Lead-Halide Perovskites Meet Donor-Acceptor Charge-Transfer Complexes

Nadège Marchal*, Wouter Van Gompel, María C. Gélvez-Rueda, Koen Vandewal, Kristof Van Hecke, Hans Gerd Boyen, Bert Conings, Roald Herckens, Sudeep Maheshwari, Ferdinand C. Grozema

*Corresponding author for this work

Research output: Contribution to journalArticleScientificpeer-review

29 Citations (Scopus)
14 Downloads (Pure)

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.

Original languageEnglish
Pages (from-to)6880-6888
Number of pages9
JournalChemistry of Materials
Volume31
Issue number17
DOIs
Publication statusPublished - 2019

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