Hybrid perovskites have shown astonishing power conversion efficiencies owed to their remarkable absorber characteristics including long carrier lifetimes, and a relatively substantial defect tolerance for solution-processed polycrystalline films. However, nonradiative charge carrier recombination at grain boundaries limits open circuit voltages and consequent performance improvements of perovskite solar cells. Here we address such recombination pathways and demonstrate a passivation effect through guanidinium-based additives to achieve extraordinarily enhanced carrier lifetimes and higher obtainable open circuit voltages. Time-resolved photoluminescence measurements yield carrier lifetimes in guanidinium-based films an order of magnitude greater than pure-methylammonium counterparts, giving rise to higher device open circuit voltages and power conversion efficiencies exceeding 17%. A reduction in defect activation energy of over 30% calculated via admittance spectroscopy and confocal fluorescence intensity mapping indicates successful passivation of recombination/trap centers at grain boundaries. We speculate that guanidinium ions serve to suppress formation of iodide vacancies and passivate under-coordinated iodine species at grain boundaries and within the bulk through their hydrogen bonding capability. These results present a simple method for suppressing nonradiative carrier loss in hybrid perovskites to further improve performances toward highly efficient solar cells.
The combination of hybrid perovskite and Cu(In,Ga)Se (CIGS) has the potential for realizing high-efficiency thin-film tandem solar cells because of the complementary tunable bandgaps and excellent photovoltaic properties of these materials. In tandem solar device architectures, the interconnecting layer plays a critical role in determining the overall cell performance, requiring both an effective electrical connection and high optical transparency. We used nanoscale interface engineering of the CIGS surface and a heavily doped poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] (PTAA) hole transport layer between the subcells that preserves open-circuit voltage and enhances both the fill factor and short-circuit current. A monolithic perovskite/CIGS tandem solar cell achieved a 22.43% efficiency, and unencapsulated devices under ambient conditions maintained 88% of their initial efficiency after 500 hours of aging under continuous 1-sun illumination.
Inorganic metal halide perovskite nanocrystals (NCs) have been employed universally in light-emitting applications during the past two years. Here, blue-emission (≈470 nm) Cs-based perovskite NCs are derived by directly mixing synthesized bromide and chloride nanocrystals with a weight ratio of 2:1. High-brightness blue perovskite light-emitting diodes (PeLEDs) are obtained by controlling the grain size of the perovskite films. Moreover, a white PeLED is demonstrated for the first time by blending orange polymer materials with the blue perovskite nanocrystals as the active layer. Exciton transfer from the blue nanocrystals to the orange polymers via Förster or Dexter energy transfer is analyzed through time resolved photoluminescence. By tuning the ratio between the perovskite nanocrystals and polymers, pure white light is achieved with the a CIE coordinate at (0.33,0.34).
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