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1.
Nano Lett ; 23(6): 2074-2080, 2023 Mar 22.
Artigo em Inglês | MEDLINE | ID: mdl-36862532

RESUMO

Terahertz (THz) radiation is a valuable tool to investigate the electronic properties of lead halide perovskites (LHPs). However, attaining high-resolution information remains elusive, as the diffraction-limited spatial resolution (∼300 µm) of conventional THz methods prevents a direct analysis of microscopic effects. Here, we employ THz scattering scanning near-field optical microscopy (THz-sSNOM) for nanoscale imaging of cesium lead bromide (CsPbBr3) thin films down to the single grain level at 600 GHz. Adopting a scattering model, we are able to derive the local THz nanoscale conductivity in a contact-free fashion. Increased THz near-field signals at CsPbBr3 grain boundaries complemented by correlative transmission electron microscopy-energy-dispersive X-ray spectroscopy elemental analysis point to the formation of halide vacancies (VBr) and Pb-Pb bonds, which induce charge carrier trapping and can lead to nonradiative recombination. Our study establishes THz-sSNOM as a powerful THz nanoscale analysis platform for thin-film semiconductors such as LHPs.

2.
ACS Appl Mater Interfaces ; 11(43): 40172-40179, 2019 Oct 30.
Artigo em Inglês | MEDLINE | ID: mdl-31581769

RESUMO

Lead halide perovskite solar cells afford high power conversion efficiencies, even though the photoactive layer is formed in a solution process. At the same time, solution processing may impose some severe dewetting issues, especially if organic, hydrophobic charge transport layers are considered. Ultimately, very narrow processing windows with a relatively large spread in device performance and a considerable lab-to-lab variation result. Here, we unambiguously identify dimethylsulfoxide (DMSO), which is commonly used as a co-solvent and complexing agent, to be the main reason for dewetting of the precursor solution on hydrophobic hole transport layers, such as polytriarylamine, in a gas-quenching-assisted deposition process. In striking contrast, we will show that N-methyl-2-pyrrolidon (NMP), which has a lower hydrophilic-lipophilic-balance, can be favorably used instead of DMSO to strongly mitigate these dewetting issues. The resulting high-quality perovskite layers are extremely tolerant with respect to the mixing ratio (NMP/dimethylformamide) and other process parameters. Thus, our findings afford an outstandingly robust, easy to use, and fail-safe deposition technique, yielding single (MAPbI3) and double (FA0.94Cs0.06PbI3) cation perovskite solar cells with high efficiencies (∼18.5%). Most notably, the statistical variation of the devices is significantly reduced, even if the deposition process is performed by different persons. We foresee that our results will further the reliable preparation of perovskite thin films and mitigate process-to-process variations that still hinder the prospects of upscaling perovskite solar technology.

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