Generation and control of ultrafast pulse trains for quasi-phase-matching high-harmonic generation

Two techniques are demonstrated to produce ultrashort pulse trains capable of quasi-phase-matching high-harmonic generation. The first technique makes use of an array of birefringent crystals and is shown to generate high-contrast pulse trains with constant pulse spacing. The second technique employs a grating-pair stretcher, a multiple-order wave plate, and a linear polarizer. Trains of up to 100 pulses are demonstrated with this technique, with almost constant inter-pulse separation. It is shown that arbitrary pulse separation can be achieved by introducing the appropriate dispersion. This principle is demonstrated by using an acousto-optic programmable dispersive filter to introduce third-and fourth-order dispersions leading to a linear and quadratic variation of the separation of pulses through the train. Chirped-pulse trains of this type may be used to quasi-phase-match high-harmonic generation in situations where the coherence length varies through the medium. (C) 2010 Optical Society of America

Weibel-induced filamentation during an ultrafast, laser-driven plasma expansion

The development of current instabilities behind the front of a cylindrically expanding plasma has been investigated experimentally via proton probing techniques. A multitude of tubelike filamentary structures is observed to form behind the front of a plasma created by irradiating solid-density wire targets with a high-intensity (I~1019??W/cm2), picosecond-duration laser pulse. These filaments exhibit a remarkable degree of stability, persisting for several tens of picoseconds, and appear to be magnetized over a filament length corresponding to several filament radii. Particle-in-cell simulations indicate that their formation can be attributed to a Weibel instability driven by a thermal anisotropy of the electron population. We suggest that these results may have implications in astrophysical scenarios, particularly concerning the problem of the generation of strong, spatially extended and sustained magnetic fields in astrophysical jets.

LIAD-fs scheme for studies of ultrafast laser interactions with gas phase biomolecules

Laser induced acoustic desorption (LIAD) has been used for the first time to study the parent ion production and fragmentation mechanisms of a biological molecule in an intense femtosecond (fs) laser field. The photoacoustic shock wave generated in the analyte substrate (thin Ta foil) has been simulated using the hydrodynamic HYADES code, and the full LIAD process has been experimentally characterised as a function of the desorption UV-laser pulse parameters. Observed neutral plumes of densities > 10(9) cm(-3) which are free from solvent or matrix contamination demonstrate the suitability and potential of the source for studying ultrafast dynamics in the gas phase using fs laser pulses. Results obtained with phenylalanine show that through manipulation of fundamental femtosecond laser parameters (such as pulse length, intensity and wavelength), energy deposition within the molecule can be controlled to allow enhancement of parent ion production or generation of characteristic fragmentation patterns. In particular by reducing the pulse length to a timescale equivalent to the fastest vibrational periods in the molecule, we demonstrate how fragmentation of the molecule can be minimised whilst maintaining a high ionisation efficiency.

Ultrafast low-loss 42-70 GHz differential SPDT switch in 0.35 μm SiGe technology

This paper presents an ultrafast wideband low-loss single-pole double-throw (SPDT) differential switch in 0.35 µ m SiGe bipolar technology. The proposed topology adopting current-steering technique results in a total measured switching time of 75 ps , which suggests a maximum switching rate of 13 Gb/s, the fastest ever reported at V-band. In addition, the switch exhibits an insertion loss lower than 1.25 dB and an isolation higher than 18 dB from 42 GHz to 70 GHz. © 2006 IEEE.

Ultrafast nonlinearities of minibands in metallodielectric Bragg resonators

The nonlinear properties of metallodielectric DBRs are investigated via optical pump-probe techniques using a widely tunable, dual-colour, high-repetition rate, ultrafast setup. As a consequence of the Bragg-arranged multilayers, the electric field penetrates to different depths of the nanostructure at different excitation resonances, strongly enhancing the intrinsic nonlinear response of the metal in comparison with bulk films. The analyzed spectral response of these structures reveals how their nonlinear behavior is dominated by the pump-induced modification of the metal dielectric function. Fitting the simulated changes of the optical resonances using transfer-matrix methods matches experiment well, and shows the key effects of the spectral dependence of the spatial mode profiles.

