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Lars Sonneveld

Publications and source records attributed to Lars Sonneveld.

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Near-field effects on cathodoluminescence outcoupling in perovskite thin films

Halide perovskite semiconductors are a promising material for high-efficiency solar cells. Their optical properties can vary within and between crystallographic grains. We present spatially-resolved cathodoluminescence (CL) spectroscopy at 2 keV and 5 keV on polycrystalline CsPbBr3 perovskite films to study these variations at the nanoscale. The CL maps show a strongly reduced intensity near the polycrystalline grain boundaries. We perform numerical simulations of the far-field emission of the electron beam-generated optical near fields using the surface profiles from AFM as input. We find that near grain boundaries the light outcoupling is strongly reduced due to enhanced internal reflection and light trapping at the curved surfaces. Lateral variations in CL intensity inside grains are due to Fabry-Perot-like resonances in the film, with the substrate acting as a back reflector. Our results show that near-field coupling and interference effects can dominate nanoscale luminescence maps of halide perovskite films. The results are broadly relevant for the analysis of cathodoluminescence and photoluminescence of corrugated thin films.

cond-mat.mtrl-sci

Facile Synthesis and On-Chip Color Tuning of CsPbBr$_{3}$@CsPbBr$_{3-x}$TFA$_{x}$ Nanoplatelets via Ion Engineering

Metal halide perovskites (MHPs) have emerged as attractive optoelectronic materials because of high fluorescence quantum yield, broad color tunability, and excellent color purity. However, the ionic nature of MHPs makes them susceptible to polar solvents, leading to defect-induced nonradiative recombination and photoluminescence (PL) quenching. Here, we present a combined in-synthesis ($\textit{in situ}$) and post-synthesis ion engineering to suppress nonradiative recombination and integrate multicolor MHP arrays on-chip through a perovskite-compatible photolithography process and $\textit{in situ}$ vapor-phase anion exchange. CsPbBr$_{3}$@CsPbBr$_{3-x}$TFA$_{x}$ nanoplatelets were grown on-chip via a single-step solution process incorporating trifluoroacetate (TFA$^{-}$) pseudohalides. X-ray photoelectron spectroscopy revealed that TFA$^{-}$ passivate uncoordinated Pb$^{2+}$ ions on nanoplatelet surface and suppresses the formation of metallic lead (Pb$^{0}$). This decreases the non-radiative recombination centers and yields a PL peak at 520 nm with a linewidth of 14.56$\% \pm$ 0.5 nm. The nanoplatelets were patterned via a top-down photolithography process and selectively masked with a PMMA/Al$_{2}$O$_{3}$ stack to enable vapor-phase anion exchange. The PL peak shifted in the unmasked regions from 520 nm to 413 nm, resulting in distinct green and blue emission arrays. Our method enables the scalable fabrication of highly luminescent, two-color MHP arrays with tailored optical properties, advancing their integration into next-generation optoelectronic devices.

cond-mat.mtrl-sci