title: Organometal halide perovskite solar cell materials rationalized: ultrafast charge generation, high and microsecond-long balanced mobilities, and slow recombination.
abstract: Organometal halide perovskite-based solar cells have recently been reported to be highly efficient, giving an overall power conversion efficiency of up to 15%. However, much of the fundamental photophysical properties underlying this performance has remained unknown. Here, we apply photoluminescence, transient absorption, time-resolved terahertz and microwave conductivity measurements to determine the time scales of generation and recombination of charge carriers as well as their transport properties in solution-processed CH3NH3PbI3 perovskite materials. We found that electron-hole pairs are generated almost instantaneously after photoexcitation and dissociate in 2 ps forming highly mobile charges (25 cm(2) V(-1) s(-1)) in the neat perovskite and in perovskite/alumina blends; almost balanced electron and hole mobilities remain very high up to the microsecond time scale. When the perovskite is introduced into a TiO2 mesoporous structure, electron injection from perovskite to the metal oxide is efficient in less than a picosecond, but the lower intrinsic electron mobility of TiO2 leads to unbalanced charge transport. Microwave conductivity measurements showed that the decay of mobile charges is very slow in CH3NH3PbI3, lasting up to tens of microseconds. These results unravel the remarkable intrinsic properties of CH3NH3PbI3 perovskite material if used as light absorber and charge transport layer. Moreover, finding a metal oxide with higher electron mobility may further increase the performance of this class of solar cells.
authors.affiliation: Division of Chemical Physics, Lund University , Box 124, 221 00 Lund, Sweden.
authors.forename: Carlito S
authors.initials: CS
authors.lastname: Ponseca
authors.forename: Tom J
authors.initials: TJ
authors.lastname: Savenije
authors.forename: Mohamed
authors.initials: M
authors.lastname: Abdellah
authors.forename: Kaibo
authors.initials: K
authors.lastname: Zheng
authors.forename: Arkady
authors.initials: A
authors.lastname: Yartsev
authors.forename: Tobjörn
authors.initials: T
authors.lastname: Pascher
authors.forename: Tobias
authors.initials: T
authors.lastname: Harlang
authors.forename: Pavel
authors.initials: P
authors.lastname: Chabera
authors.forename: Tonu
authors.initials: T
authors.lastname: Pullerits
authors.forename: Andrey
authors.initials: A
authors.lastname: Stepanov
authors.forename: Jean-Pierre
authors.initials: JP
authors.lastname: Wolf
authors.forename: Villy
authors.initials: V
authors.lastname: Sundström
mesh_terms: D011211:Electric Power Supplies; D007454:Iodides / Q000737:chemistry*; D007854:Lead / Q000737:chemistry*; D008744:Methylamines / Q000737:chemistry*; D008872:Microwaves; D012993:Solar Energy; D013997:Time Factors
chemical_list: D007454:Iodides; D008744:Methylamines; D007854:Lead; C027451:methylamine