4.6 Article

Reversible Luminochromism of an N-Heterocyclic Carbene-Protected Carbon-Centered Hexagold(I) Cluster by Solvent and Mechanical Stimuli

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ADVANCED OPTICAL MATERIALS
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WILEY-V C H VERLAG GMBH
DOI: 10.1002/adom.202301650

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gold clusters; mechanoluminochromism; N-heterocyclic carbene (NHC) ligands; stimuli-responsiveness; vapoluminochromism

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This study reports a carbon-centered gold cluster with reversible multi-stimuli responsiveness and reveals the relationship between its photophysical properties and ligand conformation through structural analysis and theoretical calculations. Additionally, the study finds that the gold cluster can emit green light even after losing crystallinity, which is a highly promising model compound for understanding the principles governing stimuli-responsiveness in metal clusters.
Luminochromic gold clusters have potential applications in sensing due to the unique optical properties arising from their geometric and electronic structures. However, the rational design of such clusters is extremely challenging, especially when the goal is to impart reversible stimuli-responsive properties to gold clusters. Herein, the reversible multi-stimuli responsiveness of a carbon-centered hexagold(I) CAu6I cluster protected by N,N'-dibenzylbenzimidazolylidene (BIBn) ligands is reported. Two types of crystals emitting blue (?(max)(em) = 479 nm) and turquoise (?(max)(em) = 497 nm) photoluminescence (PL) are obtained and found to be interconvertible by the addition and removal of solvent. Single-crystal X-ray structure analysis has revealed significant differences between the crystal structures, including the conformation of the BIBn ligands. Theoretical calculations suggest that these conformational differences directly affect the photophysical properties and that the flexibility of the BIBn ligands attached to the CAu6I core makes this possible. Furthermore, when these crystals are grounded with a spatula, they are found to emit green PL (?(max)(em) = 520 nm) following a partial loss of crystallinity. This is a remarkable example of both vapoluminochromism and mechanoluminochromism in an N-heterocyclic carbene (NHC)-protected gold cluster and holds promise as a model compound for understanding the principles governing stimuli-responsiveness in metal clusters.

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