Full‐Color and Switchable Phosphorescence of Carbene‐Metal‐Amide‐Based Bimetallic Gold(I) Complexes with Dynamic through‐Space Interaction

Regulating through‐space interactions offers a promising strategy for designing multifunctional luminescent materials. However, integrating stimuli‐responsive photophysical behaviors into such systems remains challenging. In this study, a series of carbene‐metal‐amide bimetallic Au(I) complexes featuring dynamic through‐space interactions is reported that enable aggregation‐induced emission and full‐color‐tunable photoactivated phosphorescence. Single‐crystal X‐ray diffraction combined with theoretical calculations reveals conformationally adaptive frameworks that facilitate ligand rotational freedom (carbazole) and N ‐heterocyclic carbene conformational flexibility, enabling precise modulation of intramolecular through‐space interactions. These complexes exhibit multi‐stimuli‐responsive phosphorescence, allowing reversible, on‐demand switching of emission color and intensity across molecular and macroscopic scales. By strategically blending phosphors, white‐light emission with a CIE 1931 coordinate of (0.30, 0.31) is achieved. The materials further demonstrate time‐resolved information encryption capabilities, making them ideal for light‐activated printing and high‐security anti‐counterfeiting inks. This work advances the rational design of smart luminescent platforms for applications in optoelectronics, sensing, and photonic security.