We developed novel room-temperature stimuli-responsive N-heteroacene-based liquid materials bearing a chiral alkyl chain. When these liquid materials were exposed to HCl vapor as an external stimulus, a disordered-ordered state change occurred immediately to yield self-assembled solid states from fluidic liquids. The self-assembly mechanism during this state change was evaluated by experimental in situ observations and molecular dynamics simulations over various spatiotemporal scales. These self-assembled structures led to supramolecular chirality through the influence of the chiral alkyl chain. As a result, circularly polarized luminescence (CPL) was triggered in the solid state, which was absent in the precursor liquid, thereby rendering this the first report on a stimuli-responsive CPL on/off liquid material. In addition, the initial state was recovered by exposure to air or upon heating. Moreover, the synergy between the experimental and the theoretical studies opens a new avenue to develop a novel class of stimuli-responsive materials and to discover novel phenomena in such materials.
Keywords: N-heteroacene; circularly polarized luminescence; molecular dynamics simulation; molecular modeling; quantum chemical calculation; room temperature photoluminescent liquid; stimuli-responsive liquid; time-dependent density functional theory.