Hot-electron transfer in quantum-dot heterojunction films

Gianluca Grimaldi, Ryan W. Crisp, Stephanie Brinck, Felipe Zapata, Michiko Ouwendorp, Nicolas Renaud, Nicholas Kirkwood, Wiel H. Evers, Sachin Kinge, Ivan Infante, Laurens D. A. Siebbeles and Arjan J. Houtepen ()
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Gianluca Grimaldi: Delft University of Technology
Ryan W. Crisp: Delft University of Technology
Stephanie Brinck: Vrije Universiteit
Felipe Zapata: Vrije Universiteit
Michiko Ouwendorp: Delft University of Technology
Nicolas Renaud: Delft University of Technology
Nicholas Kirkwood: Delft University of Technology
Wiel H. Evers: Delft University of Technology
Sachin Kinge: Materials Research and Development
Ivan Infante: Vrije Universiteit
Laurens D. A. Siebbeles: Delft University of Technology
Arjan J. Houtepen: Delft University of Technology

Nature Communications, 2018, vol. 9, issue 1, 1-10

Abstract: Abstract Thermalization losses limit the photon-to-power conversion of solar cells at the high-energy side of the solar spectrum, as electrons quickly lose their energy relaxing to the band edge. Hot-electron transfer could reduce these losses. Here, we demonstrate fast and efficient hot-electron transfer between lead selenide and cadmium selenide quantum dots assembled in a quantum-dot heterojunction solid. In this system, the energy structure of the absorber material and of the electron extracting material can be easily tuned via a variation of quantum-dot size, allowing us to tailor the energetics of the transfer process for device applications. The efficiency of the transfer process increases with excitation energy as a result of the more favorable competition between hot-electron transfer and electron cooling. The experimental picture is supported by time-domain density functional theory calculations, showing that electron density is transferred from lead selenide to cadmium selenide quantum dots on the sub-picosecond timescale.

Date: 2018
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DOI: 10.1038/s41467-018-04623-9

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