Infrared and electronic absorption spectra as well as ultrafast spin dynamics in isolatedCo3+(EtOH)andCo3+(EtOH,

Abstract

We present a combined theoretical and experimental study of the infrared (IR) and electronic absorption spectra in a molecular beam experiment as well as an analysis of spin dynamics in the clusters Co + 3 (EtOH) and Co + 3 (EtOH,H 2 O). The calculated IR and ground-state absorption spectra show very good agreement with experiment. By using high-level quantum chemistry methods, laser-induced ultrafast spin-flip scenarios in these structures are predicted. For the spin flip in Co + 3 (EtOH), our investigation indicates a 5 meV tolerance with respect to the laser detuning and a 6.5 meV tolerance with respect to the pulse spectral broadening, which are quite acceptable for the experimental implementation. In addition, we find that with the increase of the laser detuning the fitness of the processes gradually decays to zero on both sides but with different origins. This joint study of the homotrinuclear clusters provides insight into the experimentally observed spectra and optical properties, and steps towards the optical control of molecular magnetism for future spintronics application.

Joint Experimental and Theoretical Studies of Two Cu(II) Complexes with a 1,2,3-Triazole Derivative as Ligand: SCSC Transformation and Tunable Magnetic Properties

“…In order to clarify the magnetostructural correlations and further offer potential applications of such molecular materials in the area of tunable magnetic devices, it is an important challenge to establish the relationship between the molecular packing and magnetic properties, which requires a combination of theoretical and experimental studies. Coupled-cluster methods have been proven to produce very good agreement with experimental results in the calculations of coordinated metallic atoms in both molecular − and extended systems , in many of our previous studies. The reason lies in their ability to cope with both static correlations (which dominate magnetism) and dynamic correlations (which, among others, greatly affect the optical properties of the system). , In the present paper, we further employ these methods to investigate the polymerization behavior of discrete metal complexes through weak intermolecular interactions, so as to gain a better understanding of the relationship between molecular stacking fashions and magnetic properties.…”

Spin-electric Berry phase shift in triangular molecular magnets

“…As we mentioned in the Introduction, these systems can be possibly addressed in molecular beam experiments, similar to the ones realized in Ref. 22. An alternative experimental realization of the effect studied in this paper could possibly involve the functionalization of the MMs onto an appropriate surface/substrate, which are then electrically addressed by a nearby STM tip and electric gates.…”

“…Laser-induced nonadiabatic (femtosecond) spin dynamics in isolated triangular clusters, such as Co + 3 (EtOh), Co + 3 (EtOh), Ni 3 (CH 3 OH), and Co + (CH 3 OH) have been studied recently both theoretically (using advanced ab-initio methods) and experimentally in molecular beam experiments 22,23 . These tri-nuclear transition-metal clusters are different from the antiferromagnetic triangular molecules considered in the present paper.…”

A theoretical study of laser-induced ultrafast spin dynamics in trigonal monopyramidal iron and nickel complexes

“…The quality of the method has already been verified in a vast pool of cases. [37][38][39] (iii) Third, we perturbatively include spin-orbit coupling (SOC) and a very weak static external magnetic field B (Zeeman splitting, in order to differentiate between spin-up and spindown states) as described by the following Hamiltonian:…”