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1.
Angew Chem Int Ed Engl ; : e202412485, 2024 Aug 14.
Artículo en Inglés | MEDLINE | ID: mdl-39140456

RESUMEN

Organic-inorganic halide perovskite (OIHP) single crystals are promising for optoelectronic application, but their high surface trap density and associated ion migration hinders device performance and stability. Herein, a one-dimensional (1D) perovskites are designed and proposed as blocking layer at the crystal/electrode interface to mitigate the surface issues. As a model system, the interface ion migration in Cs0.05FA0.95PbI3 (FA=formamidinium) single-crystal perovskite solar cells (PSCs) is obviously suppressed, leading to increase of T90 lifetime from 260 to 1000 hours, five times better than previously reported results. Besides, the reduction of surface iodide ion vacancies inhibits nonradiative recombination, thus increasing the efficiency from 22.1% to 23.8%, which is one of the highest values for single-crystal PSCs. Since the deficient crystal surface is a universal and open issue, our strategy is instructive for optimizing diverse single-crystal perovskite devices.

2.
Angew Chem Int Ed Engl ; 63(9): e202314089, 2024 Feb 26.
Artículo en Inglés | MEDLINE | ID: mdl-38169141

RESUMEN

Metal halide perovskite single crystals are promising for diverse optoelectronic applications. As a universal issue of solution-grown perovskite single crystals, surface contamination causes adverse effect on material properties and device performance. Herein, learning from the self-cleaning effect of lotus leaf, we address the surface contamination issue by introducing an amphiphilic long-chain organic amine into the perovskite crystal growth solution. Self-assembly of CTAC provides a hydrophobic crystal surface, inducing spontaneous removal of residual growth solution, which results in clean surface and better optoelectronic properties of perovskite single crystals. An impressive efficiency of 23.4 % is obtained, setting a new record for FAx MA1-x PbI3 single-crystal perovskite solar cells (PSCs). Moreover, our strategy also applies to perovskite single crystals with different morphology and composition, which may contribute to improvement of other single-crystal perovskite optoelectronic devices.

3.
Angew Chem Int Ed Engl ; 62(19): e202302435, 2023 May 02.
Artículo en Inglés | MEDLINE | ID: mdl-36892282

RESUMEN

Perovskite single crystals and polycrystalline films have complementary merits and deficiencies in X-ray detection and imaging. Herein, we report preparation of dense and smooth perovskite microcrystalline films with both merits of single crystals and polycrystalline films through polycrystal-induced growth and hot-pressing treatment (HPT). Utilizing polycrystalline films as seeds, multi-inch-sized microcrystalline films can be in situ grown on diverse substrates with maximum grain size reaching 100 µm, which endows the microcrystalline films with comparable carrier mobility-lifetime (µτ) product as single crystals. As a result, self-powered X-ray detectors with impressive sensitivity of 6.1×104  µC Gyair -1 cm-2 and low detection limit of 1.5 nGyair s-1 are achieved, leading to high-contrast X-ray imaging at an ultra-low dose rate of 67 nGyair s-1 . Combining with the fast response speed (186 µs), this work may contribute to the development of perovskite-based low-dose X-ray imaging.

4.
Angew Chem Int Ed Engl ; 60(46): 24450-24455, 2021 Nov 08.
Artículo en Inglés | MEDLINE | ID: mdl-34453771

RESUMEN

We report the growth of a halide-based double perovskite, Cs2 Nax Ag1-x InCl6 :y%Mn, via a facile hydrothermal reaction at 180 °C. Through a co-doping strategy of both Na+ and Mn2+ , the as-prepared crystals exhibited a red afterglow featuring a high color purity (ca. 100 %) and a long duration time (>5400 s), three orders of magnitude longer than those solution-processed organic afterglow crystals. The energy transfer (ET) process between self-trapped excitons (STE) and activators was investigated through time-resolved spectroscopy, which suggested an ET efficiency up to 41 %. Importantly, the nominal concentration of dopants, especially in the case of Na+ , was found a useful tool to control both energy level and number distribution of traps. Cryogenic afterglow measurements suggested that the afterglow phenomenon was likely governed by thermal-activated exciton diffusion and electron tunneling process.

5.
ACS Appl Mater Interfaces ; 13(5): 6404-6410, 2021 Feb 10.
Artículo en Inglés | MEDLINE | ID: mdl-33499596

RESUMEN

Despite their low toxicity and phase stability, lead-free double perovskite nanocrystals, Cs2AgInCl6 in specific, have suffered from low quantum yield of photoluminescence. This is mainly due to two reasons, including (i) the quenching effect from metal silver which was usually formed at high temperature from Ag+ reduction in the presence of organic amines and (ii) the parity-forbidden transition of pristine double perovskites. Here, we reported a room-temperature synthesis of Cs2AgInCl6 nanocrystals in an inverse microemulsion system, where Ag+ reduction was largely suppressed. By codoping Bi and Na ions, dark self-trapping excitons (STEs) were converted into bright ones, enabling a bright phosphor of photoluminescence quantum yield up to 56%. Importantly, the doping approach at room temperature relaxed the parity-forbidden transition (1S0 → 3P2) of Bi-6s2 orbitals, revealing a fine structure of a triband excitation profile. Such spin-rule relaxation was ascribed to symmetry breaking of the doped lattice, which was evidenced by Raman spectroscopy. In a proof-of-concept experiment, the bright nanocrystals were used as a color-converting ink, which enabled a stable white light light-emitting diode to operate in various environments, even under water, for long-term service.

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