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Title: | Tailoring Interlayer Charge Transfer Dynamics in 2D Perovskites with Electroactive Spacer Molecules | Authors: | Boeije, Yorrick VAN GOMPEL, Wouter Zhang, Youcheng Ghosh, Pratyush Zelewski, Szymon J. Maufort, Arthur Roose, Bart Ooi, Zher Ying Chowdhury, Rituparno Devroey, Ilan Lenaers, Stijn Tew, Alasdair Dai, Linjie Dey, Krishanu Salway, Hayden Friend, Richard H. Sirringhaus, Henning Lutsen, Laurence Vanderzande, Dirk Rao, Akshay Stranks, Samuel D. |
Issue Date: | 2023 | Publisher: | AMER CHEMICAL SOC | Source: | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 145 (39) , p. 21330 -21343 | Abstract: | The family of hybrid organic-inorganic lead-halide perovskites are the subject of intense interest for optoelectronic applications, from light-emitting diodes to photovoltaics to X-ray detectors. Due to the inert nature of most organic molecules, the inorganic sublattice generally dominates the electronic structure and therefore the optoelectronic properties of perovskites. Here, we use optically and electronically active carbazole-based Cz-C-i molecules, where C-i indicates an alkylammonium chain and i indicates the number of CH2 units in the chain, varying from 3 to 5, as cations in the two-dimensional (2D) perovskite structure. By investigating the photophysics and charge transport characteristics of (Cz-C-i)(2)PbI4, we demonstrate a tunable electronic coupling between the inorganic lead-halide and organic layers. The strongest interlayer electronic coupling was found for (Cz-C-3)(2)PbI4, where photothermal deflection spectroscopy results remarkably reveal an organic-inorganic charge transfer state. Ultrafast transient absorption spectroscopy measurements demonstrate ultrafast hole transfer from the photoexcited lead-halide layer to the Cz-C-i molecules, the efficiency of which increases by varying the chain length from i = 5 to i = 3. The charge transfer results in long-lived carriers (10-100 ns) and quenched emission, in stark contrast to the fast (sub-ns) and efficient radiative decay of bound excitons in the more conventional 2D perovskite (PEA)(2)PbI4, in which phenylethylammonium (PEA) acts as an inert spacer. Electrical charge transport measurements further support enhanced interlayer coupling, showing increased out-of-plane carrier mobility from i = 5 to i = 3. This study paves the way for the rational design of 2D perovskites with combined inorganic-organic electronic properties through the wide range of functionalities available in the world of organics. | Notes: | Stranks, SD (corresponding author), Univ Cambridge, Dept Chem Engn & Biotechnol, Cambridge CB3 0AS, England.; Rao, AK; Stranks, SD (corresponding author), Univ Cambridge, Cavendish Lab, Dept Phys, Cambridge CB3 0HE, England. ar525@cam.ac.uk; sds65@cam.ac.uk |
Document URI: | http://hdl.handle.net/1942/41600 | ISSN: | 0002-7863 | e-ISSN: | 1520-5126 | DOI: | 10.1021/jacs.3c05974 | ISI #: | 001075431000001 | Rights: | 2023 The Authors. Published by American Chemical Society | Category: | A1 | Type: | Journal Contribution |
Appears in Collections: | Research publications |
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