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

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

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Chapter 2 Overview of the Theoretical Background 27<br />

Figure 2.1: Temperature dependence of the l<strong>in</strong>ear susceptibility of NpO 2 . The open<br />

po<strong>in</strong>ts are the measured result of [14].<br />

shown <strong>in</strong> Fig. 2.1 rises to a small cusp at the transition temperature, and<br />

stays almost constant below [22, 52]. First, the observations were ascribed<br />

to antiferromagnetic <strong>order<strong>in</strong>g</strong>. However, neutron diffraction experiments did<br />

not detect magnetic order [23], and Mössbauer measurement has given an<br />

upper limit 0.01µ B for the ordered moment.<br />

Np 4+ ions have the configuration 5f 3 , the correspond<strong>in</strong>g Hund’s rule<br />

ground state set belongs to J = 9/2. Let us immediately observe that for an<br />

odd number of <strong>electron</strong>s the symmetry classification of the <strong>electron</strong> states has<br />

to come from the theory of double groups. Without go<strong>in</strong>g <strong>in</strong>to the details,<br />

we recall the result that Γ J=9/2 = Γ 6 +2Γ 8 where Γ 8 is a four-dimensional (Γ 6<br />

is a two-dimensional) irrep of the cubic double group. The experimentally<br />

established splitt<strong>in</strong>g scheme is schematically shown <strong>in</strong> Fig. 2.2. The |Γ (1)<br />

8 〉<br />

ground state quartet is well separated from the other states.<br />

The relevant local Hilbert space is the four dimensional |Γ (1)<br />

8 〉. Its fourfold<br />

degeneracy can be understood as comb<strong>in</strong>ed of a twofold Kramers and a<br />

twofold non-Kramers degeneracy.<br />

Resonant X-ray scatter<strong>in</strong>g measurement [17] found long-range order of the<br />

Γ 5 electric quadrupole moments. However, quadrupolar <strong>order<strong>in</strong>g</strong> alone cannot<br />

resolve the Kramers degeneracy: there should rema<strong>in</strong> magnetic moments<br />

at low temperatures giv<strong>in</strong>g rise to a Curie susceptibility, and this is <strong>in</strong> contrast<br />

with the observations. Furthermore, muon sp<strong>in</strong> relaxation shows that<br />

local magnetic fields, with a pattern suggestive of magnetic octupoles, appear<br />

below the 25K transition temperature [53]. Octupolar order can resolve<br />

the Kramers degeneracy. In NpO 2 there exists only one phase transition, so<br />

the question is whether quadrupolar and octupolar order can appear at the

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