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Photoluminescence from Radiative Surface States and Excitons in Methylammonium Lead Bromide Perovskites.

ABSTRACT: In view of its band gap of 2.2 eV and its stability, methylammonium lead bromide (MAPbBr₃) is a possible candidate to serve as a light absorber in a subcell of a multijunction solar cell. Using complementary temperature-dependent time-resolved microwave conductance (TRMC) and photoluminescence (TRPL) measurements, we demonstrate that the exciton yield increases with lower temperature at the expense of the charge carrier generation yield. The low-energy emission at around 580 nm in the cubic phase and the second broad emission peak at 622 nm in the orthorhombic phase originate from radiative recombination of charges trapped in defects with mobile countercharges. We present a kinetic model describing both the decay in conductance as well as the slow ingrowth of the TRPL. Knowledge of defect states at the surface of various crystal phases is of interest to reach higher open-circuit voltages in MAPbBr₃-based cells.

SUBMITTER: Guo D

PROVIDER: S-EPMC5592651 | biostudies-literature | 2017 Sep

REPOSITORIES: biostudies-literature

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Photoluminescence from Radiative Surface States and Excitons in Methylammonium Lead Bromide Perovskites.

Guo Dengyang D Bartesaghi Davide D Wei Haotong H Hutter Eline M EM Huang Jinsong J Savenije Tom J TJ

The journal of physical chemistry letters 20170825 17

In view of its band gap of 2.2 eV and its stability, methylammonium lead bromide (MAPbBr<sub>3</sub>) is a possible candidate to serve as a light absorber in a subcell of a multijunction solar cell. Using complementary temperature-dependent time-resolved microwave conductance (TRMC) and photoluminescence (TRPL) measurements, we demonstrate that the exciton yield increases with lower temperature at the expense of the charge carrier generation yield. The low-energy emission at around 580 nm in the ...[more]

PMID: 28832152

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Project description:Highly photoluminescent hybrid lead halide perovskite nanoparticles have recently attracted wide interest in the context of high-stake applications, such as light emitting diodes (LEDs), light emitting transistors and lasers. In addition, they constitute ideal model systems to explore energy and charge transport phenomena occurring at the boundaries of nanocrystalline grains forming thin films in high-efficiency perovskite solar cells (PSCs). Here we report a complete photophysical study of CH3NH3PbBr3 perovskite nanoparticles suspended in chlorobenzene and highlight some important interaction properties. Colloidal suspensions under study were constituted of dispersed aggregates of quasi-2D platelets of a range of thicknesses, decorated with 3D-like spherical nanoparticles. These types of nanostructures possess different optical properties that afford a handle for probing them individually. The photophysics of the colloidal particles was studied by femtosecond pump-probe spectroscopy and time-correlated single-photon counting. We show here that a cascade of energy and exciton-mediated charge transfer occurs between nanostructures: upon photoexcitation, localized excitons within one nanostructure can either recombine on a ps timescale, yielding a short-lived emission, or form charge-transfer states (CTSs) across adjacent domains, resulting in longer-lived photoluminescence in the millisecond timescale. Furthermore, CTSs exhibit a clear signature in the form of a strong photoinduced electroabsorption evidenced in femtosecond transient absorption measurements. Charge transfer dynamics at the surface of the nanoparticles have been studied with various quenchers in solution. Efficient hole transfer to N,N,N',N'-tetrakis(4-methoxyphenyl)benzidine (MeO-TPD) and 1,4-bis(diphenyl-amino)benzene (BDB) donors was attested by the quenching of the nanoparticles emission. The charge transfer rate was limited by the organic layer used to stabilize the nanoparticles, which acted as a wide spacer between reactants. The forward charge transfer was found to take place in the sub-microsecond time-scale in competition with slow carrier recombination, while back transfer was shown to occur with a time-constant τ = 25 ms.

Dataset Information

Photoluminescence from Radiative Surface States and Excitons in Methylammonium Lead Bromide Perovskites.

Publications

Photoluminescence from Radiative Surface States and Excitons in Methylammonium Lead Bromide Perovskites.

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