Role of the static correlations on the ultrafast spin dynamics of 3d molecular nano-magnets

• Published in: Physica scripta 2020-06, Vol.95 (6)
• Main Authors: Dutta, D, Lefkidis, G, Hübner, W
• Format: Article
• Language: English
• Subjects: correlations; laser-induced spin dynamics; magnetism; quantum chemistry
• ISSN: 0031-8949; 1402-4896
• DOI: 10.1088/1402-4896/ab833a

We investigate the static and dynamic correlations on the synthesized heterotetranuclear magnetic cluster [Co3Ni(EtOH)]+, which, as already shown before, has a great potential to act as a magnetic nanologic element. Here we study the system with the state-of-the-art equation-of-motion coupled-cluster (EOM-CCSD) method, for which we find that although designed for dynamic correlations, it also incorporates a large part of the static correlations, and is thus an ideal method for studying optics on strongly correlated magnetic systems. We find that a major factor in the description of the static correlations is a strong d character of the molecular orbitals participating in the virtual excitations of the many-body states and propose a quantitative measure for static correlations in terms of the d → d virtual transitions. We find an inherent dependence of the static correlations on the magnetic field, the temperature, and the spin-orbit-coupling strength. Using two distinct correlation measures we study the evolution of the static and the dynamic correlations, as well as the entropy, during laser-induced ultrafast spin dynamics. Our results indicate that generally Λ processes greatly profit from strongly statically correlated intermediate states, and thus give us an insight on how to ameliorate the elementary processes when designing magnetic nanospintronics elements.