Elliptically polarized high-harmonic radiation for production of isolated attosecond pulses.

Circularly polarized attosecond pulses are powerful tool to study chiral light-matter interaction via chiral electron dynamics. However, access to isolated circularly polarized attosecond pulses enabling straightforward interpretation of measurements, still remains a challenge. In this work, we experimentally demonstrate the generation of highly elliptically polarized high-harmonics in a two-color, bi-circular, collinear laser field.

Extended ellipticity control for attosecond pulses by high harmonic generation.

Attosecond (1  as=10  s) pulses produced through high harmonic generation (HHG) are a basis for studies of electron dynamics during light-matter interaction on an electron's natural time scale. Extensively exploited HHG technology has, however, a few unsolved problems, where producing of circularly polarized or chiral attosecond pulses belongs to them. We have demonstrated experimentally a way to control the ellipticity of attosecond pulse trains produced via HHG in two-color, bi-circular laser fields.

Few-femtosecond passage of conical intersections in the benzene cation.

Observing the crucial first few femtoseconds of photochemical reactions requires tools typically not available in the femtochemistry toolkit. Such dynamics are now within reach with the instruments provided by attosecond science. Here, we apply experimental and theoretical methods to assess the ultrafast nonadiabatic vibronic processes in a prototypical complex system-the excited benzene cation.

Time-resolved high harmonic spectroscopy of dynamical symmetry breaking in bi-circular laser fields: the role of Rydberg states.

The bi-circular scheme for high harmonic generation, which combines two counter-rotating circular fields with frequency ratio 2:1, has recently permitted to generate high harmonics with essentially circular polarization, opening the way for ultrafast chiral studies. This scheme produces harmonic lines at 3N + 1 and 3N + 2 multiples of the fundamental driving frequency, while the 3N lines are forbidden owing to the three-fold symmetry of the field. It is generally established that the routinely observed signals at these forbidden harmonic lines come from a slight ellipticity in the driving fields, which breaks the three-fold symmetry.

XUV-induced reactions in benzene on sub-10 fs timescale: nonadiabatic relaxation and proton migration.

Unraveling ultrafast dynamical processes in highly excited molecular species has an impact on our understanding of chemical processes such as combustion or the chemical composition of molecular clouds in the universe. In this article we use short (<7 fs) XUV pulses to produce excited cationic states of benzene molecules and probe their dynamics using few-cycle VIS/NIR laser pulses. The excited states produced by the XUV pulses lie in an especially complex spectral region where multi-electronic effects play a dominant role.

Communication: XUV transient absorption spectroscopy of iodomethane and iodobenzene photodissociation.

Time-resolved extreme ultraviolet (XUV) transient absorption spectroscopy of iodomethane and iodobenzene photodissociation at the iodine pre-N4,5 edge is presented, using femtosecond UV pump pulses and XUV probe pulses from high harmonic generation. For both molecules the molecular core-to-valence absorption lines fade immediately, within the pump-probe time-resolution. Absorption lines converging to the atomic iodine product emerge promptly in CH3I but are time-delayed in C6H5I.

Time-resolved excited state energetics of the solvated electron in sodium-doped water clusters.

The energetics and dynamics of the first electronically excited state of solvated electron in sodium-doped water clusters has been studied, by means of time-resolved electron spectra created in a pump-probe fs-laser experiment. The Na ··· (H2O)n clusters were excited by pulses at a wavelength of 795 nm, while ionization was achieved at a wavelength of 398 nm, and the overall cross-correlation fwhm was about 50 fs. Mass-resolved electron spectra were taken using photoelectron-photoion coincidence (PEPICO) spectroscopy for cluster sizes ranging from n = 1 up to 22.

Real-time observation of interference between atomic one-electron and two-electron excitations.

We present results of real-time tracking of atomic two-electron dynamics in an autoionizing transient wave packet in krypton. A coherent superposition of two Fano resonances is excited with a femtosecond extreme-ultraviolet pulse. The evolution of the corresponding wave packet is subsequently probed with a delayed infrared pulse.

