/spl lambda/-Process-Based Spin Manipulation in Magnetic Endohedral Fullerenes

Magnetic endohedral fullerenes hold much promise as the basic elements for realizing nanoscale devices such as molecular magnets, molecular memory devices, field effect transistors, and fullerene-based quantum computers. In this paper we take Co₂@C₆₀ as an example to investigate the laser-induced, ultrafast, spin-dynamics mechanisms via processes. Fully ab initio calculations show that the spin density is localized at one of the Co atoms inside the carbon cage, indicating local spin manipulation possibility. It is found that the laser-induced ultrafast spin transfer in the endohedral fullerene can be achieved under the influence of circularly polarized light. The caging fullerene itself not only contributes to the spin localization of the whole system (on one of the two Co atoms at a time), but also amplifies the effect of the adopted laser pulse and gives an experimental possibility to produce isolated ensemble Co₂ molecules. The predicted results and the physical mechanism unveiled in the present work are expected to shed some light on the application of magnetic elements embedded in fullerenes and other related nanomaterials as functional units in spin logic devices and to allow for application-oriented spin engineering.