Proceedings of 13th Conference on Hybrid and Organic Photovoltaics (HOPV21)
Publication date: 11th May 2021
In solar cells, 33% of the energy of sunlight is lost as heat during the thermalization and cooling processes. Slow HCC is desired for thermoelectric devices and hot-carrier solar cells where extracting carriers before they have cooled could enable breaking the thermodynamic limit for single-junction solar cells. Emissive applications such as lasers, single-photon sources, and optical modulators require short HCC times for efficient radiative recombination and to prevent carrier trapping. Hot-carrier cooling (HCC) in metal halide perovskites above the Mott transition is significantly slower than in conventional semiconductors. This effect is commonly attributed to a hot-phonon bottleneck, but the influence of the lattice properties on the HCC behavior is poorly understood. Using pressure-dependent transient absorption spectroscopy, we find that at an excitation density below the Mott transition, pressure does not affect the HCC. On the contrary, above the Mott transition, HCC in methylammonium lead iodide is around 2–3 times faster at 0.3 GPa than at ambient pressure. Our electron–phonon coupling calculations reveal ∼2-fold stronger electron–phonon coupling for the inorganic cage mode at 0.3 GPa. However, our experiments reveal that pressure promotes faster HCC only above the Mott transition. Altogether, these findings suggest a change in the nature of excited carriers above the Mott transition threshold, providing insights into the electronic behavior of devices operating at such high charge-carrier densities.
Reference:
Accelerated Hot-Carrier Cooling in MAPbI3 Perovskite by Pressure-Induced Lattice Compression
Loreta A. Muscarella, Eline M. Hutter, Jarvist M. Frost, Gianluca G. Grimaldi, Jan Versluis, Huib J. Bakker, and Bruno Ehrler
The Journal of Physical Chemistry Letters 0, 12
DOI: 10.1021/acs.jpclett.1c00676
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