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.

Self-referenced spectral interferometry for single-shot measurement of sub-5-fs pulses.

We demonstrate a novel approach for the extension of self-referenced spectral interferometry to the temporal characterization of few-optical cycle pulses. The new experimental setup is characterized by low dispersion and a collinear geometry. 4-fs pulses have been characterized by performing single-shot measurements, with high dynamic range on a broad temporal region. An independent measurement of the pulse duration, obtained by using attosecond streaking, allowed us to cross-check the experimental technique.

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.

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.

A versatile apparatus for time-resolved photoemission spectroscopy via femtosecond pump-probe experiments.

A laser-based system for time-resolved photoemission spectroscopy using up to 6.2 eV photons is presented. The versatility of the laser source permits several combinations of pump and probe photon energies with pulse durations of 50-100 fs. The ultrahigh vacuum system, equipped with evaporators, a low energy electron diffraction system and an Auger spectrometer, grants the possibility to grow and characterize thin films in situ. The electron energy analyzer is a time-of-flight spectrometer with a multianode detector allowing high count rates. The performance of the whole experimental setup is investigated on Cu(100), Cu(111), and Ag(111) single crystals.

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.

Sub-two-cycle light pulses at 1.6 microm from an optical parametric amplifier.

We generate ultrabroadband pulses, spanning the 1200-2100 nm wavelength range, from an 800 nm pumped optical parametric amplifier (OPA) working at degeneracy. We compress the microjoule-level energy pulses to nearly transform-limited 8.5 fs duration by an adaptive system employing a deformable mirror. To our knowledge, these are the shortest light pulses generated at 1.6 microm.

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.

Few-optical-cycle pulses in the near-infrared from a noncollinear optical parametric amplifier.

We extend the concept of broadband phase matching in a noncollinear optical parametric amplifier (NOPA) to the near-IR. In an 800 nm pumped NOPA using periodically poled stoichiometric lithium tantalate, we amplify a spectrum spanning the 1.1-1.7 microm range and corresponding to two optical cycles of the carrier wavelength. A limited portion of the spectrum is compressed by a prism pair down to 16 fs.

Generation of broadband mid-infrared pulses from an optical parametric amplifier.

We report on the direct generation of broadband mid-IR pulses from an optical parametric amplifier. Several crystals with extended IR transparency, when pumped at 800 nm, display a broad phase-matching bandwidth around 1 mum, allowing for the generation of idler pulses spanning the 3-5 mum wavelength range. Using LiIO(3), we produce 2muJ pulses tunable in the 3-4 mum range with bandwidth supporting 30-fs transform-limited duration.

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.

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.

Conjugation length dependence of internal conversion in carotenoids: role of the intermediate state.

We report on a sub-20-fs transient absorption study of the S2(1(1)B(+)(u))-->S1(2(1)A(-)(g)) internal conversion in a series of carotenoids with a number of conjugated double bonds (N) ranging from 5 to 15. For the longer carotenoids (N>or=9), the measurements reveal the existence of an additional intermediate excited state lying between the optically allowed S2 state and the lower-lying forbidden S1 state. This state enables us to explain the nonmonotonic dependence of the S2-->S1 conversion rate on N and is expected to play an important role in photosynthetic light harvesting.

Ultrabroadband self-phase-stabilized pulses by difference-frequency generation.

Ultrabroadband near-IR (800-1700-nm) pulses are obtained by type II difference-frequency generation (DFG) between two synchronized noncollinear optical parametric amplifiers. Self-stabilization of the carrier-envelope offset phase, as expected from the DFG process, is demonstrated experimentally.

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.