Journal
ACS ENERGY LETTERS
Volume 3, Issue 9, Pages 2159-2166Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.8b01226
Keywords
-
Categories
Funding
- University at Buffalo, SUNY [57333]
- U.S. National Science Foundation [CHE-1565704]
- U.S. Department of Energy through the LANL/LDRD Program
- Center for Nonlinear Studies
Ask authors/readers for more resources
In this work, we study the role of spin-orbit coupling (SOC) in nonradiative relaxation of hot electrons and holes in methylammonium lead perovskite, MAPbI(3). For this purpose, we have developed the nonadiabatic molecular dynamics method with two component spinor wave functions that are solutions of the relativistic Kohn-Sham (KS) equations. We find that SOC enhances contributions of Pb(p(x)) and Pb(p(y)) orbitals to the conduction and valence bands. As a result, the KS orbitals become more sensitive to nuclear motions, leading to the increased nonadiabatic couplings. Consequently, SOC greatly speeds up the electron and hole relaxation, making the computed relaxation time scales consistent with available experiments. We suggest that the fast hot carrier relaxation facilitated by the SOC allows rapid transition into the long-lived triplet state that extends charge-carrier lifetime and helps achieve high-efficiency perovskite solar cells.
Authors
I am an author on this paper
Click your name to claim this paper and add it to your profile.
Reviews
Recommended
No Data Available