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1.
Angew Chem Int Ed Engl ; : e202405422, 2024 Jun 10.
Artigo em Inglês | MEDLINE | ID: mdl-38858169

RESUMO

Perovskite precursor inks suffer various forms of degradation, such as iodide anion oxidation and organic cation breakdown, hindering reliable perovskite solar cell manufacturing. Here we report that benzylhydrazine hydrochloride (BHC) not only retards the buildup of iodine as previously reported but also prevents the breakdown of organic cations. Through investigating BHC and iodine chemical reactions, we elucidate protonation and dehydration mechanisms, converting BHC to harmless volatile compounds, thus preserving perovskite film crystallization and solar cell performance. This inhibition effect lasts nearly a month with minimal BHC, contrasting control inks without BHC where organic cations fully react in less than a week. This enhanced understanding, from additive stabilization to end products, promises improved perovskite solar cell production reliability.

2.
Nano Lett ; 22(13): 5287-5293, 2022 Jul 13.
Artigo em Inglês | MEDLINE | ID: mdl-35767329

RESUMO

Perovskite quantum dots (PQDs) provide a robust solution-based approach to efficient solar cells, bright light emitting devices, and quantum sources of light. Quantifying heterogeneity and understanding coupling between dots is critical for these applications. We use double-nanohole optical trapping to size individual dots and correlate to emission energy shifts from quantum confinement. We were able to assemble a second dot in the trap, which allows us to observe the coupling between dots. We observe a systematic red-shift of 1.1 ± 0.6 meV in the emission wavelength. Theoretical analysis shows that the observed shift is consistent with resonant energy transfer and is unusually large due to moderate-to-large quantum confinement in PQDs. This demonstrates the promise of PQDs for entanglement in quantum information applications. This work enables future in situ control of PQD growth as well as studies of the coupling between small PQD assemblies with quantum information applications in mind.

3.
ACS Appl Mater Interfaces ; 14(34): 38963-38971, 2022 Aug 31.
Artigo em Inglês | MEDLINE | ID: mdl-35979625

RESUMO

Carbon-based all-inorganic CsPbIxBr3-x perovskite solar cells offer high stability against heat and humidity and a suitable band gap for tandem and semitransparent photovoltaics. In CsPbIxBr3-x perovskite films, the defects at grain boundaries (GBs) cause charge trapping, reducing the efficiency of the cell. Electronic deactivation of GB has been a conventional strategy to suppress the trapping, but at the cost of charge carrier transport through the boundaries. Here, we turn the GBs into benign charge transport pathways with the aid of bipolar charge transport semiconductors, namely, Ti3C2TX (MXene) and Spiro-OMeTAD, respectively. Thanks to the synergistic effects of both n- and p-type transport media, the charge transport is improved and balanced at the GBs. As a result, the cells achieve an efficiency of 12.7%, the highest among all low-temperature-processed carbon-based inorganic perovskite solar cells. Benign GBs also lead to enhanced light and aging stabilities. Our work demonstrates a proof-of-concept strategy of benign electronic modulation of GBs for solution-processed perovskite solar cells.

4.
Adv Mater ; 34(47): e2202390, 2022 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-36069995

RESUMO

Single-crystal halide perovskites exhibit photogenerated-carriers of high mobility and long lifetime, making them excellent candidates for applications demanding thick semiconductors, such as ionizing radiation detectors, nuclear batteries, and concentrated photovoltaics. However, charge collection depreciates with increasing thickness; therefore, tens to hundreds of volts of external bias is required to extract charges from a thick perovskite layer, leading to a considerable amount of dark current and fast degradation of perovskite absorbers. However, extending the carrier-diffusion length can mitigate many of the anticipated issues preventing the practical utilization of perovskites in the abovementioned applications. Here, single-crystal perovskite solar cells that are up to 400 times thicker than state-of-the-art perovskite polycrystalline films are fabricated, yet retain high charge-collection efficiency in the absence of an external bias. Cells with thicknesses of 110, 214, and 290 µm display power conversion efficiencies (PCEs) of 20.0, 18.4, and 14.7%, respectively. The remarkable persistence of high PCEs, despite the increase in thickness, is a result of a long electron-diffusion length in those cells, which was estimated, from the thickness-dependent short-circuit current, to be ≈0.45 mm under 1 sun illumination. These results pave the way for adapting perovskite devices to optoelectronic applications in which a thick active layer is essential.

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