Phonon fingerprints of CsPb₂Br₅

CsPb₂Br₅ is a stable, water-resistant, material derived from CsPbBr₃ perovskite and featuring two-dimensional Pb-Br framework separated by Cs layers. Both compounds can coexist at nanolength scale, which often produces conflicting optical spectroscopy results. We present a complete set of polarized Raman spectra of nonluminescent CsPb₂Br₅ single crystals that reveals the symmetry and frequency of nondegenerate Raman active phonons accessible from the basal (0 0 1) plane. The experimental results are in good agreement with density functional perturbation theory simulations, which suggests that the calculated frequencies of yet unobserved double degenerate Raman and infrared phonons are also reliable. Unlike CsPbBr₃, the lattice dynamics of CsPb₂Br₅ is stable as evidenced by the calculated phonon dispersion. The sharp Raman lines and lack of a dynamic-disorder-induced central peak in the spectra at room temperature indicate that the coupling of Cs anharmonic motion to Br atoms, known to cause the dynamic disorder in CsPbBr₃, is absent in CsPb₂Br₅.