Anharmonicity of Phonon Modes in MBE‐Grown Bi2Te3 Thin Films: A Temperature‐Dependent Raman Study

Abstract

ABSTRACTThis study examines the temperature‐dependent Raman spectra of MBE‐grown bismuth telluride (Bi2Te3) thin films, analyzing Stokes, and anti‐Stokes scattering in two polarizations to resolve symmetry‐dependent mode strengths. Density functional theory simulations of Stokes spectra identified the fundamental vibrational modes and anharmonic decay. The temperature evolution of phonon wavenumbers and linewidths revealed the role of anharmonicity: the real part of the phonon self‐energy governs the wavenumber shift (redshift) of the mode, while its imaginary part drives the linewidth broadening, both arising from cubic and quartic anharmonic processes which is associated to energy and symmetry of the mode. In contrast, the lower wavenumber and modes exhibited weaker coupling to thermal decay channels, reflected in smaller changes to their self‐energy components and longer lifetimes. The intensity of mode decreased significantly with temperature due to multi‐phonon decay, whereas and intensities remained stable. These results quantify the distinct mediation of wavenumber renormalization and lifetime effects in Bi2Te3 by the real and imaginary components of the phonon self‐energy.