From molecules to materials: SHG-CD microscopy of structured chiral films

The interplay between molecular and structural chirality as a function of local sample morphology determines the nonlinear optical properties of many organic and hybrid organic–inorganic thin films. Here, we used second harmonic generation circular dichroism (SHG-CD) microscopy of thin molecular films of 1,1′-bi-2-naphthol (R-BINOL) as a research model. Our results show that the SHG signal measured at frequencies close to the electronic transition of BINOL molecules is resonantly enhanced by more than an order of magnitude compared to the non-resonant case. The extracted resonant SHG-CD signal is dominated by the chiral response of the molecule. In contrast, structural chirality determines the non-resonant SHG-CD images. We see clear evidence that the interference of the SHG signals caused by the molecular and structural chirality can lead to a decrease in the overall SHG intensity when both SHG signals are out of phase. These findings highlight the intricate relationship between molecular and structural chirality on the one hand and structural morphology on the other hand and pave the way for novel applications by exploiting the chiroptic properties of thin films.