Proceedings of Asia-Pacific International Conference on Perovskite, Organic Photovoltaics and Optoelectronics (IPEROP24)
DOI: https://doi.org/10.29363/nanoge.iperop.2024.005
Publication date: 18th October 2023
Solution-processed organometallic halide perovskites have been widely explored for various optoelectronic applications due to excellent wavelength tunability, high absorption/emission efficiency, easy and low fabrication cost. Optically pumped amplified stimulated emission (ASE) and lasing have been demonstrated in a variety of media such as 3D, 2D, 1D, and 0D perovskites and in a number of cavity configurations. Despite these advances, solution-processed, cavity-free perovskite thin films generally demonstrate lasing with relatively high thresholds and moderate gain values due to optical losses from scattering and non-radiative recombination which originate mainly from the defect states at the surface/bulk of the perovskite materials and their irregular morphology due to grain boundaries and sample inhomogeneity.
In this work, we prepared highly uniform Cs0.25FA0.75Pb(I0.8Br0.2)3 thin films doped with various amounts of MDACl2 that has been known to stabilize the α-phase of FAPbI3, reduce the lattice strain, and minimize the density of defect centers and traps. Photoluminescence (PL) imaging and steady-state and time-resolved (TRPL) measurements, together with density functional theory (DFT) calculations and secondary ion mass spectrometry (SIMS), reveal that Cl interstitials replace iodine (I) interstitials within the perovskite layer, with some excessive chlorine accumulating near (20-25 nm) the surface. The removal of detrimental non-radiative recombination centers associated with iodine interstitials leads to dramatic improvement of the luminescent properties and stability of the material. We found that the ASE threshold is reduced by 30 times from ~ 200 μJ/cm2 to <6 μJ/cm2 while the maximum modal gain value is record-highest for the cavity-free configuration at g = 937 ± 91 cm−1 for ultrathin (T = 200 nm) spin-cast films doped with 5% of MDACl2. ASE did not degrade for over five hours of continuous measurements in the ambient environment. Ultrafast transient absorption (TA) measurements indicate that lasing originates from localized states concentrating towards the surface. [1]
Exploring light-emitting (LED) applications, we designed a novel solvent engineering method to incorporate highly luminescent fully inorganic 0D Cs4PbBr6 nanocrystals (PNCs) into a 3D CsPbBr3 film, forming the active emissive layer in single-layer perovskite light-emitting electrochemical cells. We observed a dramatic increase of the maximum external quantum efficiency (EQE) and luminance from 2.7% and 6050 cd/m2 for a 3D-only PeLEC to 8.3% and 11200 cd/m2 for a 3D-0D PNC device with only 7% by weight of 0D PNCs. The majority of this increase is driven by efficient inherent emission of 0D nanocrystals, while the concomitant morphology improvement also contributes to reduced leakage current, reduced hysteresis, and enhanced operational lifetime (half-life of 127 h), making this one of the best performing LECs reported so far. [2] These results pave the way for a rational incorporation of the extrinsic elements into perovskite materials to dramatically enhance their optical and lasing properties.
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