4.8 Article

Multiphoton Excitation of CsPbBr3 Perovskite Quantum Dots (PQDs): How Many Electrons Can One PQD Donate to Multiple Molecular Acceptors?

Journal

JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 10, Issue 11, Pages 2775-2781

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.9b01045

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Funding

  1. TUT postdoctoral programme, Tampere University, Finland

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Metastable multiexcitonic states (MESs) of semiconductor quantum dots can be involved in multielectron transfer reactions, which opens new perspectives in nanomaterials-based optoelectronic applications. Herein, we demonstrate the generation of a MES in CsPbBr3 perovskite quantum dots (PQDs) and its dissociation dynamics through multiple electron transfers to molecular electron acceptors, anthraquinones (AQs), bound to the PQD surface by a carboxylic anchor. As many as 14 excitons are produced at an excitation density of roughly 220 mu J cm(-2) without detectable PQD degradation. Addition of AQresults in the formation of PQD-AQ hybrids with excess of AQs (PQD:AQ approximate to 1:20), which opens the possibility of multielectron transfer acts from MES to AQs. We found that the electron transfer saturates after roughly five transfer acts and that the first electron transfer (ET) time constant is as short as 1 ps. However, each ET increases the Coulomb potential barrier for the next ET, which decreases the rate of ET, resulting in a saturation after five ETs.

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