White light: [{Au(L)}3] (L=3‐(2‐thienyl)pyrazolate) gives dual emission, one from an organic chromophore the other from aurophilic stacking interactions. The resulting blue–green and orange–red emissions can be tuned to approach white‐light by modulating the aggregation behavior of the cluster.

We observed an unusual reversible aggregation process showing stimuli-responsive structural dynamics and optical changes attributed to the formation of a sandwich-like Au3-Ag-Au3 cluster, which can be synthesized through both solution and mechanochemical methods. Unlike many other heteronuclear gold-silver clusters, the affinity of two cyclic Au3 complexes and a Ag(I) ion is solely bound by ligand unsupported Au-Ag bonding. The assembly/disassembly behavior, further forming nanoaggregates, is controllable by adjusting the concentration of the solution. In the solid state, the insertion of Ag(I) ion can be implemented through a mechanochemical approach, accompanied by visual color changes and reversible luminochromism. Furthermore, an uncommon solid-liquid extraction is demonstrated, showing the uniqueness of this labile Au-Ag metallophilicity and hinting at the possibility of manipulating a bonding process through a heterogeneous route.

White light: [{Au(L)}3] (L=3‐(2‐thienyl)pyrazolate) gives dual emission, one from an organic chromophore the other from aurophilic stacking interactions. The resulting blue–green and orange–red emissions can be tuned to approach white‐light by modulating the aggregation behavior of the cluster.

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Light up the world … … with white light from gold. In their Communication on page 13472 ff., D. Li and coworkers introduce an organic chromophore, thiophene, into a classical trinuclear gold(I) pyrazolate core that gives off aurophilic phosphorescence. The cooperation of dual emissions in the blue-green and orange-red regions underlies this solid-state white-light emitter, along with a red-emitting crystalline polymorph that assists the interpretation of this unusual observation in gold photochemistry.