RESUMEN
Lead halide perovskite nanocrystals (NCs) have attracted much attention as light-source materials for light-emitting diodes, lasers, and quantum light emitters. The luminescence properties of perovskite NCs and the performance of NC-based light-source devices depend on trion and biexciton dynamics. Here, we examined the size dependence of trion and biexciton binding energies by conducting low-temperature single-dot spectroscopy on three different perovskite NCs: CsPbBr3, CsPbI3, and FAPbBr3. While the photoluminescence spectral widths of the all-inorganic CsPbBr3 and CsPbI3 NCs were narrow, compared with those of the organic-inorganic hybrid FAPbBr3 NCs, the binding energies of trions and biexcitons of all three samples showed similar size dependences, independent of the A-site cation and halogen. The effective-mass approximation calculations implied the importance of dynamical dielectric screening on the formation of trions and biexcitons.
RESUMEN
Photoluminescence (PL) spectroscopy of individual semiconductor nanocrystals (NCs) is a powerful method for understanding the intrinsic optical properties of these materials. Here, we report the temperature dependence of the PL spectra of single perovskite FAPbBr3 and CsPbBr3 NCs [FA = HC(NH2)2]. The temperature dependences of the PL linewidths were mainly determined by the Fröhlich interaction between excitons and longitudinal optical phonons. For FAPbBr3 NCs, a redshift in the PL peak energy appeared between 100 and 150 K, which was because of the orthorhombic-to-tetragonal phase transition. We found that the phase transition temperature of FAPbBr3 NCs decreases with decreasing NC size.
RESUMEN
Lead halide perovskite nanocrystals (NCs) have outstanding photoluminescence (PL) properties and excellent potential for light-emitting diodes and single-photon sources. Here, we report the multiple-peak structures originating from excitons, trions, and biexcitons in low-temperature PL spectra of single CsPbBr3 NCs. We found fine-structure splitting in the PL peaks of bright excitons and biexcitons and also in the longitudinal-optical (LO)-phonon replicas of excitons. LO-phonon replicas of trions are clearly observed under strong photoexcitation, which do not show fine-structure splitting. From size-dependent analyses of these replicas, we clarified that both exciton-phonon and trion-phonon couplings become larger for smaller NCs and the coupling strengths of trions are larger than those of excitons in large NCs. These behaviors can be explained by the spatial distributions of the electron and hole wave functions in the NCs. Our findings provide essential information on electron-phonon couplings in perovskites and for the design of high-purity single-photon sources.
RESUMEN
Lead halide perovskite nanocrystals (NCs) have superior photoluminescence (PL) properties, such as high PL quantum yields and wide PL wavelength tunability, for optoelectronic applications. Here, we report the PL spectra of single formamidinium lead halide perovskite FAPbX3 (X = Br, I) NCs examined by single-dot spectroscopy at low temperature. We found four PL peaks in the low-energy region below the strong exciton PL peak that originate from two longitudinal-optical (LO) phonon replicas of the exciton PL, biexcitons, and charged excitons (trions). The binding energies of the biexcitons and trions become larger as the NCs decrease in size. The LO phonon energies show no size dependence, but the Huang-Rhys factors, which reflect the strength of the exciton-phonon coupling, become larger for smaller NCs. Our findings provide important insights into the exciton properties of perovskite NCs.
