Trains of attosecond pulses structured with time-ordered polarization states.

Ultrafast laser pulses generated at the attosecond timescale represent a unique tool to explore the fastest dynamics in matter. An accurate control of their properties, such as polarization, is fundamental to shape three-dimensional laser-driven dynamics. We introduce a technique to generate attosecond pulse trains whose polarization state varies from pulse to pulse. This is accomplished by driving high-harmonic generation with two time-delayed bichromatic counter-rotating fields with proper orbital angular momentum (OAM) content. Our simulations show that the evolution of the polarization state along the train can be controlled via OAM, pulse duration, and time delay of the driving fields. We, thus, introduce an additional control into structured attosecond pulses that provides an alternative route to explore ultrafast dynamics with potential applications in chiral and magnetic materials.