Time-Resolved Measurement of Interatomic Coulombic Decay Induced by Two-Photon Double Excitation of Ne_{2}.

The hitherto unexplored two-photon doubly excited states [Ne^{*}(2p^{-1}3s)]_{2} were experimentally identified using the seeded, fully coherent, intense extreme ultraviolet free-electron laser FERMI. These states undergo ultrafast interatomic Coulombic decay (ICD), which predominantly produces singly ionized dimers. In order to obtain the rate of ICD, the resulting yield of Ne_{2}^{+} ions was recorded as a function of delay between the extreme ultraviolet pump and UV probe laser pulses. The extracted lifetimes of the long-lived doubly excited states, 390(-130/+450) fs, and of the short-lived ones, less than 150 fs, are in good agreement with ab initio quantum mechanical calculations.

Probe of Multielectron Dynamics in Xenon by Caustics in High-Order Harmonic Generation.

We investigated the giant resonance in xenon by high-order harmonic generation spectroscopy driven by a two-color field. The addition of a nonperturbative second harmonic component parallel to the driving field breaks the symmetry between neighboring subcycles resulting in the appearance of spectral caustics at two distinct cutoff energies. By controlling the phase delay between the two color components it is possible to tailor the harmonic emission in order to amplify and isolate the spectral feature of interest. In this Letter we demonstrate how this control scheme can be used to investigate the role of electron correlations that give birth to the giant resonance in xenon. The collective excitations of the giant dipole resonance in xenon combined with the spectral manipulation associated with the two-color driving field allow us to see features that are normally not accessible and to obtain a good agreement between the experimental results and the theoretical predictions.

Slow Interatomic Coulombic Decay of Multiply Excited Neon Clusters.

Ne clusters (∼5000 atoms) were resonantly excited (2p→3s) by intense free electron laser (FEL) radiation at FERMI. Such multiply excited clusters can decay nonradiatively via energy exchange between at least two neighboring excited atoms. Benefiting from the precise tunability and narrow bandwidth of seeded FEL radiation, specific sites of the Ne clusters were probed. We found that the relaxation of cluster surface atoms proceeds via a sequence of interatomic or intermolecular Coulombic decay (ICD) processes while ICD of bulk atoms is additionally affected by the surrounding excited medium via inelastic electron scattering. For both cases, cluster excitations relax to atomic states prior to ICD, showing that this kind of ICD is rather slow (picosecond range). Controlling the average number of excitations per cluster via the FEL intensity allows a coarse tuning of the ICD rate.

High-order harmonic spectroscopy for molecular imaging of polyatomic molecules.

High-order harmonic generation is a powerful and sensitive tool for probing atomic and molecular structures, combining in the same measurement an unprecedented attosecond temporal resolution with a high spatial resolution of the order of an angstrom. Imaging of the outermost molecular orbital by high-order harmonic generation has been limited for a long time to very simple molecules, like nitrogen. Recently we demonstrated a technique that overcame several of the issues that have prevented the extension of molecular orbital tomography to more complex species, showing that molecular imaging can be applied to a triatomic molecule like carbon dioxide. Here we report on the application of such a technique to nitrous oxide (N(2)O) and acetylene (C(2)H(2)). This result represents a first step towards the imaging of fragile compounds, a category which includes most of the fundamental biological molecules.

Non-collinear high-order harmonic generation by three interfering laser beams.

High order harmonic generation (HHG) has shown its impact on several applications in Attosecond Science and Atomic and Molecular Physics. Owing to the complexity of the experimental setup for the generation and characterization of harmonics, as well as to the large computational costs of numerical modelling, HHG is generally performed and modelled in collinear geometry. Recently, several experiments have been performed exploiting non-collinear geometry, such as HHG in a grating of excited molecules created by crossing beams. In such studies, harmonics were observed at propagation directions different from those of the driving pulses; moreover the scattered harmonics were angularly dispersed.In this work we report on a new regime of HHG driven by multiple beams, where the harmonics are generated by three synchronized, intense laser pulses organized in a non-planar geometry. Although the configuration we explore is well within the strong-field regime, the scattered harmonics we observe are not angularly dispersed.

