Response of Spin to Chiral Orbit and Phonon in Organic Chiral Ferrimagnetic Crystals

Achiral organic materials show nearly negligible orbit angular momentum, whereas organic ferrimagnets with chirality and reduced electron-lattice scattering could fundamentally bridge the gap between ferromagnetism and antiferromagnetism in the rapidly emerging field of ferrimagnetic spintronics. In this work, we report enantiomeric organic chiral ferrimagnets, where the chirality results from the molecular torsion by propeller-like arrangement of the donor and acceptor molecules. The ferrimagnetism results from the difference in electron-phonon coupling of the donor and acceptor inside the chiral crystals. Because the spin polarization is significantly dependent on the chirality, the magnetization of right-handed organic chiral ferrimagnetic crystals is larger than that of left-handed ones by 300% at 10 K. In addition, the processes of both excitation and recombination are strongly related to spin, phonon, and chiral orbit in these chiral ferrimagnets. Overall, both the organic chiral ferrimagnetism and spin chiroptical activities may substantially enrich the field of organic spintronics.