The performance of three-dimensional (3D) organic-inorganic halide perovskite solar cells (PSCs) can be enhanced through surface treatment with 2D layered perovskites that have efficient charge transport. We maximized hole transport across the layers of a metastable Dion-Jacobson (DJ) 2D perovskite that tuned the orientational arrangements of asymmetric bulky organic molecules. The reduced energy barrier for hole transport increased out-of-plane transport rates by a factor of 4 to 5, and the power conversion efficiency (PCE) for the 2D PSC was 4.9%. With the metastable DJ 2D surface layer, the PCE of three common 3D PSCs was enhanced by approximately 12 to 16% and could reach approximately 24.7%. For a triple-cation–mixed-halide PSC, 90% of the initial PCE was retained after 1000 hours of 1-sun operation at ~40°C in nitrogen.
|Number of pages
|Published - Jan 7 2022
Bibliographical noteFunding Information:
The work was partially supported by the US Department of Energy under contract DE-AC36-08GO28308 with Alliance for Sustainable Energy, the manager and operator of the National Renewable Energy Laboratory. The authors acknowledge the support on 2D structure design, first-principle calculations, synthesis of PDAI2 and DMePDAI2, single-crystal synthesis and analysis, and optoelectronic characterizations (such as TRPL and TRMC) from the Center for Hybrid Organic-Inorganic Semiconductors for Energy (CHOISE), an Energy Frontier Research Center funded by the Office of Basic Energy Sciences, Office of Science within the US Department of Energy. The authors also acknowledge the support on device fabrication and characterization and general thin-film perovskite characterizations from the De-Risking Halide Perovskite Solar Cells program of the National Center for Photovoltaics, and the support on SnO2 ETL synthesis along with the corresponding device fabrication and characterization from DE-FOA-0002064 and award DEEE0008790, funded by the US Department of Energy, Office of Energy Efficiency and Renewable Energy, Solar Energy Technologies Office. Portions of this research were carried out at the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences under contract DE-AC02-76SF00515. L.D.H. and E.L.R. acknowledge funding support on UPS characterization and analysis from the Office of Naval Research under award N00014-20-1-2440. X.Z. and Y.-L.L. acknowledge support on SCLC characterization and analysis from the National Science Foundation, under grant CMMI-1824674, and funding from the Princeton Center for Complex Materials, a National Science Foundation (NSF)–MRSEC program (DMR-1420541). The DFT calculations were performed by using computational resources sponsored by the US Department of Energy’s Office of Energy Efficiency and Renewable Energy and located at the National Renewable Energy Laboratory and resources of the National Energy Research Scientific Computing Center (NERSC), a US Department of Energy Office of Science User Facility located at Lawrence Berkeley National Laboratory, operated under contract DE-AC02-05CH11231. The views expressed in the article do not necessarily represent the views of the US Department of Energy or the US government.
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