Abstract
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.
Original language | English |
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Pages (from-to) | 4118-4124 |
Number of pages | 7 |
Journal | The journal of physical chemistry letters |
Volume | 12 |
Issue number | 17 |
DOIs | |
Publication status | Published - 6 May 2021 |
Bibliographical note
Funding Information:The work of L.A.M., E.M.H., J.V., H.J.B., and B.E. is part of the Dutch Research Council (NWO) and was performed at the research institute AMOLF. The work of L.A.M. was supported by NWO Vidi Grant 016.Vidi.179.005. The authors thank Henk-Jan Boluijt for the design of Figure 1a. The authors thank Mar?a C. G?lvez-Rueda for commenting on the manuscript. J.M.F. is supported by a Royal Society University Research Fellowship (URF-R1-191292). Electronic structure calculations used the Imperial College Research Computing Service (DOI: 10.14469/hpc/2232). The work of G.G.G. was supported by the EPSRC International Centre to Centre Grant EP/S030638/1.
Funding Information:
The work of L.A.M., E.M.H., J.V., H.J.B., and B.E. is part of the Dutch Research Council (NWO) and was performed at the research institute AMOLF. The work of L.A.M. was supported by NWO Vidi Grant 016.Vidi.179.005. The authors thank Henk-Jan Boluijt for the design of a. The authors thank María C. Gélvez-Rueda for commenting on the manuscript. J.M.F. is supported by a Royal Society University Research Fellowship (URF-R1-191292). Electronic structure calculations used the Imperial College Research Computing Service (DOI: 10.14469/hpc/2232). The work of G.G.G. was supported by the EPSRC International Centre to Centre Grant EP/S030638/1.
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