Giant deformation potential induced small polaron effect in Dion–Jacobson two-dimensional lead halide perovskites

Abstract

Abstract Halide perovskites have attracted much attention recently. However, the strong lattice distortion effects in these materials have led to debates regarding the nature of charge carriers. While the behavior of carriers in bulk three-dimensional materials is well-documented, the characteristics of carriers in two-dimensional perovskites remain less understood. In this study, we provide direct and clear evidence of small polaron formation through transient spectroscopic analysis of deformation potential and dynamic lattice screening. Coherent acoustic phonon wave signals reveal a strong coupling between carriers and lattice degrees of freedom, leading to small polaron formation and a spin lifetime enhancement of up to tenfold. Utilizing optical Kerr spectroscopy and theoretical modeling, we observed a notably long polarization response time at room temperature, attributed to lattice distortion and small polarons approximately two-unit cells in size. Temperature-dependent coherent phonon dynamics and X-ray diffraction further confirmed the presence of small polarons. This discovery underscores the significance of the cooperative interplay between exciton dynamics and the small polaron field, particularly in influencing the Coulomb exchange interaction of excitons.