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Hot-carrier cooling and photoinduced refractive index changes in organic-inorganic lead halide perovskites.


ABSTRACT: Metal-halide perovskites are at the frontier of optoelectronic research due to solution processability and excellent semiconductor properties. Here we use transient absorption spectroscopy to study hot-carrier distributions in CH3NH3PbI3 and quantify key semiconductor parameters. Above bandgap, non-resonant excitation creates quasi-thermalized carrier distributions within 100 fs. During carrier cooling, a sub-bandgap transient absorption signal arises at ? 1.6 eV, which is explained by the interplay of bandgap renormalization and hot-carrier distributions. At higher excitation densities, a 'phonon bottleneck' substantially slows carrier cooling. This effect indicates a low contribution from inelastic carrier-impurity or phonon-impurity scattering in these polycrystalline materials, which supports high charge-carrier mobilities. Photoinduced reflectivity changes distort the shape of transient absorption spectra and must be included to extract physical constants. Using a simple band-filling model that accounts for these changes, we determine a small effective mass of mr=0.14 mo, which agrees with band structure calculations and high photovoltaic performance.

SUBMITTER: Price MB 

PROVIDER: S-EPMC4598728 | biostudies-literature | 2015 Sep

REPOSITORIES: biostudies-literature

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Hot-carrier cooling and photoinduced refractive index changes in organic-inorganic lead halide perovskites.

Price Michael B MB   Butkus Justinas J   Jellicoe Tom C TC   Sadhanala Aditya A   Briane Anouk A   Halpert Jonathan E JE   Broch Katharina K   Hodgkiss Justin M JM   Friend Richard H RH   Deschler Felix F  

Nature communications 20150925


Metal-halide perovskites are at the frontier of optoelectronic research due to solution processability and excellent semiconductor properties. Here we use transient absorption spectroscopy to study hot-carrier distributions in CH3NH3PbI3 and quantify key semiconductor parameters. Above bandgap, non-resonant excitation creates quasi-thermalized carrier distributions within 100 fs. During carrier cooling, a sub-bandgap transient absorption signal arises at ∼ 1.6 eV, which is explained by the inter  ...[more]

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