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1.
Nat Commun ; 15(1): 1355, 2024 Feb 14.
Artículo en Inglés | MEDLINE | ID: mdl-38355596

RESUMEN

Interstitial iodides are the most critical type of defects in perovskite solar cells that limits efficiency and stability. They can be generated during solution, film, and device processing, further accelerating degradation. Herein, we find that introducing a small amount of a zinc salt- zinc trifluoromethane sulfonate (Zn(OOSCF3)2) in the perovskite solution can control the iodide defects in resultant perovskites ink and films. CF3SOO̶ vigorously suppresses molecular iodine formation in the perovskites by reducing it to iodide. At the same time, zinc cations can precipitate excess iodide by forming a Zn-Amine complex so that the iodide interstitials in the resultant perovskite films can be suppressed. The perovskite films using these additives show improved photoluminescence quantum efficiency and reduce deep trap density, despite zinc cations reducing the perovskite grain size and iodide interstitials. The zinc additives facilitate the formation of more uniform perovskite films on large-area substrates (78-108 cm2) in the blade-coating process. Fabricated minimodules show power conversion efficiencies of 19.60% and 19.21% with aperture areas of 84 and 108 cm2, respectively, as certified by National Renewable Energy Laboratory (NREL), the highest efficiency certified for minimodules of these sizes.

2.
Nature ; 616(7958): 712-718, 2023 04.
Artículo en Inglés | MEDLINE | ID: mdl-37020031

RESUMEN

Metal-halide perovskites (MHPs) have been successfully exploited for converting photons to charges or vice versa in applications of solar cells, light-emitting diodes and solar fuels1-3, for which all these applications involve strong light. Here we show that self-powered polycrystalline perovskite photodetectors can rival the commercial silicon photomultipliers (SiPMs) for photon counting. The photon-counting capability of perovskite photon-counting detectors (PCDs) is mainly determined by shallow traps, despite that deep traps also limit charge-collection efficiency. Two shallow traps with energy depth of 5.8 ± 0.8 millielectronvolts (meV) and 57.2 ± 0.1 meV are identified in polycrystalline methylammonium lead triiodide, which mainly stay at grain boundaries and the surface, respectively. We show that these shallow traps can be reduced by grain-size enhancement and surface passivation using diphenyl sulfide, respectively. It greatly suppresses dark count rate (DCR) from >20,000 counts per second per square millimetre (cps mm-2) to 2 cps mm-2 at room temperature, enabling much better response to weak light than SiPMs. The perovskite PCDs can collect γ-ray spectra with better energy resolution than SiPMs and maintain performance at high temperatures up to 85 °C. The zero-bias operation of perovskite detectors enables no drift of noise and detection property. This study opens a new application of photon counting for perovskites that uses their unique defect properties.

3.
Adv Mater ; 34(49): e2205769, 2022 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-36177689

RESUMEN

Tin-lead (Sn-Pb) narrow-bandgap (NBG) perovskites show great potential in both single-junction and all-perovskite tandem solar cells. Sn-Pb perovskite solar cells (PSCs) are still limited by low charge collection efficiency and poor stability. Here, a ternary Sn (II) alloy of SnOCl is reported as the hole-transport material (HTM) with a work function of 4.95 eV for Sn-Pb PSCs. The solution-processed SnOCl layer has a texture structure that not only reduces the optical loss of the devices, but also changes grain growth of Sn-Pb perovskites and boosts the carrier diffusion length to 3.63 µm. The formation of small perovskite grains at the HTM/perovskite interface is suppressed. These result in an almost constant internal quantum efficiency (IQE) of 96 ± 2% across the absorption spectrum of Sn-Pb perovskites. The SnOCl HTM significantly enhances the stability of Sn-Pb PSCs with 87% of its initial efficiency retained after 1-sun illumination for 1200 h, and keeps 85% efficiency under 85 °C thermal stress for 1500 h. The hybrid HTM further improves the stabilized efficiencies of single-junction Sn-Pb PSCs and all-perovskite tandem solar cells to 23.2% and 25.9%, respectively. This discovery opens an avenue to the multicomponent metal alloys as HTM in PSCs.