Trajectory-resolved Coulomb focusing in tunnel ionization of atoms with intense, elliptically polarized laser pulses.

In strong-field light-matter interactions, the strong laser field dominates the dynamics. However, recent experiments indicate that the Coulomb force can play an important role as well. In this Letter, we have studied the photoelectron momentum distributions produced from noble gases in elliptically polarized, 800 nm laser light. By performing a complete mapping of the three-dimensional electron momentum, we find that Coulomb focusing significantly narrows the lateral momentum spread. We find a surprisingly sensitive dependence of Coulomb focusing on the initial transverse momentum distribution, i.e., the momentum at the moment of birth of the photoelectron. We also observe a strong signature of the low-energy structure in the above threshold ionization spectrum.

Ultrafast spectroscopy of linear carbon chains: the case of dinaphthylpolyynes.

The dynamics of excited states in α,ω-dinaphthylpolyyne, a class of linear sp-carbon chains, has been investigated by ultrafast transient absorption spectroscopy and DFT//TDDFT calculations. We show that the role of molecular conformers, in which end-capped naphthalene rings are planar or perpendicular to the polyyne plane, is fundamental for understanding both the steady state properties, such as UV-Vis absorption spectra and vibronic transitions, and the ultrafast transient absorption features. In particular, we observed in one of the conformers the ultrafast formation of a narrow photo-induced absorption band rising within 30 ps. This band can be assigned to an inter-system crossing event leading to the formation of triplet excited states.

Polarization pulse shaping induced by impulsive molecular alignment in optical filamentation and application to high-order harmonic generation.

We investigated theoretically and experimentally the ultrafast birefringence induced by impulsive alignment in a molecular gas during optical filamentation. This phenomenon is able to substantially affect the polarization state of an ultrashort laser pulse that propagates through the aligned medium at suitable delays from a first aligning pulse. We exploited this modulation of the polarization state in order to effectively control the high-order harmonic generation (HHG) process, which is strongly dependent on the driving pulse polarization. These results open new and fascinating perspectives for the tailoring of strong-field phenomena by means of polarization pulse shaping.

Efficient continuum generation exceeding 200 eV by intense ultrashort two-color driver.

A temporal gating on the high-order harmonic emission process is achieved using an intense 20 fs, 1.45 microm pulse (IR) in combination with an intense 13 fs, 800 nm pulse [visible (VIS)]. Exploiting this two-color gating scheme, a coherent continuous emission extending up to 160 eV using Ar gas and 200 eV using Ne gas is efficiently generated. The IR pulse contributes to significantly extending the harmonic emission to higher photon energies, whereas the VIS pulse improves the conversion efficiency of the process. These results indicate the possibility to produce bright attosecond pulses approaching the soft X spectral region.

Molecular rotovibrational dynamics excited in optical filamentation.

The rotovibrational dynamics excited by optical filamentation in molecular gases is studied in the temporal domain. Two time-delayed replicas of the same laser pulse have been used to generate a first filament, for the rotovibrational excitation of the sample, and a second collinear filament probing the Raman dynamics. The Fermi doublet structure in CO(2) as well as the very fast stretching mode of H(2) were clearly resolved.

Rotational Raman effects in the wake of optical filamentation.

The spatiotemporal effects generated in the wake of a laser filament propagating in nitrogen are investigated. At suitable time delays, a probe light pulse propagating along the wake experiences a strong spatial confinement and a noticeable spectral broadening at the same time. Numerical simulations, well reproducing the experimental findings, show the key role of the impulsive rotational Raman response in the observed phenomena.

Millijoule-level phase-stabilized few-optical-cycle infrared parametric source.

Ultrabroadband self-phase-stabilized near-IR pulses have been generated by difference-frequency generation of a filament broadened supercontinuum followed by two-stage optical parametric amplification. Pulses with energy up to 1.2 mJ and duration down to 17 fs are demonstrated. These characteristics make such a source suited as a driver for high-order harmonic generation and isolated attosecond pulse production.

