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Frontiers of attosecond science are constantly shifting, thus addressing moreand more intricate effects with increasing resolution. Ultrashort pulses offera practical way to prepare complex superpositions of quantum states, follow,and steer their dynamics. In this contribution, an ultrafast spin-flip processtriggered by sub-femtosecond (fs) excitation and strong spin-orbit couplingbetween 2p core-excited states of a transition metal complex is investigatedusing density matrix-based time-dependent restricted active space configurationinteraction theory. The effect of the nuclear vibrations is incorporated makinguse of an electronic system plus vibrational bath partitioning. The differencesbetween isolated sub-fs pulses and pulse trains as well as influence of variouspulse characteristics on the initiated dynamics are discussed. The effect understudy can be potentially used for ultrafast clocking in sub-few fs experiments.

Ultrafast dissipative spin-state dynamics triggered by X-ray pulse trains