$edge XAS
{5.2.3}Spin resolved O $K-$XAS
{5.3}Anomalous Spin Polarization in CrO$_2$
{5.3.1}Dualistic electronic nature in CrO$_2$
{5.3.2}Electron correlations and band effect in TMO
{5.3.3}Localized character of $3d$ states in CrO$_2$
{5.3.4}Role of the oxygen $2p$ band
{5.4}Conclusions
Appendix
{A}Methods of Calculation in Fe$_3$O$_4$
{B}Multiplet calculation program: Xtls
{B.1}Introduction}
{B.2}Installation}
{B.3}The format of the parameter description file (X-card)
{C}List of Publications

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