Ab initio calculations of the crystal field and phonon dispersions in CePdAl and LaPdAl.

CePdAl crystallizes in the CaBeGe-type tetragonal structure (P4/nmm, 129) and undergoes a phase transition to the orthorhombic Cmme structure at around 13 K. Its inelastic neutron spectra reveal an additional magnetic excitation that was ascribed to electron-phonon interaction leading to a formation of a new quantum quasi-bound vibron state. We present the first-principles calculations of the crystal field excitations and lattice dynamics calculations of the phonon dispersions to compare with the experimental data. The calculated crystal field energy splitting in CePdAl agrees well with the model used to describe the experimental neutron scattering spectra. The first excited crystal field level moves to higher energies when undergoing the transformation from tetragonal to orthorhombic structure, in agreement with the experiment. The analysis based on calculated elastic constants and lattice dynamics calculations show that in both tetragonal and orthorhombic structures there are no imaginary modes for any q-wave vector within the Brillouin zone, and therefore the lattice structures are stable. The phonon dispersions and density of states are calculated for both crystal structures of CePdAl and its nonmagnetic counterpart LaPdAl. The results generally agree well with the experimental data including the high phonon density of states around 12 meV. The phonon density of states is also used to calculate the mean squared displacement, Debye temperature, lattice heat capacity and compared with similar properties of the available experiment.