RESUMEN
Two-dimensional (2D) halide perovskites represent the natural semiconductor quantum wells (QWs), which hold great promise for optoelectronics. However, due to the hybrid structure of Ruddlesden-Popper 2D perovskites, the intrinsic nature of hot-carrier kinetics remains shielded within. Herein, we adopt CsPbBr3 nanoplates as a model system to reveal the intrinsic carrier dynamics in inorganic perovskite QWs. Interestingly, we revealed an ultrafast and hot-phonon-bottleneck (HPB)-free carrier cooling in monodisperse CsPbBr3 QWs, which is in sharp contrast to the bulk and nanocrystalline perovskites. The absence of HPB was attributed to the efficient out-of-plane triplet-exciton-LO-phonon coupling in 2D perovskites because of the structural anisotropy. Accordingly, the HPB can be activated by shutting down the out-of-plane energy loss route through forming the layer-stacked perovskite superlattice. The controllable on and off of HPB may provide new possibilities in optoelectronic devices and these findings deepen the understanding of a hot-carrier cooling mechanism in 2D perovskites.
RESUMEN
Sn-doped lead halide perovskites (LHPs) have attracted considerable attention for their lower bandgap and lower toxicity. While it is well-established that Sn doping easily introduces a lot of structural defects into LHP films, the extent to which these defects impact carrier dynamics has yet to be fully elucidated. Herein, we take Sn-doped MAPbBr3 films as an example to explore the influence of Sn doping on their carrier dynamics. The results show that Sn doping can simultaneously introduce many fillable electron traps and unfillable hole traps, consequently instigating an ultrafast carrier capture process. This further elicits long-lived internal charge separation between band edge and trap states or between two kinds of trap states, thereby enabling these carriers to persist for up to â¼2.6 µs. Our findings suggest that Sn doping potentially serves as an effective strategy to prolong the carrier lifetime in LHPs, which could pave the way for potential applications within Sn-based perovskites.
RESUMEN
Perovskite materials have demonstrated great potential for ultrafast scintillators with high light yield. However, the decay time of perovskite still cannot be further minimized into sub-nanosecond region, while sub-nanosecond scintillators are highly demanded in various radiation detection, including high speed X-ray imaging, time-of-flight based tomography or particle discrimination, and timing resolution measurement in synchrotron radiation facilities, etc. Here, a rational design strategy is showed to shorten the scintillation decay time, by maximizing the dielectric difference between organic amines and Pb-Br octahedral emitters in 2D organic-inorganic hybrid perovskites (OIHP). Benzimidazole (BM) with low dielectric constant inserted between [PbBr6 ]2- layers, resulting in a surprisingly large exciton binding energy (360.3 ± 4.8 meV) of 2D OIHP BM2 PbBr4 . The emitting decay time is shortened as 0.97 ns, which is smallest among all the perovskite materials. Moreover, the light yield is 3190 photons MeV-1 , which is greatly higher than conventional ultrafast scintillator BaF2 (1500 photons MeV-1 ). The rare combination of ultrafast decay time and considerable light yield renders BM2 PbBr4 excellent performance in γ-ray, neutron, α-particle detection, and the best theoretical coincidence time resolution of 65.1 ps, which is only half of the reference sample LYSO (141.3 ps).
RESUMEN
Accurate characterization of the longitudinal (along the thickness direction) carrier transport property is of significant importance for evaluating the quality and performance of perovskite thin films. Herein, we report the development of a modified transient reflection (TR) spectroscopy method to realize the direct observation and determination of the longitudinal carrier transport process in MAPbI3 polycrystalline thin films. Unlike the traditional TR spectroscopy, the carrier transport dynamics along the film thickness is resolved by making the pump (excitation) and probe beams spatially separated on each side of the film, so that the carrier transport from the excitation side to the probe side is directly captured. Utilizing this method, the longitudinal carrier diffusion coefficients (D) in various perovskite films with different thicknesses and grain sizes (extracted from SEM images) are determined, showing D values of â¼1.5 to 1.8 cm2 s-1 (â¼0.5 to 0.8 cm2 s-1) for films with grain size larger (smaller) than the thickness. This empirical correlation between the longitudinal D and film thickness/grain size provides a reference for quick quality screening and evaluation of perovskite polycrystalline thin films.