Semiclassical model for attosecond angular streaking.

Attosecond angular streaking is a new technique to achieve unsurpassed time accuracy of only a few attoseconds. Recently this has been successfully used to set an upper limit on the electron tunneling delay time in strong laser field ionization. The measurement technique can be modeled with either the time-dependent Schrödinger equation (TDSE) or a more simple semiclassical approach that describes the process in two steps in analogy to the three-step model in high harmonic generation (HHG): step one is the tunnel ionization and step two is the classical motion in the strong laser field. Here we describe in detail a semiclassical model which is based on the ADK theory for the tunneling step, with subsequent classical propagation of the electron in the laser field. We take into account different ellipticities of the laser field and a possible wavelength-dependent ellipticity that is typically observed for pulses in the two-optical-cycle regime. This semiclassical model shows excellent agreement with the experimental result.

Spectral signature of short attosecond pulse trains.

We report experimental measurements of high-order harmonic spectra generated in Ar using a carrier-envelope-offset (CEO) stabilized 12 fs, 800 nm laser field and a fraction (less than 10%) of its second harmonic. Additional spectral peaks are observed between the harmonic peaks, which are due to interferences between multiple pulses in the train. The position of these peaks varies with the CEO and their number is directly related to the number of pulses in the train. An analytical model, as well as numerical simulations, support our interpretation.

Attosecond ionization and tunneling delay time measurements in helium.

It is well established that electrons can escape from atoms through tunneling under the influence of strong laser fields, but the timing of the process has been controversial and far too rapid to probe in detail. We used attosecond angular streaking to place an upper limit of 34 attoseconds and an intensity-averaged upper limit of 12 attoseconds on the tunneling delay time in strong field ionization of a helium atom. The ionization field derives from 5.5-femtosecond-long near-infrared laser pulses with peak intensities ranging from 2.3 x 10(14) to 3.5 x 10(14) watts per square centimeter (corresponding to a Keldysh parameter variation from 1.45 to 1.17, associated with the onset of efficient tunneling). The technique relies on establishing an absolute reference point in the laboratory frame by elliptical polarization of the laser pulse, from which field-induced momentum shifts of the emergent electron can be assigned to a temporal delay on the basis of the known oscillation of the field vector.

Generation of intense few-cycle laser pulses through filamentation - parameter dependence.

Intense few-cycle laser pulses as short as 5.1 fs are generated though self-filamentation in a noble gas atmosphere. We study the dependence of the laser pulse fidelity on the driving pulse profile and chirp as well as on the gas parameters, quantify their pointing stability and spatial quality.

Spectrally resolved femtosecond 2-colour 3-pulse photon echoes: a new spectroscopic tool to study molecular dynamics.

We present a new multidimensional femtosecond spectroscopy technique based on spectrally resolved 2-colour 3-pulse photon echoes for investigating molecular dynamics in a variety of systems including proteins. In this technique the sample is illuminated by two femtosecond 'pump' pulses with wave vectors k1, k2 and wavelength lambda(pump) and a femtosecond 'probe' pulse with wave vector k3 and wavelength lambda(probe). Nonlinear signals are generated in the phase-matching directions k4 = - k1 + k2 + k3 and k6 = - k3 + k1 + k2. These signals are analysed in spectrometers equipped with CCD detectors and the spectra of the signals are recorded for various values of (i) the delay t12 between pulses 1 and 2, (ii) the delay t23 between pulses 2 and 3, and (iii) the wavelengths lambda(pump), lambda(probe). The technique has been used for studying vibrational and electronic dynamics of dye molecules, such as cresyl violet in methanol, and ultra-fast transient processes that occur during the photo-dissociation of carbonmonoxy myoglobin (MbCO) into myoglobin (Mb) and CO.