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Sirtl, Maximilian T. ORCID logoORCID: https://orcid.org/0000-0002-2860-4223; Hooijer, Rik ORCID logoORCID: https://orcid.org/0000-0002-0038-2649; Armer, Melina ORCID logoORCID: https://orcid.org/0000-0002-1716-4648; Ebadi, Firouzeh G. ORCID logoORCID: https://orcid.org/0000-0002-7374-4479; Mohammadi, Mahdi; Maheu, Clément ORCID logoORCID: https://orcid.org/0000-0001-5417-5672; Weis, Andreas ORCID logoORCID: https://orcid.org/0000-0003-0128-4116; van Gorkom, Bas T.; Häringer, Sebastian ORCID logoORCID: https://orcid.org/0000-0001-6379-5371; Janssen, René A. J. ORCID logoORCID: https://orcid.org/0000-0002-1920-5124; Mayer, Thomas; Dyakonov, Vladimir ORCID logoORCID: https://orcid.org/0000-0001-8725-9573; Tress, Wolfgang ORCID logoORCID: https://orcid.org/0000-0002-4010-239X und Bein, Thomas ORCID logoORCID: https://orcid.org/0000-0001-7248-5906 (2022): 2D/3D Hybrid Cs2AgBiBr6 Double Perovskite Solar Cells: Improved Energy Level Alignment for Higher Contact‐Selectivity and Large Open Circuit Voltage. In: Advanced Energy Materials, Bd. 12, Nr. 7 [PDF, 2MB]

Abstract

Since their introduction in 2017, the efficiency of lead-free halide perovskite solar cells based on Cs2AgBiBr6 has not exceeded 3%. The limiting bottlenecks are attributed to a low electron diffusion length, self-trapping events and poor selectivity of the contacts, leading to large non-radiative VOC losses. Here, 2D/3D hybrid double perovskites are introduced for the first time, using phenethyl ammonium as the constituting cation. The resulting solar cells show an increased efficiency of up to 2.5% for the champion cells and 2.03% on average, marking an improvement by 10% compared to the 3D reference on mesoporous TiO2. The effect is mainly due to a VOC improvement by up to 70 mV on average, yielding a maximum VOC of 1.18 V using different concentrations of phenethylammonium bromide. While these are among the highest reported VOC values for Cs2AgBiBr6 solar cells, the effect is attributed to a change in recombination behavior within the full device and a better selectivity at the interface toward the hole transporting material (HTM). This explanation is supported by voltage-dependent external quantum efficiency, as well as photoelectron spectroscopy, revealing a better energy level alignment and thus a better hole-extraction and improved electron blocking at the HTM interface.

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