Enabling coherence of polarized spin and photon in chiral nanoclusters through chirality-mediated magnetization control

Metal nanoclusters have emerged as pivotal materials in catalysis, sensing, luminescence, and bioimaging, largely due to the unique synergy between their polymetallic cores, ligand shells, and the resulting interfacial regions. This study investigates the mechanisms of angular momentum transfer from metal centers to organic ligands within enantiomeric nanocluster magnets, specifically focusing on its dependence on spin–photon–chiral orbit interactions. The strong interaction between the Cu4 core and the surrounding chiral organic ligands in the R/S-Cu4 (R/S refers to the chirality of the chiral ligand) nanocluster induces electron–phonon coupling dependent spin polarization that exhibits a marked disparity between enantiomers. Intensified electron–phonon coupling tends to quench the influence of the chiral orbit on spin states. Conversely, reducing the temperature leads to the attenuation of these vibrational interactions, thereby promoting more efficient spin–photon coupling. These findings offer fundamental insights into the complex interplay between spin degrees of freedom, lattice dynamics, and polarized photons in chiral nanoclusters.