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Please use this identifier to cite or link to this item: http://hdl.handle.net/1942/29210

Title: Lead-Halide Perovskites Meet Donor–Acceptor Charge-Transfer Complexes
Authors: Nadège, Marchal
Van Gompel, Wouter
Gélvez-Rueda, María
Vandewal, Koen
Van Hecke, Kristof
Boyen, Hans-Gerhard
Conings, Bert
Herckens, Roald
Maheshwari, Sudeep
Lutsen, Laurence
Quarti, Claudio
Grozema, Ferdinand
Vanderzande, Dirk
Beljonne, David
Issue Date: 2019
Citation: Chemistry of materials, 31 (17), p. 6880-6888
Abstract: Low-dimensional lead halide hybrid perovskites are nowadays in the spotlight because of their improved stability and extensive chemical flexibility compared to their 3D perovskite counterparts, the current challenge being to design functionalized organic cations. Here, we report on the synthesis and full characterization of a perovskite-like hybrid (a perovskitoid) where the 1D lead iodide layout is patterned with a donor−acceptor charge transfer complex (CTC) between pyrene and tetracyanoquinodimethane, with a chemical formula of (C20H17NH3)PbI3·(C12H4N4). By combining multiple structural analysis and spectroscopic techniques with ab initio modeling, we show that the electronic, optical, and charge-transport properties of the hybrid materials are dominated by the organic CTC, with the inorganic backbone primarily acting as a template for the organization of the donor and acceptor molecules. Interestingly, time-resolved microwave conductivity (TRMC) measurements show an enhanced photocurrent generation in the 1D hybrid compared to the pure organic charge-transfer salt, likely associated with transient localization of the holes on the lead-iodide octahedra. This observation is in line with the close energy resonance between the valence crystal orbitals of the lead-iodide lattice and the frontier occupied molecular orbitals of pyrene predicted by the DFT calculations. Therefore, it paves the way toward the design of new hybrid low-dimensionality perovskites offering a synergic combination of organic and inorganic functionalities.
Notes: Marchal, N (reprint author), Univ Mons, Lab Chem Novel Mat, Pl Parc 20, B-7000 Mons, Belgium. nadege.marchal@umons.ac.be
URI: http://hdl.handle.net/1942/29210
DOI: 10.1021/acs.chemmater.9b01289
ISI #: 000485830300057
ISSN: 0897-4756
Category: A1
Type: Journal Contribution
Appears in Collections: Research publications

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