Ab initio theory for femtosecond spin dynamics, angle-resolved fidelity analysis, and the magneto-optical Kerr effect in the Ni-3(CH3OH) and Co-3(+) (CH3OH) clusters

作者：Chaudhuri, D.^*; Jin, W.; Lefkidis, G.; Huebner, W.

来源：Journal of Chemical Physics, 2015, 143(17): 174303.

DOI：10.1063/1.4932949

• EFFECTIVE CORE POTENTIALS
• SMALL NI-N
• MOLECULAR CALCULATIONS
• ELECTRONIC-STRUCTURE
• LASER-PULSES
• ULTRAFAST
• NICKEL
• METHANOL
• SPECTROSCOPY
• MAGNETISM

We present a systematic analysis of the ab initio controlled femtosecond spin dynamics in Ni-3(CH3OH) and Co-3(+)(CH3OH) clusters achieved by a spin-orbit-coupling enabled. process. The distortion caused by the attachment of CH3OH to one of the active magnetic centers of the Ni-3 and the Co-3(+) clusters induces asymmetric geometries which result in well localized spin densities on the magnetic centers. With the use of high-level quantum chemistry methods, successful spin-flip scenarios are demonstrated for both clusters. In order to assess the experimental accessibility of those effects, we compute their tolerance with respect to two laser pulse parameters, i. e., the energy detuning as well as the deviation of the polar angle phi from its optimized value. Finally, we calculate the magneto-optical Kerr effect in order to connect to the susceptibility tensor chi as an experimentally measurable quantity.

• 出版日期2015-11-7
• 单位陕西师范大学