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.

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.

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.

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.

Effects of laser irradiation on hematoporphyrin-treated normal and transformed thyroid cells in culture.

Laser irradiation of tissues treated in vivo with the hematoporphyrin derivative (HPD) is known to result in a cytocidal effect, reportedly more pronounced in the tumor than in the surrounding normal tissues. In order to ascertain if this phenomenon had a clear cellular basis, it has been now reproduced in vitro in a model system consisting of normal and transformed cell lines. Epithelial rat thyroid cells were infected and transformed with a RNA oncogenic virus. Both the original (normal) and the viral-transformed (tumorigenic) cells were incubated with HPD and exposed to two types of laser irradiation: 631 nm, continuous wave; and 337.1 nm, pulsed. Under the conditions tested, the percentage survival of the transformed cells was found to be lower (up to approximately 3 times) than that of the normal cells. The cytocidal effect was greater using the pulsed than using the continuous-wave irradiation. The difference between normal and tumor cells was more evident at 30 micrograms than at 50 micrograms of HPD per ml. The HPD not followed by laser irradiation had no effect on the cell growth rate. The findings of a significant difference in the sensitivity to photoactivated HPD between normal and tumor cells under strictly controlled and highly comparable conditions opens new possibilities to the study of the cellular and molecular mechanisms involved in the phototherapy of tumors. Furthermore, studies in vitro on the active components of the photosensitizer and on their selectivity towards the tumor cells, explained at a cellular level, will lead to better approaches to photochemotherapy in vivo.

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.

Spectral features and modeling of high-order harmonics generated by sub-10-fs pulses

Harmonic radiation generated in a neon gas jet by sub-10-fs laser pulses was investigated both experimentally and theoretically. The spectral profile of the harmonics with respect to the order, their intensity and relative spectral shifts were measured as a function of the position of the gas jet. The results point out spectral features typical of the quasi-single-cycle excitation regime. A nonadiabatic three-dimensional numerical model was developed, which provides harmonic spectra in remarkable agreement with the experiments.

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.

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.

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.

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.

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.