Mn Doping in Low-Dimensional Perovskites: A Switch for Controlling Dopant and Host Emission

Abstract

The growth of solid-state photonics relies on the design of highly efficient devices with tunable photoluminescence (PL) based on thermally stable phosphors. In this study, a room-temperature, all-ambient synthesis of Mn-doped hybrid lead halide perovskite phosphors is presented. By applying temperature-dependent (4.2–300 K) steady-state and transient PL measurements, the photophysical pathways of the hybrid system were identified and the carrier recombination processes at play were defined. At higher Mn-doping concentrations (>4%), the excitonic white light host emission nearly disappears, and a bright Mn transition appears at ∼650 nm with a record PL quantum yield of ∼87.4%. The intense sensitized Mn luminescence results from rapid and efficient exciton-to-dopant energy transfer, as evidenced by time-gated and femtosecond fluorescence upconversion measurements. A millisecond PL decay time attributed to the Mn dopant and a microsecond PL decay time associated with the excitonic emission of the host were found, indicating energy and reverse energy transfer in the system. These findings provide unique insights into the chemical tailoring of the Mn-dopant emission by investigating the coupling between the host semiconductor and the dopant ion, a stepping stone toward the development of high-performance solid-state light-emitting diodes and scintillators.