Ultrafast photo-excitation dynamics in isolated, neutral water clusters.

Using the efficient nonlinear conversion scheme which was recently developed in our group [M. Beutler, M. Ghotbi, F.

Efficient spectral conversion and temporal compression of femtosecond pulses in SF6.

An uniquely high conversion efficiency of fundamental radiation from a Ti:sapphire laser to a supercontinuum is achieved through filamentary propagation in sulfur hexafluoride (SF6) to generate a uniform over-octave spectrum. Two different parts of the supercontinuum, firstly around the fundamental wavelength of 800 nm and secondly within the newly generated frequency range around 550 nm, are shown to be compressible down to minimal pulse duration of about 10 fs demonstrating a potential of the method for single-cycle pulses generation.

Cascaded interactions between Raman induced solitons and dispersive waves in photonic crystal fibers at the advanced stage of supercontinuum generation.

The complex mechanism of multiple interactions between solitary and dispersive waves at the advanced stage of supercontinuum generation in photonic crystal fiber is studied in experiment and numerical simulations. Injection of high power negatively chirped pulses near zero dispersion frequency results in an effective soliton fission process with multiple interactions between red shifted Raman solitons and dispersive waves. These interactions may result in relative acceleration of solitons with further collisions between them of quasi-elastic or quasi-plastic kinds.

Supercontinuum spectrum control in microstructure fibers by initial chirp management.

Experiments and numerical simulation were performed for verification of the role of femtosecond pulse chirp for supercontinuum generation in photonic crystal fiber. We demonstrate that injection of high power negatively chirped pulses near zero dispersion point brings an advantage over positively chirped pulses resulting in additional collision between solitons and in development of a significantly broader spectrum. Coupling between Raman induced solitons and dispersive waves generated by higher order dispersion was proven to be the key mechanism behind the results.

Ultrafast dynamics in Na-doped water clusters and the solvated electron.

The lifetimes of the first electronically excited state of (H(2)O)(n)...

Fragmentation and ionization dynamics of C60 in elliptically polarized femtosecond laser fields.

Ionization and fragmentation of C60 fullerenes is studied in elliptically polarized, intense fs laser fields at 797 nm [I=(0.5-4.3)x10;{14} W cm;{-2}] and contrasted with Xe+, utilizing time-of-flight mass spectrometry.

Ultrafast energy redistribution in C(60) fullerenes: a real time study by two-color femtosecond spectroscopy.

Strong-field excitation and energy redistribution dynamics of C(60) fullerenes are studied by means of time-resolved mass spectrometry in a two-color femtosecond pump-probe setup. Resonant pre-excitation of the electronic system via the first dipole-allowed HOMO-->LUMO+1(t(1g)) (HOMO denotes highest occupied molecular orbital and LUMO denotes lowest unoccupied molecular orbital) transition with ultrashort 25 fs pulses at 399 nm of some 10(12) W cm(-2) results in a highly nonequilibrium distribution of excited electrons and vibrational modes in the neutral species. The subsequent coupling among the electronic and nuclear degrees of freedom is monitored by probing the system with time-delayed 27 fs pulses at 797 nm of some 10(13) W cm(-2).

Femtosecond regenerative amplification in Cr:forsterite.

We describe an oscillator-amplifier laser system for the generation of high-power femtosecond pulses near 1.25 microm based on chromium-doped forsterite. Chirped-pulse amplification at a 1-kHz repetition rate raises the pulse energy to >350 microJ.

Powerful and tunable operation of a 1-2-kHz repetition-rate gain-switched Cr:forsterite laser and its frequency doubling.

We present a comprehensive study of the optimum operating regime in gain-switched Cr:forsterite lasers pumped at kilohertz repetition rates, comparing five crystals of similar quality but different dopant levels. The optimization of the cavity design includes selection of the proper pump fluence to account for excited-state absorption, optimum matching of the pump and laser modes, and consideration of thermal effects. As a result >1-W average output power is demonstrated at 2 kHz.

