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Ph.D. THESIS Multipolar ordering in f-electron systems

Ph.D. THESIS Multipolar ordering in f-electron systems

Ph.D. THESIS Multipolar ordering in f-electron systems

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Contents<br />

1 Introduction 3<br />

2 Overview of the Theoretical Background 5<br />

2.1 General Considerations . . . . . . . . . . . . . . . . . . . . . . 5<br />

2.2 Crystal Field Theory . . . . . . . . . . . . . . . . . . . . . . . 8<br />

2.2.1 Stevens Equivalents . . . . . . . . . . . . . . . . . . . . 9<br />

2.2.2 Crystal Field Splitt<strong>in</strong>g . . . . . . . . . . . . . . . . . . 11<br />

2.3 Local Order Parameters . . . . . . . . . . . . . . . . . . . . . 14<br />

2.4 Interactions Between the Multipoles . . . . . . . . . . . . . . . 17<br />

2.5 <strong>Ph</strong>ase Transitions . . . . . . . . . . . . . . . . . . . . . . . . . 21<br />

2.6 Review of f-<strong>electron</strong> Systems . . . . . . . . . . . . . . . . . . 25<br />

2.6.1 NpO 2 . . . . . . . . . . . . . . . . . . . . . . . . . . . 26<br />

2.6.2 Pr-filled Skutterudites . . . . . . . . . . . . . . . . . . 29<br />

2.6.3 URu 2 Si 2 . . . . . . . . . . . . . . . . . . . . . . . . . . 32<br />

3 Octupolar Order<strong>in</strong>g of Γ 8 Ions 36<br />

3.1 Octupolar Moments <strong>in</strong> the Γ 8 Quartet State . . . . . . . . . . 37<br />

3.2 The Octupolar–Quadrupolar Model . . . . . . . . . . . . . . . 41<br />

3.2.1 The Case of Zero Magnetic Field . . . . . . . . . . . . 42<br />

3.2.2 The Case of H‖(111) Magnetic Field . . . . . . . . . . 46<br />

3.3 The Effect of Magnetic Field with Arbitrary Direction on the<br />

Octupolar Order<strong>in</strong>g . . . . . . . . . . . . . . . . . . . . . . . . 50<br />

3.3.1 Ground State Calculation . . . . . . . . . . . . . . . . 51<br />

3.3.2 Field Induced Multipoles . . . . . . . . . . . . . . . . . 53<br />

3.3.3 Connection with the Mean-Field Results . . . . . . . . 55<br />

3.4 Symmetry Classification of Multipoles <strong>in</strong> External Magnetic<br />

Field . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 57<br />

3.4.1 Symmetry Related Expansion of the Helmholtz Potential:<br />

Method I. . . . . . . . . . . . . . . . . . . . . . . 59<br />

3.4.2 Inclusion of the Time Reversal: Method II. . . . . . . . 64<br />

3.4.3 Remarks . . . . . . . . . . . . . . . . . . . . . . . . . . 66<br />

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