  Using a synergistic combination of experimental and computational methods, we
shed light on the unusual solubility of (Cr,Ti)3AlC2 MAX phase, showing that it
may accommodate Cr only at very low concentrations (<2at%) or at the exact
Cr/(Cr+Ti) ratio of 2/3, even when the ratio of reactants is far from this
stoichiometry (1/2 < Cr/(Cr+Ti) < 5/6). In both phases Cr exclusively occupies
the 4f sites, bridging carbide layers with the Al layer. Despite this, the
peculiar stability of (Cr2/3Ti1/3)3AlC2 is attributed to the formation of
strong, spin-polarised Cr-C bonds, which result in volume reduction and marked
increase in c/a ratio.