Observation of Ultrafast Charge Migration in an Amino Acid

We present the first direct measurement of ultrafast charge migration in a biomolecular building block the amino acid phenylalanine. Using an extreme ultraviolet pulse of 1.5 fs duration to ionize molecules isolated in the gas phase, the location of the resulting hole was probed by a 6 fs visible/near-infrared pulse. By measuring the yield of a doubly charged ion as a function of the delay between the two pulses, the positive hole was observed to migrate to one end of the cation within 30 fs. This process is likely to originate from even faster coherent charge oscillations in the molecule being dephased by bond stretching which eventually localizes the final position of the charge. This demonstration offers a clear template for observing and controlling this phenomenon in the future.

Longitudinal proton probing of ultrafast and high-contrast laser-solid interactions

We have performed an experiment aimed at measuring self-generated magnetic fields produced in solids by high electron currents following high-intensity and high contrast short-pulse laser irradiation. This was done using longitudinal high resolution proton deflectometry. The experiment was performed at the Titan-JLF laser facility with a high-power short-pulse beam (700 fs, ~ 110 J) split into two beams irradiating two solid targets. One beam is used for the generation of protons and the other beam for the generation of the ultra-high currents of electrons and of the associated magnetic fields. This capability allows us to study the spatio-temporal evolution of the magnetic fields and its dependence on the laser intensity and target material. © Owned by the authors, published by EDP Sciences, 2013.

Pressure effect on vibrational frequency and dephasing of 1-alkyl-3-methylimidazolium hexafluorophosphate ionic liquids

Raman spectra in the range of the totally symmetric stretching mode of the [PF6]− anion, νs(PF6), have been measured for 1-alkyl-3-methylimidazolium ionic liquids [CnC1im][PF6], for n = 4, 6, and 8, as a function of pressure at room temperature. The ionic liquids [C6C1im][PF6] and [C8C1im][PF6] remain in an amorphous phase up to 3.5 GPa, in contrast to [C4C1im][PF6], whichcrystallizes above ∼0.5 GPa. Equations of state based either on a group contribution model or Carnahan-Starling-van der Waals model have been used to estimate the densities of the ionic liquids at high pressures. The shifts of the vibrational frequency of νs(PF6) with density observed in [C6C1im][PF6] and in [C8C1im][PF6] have been calculated by a hard-sphere model of a pseudo-diatomic solute under short-range repulsive interactions with the neighboring particles. The stochastic model of Kubo for vibrational dephasing has been used to obtain the amplitude of vibrational frequency fluctuation, ⟨Δω 2⟩, and the relaxation time of frequency fluctuation, τ c , as a function of density by Raman band shape analysis of the νs(PF6) mode of [C6C1im][PF6] and [C8C1im][PF6].

Population trapping in bound states during IR-assisted ultrafast photoionization of Ne+

We have investigated the photoionization of Ne+ in the combined field of a short infrared laser pulse and a delayed ultrashort pulse of the infrared laser's 23rd harmonic. We observe an ionization yield compatible with a picture in which one electron gets excited into Rydberg states by the harmonic laser field and is subsequently removed by the infrared laser field. Modulations are seen in the ionization yield as a function of time delay. These modulations originate from the trapping of population in low members of the Rydberg series with different states being populated at different ranges of delay times. The calculations further demonstrate that single-threshold calculations cannot reproduce the Ne+ photoionization yields obtained in multithreshold calculations.

Ultrafast Electron Dynamics in Phenylalanine Initiated by Attosecond Pulses

In the last decade attosecond technology has opened up the investigation of ultrafast electronic processes in atoms, simple molecules and solids. Here we report the application of isolated attosecond pulses to prompt ionization of the amino acid phenylalanine, and the subsequent detection of ultrafast dynamics on a sub-4.5-fs temporal scale, which is shorter than the vibrational response of the molecule. The ability to initiate and observe such electronic dynamics in polyatomic molecules represents a crucial step forward in attosecond science, which is progressively moving towards the investigation of more and more complex systems.

