Stefan Haessler

Phase distortions of attosecond pulses produced by resonance-enhanced high harmonic generation

Resonant enhancement of high harmonic generation can be obtained in plasmas containing ions with strong radiative transitions resonant with harmonic orders. The mechanism for this enhancement is still debated. We perform the first temporal characterization of the attosecond emission from a tin plasma under near-resonant conditions for two different resonance detunings. We show that the resonance considerably changes the relative phase of neighboring harmonics. For very small detunings, their phase locking may even be lost, evidencing strong phase distortions in the emission process and a modified attosecond structure. These features are well reproduced by our simulations, allowing their interpretation in terms of the phase of the recombination dipole moment.

Spectrally resolved multi-channel contributions to the harmonic emission in N 2

When generated in molecules, high-order harmonics can be emitted through different ionization channels. The coherent and ultrafast electron dynamics occurring in the ion during the generation process is directly imprinted in the harmonic signal, i.e. in its amplitude and spectral phase. In aligned N2 molecules, we find evidence for a fast variation of this phase as a function of the harmonic order when varying the driving laser intensity. Basing our analysis on a three-step model, we find that this phase variation is a signature of transitions from a single- to a multi-channel regime. In particular, we show that significant nuclear dynamics may occur in the ionization channels on the attosecond timescale, affecting both the amplitude and the phase of the harmonic signal.

Polarization-resolved pump-probe spectroscopy with high harmonics

High harmonic generation in gases can be used as a probe of the electronic structure of the emitting medium, with attosecond temporal resolution and angstrom spatial resolution. The prospect of measuring molecular dynamics by pump-probe spectroscopy with such precision is attracting a lot of interest. An important issue in pump-probe spectroscopy lies in the ability to detect small signals: the detected signal can be easily dominated by the contributions from non-excited molecules or from a carrier gas. In this paper, we demonstrate that polarization-resolved pump-probe spectroscopy can be used to overcome this issue. We study high harmonic generation from rotationally excited molecules. We show that by measuring the harmonic field that is generated orthogonally to the driving laser field, the contrast in the detection of alignment revivals in nitrogen can be increased by a factor 4. We use this configuration to measure alignment revivals in an argon-nitrogen mixture, in which the total harmonic signal is dominated by the contributions from argon.

Femtosecond envelope of the high-harmonic emission from ablation plasmas

We characterize the temporal profile of the high-order harmonic emission from ablation plasma plumes using cross-correlations with the infrared (IR) laser beam provided by two-photon harmonic+IR ionization of rare gas atoms. We study both non-resonant plasmas (lead, gold and chrome) and resonant plasmas (indium and tin), i.e. plasmas presenting in the singly charged ions a strong radiative transition coinciding with a harmonic order. The cross-correlation traces are found to be very similar for all harmonic orders and all plasma targets. The recovered harmonic pulse durations are very similar to the driving laser, with a tendency towards being shorter, demonstrating that the emission is a directly laser-driven process even in the case of resonant harmonics. This provides a valuable input for theories describing resonant-harmonic emission and opens the perspective of a very high flux tabletop XUV source for applications.

Attosecond chirp-encoded dynamics of light nuclei

We study the spectral phase of high-order harmonic emission as an observable for probing ultrafast nuclear dynamics after the ionization of a molecule. Using a strong-field approximation theory that includes nuclear dynamics, we relate the harmonic phase to the phase of the overlap integral of the nuclear wavefunctions of the initial neutral molecule and the molecular ion after an attosecond probe delay. We determine experimentally the group delay of the high harmonic emission from D2 and H2 molecules, which allows us to verify the relation between harmonic frequency and the attosecond delay. The small difference in the harmonic phase between H2 and D2 calculated theoretically is consistent with our experimental results.

X-SEA-F-SPIDER characterization of over octave spanning pulses in the infrared range.

We show a practical implementation of a pulse characterization method for sub-cycle pulse measurements in the infrared spectral range based on spectral shearing interferometry. We employ spatially-encoded arrangement filter-based spectral phase interferometry for direct electric field reconstruction with external ancila pulses (X-SEA-F-SPIDER). We show merits and limitations of the setup and an in-depth comparison to another widely used temporal characterization technique - Second-Harmonic Generation Frequency Resolved Optical Gating (SHG-FROG). The X-SEA-F-SPIDER implementation presented in this paper allows measurement of sub-cycle pulses with over one octave wide spectrum spanning the 900-2400 nm range without adding any extra dispersion due to the pulse characterization apparatus.

Strong field applications of Gigawatt self-compressed pulses from a Kagome fiber

Nonlinear self-compression of 1.7-µm pulses in a gas-filled Kagome fiber down to a single cycle duration and pulse energies up to 100 µJ provides a uniquely simple driver source for high-harmonic generation and above-threshold ionization experiments.

Photoionization Time Delays

The material presented in this chapter is based on important advances realized in “attophysics” which make feasible to follow the motion of electrons in atoms and molecules with attosecond-level time resolution. In this context, time-delays have been recently determined in the process of photoionization by extreme-ultra-violet (XUV) pulses and the question of the significance of these measured delays arises. As we shall outline here, numerical experiments show that they are intimately related to the structure of the ionized species’ continuous spectrum. Another point addressed here is that, in experiments, the measurements have the common characteristic to be performed in the presence of an auxiliary infra-red (IR) field, used to “clock” the timing of the process. This implies to adapt the theory treatment to handle such “two-color” photoionization processes. We review a systematic analysis of these features that are characteristic of this class of electronic transitions, when viewed in the time domain.

SEA-SPIDER Characterization of Over Octave Spanning Pulses in the Mid-IR

We show a pulse characterization method for sub-cycle pulse measurements based on spectral shearing interferometry which allows measurement of undistorted sub-cycle self-compressed pulses in Kagome fiber with spectrum spanning 1.1-2.6 μm range.

Standoff Sources of Coherent Radiation Initiated by Femtosecond Filaments

we present the results of experimental and theoretical investigations for remote initiation of lasing in nitrogen and air by femtosecond filaments generated by laser pulses with different wavelengths, polarization and applying adaptive control methods