Elemental sensitivity in soft x-ray imaging with a laser-plasma source and a color center detector.

Elemental sensitivity in soft x-ray imaging of thin foils with known thickness is observed using an ultrafast laser-plasma source and a LiF crystal as detector. Measurements are well reproduced by a simple theoretical model. This technique can be exploited for high spatial resolution, wide field of view imaging in the soft x-ray region, and it is suitable for the characterization of thin objects with thicknesses ranging from hundreds down to tens of nanometers.

Hollow-fiber compression of visible, 200 fs laser pulses to 40 fs pulse duration.

We demonstrate the use of a very simple, compact, and versatile method, based on the hollow-fiber compression technique, to shorten the temporal length of visible laser pulses of 100-300 fs to pulse durations shorter than approximately 50 fs. In particular, 200 fs, frequency-doubled, Nd:glass laser pulses (527 nm) were spectrally broadened to final bandwidths as large as 25 nm by nonlinear propagation through an Ar-filled hollow fiber. A compact, dispersive, prism-pair compressor was then used to produce as short as 40 fs, 150 microJ pulses. A very satisfactory agreement between numerical simulations and measurements is found.

Isolated single-cycle attosecond pulses.

We generated single-cycle isolated attosecond pulses around approximately 36 electron volts using phase-stabilized 5-femtosecond driving pulses with a modulated polarization state. Using a complete temporal characterization technique, we demonstrated the compression of the generated pulses for as low as 130 attoseconds, corresponding to less than 1.2 optical cycles. Numerical simulations of the generation process show that the carrier-envelope phase of the attosecond pulses is stable. The availability of single-cycle isolated attosecond pulses opens the way to a new regime in ultrafast physics, in which the strong-field electron dynamics in atoms and molecules is driven by the electric field of the attosecond pulses rather than by their intensity profile.

Generation of high-energy self-phase-stabilized pulses by difference-frequency generation followed by optical parametric amplification.

We produce ultrabroadband self-phase-stabilized near-IR pulses by a novel approach where a seed pulse, obtained by difference-frequency generation of a hollow-fiber broadened supercontinuum, is amplified by a two-stage optical parametric amplifier. Energies up to 20 microJ with a pulse spectrum extending from 1.2 to 1.6 microm are demonstrated, and a route for substantial energy scaling is indicated.

High-energy, few-optical-cycle pulses at 1.5 microm with passive carrier-envelope phase stabilization.

We report on a source of ultrabroadband self-phase-stabilized near-IR pulses by difference-frequency generation of a hollow-fiber broadened supercontinuum followed by two-stage optical parametric amplification. We demonstrate energies up to 200 microJ with 15 fs pulse width, making this source suited as a driver for attosecond pulse generation.

Controlling two-center interference in molecular high harmonic generation.

We experimentally investigate the process of intramolecular quantum interference in high-order harmonic generation in impulsively aligned CO2 molecules. The recombination interference effect is clearly seen through the order dependence of the harmonic yield in an aligned sample. The experimental results can be well modeled assuming that the effective de Broglie wavelength of the returning electron wave is not significantly altered by the Coulomb field of the molecular ion. We demonstrate that such interference effects can be effectively controlled by changing the ellipticity of the driving laser field.

Measurement of harmonic phase differences by interference of attosecond light pulses.

By using a self-referencing technique, we have experimentally measured the influence of the carrier-envelope phase of femtosecond light pulses on the phase of the electric field of the radiation produced by high-order harmonic generation. We show that, in particular experimental conditions, the temporal evolution of the electric field of the attosecond pulses, is directly controlled by the carrier-envelope phase of the driving pulses.

Observation of carrier-envelope phase phenomena in the multi-optical-cycle regime.

So far the role of the carrier-envelope phase of a light pulse has been clearly experimentally evidenced only in the sub-6-fs temporal regime. Here we show, both experimentally and theoretically, the influence of the carrier-envelope phase of a multi-optical-cycle light pulse on high-order harmonic generation. For the first time, we demonstrate that the short and long electron quantum paths contributing to harmonic generation are influenced in a different way by the pulse carrier-envelope phase.