A momentum-resolved view of polaron formation in materials (2402.01468v1)

Abstract: A combined experimental and computational methodology for interrogating the phonon contribution to polaron formation in real materials is developed. Using LiF as an example, we show that the recent ab-initio theory of Sio et. al [PRL 122, 246403 (2019)] makes predictions of the momentum- and branch dependent phonon amplitides in polaron quasiparticles that are testable using ultrafast electron diffuse scattering (UEDS) and related techniques. The large electron polaron in LiF has UEDS signatures that are qualitatively similar to those expected from a simple point-defect model, but the small hole polaron exhibits a profoundly anisotropic UEDS pattern that is in poor agreement with a point-defect model. We also show that these polaron diffuse scattering signatures are directly emblematic of the underlying polaron wavefunction. The combination of new time and momentum resolved experimental probes of nonequilibrium phonons with novel computational methods promises to complement the qualitative results obtained via model Hamiltonians with a first principles, material-specific quantiative understanding of polarons and their properties.