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Lead-halide perovskites meet donor-acceptor charge-transfer complexes

(2019) CHEMISTRY OF MATERIALS. 31(17). p.6880-6888
Author
Organization
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 center dot(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.
Keywords
ORGANIC-INORGANIC PEROVSKITES, HYBRID PEROVSKITES, QUANTUM CONFINEMENT, OPTICAL-PROPERTIES, CARRIERS, DESIGN

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MLA
Marchal, Nadege, et al. “Lead-Halide Perovskites Meet Donor-Acceptor Charge-Transfer Complexes.” CHEMISTRY OF MATERIALS, vol. 31, no. 17, 2019, pp. 6880–88.
APA
Marchal, N., Van Gompel, W., Gelvez-Rueda, M. C., Vandewal, K., Van Hecke, K., Boyen, H.-G., … Beljonne, D. (2019). Lead-halide perovskites meet donor-acceptor charge-transfer complexes. CHEMISTRY OF MATERIALS, 31(17), 6880–6888.
Chicago author-date
Marchal, Nadege, Wouter Van Gompel, Maria C Gelvez-Rueda, Koen Vandewal, Kristof Van Hecke, Hans-Gerd Boyen, Bert Conings, et al. 2019. “Lead-Halide Perovskites Meet Donor-Acceptor Charge-Transfer Complexes.” CHEMISTRY OF MATERIALS 31 (17): 6880–88.
Chicago author-date (all authors)
Marchal, Nadege, Wouter Van Gompel, Maria C Gelvez-Rueda, Koen Vandewal, Kristof Van Hecke, Hans-Gerd Boyen, Bert Conings, Roald Herckens, Sudeep Maheshwar, Laurence Lutsen, Claudio Quarti, Ferdinand C Grozema, Dirk Vanderzande, and David Beljonne. 2019. “Lead-Halide Perovskites Meet Donor-Acceptor Charge-Transfer Complexes.” CHEMISTRY OF MATERIALS 31 (17): 6880–6888.
Vancouver
1.
Marchal N, Van Gompel W, Gelvez-Rueda MC, Vandewal K, Van Hecke K, Boyen H-G, et al. Lead-halide perovskites meet donor-acceptor charge-transfer complexes. CHEMISTRY OF MATERIALS. 2019;31(17):6880–8.
IEEE
[1]
N. Marchal et al., “Lead-halide perovskites meet donor-acceptor charge-transfer complexes,” CHEMISTRY OF MATERIALS, vol. 31, no. 17, pp. 6880–6888, 2019.
@article{8645673,
  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 center dot(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.},
  author       = {Marchal, Nadege and Van Gompel, Wouter and Gelvez-Rueda, Maria C and Vandewal, Koen and Van Hecke, Kristof and Boyen, Hans-Gerd and Conings, Bert and Herckens, Roald and Maheshwar, Sudeep and Lutsen, Laurence and Quarti, Claudio and Grozema, Ferdinand C and Vanderzande, Dirk and Beljonne, David},
  issn         = {0897-4756},
  journal      = {CHEMISTRY OF MATERIALS},
  keywords     = {ORGANIC-INORGANIC PEROVSKITES,HYBRID PEROVSKITES,QUANTUM CONFINEMENT,OPTICAL-PROPERTIES,CARRIERS,DESIGN},
  language     = {eng},
  number       = {17},
  pages        = {6880--6888},
  title        = {Lead-halide perovskites meet donor-acceptor charge-transfer complexes},
  url          = {http://dx.doi.org/10.1021/acs.chemmater.9b01289},
  volume       = {31},
  year         = {2019},
}

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