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Benzodithiophene-Based Spacers for Layered and Quasi-Layered Lead Halide Perovskite Solar Cells.

ABSTRACT: Incorporating extended pi-conjugated organic cations in layered lead halide perovskites is a recent trend promising to merge the fields of organic semiconductors and lead halide perovskites. Herein, we integrate benzodithiophene (BDT) into Ruddlesden-Popper (RP) layered and quasi-layered lead iodide thin films (with methylammonium, MA) of the form (BDT)₂ MA_n-1 Pb_n I_3n+1 . The importance of tuning the ligand chemical structure is shown as an alkyl chain length of at least six carbon atoms is required to form a photoactive RP (n=1) phase. With N=20 or 100, as prepared in the precursor solution following the formula (BDT)₂ MA_N-1 Pb_N I_3N+1 , the performance and stability of devices surpassed those with phenylethylammonium (PEA). For N=100, the BDT cation gave a power conversion efficiency of up to 14.7 % vs. 13.7 % with PEA. Transient photocurrent, UV photoelectron spectroscopy, and Fourier transform infrared spectroscopy point to improved charge transport in the device active layer and additional electronic states close to the valence band, suggesting the formation of a Lewis adduct between the BDT and surface iodide vacancies.

SUBMITTER: Primera Darwich B

PROVIDER: S-EPMC8361775 | biostudies-literature | 2021 Jul

REPOSITORIES: biostudies-literature

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Benzodithiophene-Based Spacers for Layered and Quasi-Layered Lead Halide Perovskite Solar Cells.

Primera Darwich Barbara B Guijarro Nestor N Cho Han-Hee HH Yao Liang L Monnier Luc L Schouwink Pascal P Mensi Mounir M Yum Jun-Ho JH Sivula Kevin K

ChemSusChem 20210621 14

Incorporating extended pi-conjugated organic cations in layered lead halide perovskites is a recent trend promising to merge the fields of organic semiconductors and lead halide perovskites. Herein, we integrate benzodithiophene (BDT) into Ruddlesden-Popper (RP) layered and quasi-layered lead iodide thin films (with methylammonium, MA) of the form (BDT)2 MAn-1 Pbn I3n+1 . The importance of tuning the ligand chemical structure is shown as an alkyl chain ...[more]

PMID: 34075712

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Project description:Organic-inorganic semiconductors, which adopt the perovskite crystal structure, have perturbed the landscape of contemporary photovoltaics research. High-efficiency solar cells can be produced with solution-processed active layers. The materials are earth abundant, and the simple processing required suggests that high-throughput and low-cost manufacture at scale should be possible. While these materials bear considerable similarity to traditional inorganic semiconductors, there are notable differences in their optoelectronic behavior. A key distinction of these materials is that they are physically soft, leading to considerable thermally activated motion. In this Account, we discuss the internal motion of methylammonium lead iodide (CH3NH3PbI3) and formamidinium lead iodide ([CH(NH2)2]PbI3), covering: (i) molecular rotation-libration in the cuboctahedral cavity; (ii) drift and diffusion of large electron and hole polarons; (iii) transport of charged ionic defects. These processes give rise to a range of properties that are unconventional for photovoltaic materials, including frequency-dependent permittivity, low electron-hole recombination rates, and current-voltage hysteresis. Multiscale simulations, drawing from electronic structure, ab initio molecular dynamic and Monte Carlo computational techniques, have been combined with neutron diffraction measurements, quasi-elastic neutron scattering, and ultrafast vibrational spectroscopy to qualify the nature and time scales of the motions. Electron and hole motion occurs on a femtosecond time scale. Molecular libration is a sub-picosecond process. Molecular rotations occur with a time constant of several picoseconds depending on the cation. Recent experimental evidence and theoretical models for simultaneous electron and ion transport in these materials has been presented, suggesting they are mixed-mode conductors with similarities to fast-ion conducting metal oxide perovskites developed for battery and fuel cell applications. We expound on the implications of these effects for the photovoltaic action. The temporal behavior displayed by hybrid perovskites introduces a sensitivity in materials characterization to the time and length scale of the measurement, as well as the history of each sample. It also poses significant challenges for accurate materials modeling and device simulations. There are large differences between the average and local crystal structures, and the nature of charge transport is too complex to be described by common one-dimensional drift-diffusion models. Herein, we critically discuss the atomistic origin of the dynamic processes and the associated chemical disorder intrinsic to crystalline hybrid perovskite semiconductors.

Dataset Information

Benzodithiophene-Based Spacers for Layered and Quasi-Layered Lead Halide Perovskite Solar Cells.

Publications

Benzodithiophene-Based Spacers for Layered and Quasi-Layered Lead Halide Perovskite Solar Cells.

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