Willem Boutu

Isolated attosecond pulses using a detuned second-harmonic field.

Calculations are presented for the generation of an isolated attosecond pulse in a multicycle two-color strong-field regime. We show that the recollision of the electron wave packet can be confined to half an optical cycle using pulses of up to 40 fs in duration. The scheme is proven to be efficient using two intense beams, one producing a strong field at omega and the other a strong field detuned from 2omega. The slight detuning deltaomega of the second harmonic is used to break the symmetry of the electric field over many optical cycles and provides a coherent control for the formation of an isolated attosecond pulse.

Polarization-resolved pump-probe spectroscopy with high harmonics

High harmonic generation in gases can be used as a probe of the electronic structure of the emitting medium, with attosecond temporal resolution and angstrom spatial resolution. The prospect of measuring molecular dynamics by pump-probe spectroscopy with such precision is attracting a lot of interest. An important issue in pump-probe spectroscopy lies in the ability to detect small signals: the detected signal can be easily dominated by the contributions from non-excited molecules or from a carrier gas. In this paper, we demonstrate that polarization-resolved pump-probe spectroscopy can be used to overcome this issue. We study high harmonic generation from rotationally excited molecules. We show that by measuring the harmonic field that is generated orthogonally to the driving laser field, the contrast in the detection of alignment revivals in nitrogen can be increased by a factor 4. We use this configuration to measure alignment revivals in an argon-nitrogen mixture, in which the total harmonic signal is dominated by the contributions from argon.

Attosecond chirp-encoded dynamics of light nuclei

We study the spectral phase of high-order harmonic emission as an observable for probing ultrafast nuclear dynamics after the ionization of a molecule. Using a strong-field approximation theory that includes nuclear dynamics, we relate the harmonic phase to the phase of the overlap integral of the nuclear wavefunctions of the initial neutral molecule and the molecular ion after an attosecond probe delay. We determine experimentally the group delay of the high harmonic emission from D2 and H2 molecules, which allows us to verify the relation between harmonic frequency and the attosecond delay. The small difference in the harmonic phase between H2 and D2 calculated theoretically is consistent with our experimental results.

Impact of wave front and coherence optimization in coherent diffractive imaging

We present single shot nanoscale imaging using a table-top femtosecond soft X-ray laser harmonic source at a wavelength of 32 nm. We show that the phase retrieval process in coherent diffractive imaging critically depends on beam quality. Coherence and image fidelity are measured from single-shot coherent diffraction patterns of isolated nano-patterned slits. Impact of flux, wave front and coherence of the soft X-ray beam on the phase retrieval process and the image quality are discussed. After beam improvements, a final image reconstruction is presented with a spatial resolution of 78 nm (half period) in a single 20 fs laser harmonic shot.

Measurement and optimization of isolated attosecond pulse contrast

An experimental method is presented to experimentally measure and control the carrier-envelope-phase (CEP)-dependent pulse-energy contrast of isolated attosecond pulses. By scanning the CEP and measuring the photoelectron spectrum produced by the combined action of the attosecond pulses and the high-harmonic driving laser pulses at zero relative time delay, one can extract the pulse-energy ratio between the main attosecond pulse and its neighboring satellite pulses arriving in preceding or subsequent half-cycles of the driver pulse. Moreover, this method allows fast and efficient in situ retrieval of the optimal CEP for high-contrast isolated attosecond pulse generation.

High-order-harmonic generation in gas with a flat-top laser beam

We present experimental and numerical results on high-order-harmonic generation with a flat-top laser beam. We show that a simple binary tunable phase plate, made of two concentric glass plates, can produce a flat-top profile at the focus of a Gaussian infrared beam. Both experiments and numerical calculations show that there is a scaling law between the harmonic generation efficiency and the increase of the generation volume.

Fourier transform holography with high harmonic spectra for attosecond imaging applications

We demonstrate a method of using a Fourier holographic technique to utilize attosecond soft x-ray pulses to image nanometer-scale objects. A discrete frequency comb of laser-generated high-order harmonics, yielding a train of attosecond pulses, has been used to record spatially and spectrally resolved images. The individual wavelengths were also combined to form a single image, albeit with lower spatial resolution, demonstrating the applicability of the method to using isolated attosecond pulses with continuous bandwidths.

Scaling of the generation of high-order harmonics in large gas media with focal length

We present theoretical and experimental results on high-order harmonic generation in a low-density few-centimeter-long gas medium (L{sub med}{<=} 10 cm). We study the dependence with focal length of harmonic efficiency. Theoretically, we consider in detail the generation of the 25th harmonic of a short pulse Ti:sapphire laser in argon. Within the strong-field approximation for the atomic dipole, and a complete account of the macroscopic propagation, we compute the number of photons produced as a function of the medium parameters and the focusing conditions. The simulations show that, at constant intensity, the emission of the 25th harmonic scales with the focal length as {approx}f{sup 4} at low pressure (P=2 Torr) and as {approx}f{sup 6} at higher pressure (P=5 Torr). At constant laser energy, we find that the harmonic signal scales approximately as f{sup 2} at low pressure and as f{sup 4} at higher pressure. Those numerical results are compared with experimental data.

Frequency conversion of subnanojoule femtosecond pulses in microstructure fibers

We experimentally demonstrate highly efficient multiplex frequency conversion of unamplified subnanojoule femtosecond pulses of Ti:sapphire laser radiation in fused silica microstructure fibers. Nonlinear optical spectral transformation of femtosecond pulses in an array of fused silica threadlike channels in these microstructure fibers results in the generation of isolated anti-Stokes spectral components within the wavelength range of 400–500 nm. An efficiency of frequency conversion of about 20% is achieved for 800-nm pump pulses with an energy of 0.7 nJ and a pulse duration of 70 fs.

Shot-to-shot intensity and wavefront stability of high-harmonic generation

We report on the shot-to-shot stability of intensity and spatial phase of high-harmonic generation (HHG). The intensity stability is measured for each high-harmonic (HH) order with a spectrometer. Additionally, the spatial phase is measured with an XUV wavefront sensor for a single HH order measured in a single shot, which according to our knowledge was not reported before with a Hartmann wavefront sensor. Furthermore, we compare the single-shot measurement of the spatial phase with time-integrated measurements and we show that the XUV wavefront sensor is a useful tool to simultaneously optimize the spatial phase and intensity of HHG within the available HHG parameter range used in this study.