Ultrafast carrier thermalization in lead iodide perovskite probed with two-dimensional electronic spectroscopy
Authors
Richter, Johannes
Branchi, F
Valduga de Almeida Camargo, F
Zhao, Baodan
Cerullo, G
Journal Title
Nature Communications
ISSN
2041-1723
Publisher
Nature Publishing Group
Volume
8
Number
376
Language
English
Type
Article
This Version
VoR
Metadata
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Richter, J., Branchi, F., Valduga de Almeida Camargo, F., Zhao, B., Friend, R., Cerullo, G., & Deschler, F. (2017). Ultrafast carrier thermalization in lead iodide perovskite probed with two-dimensional electronic spectroscopy. Nature Communications, 8 (376)https://doi.org/10.1038/s41467-017-00546-z
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 cm$^2$ V$^{−1}$s$^{−1}$ at carrier densities lower than 2 × 10$^{19}$ cm$^{−3}$ and limit the time for carrier extraction in hot carrier solar cells.
Relationships
Is supplemented by: https://doi.org/10.17863/CAM.11883
Sponsorship
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.
Funder references
EPSRC (EP/M005143/1)
EPSRC (1492283)
Embargo Lift Date
2100-01-01
Identifiers
External DOI: https://doi.org/10.1038/s41467-017-00546-z
This record's URL: https://www.repository.cam.ac.uk/handle/1810/265674
Rights
Attribution 4.0 International, Attribution 4.0 International, Attribution 4.0 International, Attribution 4.0 International