Chromium-doped forsterite laser with 1.1 W of continuous-wave output power at room temperature.

We demonstrate stable continuous-wave operation of a Cr:forsterite laser pumped by a cw Nd:YAG laser at 288 K. We use no choppers to limit the duty cycle of the cw system. The proper adjustment of the pump- and cavity-mode overlap based on the ABCD concept simulation eliminates the output power decrease at the high-level pump power.

Coherent control of bond breaking in amino acid complexes with tailored femtosecond pulses.

Intense femtosecond laser pulses, judiciously tailored in an adaptive, optimal control feedback loop were used to break preferentially the acyl-N ("peptide") bond of Ac-Phe-NHMe that may be regarded as a dipeptide model. We show that coherent excitation of complex wave packets in the strong-field regime allows to cleave strong backbone bonds in the molecular system preferentially, while keeping other more labile bonds intact. These results show the potential of pulse shaping as a powerful complementary analytical tool for protein sequencing of large biopolymers in addition to the well-known mass spectrometry and chemical analysis.

Chirped-pulse stimulated Raman scattering in barium nitrate with subsequent recompression.

We report a 30% internal conversion efficiency for the first Stokes pulse in stimulated Raman scattering of femtosecond pulses that are dispersively stretched to 250 ps, obtained by use of an all-solid-state laser system. A transfer of the linear chirp is observed, leading to a Raman pulse duration of 190 fs after recompression. Compressed pulse energies of 80 muJ at a repetition rate of 1 kHz are obtained, with a potential for an easy increase to more than 150 muJ.

Coupled ultrafast lattice and polarization dynamics in ferroelectric nanolayers.

We report the first analysis of the polarization and lattice dynamics in a metal/ferroelectric/metal nanolayer system by femtosecond x-ray diffraction. Two Bragg reflections provide information on the coupled dynamics of the two relevant phonon modes for ferroelectricity in perovskites, the tetragonal distortion and the soft mode. Optical excitation of the SrRuO(3) metal layers generates giant stress (>1 GPa) compressing the PbZr(0.

Ultrafast changes of molecular crystal structure induced by dipole solvation.

Femtosecond photoexcitation of organic chromophores in a molecular crystal induces strong changes of the electronic dipole moment via intramolecular charge transfer as is evident from transient vibrational spectra. The structural response of the crystal to the dipole change is mapped directly for the first time by ultrafast x-ray diffraction or diffuse scattering. Changes of diffracted and transmitted x-ray intensity demonstrate an angular rearrangement of molecules around excited dipoles following the 10 ps kinetics of charge transfer and leaving lattice plane spacings unchanged.

Control of giant breathing motion in c60 with temporally shaped laser pulses.

Femtosecond laser pulses tailored with closed-loop, optimal control feedback were used to excite oscillations in C60 with large amplitude by coherent heating of nuclear motion. A characteristic pulse sequence results in significant enhancement of C2 evaporation, a typical energy loss channel of vibrationally hot C60. The separation between subsequent pulses in combination with complementary two-color pump-probe data and time-dependent density functional theory calculations give direct information on the multielectron excitation via the t(1g) resonance followed by efficient coupling to the radial symmetric a(g)(1) breathing mode.

Self-compression by femtosecond pulse filamentation: experiments versus numerical simulations.

We analyze pulse self-compression in femtosecond filaments, both experimentally and numerically. We experimentally demonstrate the compression of 45 fs pulses down to a duration of 7.4 fs at millijoule pulse energies.

C60 in intense short pulse laser fields down to 9 fs: excitation on time scales below e-e and e-phonon coupling.

The interaction of C60 fullerenes with 765-797 nm laser pulses as short as 9 fs at intensities of up to 3.7 x 10(14) W cm(-2) is investigated with photoion spectroscopy. The excitation time thus addressed lies well below the characteristic time scales for electron-electron and electron-phonon couplings.