Ultrafast charge dynamics in an amino acid induced by attosecond pulses

In the past few years, attosecond techniques have been implemented for the investigation of ultrafast dynamics in molecules. The generation of isolated attosecond pulses characterized by a relatively high photon flux has opened up new possibilities in the study of molecular dynamics. In this paper, we report on experimental and theoretical results of ultrafast charge dynamics in a biochemically relevant molecule, namely, the amino acid phenylalanine. The data represent the first experimental demonstration of the generation and observation of a charge migration process in a complexmolecule, where electron dynamics precede nuclear motion. The application of attosecond technology to the investigation of electron dynamics in biologically relevant molecules represents a multidisciplinary work, which can open new research frontiers: those in which few-femtosecond and even subfemtosecond electron processes determine the fate of biomolecules. It can also open new perspectives for the development of new technologies, for example, in molecular electronics, where electron processes on an ultrafast temporal scale are essential to trigger and control the electron current on the scale of the molecule.

Ultrafast Non-Radiative Decay of Gas-Phase Nucleosides

The ultrafast photo-physical properties of DNA are crucial in providing a stable basis for life. Although the DNA bases efficiently absorb ultraviolet (UV) radiation, this energy can be dissipated to the surrounding environment by the rapid conversion of electronic energy to vibrational energy within about a picosecond. The intrinsic nature of this internal conversion process has previously been demonstrated through gas phase experiments on the bases, supported by theoretical calculations. De-excitation rates appear to be accelerated when individual bases are hydrogen bonded to solvent molecules or their complementary Watson-Crick pair. In this paper, the first gas-phase measurements of electronic relaxation in DNA nucleosides following UV excitation are reported. Using a pump-probe ionization scheme, the lifetimes for internal conversion to the ground state following excitation at 267 nm are found to be reduced by around a factor of two for adenosine, cytidine and thymidine compared with the isolated bases. These results are discussed in terms of a recent proposition that a charge transfer state provides an additional internal conversion pathway mediated by proton transfer through a sugar to base hydrogen bond.

LIAD-fs: A novel method for studies of ultrafast processes in gas phase neutral biomolecules

A new experimental technique for femtosecond (fs) pulse studies of gas phase biomolecules is reported. Using Laser-Induced Acoustic Desorption (LIAD) to produce a plume of neutral molecules, a time-delayed fs pulse is employed for ionisation/fragmentation, with subsequent products extracted and mass analysed electrostatically. By varying critical laser pulse parameters, this technique can be used to implement control over molecular fragmentation for a range of small biomolecules, with specific studies of amino acids demonstrated.

Ultrafast charge dynamics initiated by high-intensity, ultrashort laser-matter interaction

The interaction of high‐intensity laser pulses with matter releases instantaneously ultra‐large currents of highly energetic electrons, leading to the generation of highly‐transient, large‐amplitude electric and magnetic fields. We report results of recent experiment in which such charge dynamics have been studied by using proton probing techniques able to provide maps of the electrostatic fields with high spatial and temporal resolution. The dynamics of ponderomotive channelling in underdense plasmas have been studied in this way, as also the processes of Debye sheath formation and MeV ion front expansion at the rear of laser‐irradiated thin metallic foils. An application employing laser‐driven impulsive fields for energy‐selective ion beam focusing is also presented.

Investigations of ultrafast charge dynamics in laser-irradiated targets by a self probing technique employing laser driven protons

The divergent and broadband proton beams produced by the target normal sheath acceleration mechanism provide the unique opportunity to probe, in a point-projection imaging scheme, the dynamics of the transient electric and magnetic fields produced during laser-plasma interactions. Commonly such experimental setup entails two intense laser beams, where the interaction produced by one beam is probed with the protons produced by the second. We present here experimental studies of the ultra-fast charge dynamics along a wire connected to laser irradiated target carried out by employing a ‘self’ proton probing arrangement – i.e. by connecting the wire to the target generating the probe protons. The experimental data shows that an electromagnetic pulse carrying a significant amount of charge is launched along the wire, which travels as a unified pulse of 10s of ps duration with a velocity close to speed of light. The experimental capabilities and the analysis procedure of this specific type of proton probing technique are discussed.