Ultralow Thermal Conductivity of 2D Dion–Jacobson (PDA)(FA)n−1PbnI3n+1 Perovskite Films

Two-dimensional (2D) perovskites exhibit enhanced thermal stability compared to three-dimensional perovskites, especially the emerging 2D Dion–Jacobson (DJ) phase perovskite. However, the heat transfer mechanisms in DJ phase perovskites are rarely reported. Herein, we determine thermal conductivities of (PDA)(FA) n − 1 Pb n I 3 n + 1 films with n = 1−6 by time-domain thermoreflectance. The measured results indicate that the thermal conductivities of these films are extremely low, showing a trend from decline to rise with increasing n values, and reaching to the lowest when n = 2. We measure the propagation of acoustic phonons in films with n = 1−3 by time-domain Brillouin scattering and find phonon velocity plays a key role in the thermal conductivity, which can be explained by the mismatch of spring constants between the inorganic layer and the organic layer using the bead-spring model. The gradually increasing thermal conductivity for larger n values is attributed to the gradual transformation of the grain orientation from horizontal to vertical, which is demonstrated by the grazing-incidence wide-angle x ray scattering (GIWAXS) results. Our work deepens the understanding of the thermal transport process in 2D DJ phase perovskite films and provides insights into thermal management solutions for their devices.