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Two distinct “light switch” molecules are turned on in the presence of different G ‐ quadruplex DNA structures. When irradiated with visible light, the photochemical “light switch” undergoes selective ligand loss when bound to mixed ‐ hybrid G ‐ quadruplex DNA, followed by DNA metalation. The photophysical “light switch” brightly emits when bound to parallel G ‐ quadruplex DNA. More information can be found in the Full Paper by E. C. Glazer et al. on page 550 ff. [ABSTRACT FROM AUTHOR]