title: Electron-Rotor Interaction in Organic-Inorganic Lead Iodide Perovskites Discovered by Isotope Effects.
abstract: We report on the carrier-rotor coupling effect in perovskite organic-inorganic hybrid lead iodide (CH3NH3PbI3) compounds discovered by isotope effects. Deuterated organic-inorganic perovskite compounds including CH3ND3PbI3, CD3NH3PbI3, and CD3ND3PbI3 were synthesized. Devices made from regular CH3NH3PbI3 and deuterated CH3ND3PbI3 exhibit comparable performance in band gap, current-voltage, carrier mobility, and power conversion efficiency. However, a time-resolved photoluminescence (TRPL) study reveals that CH3NH3PbI3 exhibits notably longer carrier lifetime than that of CH3ND3PbI3, in both thin-film and single-crystal formats. Furthermore, the comparison in carrier lifetime between CD3NH3PbI3 and CH3ND3PbI3 single crystals suggests that vibrational modes in methylammonium (MA(+)) have little impact on carrier lifetime. In contrast, the fully deuterated compound CD3ND3PbI3 reconfirmed the trend of decreasing carrier lifetime upon the increasing moment of inertia of cationic MA(+). Polaron model elucidates the electron-rotor interaction.
authors.affiliation: Department of Chemistry and Biochemistry, Northern Illinois University , DeKalb, Illinois 60115, United States.
authors.forename: Jue
authors.initials: J
authors.lastname: Gong
authors.affiliation: Chemistry and Nanoscience Center, National Renewable Energy Laboratory , Golden, Colorado 80401, United States.
authors.forename: Mengjin
authors.initials: M
authors.lastname: Yang
authors.affiliation: School of Physics, State Key Laboratory of Crystal Materials, Shandong University , Jinan 250100, China.
authors.forename: Xiangchao
authors.initials: X
authors.lastname: Ma
authors.affiliation: Center for Nanoscale Materials, Argonne National Laboratory , Argonne, Illinois 60439, United States.
authors.forename: Richard D
authors.initials: RD
authors.lastname: Schaller
authors.affiliation: Center for High Pressure Science and Technology Advanced Research , Shanghai 201203, China.
authors.forename: Gang
authors.initials: G
authors.lastname: Liu
authors.affiliation: Center for High Pressure Science and Technology Advanced Research , Shanghai 201203, China.
authors.forename: Lingping
authors.initials: L
authors.lastname: Kong
authors.affiliation: Chemistry and Nanoscience Center, National Renewable Energy Laboratory , Golden, Colorado 80401, United States.
authors.forename: Ye
authors.initials: Y
authors.lastname: Yang
authors.affiliation: Chemistry and Nanoscience Center, National Renewable Energy Laboratory , Golden, Colorado 80401, United States.
authors.forename: Matthew C
authors.initials: MC
authors.lastname: Beard
authors.affiliation: Department of Chemistry and Biochemistry, Northern Illinois University , DeKalb, Illinois 60115, United States.
authors.forename: Michael
authors.initials: M
authors.lastname: Lesslie
authors.affiliation: School of Physics, State Key Laboratory of Crystal Materials, Shandong University , Jinan 250100, China.
authors.forename: Ying
authors.initials: Y
authors.lastname: Dai
authors.affiliation: School of Physics, State Key Laboratory of Crystal Materials, Shandong University , Jinan 250100, China.
authors.forename: Baibiao
authors.initials: B
authors.lastname: Huang
authors.affiliation: Chemistry and Nanoscience Center, National Renewable Energy Laboratory , Golden, Colorado 80401, United States.
authors.forename: Kai
authors.initials: K
authors.lastname: Zhu
authors.affiliation: Department of Chemistry and Biochemistry, Northern Illinois University , DeKalb, Illinois 60115, United States.
authors.forename: Tao
authors.initials: T
authors.lastname: Xu