No Arabic abstract
Self-action nonlinearity is a key aspect -- either as a foundational element or a detrimental factor -- of several optical spectroscopies and photonic devices. Supercontinuum generation, wavelength converters and chirped pulse amplification are just a few examples. The recent advent of Free Electron Lasers (FEL) fostered building on nonlinearity to propose new concepts and extend optical wavelengths paradigms for extreme ultraviolet (EUV) and X-ray regimes. No evidence for intrapulse dynamics, however, has been reported at such short wavelengths, where the light-matter interactions are ruled by the sharp absorption edges of core-electrons. Here, we provide experimental evidence for self-phase modulation of femtosecond FEL pulses, which we exploit for fine self-driven spectral tunability by interaction with sub-micrometric foils of selected monoatomic materials. Moving the pulse wavelength across the absorption edge, the spectral profile changes from a non-linear spectral blue-shift to a red-shifted broadening. These findings are rationalized accounting for ultrafast ionization and delayed thermal response of highly excited electrons above and below threshold, respectively.
We demonstrate experimentally the full tunability of a coherent femtosecond source in the whole ultraviolet spectral region. The experiment relies on the technique of high-order harmonic generation driven by a near-infrared parametric laser source in krypton gas. By tuning the drive wavelength in the range between 1100 to 1900 nm, we generated intense harmonics from near to extreme ultraviolet. A number of photons per shot of the order of 10^7 has been measured for the first harmonic orders. Many novel scientific prospects are expected to benefit from the use of such a table-top tunable source.
We utilize coherent femtosecond extreme ultraviolet (EUV) pulses derived from a free electron laser (FEL) to generate transient periodic magnetization patterns with periods as short as 44 nm. Combining spatially periodic excitation with resonant probing at the dichroic M-edge of cobalt allows us to create and probe transient gratings of electronic and magnetic excitations in a CoGd alloy. In a demagnetized sample, we observe an electronic excitation with 50 fs rise time close to the FEL pulse duration and ~0.5 ps decay time within the range for the electron-phonon relaxation in metals. When the experiment is performed on a sample magnetized to saturation in an external field, we observe a magnetization grating, which appears on a sub-picosecond time scale as the sample is demagnetized at the maxima of the EUV intensity and then decays on the time scale of tens of picoseconds via thermal diffusion. The described approach opens prospects for studying dynamics of ultrafast magnetic phenomena on nanometer length scales.
We use caustic beam shaping on 100 fs pulses to experimentally generate non-paraxial accelerating beams along a 60 degree circular arc, moving laterally by 14 mum over a 28 mum propagation length. This is the highest degree of transverse acceleration reported to our knowledge. Using diffraction integral theory and numerical beam propagation simulations, we show that circular acceleration trajectories represent a unique class of non-paraxial diffraction-free beam profile which also preserves the femtosecond temporal structure in the vicinity of the caustic.
We exploit inverse Raman scattering and solvated electron absorption to perform a quantitative characterization of the energy loss and ionization dynamics in water with tightly focused near-infrared femtosecond pulses. A comparison between experimental data and numerical simulations suggests that the ionization energy of water is 8 eV, rather than the commonly used value of 6.5 eV. We also introduce an equation for the Raman gain valid for ultra-short pulses that validates our experimental procedure.
We present an analysis of two experimental approaches to controlling the directionality of molecular rotation with ultrashort laser pulses. The two methods are based on the molecular interaction with either a pair of pulses (a double kick scheme) or a longer pulse sequence (a chiral pulse train scheme). In both cases, rotational control is achieved by varying the polarization of and the time delay between the consecutive laser pulses. Using the technique of polarization sensitive resonance-enhanced multi-photon ionization, we show that both methods produce significant rotational directionality. We demonstrate that increasing the number of excitation pulses supplements the ability to control the sense of molecular rotation with quantum state selectivity, i.e. predominant excitation of a single rotational state. We also demonstrate the ability of both techniques to generate counter-rotation of molecular nuclear spin isomers (here, ortho- and para-nitrogen) and molecular isotopologues (here, 14N_2 and 15N_2).