Ultrafast carrier thermalization in lead iodide perovskite probed with two-dimensional electronic spectroscopy

Johannes M. Richter, Federico Branchi, Franco Valduga de Almeida Camargo, Baodan Zhao, Richard H. Friend, Giulio Cerullo () and Felix Deschler ()
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Johannes M. Richter: University of Cambridge
Federico Branchi: Politecnico di Milano
Franco Valduga de Almeida Camargo: Politecnico di Milano
Baodan Zhao: University of Cambridge
Richard H. Friend: University of Cambridge
Giulio Cerullo: Politecnico di Milano
Felix Deschler: University of Cambridge

Nature Communications, 2017, vol. 8, issue 1, 1-7

Abstract: Abstract In band-like semiconductors, charge carriers form a thermal energy distribution rapidly after optical excitation. In hybrid perovskites, the cooling of such thermal carrier distributions occurs on timescales of about 300 fs via carrier-phonon scattering. However, the initial build-up of the thermal distribution proved difficult to resolve with pump–probe techniques due to the requirement of high resolution, both in time and pump energy. Here, we use two-dimensional electronic spectroscopy with sub-10 fs resolution to directly observe the carrier interactions that lead to a thermal carrier distribution. We find that thermalization occurs dominantly via carrier-carrier scattering under the investigated fluences and report the dependence of carrier scattering rates on excess energy and carrier density. We extract characteristic carrier thermalization times from below 10 to 85 fs. These values allow for mobilities of 500 cm2 V−1 s−1 at carrier densities lower than 2 × 1019 cm−3 and limit the time for carrier extraction in hot carrier solar cells.

Date: 2017
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DOI: 10.1038/s41467-017-00546-z

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