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Ultrafast processes in matter can be captured and even controlled by using sequences of few-cycle optical pulses, which need to be well characterized, both in amplitude and phase. The same degree of control has not yet been achieved for few-cycle extreme ultraviolet pulses generated by high-order harmonic generation in gases, with duration in the attosecond range. Here, we show that by varying the spectral phase and carrier-envelope phase (CEP) of a high-repetition rate laser, using dispersion in glass, we achieve a high degree of control of the relative phase and CEP between consecutive attosecond pulses. The experimental results are supported by a detailed theoretical analysis based upon the semiclassical three-step model for high-order harmonic generation.
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We study the photoionization of argon atoms close to the 3s$^2$3p$^6$ $rightarrow$ 3s$^1$3p$^6$4p $leftrightarrow$ 3s$^2$3p$^5$ $varepsilon ell$, $ell$=s,d Fano window resonance. An interferometric technique using an attosecond pulse train, i.e. a frequency comb in the extreme ultraviolet range, and a weak infrared probe field allows us to study both amplitude and phase of the photoionization probability amplitude as a function of photon energy. A theoretical calculation of the ionization process accounting for several continuum channels and bandwidth effects reproduces well the experimental observations and shows that the phase variation of the resonant two-photon amplitude depends on the interaction between the channels involved in the autoionization process.
We study the higher-harmonic generation (HHG) using elliptically polarized two-color driving fields. The HHG via bi-chromatic counter-rotating laser fields is a promising source of circularly polarized ultrashort XUV radiation at the attosecond time scale. The ellipticity or the polarization of the attosecond pulses can be tweaked by modifying the emitted harmonics ellipticity, which can be controlled by varying the driver fields. We propose a simple setup to control the polarization of the driving fields, which eventually changes the ellipticity of the attosecond pulses. A well-defined scaling law for the ellipticity of the attosecond pulse as a function of the rotation angle of the quarter-wave plate is also deduced by solving the time-dependent Schrodinger equation (TDSE) in two dimensions. The scaling law can further be explored to obtain the attosecond pulses of the desired degree of polarization, ranging from linear to elliptical to circular polarization.
The recent development of ultrafast extreme ultraviolet (XUV) coherent light sources bears great potential for a better understanding of the structure and dynamics of matter. Promising routes are advanced coherent control and nonlinear spectroscopy schemes in the XUV energy range, yielding unprecedented spatial and temporal resolution. However, their implementation has been hampered by the experimental challenge of generating XUV pulse sequences with precisely controlled timing and phase properties. In particular, direct control and manipulation of the phase of individual pulses within a XUV pulse sequence opens exciting possibilities for coherent control and multidimensional spectroscopy, but has not been accomplished. Here, we overcome these constraints in a highly time-stabilized and phase-modulated XUV-pump, XUV-probe experiment, which directly probes the evolution and dephasing of an inner subshell electronic coherence. This approach, avoiding any XUV optics for direct pulse manipulation, opens up extensive applications of advanced nonlinear optics and spectroscopy at XUV wavelengths.
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 neighbouring 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.
Trains of ultrashort laser pulses separated by the time of rotational revival (typically, tens of picoseconds) have been exploited for creating ensembles of aligned molecules. In this work we introduce a chiral pulse train - a sequence of linearly polarized pulses with the polarization direction rotating from pulse to pulse by a controllable angle. The chirality of such a train, expressed through the period and direction of its polarization rotation, is used as a new control parameter for achieving selectivity and directionality of laser-induced rotational excitation. The method employs chiral trains with a large number of pulses separated on the time scale much shorter than the rotational revival (a few hundred femtosecond), enabling the use of conventional pulse shapers.
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