Photoluminescence Quenching in CsPbCl₃ upon Fe Doping: Colloidal Synthesis, Structural and Optical Properties

Abstract

Doped perovskite lead halide nanocrystals (PHNCs) are promising materials for various optoelectronic applications, but the major challenge faced by the researchers is the inability to dope foreign elements into perovskite lattice because of the strong lead-halide bond energies. In this work, we have used Fe as a dopant in CsPbCl 3 to explore different doping techniques based on the colloidal synthesis of PHNCs to investigate the advantages and disadvantages of different techniques. We are able to dope a relatively higher amount of Fe (~10%) than reported and observe clear optical signatures when the precursor does not have pre-existing PbÀ Cl bonds. We prove that there are two competing processes inside a doped PHNC -one is the effect of dopant energy levels, and the other is surface passivation by halide ions. Using the most optimal synthesis strategy, we show that although Fe does act as a luminescence quencher in perovskite similar to II-VI quantum dots (QDs), the quenching requires much more Fe compared to trace amounts of Fe required in traditional QDs. Our work will assist in giving an overall comparative idea of doping and finding the most optimized strategy and help identify the underlying physical processes in perovskite based QDs.

Insights into the Impact of Fe-Doped CsPbCl3 Perovskites on Stability and Luminescence: A First-Principles Investigation

“…Moreover, spin polarization is considered in our calculation. In this work, according to the Fe low doping concentration from the experimental report, we investigate the physical properties of only three structures, which are CsPbCl 3 ( x = 0), CsPb 0.963 Fe 0.037 Cl 3 ( x = 0.037), and CsPb 0.926 Fe 0.074 Cl 3 ( x = 0.074) corresponding to Fe doping concentrations of 0, 3.7, and 7.4%, respectively. 3 × 3 × 3 supercells of 135 atoms are used for the computation of CsPb 1– x Fe x Cl 3 .…”

Thermally Evaporated CsPbCl3 Perovskite on Si/SiO2 with Wide Spectrum Photoresponse from Ultraviolet (UV) to Near-Infrared (NIR)

“…Moreover, the photophysical properties of the metal halide perovskite can be further modulated by the incorporation of optically active dopants, such as lanthanide (Ln 3+ ) and transition metal ions (Mn 2+ , Fe 2+ , Cd 2+ ). − Since the first reported successful doping of Ln 3+ in CsPbX 3 perovskite quantum dots (PQDs), Ln 3+ doped perovskites have been extensively investigated for their promising applications in optoelectronics. , In Ln 3+ doped perovskite NCs, the large absorption cross section (1 × 10 –14 to 1 × 10 –13 cm 2 ) of the perovskite NCs is of great advantage for harvesting energy needed to excite the Ln 3+ dopants whose sensitized intra-atomic f–f transitions will lead to long-lived and narrow-band emissions valuable in optoelectronics devices like solar cells and light-emitting diodes . Particularly, Yb 3+ doped CsPbX 3 PQDs exhibit efficient near-infrared (NIR) emissions with PLQY of 173% via a unique quantum cutting (QC) process, which is a highly efficient picosecond energy transfer and two-photon excitation process from the perovskite host to the Yb 3+ dopant 2 F 5/2 excited level .…”