Single-component dual emission and full-spectrum color tuning from through-space charge transfer in asymmetric [2.2]paracyclophanes

M and persists in a rigid polymer matrix. By utilizing solvent polarity to alter the thermodynamic equilibrium between these states, we demonstrate continuous color tuning across the visible spectrum, including the generation of single-molecule white light with CIE coordinates of (0.33, 0.32). Furthermore, we report a negative thermal quenching effect, in which the emission intensity rises rather than falls on heating, achieving photoluminescence quantum yields as high as 88%, a response documented in inorganic phosphors and semiconductors but rare among discrete organic emitters in solution. Translating thermal and dielectric fluctuations into ratiometric spectral readouts positions cyclophanes as a general scaffold for stimuli-responsive optoelectronics.