Optimization of the Photoresponse in a Molecular Ferroelectric

Molecular ferroelectrics bear significant potential for applications, in particular if they can be stimulated by light. One strategy to design molecular photoferroelectrics consists of combining organic cations with a photosensitive unit, such as a molecular photoswitch. The recently reported (DMA)(PIP)[Fe(CN) 5 NO] constitutes such a molecular ferroelectric, where the [Fe(CN) 5 NO] 2− can undergo photoisomerization of the NO ligand, into two metastable states called MS1 (isonitrosyl) and MS2 (side‐on NO). We show how to maximize the conversion from the nitrosyl ground state toward these two isomers using polarized light, and report the structures of the resulting photoisomers, MS1 and MS2.