The combination of physical properties sensitive to molecular chirality in a single system allows the observation of fascinating phenomena such as magneto‐chiral dichroism (MChD) and circularly polarized luminescence (CPL) having potential applications for optical data readout and display technology. Homochiral monodimensional coordination polymers of YbIIIwere designed from a 2,15‐bis‐ethynyl‐hexahelicenic scaffold decorated with two terminal 4‐pyridyl units. Thanks to the coordination of the chiral organic chromophore to Yb(hfac)3units (hfac−=1,1,1,5,5,5‐hexafluoroacetylaconate), efficient NIR‐CPL activity is observed. Moreover, the specific crystal field around the YbIIIinduces a strong magnetic anisotropy which leads to a single‐molecule magnet (SMM) behaviour and a remarkable room temperature MChD. The MChD‐structural correlation is supported by computational investigations.
The formation of helical self-assembled fibres by a C3 symmetric molecule incorporating three tetrathiafulvalene units is shown to be influenced dramatically by the processing conditions, leading to a variety of different chiral forms, including unprecedented croissants.