Circular dichroism in multiphoton ionization of resonantly excited helium ions near channel closing.

The circular dichroism (CD) of photoelectrons generated by near-infrared (NIR) laser pulses using multiphoton ionization of excited He ions in the 3p(m= +1) state is investigated. The ions were prepared by circularly polarized extreme ultraviolet (XUV) pulses. For circularly polarized NIR pulses co- and counter-rotating relative to the polarization of the XUV pulse, a complex variation of the CD is observed as a result of intensity- and polarization-dependent Freeman resonances, with and without additional dichroic AC-Stark shifts.

Ultrafast Resonant State Formation by the Coupling of Rydberg and Dark Autoionizing States.

Studying the dynamics of dark states is challenging due to their inability to undergo single-photon emission or absorption. This challenge is made even more difficult for dark autoionizing states owing to their ultrashort lifetime of a few femtoseconds. High-order harmonic spectroscopy recently appeared as a novel method to probe the ultrafast dynamics of a single atomic or molecular state.

Attosecond pulse shaping using a seeded free-electron laser.

Attosecond pulses are central to the investigation of valence- and core-electron dynamics on their natural timescales. The reproducible generation and characterization of attosecond waveforms has been demonstrated so far only through the process of high-order harmonic generation. Several methods for shaping attosecond waveforms have been proposed, including the use of metallic filters, multilayer mirrors and manipulation of the driving field.

Complete Characterization of Phase and Amplitude of Bichromatic Extreme Ultraviolet Light.

Intense, mutually coherent beams of multiharmonic extreme ultraviolet light can now be created using seeded free-electron lasers, and the phase difference between harmonics can be tuned with attosecond accuracy. However, the absolute value of the phase is generally not determined. We present a method for determining precisely the absolute phase relationship of a fundamental wavelength and its second harmonic, as well as the amplitude ratio.

Symmetry breakdown of electron emission in extreme ultraviolet photoionization of argon.

Short wavelength free-electron lasers (FELs), providing pulses of ultrahigh photon intensity, have revolutionized spectroscopy on ionic targets. Their exceptional photon flux enables multiple photon absorptions within a single femtosecond pulse, which in turn allows for deep insights into the photoionization process itself as well as into evolving ionic states of a target. Here we employ ultraintense pulses from the FEL FERMI to spectroscopically investigate the sequential emission of electrons from gaseous, atomic argon in the neutral as well as the ionic ground state.