Nirit Dudovich's Lab

Attosecond transient absorption resolves the instantaneous response of a quantum system as it interacts with a laser field, by mapping its sub-cycle dynamics onto the absorption spectrum of attosecond pulses. However, the quantum dynamics are imprinted in the amplitude, phase and polarization state of the attosecond pulses. Here we introduce attosecond transient interferometry and measure the transient phase, as we follow its evolution within the optical cycle. We demonstrate how such phase information enables us to decouple the multiple quantum paths induced in a light-driven system, isolating their coherent contribution and retrieving their temporal evolution. Applying attosecond transient interferometry reveals the Stark shift dynamics in helium and retrieves long-term electronic coherences in neon. Finally, we present a vectorial generalization of our scheme, theoretically demonstrating the ability to isolate the underlying anomalous current in light-driven topological materials. Our scheme provides a direct insight into the interplay of light-induced dynamics and topology. Attosecond transient interferometry holds the potential to considerably extend the scope of attosecond metrology, revealing the underlying coherences in light-driven complex systems.

In this chapter, we introduce all-optical attosecond interferometry using high-harmonic generation (HHG). Interferometry provides an access to phase information, enabling the reconstruction of ultrafast electron dynamics with attosecond precision. We discuss two main pathwaysinternal and external attosecond interferometry. In internal interferometry, the manipulation of quantum paths within the HHG mechanism enables phase-resolved studies of strong-field processes, such as field-induced tunneling. In external interferometry, the phase of the light emitted during the HHG process can be determined using optical interference in the extreme-ultraviolet regime. Both pathways have significantly progressed the state of the art of ultrafast spectroscopy, as evidenced by numerous examples described in this chapter. All-optical attosecond interferometry is applicable to a wide range of systems, such as atomic and molecular gases and condensed-matter systems. Combining the two pathways has the potential to access to hitherto elusive ultrafast multi-electron and chiral phenomena.

Strong laser pulses enable probing molecules with their own electrons. The oscillating electric field tears electrons off a molecule, accelerates them, and drives them back toward their parent ion within a few femtoseconds. The electrons are then diffracted by the molecular potential, encoding its structure and dynamics with angstrom and attosecond resolutions. Using elliptically polarized laser pulses, we show that laser-induced electron diffraction is sensitive to the chirality of the target. The field selectively ionizes molecules of a given orientation and drives the electrons along different sets of trajectories, leading them to recollide from different directions. Depending on the handedness of the molecule, the electrons are preferentially diffracted forward or backward along the light propagation axis. This asymmetry, reaching several percent, can be reversed for electrons recolliding from two ends of the molecule. The chiral sensitivity of laser-induced electron diffraction opens a new path to resolve ultrafast chiral dynamics.