Photoinduced Single- and Multiple-Electron Dynamics Processes Enhanced by Quantum Confinement in Lead Halide Perovskite Quantum Dots.
Methylammonium lead iodide perovskite (MAPbI3) is a promising material for photovoltaic devices. A modification of MAPbI3into confined nanostructures is expected to further increase efficiency of solar energy conversion. Photoexcited dynamic processes in a MAPbI3quantum dot (QD) have been modeled by many-body perturbation theory and nonadiabatic dynamics. A photoexcitation is followed by either exciton cooling (EC), its radiative (RR) or nonradiative recombination (NRR), or multiexciton generation (MEG) processes. Computed times of these processes fall in the order of MEG < EC < RR < NRR, where MEG is on the order of a few femtoseconds, EC is in the picosecond range, while RR and NRR are on the order of nanoseconds. Computed time scales indicate which electronic transition pathways can contribute to increase in charge collection efficiency. Simulated mechanisms of relaxation and their rates show that quantum confinement promotes MEG in MAPbI3QDs.
Department of Chemistry, University of South Dakota , Vermillion, South Dakota 57069, United States.
Dayton J
DJ
Vogel
Department of Physics, North Dakota State University , Fargo, North Dakota 58102, United States.
Andrei
A
Kryjevski
L.N. Gumilyov Eurasian National University , Astana 010008, Kazakhstan.|National University of Science and Technology "MISIS" , Moscow, 119049 Russian Federation.
Talgat
T
Inerbaev
Department of Chemistry, University of South Dakota , Vermillion, South Dakota 57069, United States.|Department of Chemistry and Biochemistry, North Dakota State University , Fargo, North Dakota 58102, United States.
Dmitri S
http://orcid.org/0000-0001-7847-5549
DS
Kilin