Electronic structure, metamagnetism and thermopower of LaSiFe$_{12}$ and interstitially doped LaSiFe$_{12}$

Abstract: We present a systematic investigation of the effect of H, B, C, and N interstitials on the electronic, lattice and magnetic properties of La(Fe,Si)${13}$ using density functional theory. The parent LaSiFe${12}$ alloy has a shallow, double-well free energy function that is the basis of itinerant metamagnetism. On increasing the dopant concentration, the resulting lattice expansion causes an initial increase in magnetisation for all interstitials that is only maintained at higher levels of doping in the case of hydrogen. Strong s-p band hybridisation occurs at high B,C and N concentrations. We thus find that the electronic effects of hydrogen doping are much less pronounced than those of other interstitials, and result in the double-well structure of the free energy function being least sensitive to the amount of hydrogen. This microscopic picture accounts for the vanishing first order nature of the transition by B,C, and N dopants as observed experimentally. We use our calculated electronic density of states for LaSiFe$_{12}$ and the hydrogenated alloy to infer changes in magneto-elastic coupling and in phonon entropy on heating through $T_C$ by calculating the fermionic entropy due to the itinerant electrons. Lastly, we predict the electron thermopower in a spin-mixing, high temperature limit and compare our findings to recent literature data.