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Probing single-molecule electron–hole transfer dynamics at a molecule–NiO semiconductor nanocrystalline interface

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Abstract

Interfacial charge transfer dynamics in dye-sensitized NiO nanoparticles are being investigated for photocathodes in p-type dye-sensitized solar cells. In the photoreaction, after fast electron transfer from NiO to a molecule, the recombination of the hole in the nanoparticles with the electron in a reduced molecule plays an important role in the charge separation process and solar energy harvesting. Nevertheless, knowledge of the interfacial charge recombination (CR) rate and its mechanism is still limited due to the complex photoinduced electron and hole dynamics and lack of characterization of the inhomogeneity of the dynamics. Here, we report our work on probing interfacial charge recombination dynamics in Zn(II)–5,10,15,20-tetra(3-carboxyphenyl)porphyrin (m-ZnTCPP) dye-sensitized NiO nanoparticles by correlating single-molecule fluorescence blinking dynamics with charge transfer dynamics using single-molecule photon-stamping spectroscopy. The correlated analyses of single-molecule fluorescence intensity, lifetime, and blinking reveal the intrinsic distribution and temporal fluctuation of interfacial charge transfer reactivity, which are closely related to site-specific molecular interactions and dynamics.

Graphical abstract: Probing single-molecule electron–hole transfer dynamics at a molecule–NiO semiconductor nanocrystalline interface

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Publication details

The article was received on 08 Mar 2017, accepted on 29 May 2017 and first published on 30 May 2017


Article type: Paper
DOI: 10.1039/C7CP01476G
Citation: Phys. Chem. Chem. Phys., 2017, Advance Article
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    Probing single-molecule electron–hole transfer dynamics at a molecule–NiO semiconductor nanocrystalline interface

    B. Dhital, V. G. Rao and H. P. Lu, Phys. Chem. Chem. Phys., 2017, Advance Article , DOI: 10.1039/C7CP01476G

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