Complex Emissive Properties of Novel Azulene‐Dimethylaniline Dyads: Insights from Experimental and Computational Studies

Stimuli‐responsive fluorescent materials are of great interest for sensing applications. Azulene‐based molecular platforms feature a unique combination of optical, luminescence, and stimuli‐responsive properties. In particular, they often display both pH‐ and excitation wavelength‐dependent luminescent properties. Herein, the syntheses of two novel azulene derivatives 4‐(azulen‐2‐yl)‐ N , N ‐dimethylaniline ( 1 ) and 4‐(azulen‐1‐yl)‐ N , N ‐dimethylaniline ( 2 ) is presented via Suzuki–Miyaura cross coupling reactions. Combined experimental and theoretical investigations have been performed to elucidate the complex emissive properties exhibited by 4‐(azulen‐2‐yl)‐ N , N ‐dimethylaniline and 4‐(azulen‐1‐yl)‐ N , N ‐dimethylaniline, as well as those of their protonated forms. An in‐depth understanding of their stimuli‐responsive fluorescent properties is provided which is crucial for the future development of optical sensors.