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Artigo em Inglês | MEDLINE | ID: mdl-32045195


The two-step solution-based process has demonstrated substantial success in fabricating high-efficiency perovskite solar cells in recent years. Despite the high performance, the underlying mechanisms that govern the formation of perovskite films and corresponding device performance are yet to be fully understood. Particularly, organic cation composition used in the two-step solution processing of mixed-cation lead halide perovskite solar cells plays a critical role in the perovskite film formation and the resultant device performance. However, little is understood about the impacts of organic cation composition on the current density-voltage (J-V) hysteretic behavior and stability of perovskite solar cells. To address this need, here, we study the effect of mixed organic cations, that is, the fraction of formamidinium (FA) and methylammonium (MA) contents, used for the two-step solution-processed perovskite thin films on solar cell performance, including efficiency, J-V hysteresis, and stability. In addition to the efficiency variations, we find that perovskite solar cells based on FA-rich and MA-rich stoichiometries show distinct characteristics in J-V hysteresis and stability. The origins of such a discrepancy are attributed to the thermodynamically driven conversion from lead iodide to perovskites, which is determined by the combination of organic cations. The perovskite solar cells based on the mixed cation FA0.6MA0.4PbI3 composition show a champion power conversion efficiency of over 21% and robust stability (retaining more than 90% of initial efficiency) under maximum power-point tracking in dry nitrogen for more than 500 h. Our work provides insights on understanding the formation of perovskite films in the two-step process, which may benefit further investigation on perovskite solar cells.

J Chem Phys ; 152(6): 064705, 2020 Feb 14.
Artigo em Inglês | MEDLINE | ID: mdl-32061228


Narrow bandgap mixed tin (Sn) + lead (Pb) perovskites are necessary for the bottom sub-cell absorber in high efficiency all-perovskite polycrystalline tandem solar cells. We report on the impact of mixed cation composition and atmospheric exposure of perovskite films on sub-gap absorption in films and performance of solar cells based on narrow bandgap mixed formamidinium (FA) + methylammonium (MA) and Sn + Pb halide perovskites, (FASnI3)x(MAPbI3)1-x. Structural and optical properties of 0.3 ≤ x ≤ 0.8 (FASnI3)x(MAPbI3)1-x perovskite thin film absorbers with bandgaps ranging from 1.25 eV (x = 0.6) to 1.34 eV (x = 0.3) are probed with and without atmospheric exposure. Urbach energy, which quantifies the amount of sub-gap absorption, is tracked for pristine perovskite films as a function of composition, with x = 0.6 and 0.3 demonstrating the lowest and highest Urbach energies of 23 meV and 36 meV, respectively. Films with x = 0.5 and 0.6 compositions show less degradation upon atmospheric exposure than higher or lower Sn-content films having greater sub-gap absorption. The corresponding solar cells based on the x = 0.6 absorber show the highest device performance. Despite having a low Urbach energy, higher Sn-content solar cells show reduced device performances as the amount of degradation via oxidation is the most substantial.

Angew Chem Int Ed Engl ; 56(26): 7674-7678, 2017 06 19.
Artigo em Inglês | MEDLINE | ID: mdl-28524450


Methylammonium-mediated phase-evolution behavior of FA1-x MAx PbI3 mixed-organic-cation perovskite (MOCP) is studied. It is found that by simply enriching the MOCP precursor solutions with excess methylammonium cations, the MOCPs form via a dynamic composition-tuning process that is key to obtaining MOCP thin films with superior properties. This simple chemical approach addresses several key challenges, such as control over phase purity, uniformity, grain size, composition, etc., associated with the solution-growth of MOCP thin films with targeted compositions.