A ttosecond electron wavepackets are produced when an intense laser field ionizes an atom or a molecule 1 . When the laser field drives the wavepackets back to the parent ion, they interfere with the bound wavefunction, producing coherent subfemtosecond extreme-ultraviolet light bursts. When only a single return is possible 2,3 , an isolated attosecond pulse is generated. Here we demonstrate that by modulating the polarization of a carrier-envelope phase-stabilized short laser pulse 4 , we can finely control the electron-wavepacket dynamics. We use high-order harmonic generation to probe these dynamics. Under optimized conditions, we observe the signature of a single return of the electron wavepacket over a large range of energies. This temporally confines the extreme-ultraviolet emission to an isolated attosecond pulse with a broad and tunable bandwidth. Our approach is very general, and extends the bandwidth of attosecond isolated pulses in such a way that pulses of a few attoseconds seem achievable. Similar temporal resolution could also be achieved by directly using the broadband electron wavepacket. This opens up a new regime for timeresolved tomography of atomic or molecular wavefunctions 5,6 and ultrafast dynamics.During high-order harmonic generation (HHG) in gas 7 , short electron wavepackets (EWPs) are periodically released by high-field ionization. Their subsequent coherent interaction with the remaining bound wavefunction leads to coherent extremeultraviolet (XUV) emission. The T 0 /2 periodicity of this process (T 0 being the laser optical period) ensures that only odd harmonics of the fundamental radiation are emitted. Temporally, the XUV pulses are emitted as a train of chirped attosecond pulses [8][9][10] (1 attosecond = 10 −18 s). For both plateau (low energy) and cut-off (high energy) harmonics, specific focusing conditions ensure that only a single attosecond pulse is emitted every half cycle 11,12 . Extracting an isolated attosecond pulse from this train requires breaking the periodicity of the process, so that XUV emission is only possible within a single half cycle of the fundamental pulse. In this way, isolated 250-attosecond-long Figure 1 Spectra generated in argon. Spectra emitted from an argon medium irradiated with a polarization-modulated pulse (τ = 5 fs, δ = 6.2 fs, β = 0 • ) as a function of the CEP shift. For some CEPs, harmonic peaks appear, whereas for other CEPs, they broaden up to a continuum.pulses were recently obtained 13 by selecting the (highly intensity dependent) cut-off harmonics generated in neon by a 5-fs linearly polarized, fundamental pulse with stabilized carrierenvelope phase (CEP). With this technique, the minimum pulse duration achievable is limited by the (∼10 eV) bandwidth of the selected cut-off harmonics, which prevents us reaching the sub-100-attosecond domain.To isolate a broadband attosecond pulse, we used a different approach 2 . Our approach relies on the strong HHG sensitivity on the ellipticity, ε, of the fundamental field, which is largely nature phy...

We suggest a high-order harmonic generation (HHG) model describing enhancement of the generation efficiency for the harmonic resonant with the transition between the ground and autoionizing state of the generating ion. The results of numerical and analytical calculations based on this model are in good quantitative agreement with the experiments showing HHG enhancement up to 2 orders of magnitude. Moreover, this model reproduces well the essential difference in HHG efficiency for different ions. We show that intense but relatively long attosecond pulses can be generated using the enhanced harmonics.

Abstract. 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 neighboring 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.

By experimentally studying high-order harmonic beams generated in gases, we show how the spatial characteristics of these ultrashort extreme-ultraviolet (XUV) beams can be finely controlled when a single fundamental beam generates harmonics in a thin gas medium. We demonstrate that these XUV beams can be emitted as converging beams and thereby get focused after generation. We study this optics-less focusing using a spatially chirped beam that acts as a probe located inside the harmonic generation medium. We analyze the XUV beam evolution with an analytical model and obtain very good agreement with experimental measurements. The XUV foci sizes and positions vary strongly with the harmonic order, and the XUV waist can be located at arbitrarily large distances from the generating medium. We discuss how intense XUV fields can be obtained with optics-less focusing and how the order-dependent XUV beam characteristics are compatible with broadband XUV irradiation and attosecond science.

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We investigate numerically and analytically the polarization properties of high-order harmonics generated by an atom in intense elliptically polarized laser field. The offset angle of the harmonic polarization ellipse can be well described with the semiclassic "simple-man" high-harmonic generation model. The harmonic ellipticity itself, however, can be hardly understood within this model. We show that this ellipticity originates from quantum-mechanical uncertainty of the electron motion. We develop a theoretical approach describing this ellipticity and, more generally, the time evolution of the high-harmonic polarization state within the laser cycle. The analytical results are verified with the exact numerical solution; to make the comparison accurately, we develop a specific technique for separating the contributions of quantum paths in the numerical calculation.

We study high-order harmonic generation from a laser-produced tin plasma using 780 and 390 nm, 40 fs, 1 kHz pulses. Varying the chirp of the laser radiation, we observe variation of the harmonic frequency and intensity. The enhanced 16th and 17th harmonics are attributed to the influence of the strong ionic transitions of tin. Theoretical calculations of the photoabsorption spectra reveal the decisive role of Sn II and Sn III transitions in the enhancement of single harmonics. Varying the fundamental frequency we study numerically the spectral width where the harmonic is enhanced. We find, both theoretically and experimentally, that this width is wider than the one of the corresponding resonance in the photoabsorption spectrum. The resonance line modification can be explained by the Stark shift of the autoionizing state in the laser field, as well as the photoionization of this state.

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