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Nanoparticle surfactants for kinetically arrested photoactive assemblies to track light-induced electron transfer

Huang, J; Foldes, T; McCune, JA; Xu, DD; de Nijs, B; Chikkaraddy, R; Collins, SM; ... Sokolowski, K; + view all (2021) Nanoparticle surfactants for kinetically arrested photoactive assemblies to track light-induced electron transfer. Nature Nanotechnology , 16 pp. 1121-1129. 10.1038/s41565-021-00949-6. Green open access

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Abstract

Nature controls the assembly of complex architectures through self-limiting processes; however, few artificial strategies to mimic these processes have been reported to date. Here we demonstrate a system comprising two types of nanocrystal (NC), where the self-limiting assembly of one NC component controls the aggregation of the other. Our strategy uses semiconducting InP/ZnS core–shell NCs (3 nm) as effective assembly modulators and functional nanoparticle surfactants in cucurbit[n]uril-triggered aggregation of AuNCs (5–60 nm), allowing the rapid formation (within seconds) of colloidally stable hybrid aggregates. The resultant assemblies efficiently harvest light within the semiconductor substructures, inducing out-of-equilibrium electron transfer processes, which can now be simultaneously monitored through the incorporated surface-enhanced Raman spectroscopy–active plasmonic compartments. Spatial confinement of electron mediators (for example, methyl viologen (MV2+)) within the hybrids enables the direct observation of photogenerated radical species as well as molecular recognition in real time, providing experimental evidence for the formation of elusive σ–(MV+)2 dimeric species. This approach paves the way for widespread use of analogous hybrids for the long-term real-time tracking of interfacial charge transfer processes, such as the light-driven generation of radicals and catalysis with operando spectroscopies under irreversible conditions.

Type: Article
Title: Nanoparticle surfactants for kinetically arrested photoactive assemblies to track light-induced electron transfer
Open access status: An open access version is available from UCL Discovery
DOI: 10.1038/s41565-021-00949-6
Publisher version: https://doi.org/10.1038/s41565-021-00949-6
Language: English
Additional information: This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions.
Keywords: METHYL VIOLOGEN, NANOCRYSTALS, REDUCTION, CHEMISTRY, GROWTH
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Physics and Astronomy
URI: https://discovery.ucl.ac.uk/id/eprint/10137512
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