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

TL;DR

This paper investigates ultrafast spin-flip dynamics in a transition metal complex triggered by sub-femtosecond X-ray pulses, revealing potential applications in ultrafast clocking and quantum control.

Contribution

It introduces a density matrix-based method to study spin dynamics induced by ultrashort X-ray pulses, including vibrational effects and pulse train influences.

Findings

Ultrafast spin-flip occurs within sub-femtosecond timescales.

Pulse trains and pulse characteristics significantly affect spin dynamics.

Vibrational effects modulate the spin-flip process.

Abstract

Frontiers of attosecond science are constantly shifting, thus addressing more and more intricate effects with increasing resolution. Ultrashort pulses offer a practical way to prepare complex superpositions of quantum states, follow, and steer their dynamics. In this contribution, an ultrafast spin-flip process triggered by sub-femtosecond (fs) excitation and strong spin-orbit coupling between 2p core-excited states of a transition metal complex is investigated using density matrix-based time-dependent restricted active space configuration interaction theory. The effect of the nuclear vibrations is incorporated making use of an electronic system plus vibrational bath partitioning. The differences between isolated sub-fs pulses and pulse trains as well as influence of various pulse characteristics on the initiated dynamics are discussed. The effect under study can be potentially used for ultrafast clocking in sub-few fs experiments.