  To understand the mechanisms by which Fe and Cr additions increase the
corrosion rate of irradiated Zr alloys, a combination of experimental (atom
probe tomography, x-ray diffraction and thermoelectric power measurements) and
modelling (density functional theory) techniques are employed to investigate
the non-equilibrium solubility and clustering of Fe and Cr in binary Zr alloys.
Cr occupies both interstitial and substitutional sites in the {\alpha}-Zr
lattice, Fe favours interstitial sites, and a low-symmetry site that was not
previously modelled is found to be the most favourable for Fe. Lattice
expansion as a function of alloying concentration (in the dilute regime) is
strongly anisotropic for Fe additions, expanding the $c$-axis while contracting
the $a$-axis. Defect clusters are observed at higher solution concentrations,
which induce a smaller amount of lattice strain compared to the dilute defects.
In the presence of a Zr vacancy, all two-atom clusters are more soluble than
individual point defects and as many as four Fe or three Cr atoms could be
accommodated in a single Zr vacancy. The Zr vacancy is critical for the
increased solubility of defect clusters, the implications for irradiation
induced microstructure changes in Zr alloys are discussed.
