The gap between laser dyes and luminescent polymers—on the way to the polymer laser diode‒is bridged by conjugated oligothiophenes, according to the results reported here. Evidence for optically pumped spectral narrowing in ultrathin single crystals of α‐octithiophene (α‐8T) is presented. For example, the gain narrowing of two narrow emission lines that appear when the crystals are pumped can be described in the usual framework of stimulated emission. In contrast to dye‐doped crystals, α‐8T provides both the emitter and the optical cavity.
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