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 Yb^IIIwere 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 Yb^IIIinduces 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.

A thin layer of ordered DNA acts as an efficient spin filter for photoemitted electrons from a gold surface.

Magnetochiral dichroism (MChD), a fascinating manifestation of the light-matter interaction characteristic for chiral systems under magnetic fields, has become a well-established optical phenomenon reported for many different materials. However, its interpretation remains essentially phenomenological and qualitative, because the existing microscopic theory has not been quantitatively confirmed by confronting calculations based on this theory with experimental data. Here, we report the experimental low-temperature MChD spectra of two archetypal chiral paramagnetic crystals taken as model systems, tris(1,2-diaminoethane)nickel(II) and cobalt(II) nitrate, for light propagating parallel or perpendicular to the c axis of the crystals, and the calculation of the MChD spectra for the Ni(II) derivative by state-of-the-art quantum chemical calculations. By incorporating vibronic coupling, we find good agreement between experiment and theory, which opens the way for MChD to develop into a powerful chiral spectroscopic tool and provide fundamental insights for the chemical design of new magnetochiral materials for technological applications.