Unusual Thermo‐Enhanced Second Harmonic Generation in Organic Configurationally‐Locked Polyene Crystals

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To modulate nonlinear optical (NLO) effects of crystalline material holds great application potential in the photoelectronic and optical fields. Organic configurationally-locked polyene represents an exciting NLO family with large second harmonic generation (SHG) effects, whereas it is a huge blank to switch and modulate their NLO property through external stimuli. For the first time, here present unusual thermo-enhanced SHG activities are presented in a polyene-based NLO compound, 2-{3-[2-(4-pyrrolidinphenyl)vinyl]-5,5-dimethylcyclohex-2-enylidene}malononitrile (1), giving a record-high magnitude of SHG enhancement up to ≈170% during its isomorphic phase transition. Theoretical analysis discloses this behavior stems from the reduced degree of torsion in the π-conjugated structures in 1, as verified by dihedral angles between its pyrrolidine and phenyl planes. As the first study on thermo-enhanced SHG properties of organic crystals, this work affords a new avenue of modulating physical properties to fabricate high-performance photoelectronic and optical devices.