Calculation of the spectral, structural, and electronic properties of NaCrSi2O6 and LiCrSi2O6 crystals

•Combined analysis based on crystal field theory and DFT independent methods have been used for (Na, Li)CrSi2O6 crystals.•Crystal field parameters modeling and energy levels scheme simulation of two Cr3+-bearing system have been made.•Structural and electronic properties of considered materials were predicted.

Spectral, structural and electronic properties of two Cr3+-bearing systems (NaCrSi2O6, LiCrSi2O6) have been theoretically modeled using two different approaches: semi-empirical model of crystal field, in the framework of the Exchange Charge Model and two ab initio DFT-based calculations, as implemented in the CASTEP module [1] of Materials Studio package [2] and, for reliability, CRYSTAL09 code [3]. The first one allows for calculations of the electronic levels of sixfold coordinated Cr3+ ions in a crystal field of host’s ligands and direct comparison with experimental absorption spectra [4]. The latter two allow for the analysis of the band structure and density of states (DOS), after optimization of the crystal lattice structures of these materials. In particular, a special attention was paid to the energetic position of the Cr3+ 3d states. All obtained results are compared with corresponding experimental values and discussed.