3.

8 The f 2 Configuration 121

is possibly quadrupolar. The fact that the third-order magnetic sus-

ceptibility x3 shows a positive divergency at Tt,[331], may (but again,
may not) support the quadrupolar scenario (the relationship between
a x3 anomaly and quadrupolar ordering is demonstrated in the solu-
tion to Problem 2.8, p. 74). We return to the question of quadrupolar
ordering in Sea. 3.9 and 3.10.1. We are going to see that there are well-
established cases of quadrupole order, and also of coexisting quadrupole
and magnetic order22. However, the case of URu2Si2 is less clear-cut
than some of the others, and the nature of its ordered phases is still
debatable.

3.8.4 Exchange Induced Magnetism

PrRunSiz is isostructural with URu2Si2 and it contains Pr3+ 4 4f2
ions, thus we might think that the two systems ought to show similar
behaviour. In fact, they could hardly be more different. PrRuzSiz is a
ferromagnet below Tc = 14K, and the T = 0 ionic moment23 is fairly
large: 2 . 7 6 ~[300].
~
It is thought that the crystal field ground state of a Pr3+ ion is
a singlet; however, this time it is a rtl state, separated by a gap A
from the rt2 singlet [300]. Apparently, it is a good approximation to
take Irtl) = (1/d%(l4) +
I - 4)), and lrt2) = (l/fiW)- I - 4)),
as before. Thus the large moments are there, only they are mixed
into non-magnetic combinations. If we can de-mix across the crystal
field gap, we should expect that the resulting moments interact with a
strongly anisotropic exchange coupling like -I Jf Jf . Using the mean
field approximation, the single-ion energy expression is

(3.71)
where a = z I ( J z ) , z being the coordination number. Doing the cal-
culation, one finds that the system has a magnetically ordered ground
22As a rule, these two kinds of order should set in at different temperatures since
they are of completely different nature: magnetism breaks time reversal invariance,
while quadrupole order does not. It is possible that there are two closely spaced
transitions in URu2Siz , which cannot be resolved experimentally.
23Thiscomes from Mossbauer measurements. Bulk magnetization would give the
somewhat smaller 2 . 6 9 ~ Though
~. it is clear that Pr makes the substance magnetic,
the Ru 4d bands become polarized, and this accounts for the discrepancy [300].