4.
Sci Adv ; 8(38): eabo5977, 2022 Sep 23.
Artículo en Inglés | MEDLINE | ID: mdl-36149953

RESUMEN

The formation of voids in perovskite films close to the buried interface has been reported during film deposition. These voids are thought to limits the efficiency and stability of perovskite solar cells (PSCs). Here, we studied the voids formed during operation in perovskite films that were optimized during the solution deposition process to avoid voids. New voids formed during operation are found to assemble along grain boundaries at the bottom interface, caused by the loss of residual solvent and conversion of amorphous phase to crystalline phase. Unexpectedly, the formation of these voids did not negatively affect the stability of PSCs. Decreasing the amorphous region in perovskites by thermal annealing decreased the positive iodide interstitial density, and improved the light stability of PSCs. The annealed devices maintained 90% of their initial efficiency and light soaking for 1900 hours at open circuit condition under 1-sun illumination at 50°C.

5.
Adv Mater ; 34(30): e2202954, 2022 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-35652351

RESUMEN

Perovskite solar cells (PSCs) are promising to reduce the cost of photovoltaic system due to their low-cost raw materials and high-throughput solution process; however, fabrication of all the active layers in perovskite modules using a scalable solution process has not yet been demonstrated. Herein, the fabrication of highly efficient PSCs and modules in ambient conditions is reported, with all layers bladed except the metal electrode, by blading a 36 ± 9 nm-thick electron-transport layer (ETL) on perovskite films with a roughness of ≈80 nm. A combination of additives in phenyl-C61 -butyric acid methyl ester (PCBM) allows the PCBM to conformally cover the perovskites and still have a good electrical conductivity. Amine-functionalized molecules are added to enhance both the dispersity of PCBM and the affinity to perovskites. A PCBM dopant of 4-(2,3-dihydro-1,3-dimethyl-1H-benzimidazol-2-yl)-N,N-dimethylbenzenamine (N-DMBI) recovers the conductivity loss induced by the small amine molecules. PSCs (0.08 cm2 ) fabricated by the all-blading process reache an average efficiency of 22.4 ± 0.5% and a champion efficiency of 23.1% for perovskites with a bandgap of 1.51 eV, with much better stability compared to evaporated ETL PSCs. The all-bladed minimodule (25.03 cm2 ) shows an aperture efficiency of ≈19.3%, showing the good uniformity of the bladed ETLs.

6.
Nanoscale ; 10(35): 16919-16927, 2018 Sep 13.
Artículo en Inglés | MEDLINE | ID: mdl-30178805

RESUMEN

Metal halide perovskite nanocrystals have recently emerged as promising materials for light emitting displays and lasing applications due to their narrow emission wavelengths, high photoluminescence quantum yields, and readily adjustable emission wavelengths. For these metal halide perovskite nanocrystals to be useful in commercial applications, their stability must be increased and the photoluminescence quantum yields of the iodide (red emitting) and chloride (blue emitting) containing derivatives must also be increased. The photoluminescence quantum yields of blue emitting CsPbCl3 nanoparticles lag behind those of green emitting CsPbBr3 nanoparticles, with maximum photoluminescence quantum yields of 1-10% previously reported for CsPbCl3 as compared to 80-100% for CsPbBr3. Herein, we show that alkyltrichlorosilanes (R-SiCl3) can be used as Cl-sources for rapid anion exchange with host CsPbBr3 nanocrystals. This anion exchange reaction is advantageous in that it can be performed at room temperature and results in highly dispersible nanoparticles coated with siloxane shells. CsPbCl3 nanoparticles produced through Cl-exchange with R-SiCl3 show significantly improved long-term stability and high photoluminescence quantum yields of up to 12%. These siloxane coated nanocrystals are even stable in the presence of water, whereas CsPbCl3 nanoparticles synthesized through other routes rapidly degrade in the presence of water.

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