Issue 6, 2023

Overall structure of Au12Ag60(S-c-C6H11)31Br9(Dppp)6: achieving a stronger assembly of icosahedral M13 units

Abstract

Precise atomically assembled nanoclusters provide a great platform to elucidate the evolution of the assembly of building blocks. Herein, a large icosahedral (M13)-based silver–gold alloy nanocluster [Au12Ag60(S-c-C6H11)31Br9(Dppp)6]Br2 (dppp = 1,3-bis(diphenylphosphino)propane) is reported. Structurally, Au12Ag60 consists of an Au12Ag40 kernel, which is viewed as the interpenetration of ten twisted complete icosahedrons (M13) and two missing icosahedrons (M12), and this is surrounded by a complex metal–organic shell. Benefiting from the extra doping of eight to twelve Au atoms, the octameric assembly was increased to a twelve-mer assembly. The time-dependent density functional theory (TDDFT) method with a Tamm–Dancoff approximation (TDA) was performed to investigate the difference in the optical properties of Au12Ag60 and Au8Ag57. The results indicate that the difference in the amount of Au atoms results in different optical properties. Furthermore, transient absorption spectroscopy (TA) was also performed, revealing that a twelve-mer assembly greatly enhances the excited-state lifetime. The [Au12Ag60(S-c-C6H11)31Br9(Dppp)6]Br2 alloy nanocluster has provided a breakthrough in the number of icosahedral M13 assemblies, i.e., achieving a twelve-mer assembly, helping to elucidate the fusion growth of M13-based assembled nanoclusters as well as their geometric/electronic structure correlations, which will promote further research on the assembly of M13 nano-building blocks, especially on their optical properties.

Graphical abstract: Overall structure of Au12Ag60(S-c-C6H11)31Br9(Dppp)6: achieving a stronger assembly of icosahedral M13 units

Supplementary files

Article information

Article type
Paper
Submitted
26 11 2022
Accepted
28 12 2022
First published
29 12 2022

Nanoscale, 2023,15, 2633-2641

Overall structure of Au12Ag60(S-c-C6H11)31Br9(Dppp)6: achieving a stronger assembly of icosahedral M13 units

M. Zhou, K. Li, P. Wang, H. Zhou, S. Jin, Y. Pei and M. Zhu, Nanoscale, 2023, 15, 2633 DOI: 10.1039/D2NR06613K

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