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


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Authors

Price, Michael B 
Butkus, Justinas 
Jellicoe, Tom C 
Briane, Anouk 

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.

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Keywords

0912 Materials Engineering

Journal Title

Nat Commun

Conference Name

Journal ISSN

2041-1723
2041-1723

Volume Title

6

Publisher

Springer Science and Business Media LLC
Sponsorship
Engineering and Physical Sciences Research Council (EP/M005143/1)
EPSRC (via Brunel University London) (unknown)
Engineering and Physical Sciences Research Council (EP/G060738/1)
We thank the Engineering and Physical Sciences Research Council, and the Winton Programme (Cambridge) for the Physics of Sustainability for funding. M.B.P. wants to thank the Cambridge Commonwealth Trust and the Rutherford Foundation of New Zealand for funding. F.D. acknowledges funding from a Herchel Smith Research Fellowship.