La₂Pd₃Ge₅ and Nd₂Pd₃Ge₅ Compounds: Chemical Bonding and Physical Properties

Abstract

The two La₂Pd₃Ge₅ and Nd₂Pd₃Ge₅ compounds, crystallizing in the oI40-U₂Co₃Ge₅ crystal structure, were targeted for analysis of their chemical bonding and physical properties. The compounds of interest were obtained by arc melting and characterized by differential thermal analysis, scanning electron microscopy, and X-ray diffraction both on powder and on a single crystal (for the La analogue), to ensure the high quality of the samples and accurate crystallographic data. Chemical bonding was studied by analyzing the electronic structure and effective QTAIM charges of La₂Pd₃Ge₅. A significant charge transfer mainly occurs from La to Pd so that Ge species assume tiny negative charges. This result, together with the -(I)COHP analysis, suggests that, in addition to the expected homopolar Ge bonds within zigzag chains, heteropolar interactions between Ge and the surrounding La and Pd occur with multicenter character. Covalent La-Pd interactions increase the complexity of chemical bonding, which could not be adequately described by the simplified, formally obeyed, Zintl-Klemm scheme. Electric resistivity, specific heat, magnetization, and magnetic susceptibility as a function of temperature indicate for both compounds a metallic-like behavior. For Nd₂Pd₃Ge₅, two low-temperature phase transitions are detected, leading to an antiferromagnetic ground state.