While it may at first seem counterintuitive, magnetic behavior and even magnetic
order is possible even in compounds which have no magnetic components. The
reason for this is that at low densities, a free electron gas undergoes a
series of many-body instabilities which include the formation of an ordered
electron lattice (the Wigner lattice) and then ferromagnetic order. The phase
diagram at the right shows the regimes of stability for these phenomena in
three dimensional electron systems, as functions of temperature and electron
density.
Recently ferromagnetism was found in single crystals of semiconducting
CaB6, in which small amounts of La were introduced to create
mobile electrons at densities of about 1019cm3, or
with electronic separations of ~50 Bohr radii. Since this density is comparable
to those expected to yield magnetically ordered Wigner lattices,
there was much excitement about this result, especially the Curie temperatures
which were found to be as large as 900 K in this system. We carried out a
detailed study of the relationship between the spontaneous moment, determined
by low temperature magnetization measurements and the electron concentration,
taken from Hall effect measurements. As the figure at the left shows, there
is no clear relationship between the moment and the density of electrons.
The reason for this was revealed in an electron microscopy study of the crystal
surfaces, as shown in the figure at the right. Microprobe measurements show
that macroscopic amounts of Fe and Ni are deposited on the crystal facets
and surfaces during the synthesis of the crystals. Unfortunately, it now appears
that the ferromagnetic order found in doped alkali earth hexaborides is at
least partially extrinsic and due to accidental contamination by ferromagnetic
elements.
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The properties of magnetic moments, whether introduced intentionally or not,
are subtle and interesting. We have explored several families of intermetallic
compounds, which as small gap insulators or low carrier density semimetals,
might have the potential to be driven magnetic at low carrier concentrations.
One example is the half-Heusler compounds, RXN, where R and X are transition
metal atoms and N is a pnictogen. Electronic structure calculations suggested
that if the total number of valence electrons per formula unit is 17 or more,
and if the d-electrons from the R and X elements total 10 that semiconducting
behavior should be found, and that only the defect states could lead to weak
magnetic behavior. We have confirmed this prediction by synthesizing and studying
the transport and magnetic properties of high quality single crystal and polycrystalline
specimens of HfNiSn, TiNiSN, and TiPtSn. The figure at left demonstrates the
intrinsically semiconducting behavior of the undoped hosts.
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Perhaps the most striking attribute of these low carrier density systems is
their linear magnetoresistance, found only at the lowest temperatures and
only in samples – both single crystal and polycrystalline - with substantial
doping levels. An example is shown at the right for a collection of different
single crystals. On general grounds, the magnetoresistance is not expected
to be linear, or any odd function of field, since the magnetoresistance should
not depend on the sign of the field. It is in principle possible that orbital
or magnetic order occurs in these materials, introducing an internal symmetry
breaking field. However, we believe that the linear magnetoresistance results
from phase separation on small length scales into conducting regions superposed
on an insulating matrix. To read more about linear magnetoresistance, please
see Parish and Littlewood, Nature
426, 162 (2003). A linear
and nonsaturating magnetoresistance might serve as the basis for a magnetic
field sensor device, especially for large magnetic fields such as those produced
at the National High Magnetic Field Laboratory. For more about this type of
application see Xu, et al, Nature
417, 421 (2002).