Many
Heusler compounds are predicted to be half-metallic ferromagnets
and thus find extensive interest as materials for spintronic applications,
an example of which is the Co2Cr1–x
Fe
x
Al series. So far, bulk samples
of that series, in particular, Cr-rich samples, do not verify those
predictions, and various studies have yielded results that are fraught
with anomalies. Thin films as well do not meet expectations, neither
in magnetoresistance ratio nor in degree of spin polarization and
magnetic moments. Polycrystalline samples of Co2CrAl, Co2FeAl, and Co2Cr0.6Fe0.4Al
were found to be phase segregated, a hurdle easily tackled by using
the optical floating zone (FZ) technique. Hence, in this work, we
have carried out crystal growth of Co2Cr1–x
Fe
x
Al Heusler compounds,
as a step toward understanding the intrinsic material properties of
this series. Our results demonstrate that, although the phase segregation
is eliminated in the FZ grown samples, an unexpected phase transformation
via spinodal decomposition takes place in Cr-rich samples. This phase
decomposition is found to strongly affect the magnetic properties
and as well as other physical properties, e.g., spin polarization.
Our finding presents new insight into the phase dynamics of this system
and provides answers to many of the issues in this series of half-metallic
ferromagnets.