Mummaneni, Bharadwaj ChowdaryBharadwaj ChowdaryMummaneniChen, SihuaiSihuaiChenHübner, WolfgangWolfgangHübnerLefkidis, GeorgiosGeorgiosLefkidis2024-07-292024-07-292024https://publica.fraunhofer.de/handle/publica/47215210.1039/d4cp01086h2-s2.0-8519703634938940727In the quest to harness the potential of nanospintronic applications, we analyze and investigate the spin channels for the ultrafast spin dynamics in mononuclear Cu2+(tdp)Cl2 (Cutdp) and Cu2+(tdp)Cl2·MeCN (Cutdp·MeCN) using a high-level ab initio many-body theory. In that spirit, we select two slightly different polymerizations arising from one parent complex. We establish the difference in magnetic behavior between the two complexes which arises solely from the geometrical differences. We calculate the static magnetic properties, such as the magnetic anisotropy of the complexes, which is analyzed by means of the magnetic moment of the ground state. The asymmetry of the core Cu-Cl-Cu-Cl axial plane unit is also reflected in the ground state absorption spectra of the two complexes. Comparisons with the experimental data are in good agreement with the exception of one peak in the theoretical calculations for each of the complexes, confirming the reliability of theoretical methods employed. A major finding in this work is the distinction between classical and coherent superpositions of Λ processes. We employ the selective blocking and retention (SBR) technique to find the unique path or paths for spin dynamic scenarios like spin flip and spin transfer. Additionally, we also present two different scenarios in which intermediate states are involved in spin dynamic processes, (i) classical superposition of Λ processes (i.e., there are many unique paths for transition, even with just one intermediate state the transition completes successfully), and (ii) collective coherent superposition of Λ processes (i.e., there is only one path for the transition, which requires more than one intermediate state to be in a specific coherent superposition). As a consequence, we gain insight into the type of correlations (static or dynamic) involved in a particular spin dynamic scenario.enjournal article