4.8 Article

Template-assisted alloying of atom-precise silver nanoclusters: a new approach to generate cluster functionality

Journal

CHEMICAL SCIENCE
Volume 13, Issue 38, Pages 11394-11404

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/d2sc04390d

Keywords

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Funding

  1. NPDF fund from SERB [PDF/2020/001085]

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A new synthetic approach using site-specific alloying has been revealed to acquire the atomic design of new functional Ag(i) nanoclusters. This approach allows precise control over the surface charge, size, and shape of the template, resulting in the self-assembly of Ag(i) with a similar core structure. The introduction of strongly interacted peripheral motif units enhances the rigidity of the cluster skeleton, reducing non-radiative transitions and facilitating room-temperature emission properties. The electron-donating effect of the peripheral motif units reduces the bandgap and influences intercluster charge carrier transport. This novel synthetic approach paves the way for well-functioning nanocluster design.
To acquire the atomic design of new functional Ag(i) nanoclusters (NCs), a new synthetic approach of site-specific alloying has been unveiled, by which the neutral CO2 templated Ag-20 core is confined through Cu containing two peripheral motif units. The impact of surface charge, size and shape of the template on the self-assembly of Ag(i) has been precisely controlled here for the first time and as a result, a similar pentagonal gyrobicupola-like Ag-20 core is formed while varying the templates (S2-, CO32- and CO2). However, the surface charge generated on the Ag(i) core due to the presence of a neutral template opens up the possibility of this novel alloying process. The introduction of strongly interacted peripheral motif units (DMA-CuS-) on the Ag-20 core enforces more rigidity in the skeleton that reduces the probability of non-radiative transition in the excited state by lowering the intramolecular vibration. In addition to this, the incorporation of electron-donating peripheral motif units modulates the frontier molecular arrangement that helps in attaining the synergy which would ultimately turn on the room-temperature emission properties. The electron-donating effect of the peripheral motif units further leads to a sharp reduction of the bandgap and the symmetric position of the heterometal in the cluster minimizes the intercluster distances which further influences the intercluster charge carrier transport. So, the precise structure-property correlation with this novel synthetic approach will pave the way for a well-functioning NC design.

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