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

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Richter, JM 
Branchi, F 
Valduga de Almeida Camargo, F 
Zhao, B 
Friend, RH 


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−1s−1 at carrier densities lower than 2 × 1019 cm−3 and limit the time for carrier extraction in hot carrier solar cells.



0299 Other Physical Sciences, Bioengineering

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Nature Communications

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Nature Publishing Group
Engineering and Physical Sciences Research Council (EP/M005143/1)
EPSRC (1492283)
European Commission Horizon 2020 (H2020) Future and Emerging Technologies (FET) (696656)
This project has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement no 654148 Laserlab-Europe (CUSBO 002151). We acknowledge further financial support from the Engineering and Physical Sciences Research Council of the UK (EPSRC). G.C. acknowledges support by the European Union Horizon 2020 Programme under Grant Agreement No. 696656 Graphene Flagship and by the European Research Council Advanced Grant STRATUS (ERC-2011-AdG No. 291198). J.M.R. and F.D. thank the Winton Programme for the Physics of Sustainability (University of Cambridge). J.M.R. thanks the Cambridge Home European Scheme for financial support. F.D. acknowledges funding from a Herchel Smith Research Fellowship and a Winton Advanced Research Fellowship. We thank Cristian Manzoni for fruitful discussions.
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