Han Yulun, Kilin Dmitri S
Department of Chemistry and Biochemistry, North Dakota State University, Fargo, North Dakota 58102, United States.
J Phys Chem Lett. 2020 Dec 3;11(23):9983-9989. doi: 10.1021/acs.jpclett.0c02973. Epub 2020 Nov 12.
Lead halide perovskites have attracted much attention as an active material in solar cells. In this first-principles study, we consider a cesium lead halide perovskite slab interfacing with electron transport and hole transport layers, relevant to the practical photovoltaic architecture. We apply external electric fields normal to the surface of the perovskite slab and explore the induced changes onto optoelectronic properties. It is found that the bandgap increases linearly and the conductivity diminishes exponentially with decreasing electric field strengths. Furthermore, we study the influence of electric fields onto nonradiative relaxation of photoexcited electrons and holes using the reduced density matrix in the formalism of Redfield theory. Our calculations provide relaxation rates and relaxation pathways, illustrating the mechanisms of modulations of electric field strengths onto charge carrier dynamics. Our results show that holes have longer lifetimes than electrons at various external electric fields. It is also found that the patterns of charge carrier dynamics depend on the direction of external electric fields. Specifically, in comparison with the system under zero field, our findings show that (i) the positive electric field facilitates the relaxation of electrons and holes and (ii) the negative electric field facilitates the relaxation of electrons but inhibits the relaxation of holes.
