In its initial phase in 2009, the inorganic‐organic hybrid perovskite solar cells (PSCs) delivered a 3.8% power conversion efficiency (PCE), which is far below the present 25.7% PCE obtained in 2022. The significant improvement of the efficiency of PSCs in such a short period has stimulated significant interest in the photovoltaic community. However, the performance of current PSCs is behind the commercially available and widely used solar cells in terms of stability and scalability. Among various commonly studied perovskite materials, methylammonium lead iodide (MAPbI3) is the most widely studied. This review will focus on the common solar cell structures (mesoporous, inverted planar p‐i‐n, planar n‐i‐p) using MAPbI3perovskite as an active layer and the effect of these solar cell structures on their performances. Furthermore, some commonly‐used strategies are outlined for improving the device performance, such as optimizing the deposition technique of the charge transporting and the active layers, modifying the properties of the carrier transporting layer and the perovskite layer by interface engineering and doping, optimizing the perovskite surface morphology, along with others. This article will also discuss the hole transport free and electron transport free MAPbI3PSCs.
- NSF-PAR ID:
- 10142694
- Date Published:
- Journal Name:
- Chemical Society Reviews
- Volume:
- 48
- Issue:
- 18
- ISSN:
- 0306-0012
- Page Range / eLocation ID:
- 4854 to 4891
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract -
Photoinduced nonequilibrium processes in nanoscale materials play key roles in photovoltaic and photocatalytic applications. This review summarizes recent theoretical investigations of excited state dynamics in metal halide perovskites (MHPs), carried out using a state-of-the-art methodology combining nonadiabatic molecular dynamics with real-time time-dependent density functional theory. The simulations allow one to study evolution of charge carriers at the ab initio level and in the time-domain, in direct connection with time-resolved spectroscopy experiments. Eliminating the need for the common approximations, such as harmonic phonons, a choice of the reaction coordinate, weak electron–phonon coupling, a particular kinetic mechanism, and perturbative calculation of rate constants, we model full-dimensional quantum dynamics of electrons coupled to semiclassical vibrations. We study realistic aspects of material composition and structure and their influence on various nonequilibrium processes, including nonradiative trapping and relaxation of charge carriers, hot carrier cooling and luminescence, Auger-type charge–charge scattering, multiple excitons generation and recombination, charge and energy transfer between donor and acceptor materials, and charge recombination inside individual materials and across donor/acceptor interfaces. These phenomena are illustrated with representative materials and interfaces. Focus is placed on response to external perturbations, formation of point defects and their passivation, mixed stoichiometries, dopants, grain boundaries, and interfaces of MHPs with charge transport layers, and quantum confinement. In addition to bulk materials, perovskite quantum dots and 2D perovskites with different layer and spacer cation structures, edge passivation, and dielectric screening are discussed. The atomistic insights into excited state dynamics under realistic conditions provide the fundamental understanding needed for design of advanced solar energy and optoelectronic devices.more » « less
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1039/c9cs00254e
