Electrochemical Modulation of the Photophysics of Surface-Localized Trap States in Core/Shell/(Shell) Quantum Dot Films
Ward Van Der Stam (TU Delft - ChemE/Opto-electronic Materials)
Gianluca Grimaldi (TU Delft - ChemE/Opto-electronic Materials)
Jaco J. Geuchies (TU Delft - ChemE/Opto-electronic Materials)
Solrun Gudjonsdottir (TU Delft - ChemE/Opto-electronic Materials)
Pieter T. Van Uffelen (Student TU Delft)
Mandy Van Overeem (Student TU Delft)
Baldur Brynjarsson (Student TU Delft)
Nicholas Kirkwood (TU Delft - ChemE/Opto-electronic Materials)
Arjan J. Houtepen (TU Delft - ChemE/Opto-electronic Materials)
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Abstract
In this work, we systematically study the spectroelectrochemical response of CdSe quantum dots (QDs), CdSe/CdS core/shell QDs with varying CdS shell thicknesses, and CdSe/CdS/ZnS core/shell/shell QDs in order to elucidate the influence of localized surface trap states on the optoelectronic properties. By correlating the differential absorbance and the photoluminescence upon electrochemically raising the Fermi level, we reveal that trap states near the conduction band (CB) edge give rise to nonradiative recombination pathways regardless of the CdS shell thickness, evidenced by quenching of the photoluminescence before the CB edge is populated with electrons. This points in the direction of shallow trap states localized on the CdS shell surface that give rise to nonradiative recombination pathways. We suggest that these shallow trap states reduce the quantum yield because of enhanced hole trapping when the Fermi level is raised electrochemically. We show that these shallow trap states are removed when additional wide band gap ZnS shells are grown around the CdSe/CdS core/shell QDs.
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