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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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