Phonons in Copper Diphosphide (CuP2): Raman Spectroscopy and Lattice Dynamics Calculations.

Abstract

Copper diphosphide (CuP2) is an emerging binary semiconductor with promising properties for energy conversion and storage applications. While functionality and possible applications of CuP2 have been studied, there is a curious gap in the investigation of its vibrational properties. In this work, we provide a reference Raman spectrum of CuP2, with a complete analysis of all Raman active modes from both experimental and theoretical perspectives. Raman measurements have been performed on polycrystalline CuP2 thin films with close to stoichiometric composition. Detailed deconvolution of the Raman spectrum with Lorentzian curves has allowed identification of all theoretically predicted Raman active modes (9Ag and 9Bg), including their positions and symmetry assignment. Furthermore, calculations of the phonon density of states (PDOS), as well as the phonon dispersions, provide a microscopic understanding of the experimentally observed phonon lines, in addition to the assignment to the specific lattice eigenmodes. We further provide the theoretically predicted positions of the infrared (IR) active modes, along with the simulated IR spectrum from density functional theory (DFT). Overall good agreement is found between the experimental and DFT-calculated Raman spectra of CuP2, providing a reference platform for future investigations on this material.