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Ultrafast Electron Dynamics in Phenylalanine Initiated by Attosecond Pulses
Abstract: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.One Sentence Summary: Ultrafast electron dynamics on a sub-4.5-fs temporal scale, which precedes any nuclear motion, is initiated in an amino acid by attosecond pulses.
The attosecond streak camera method is usually implemented to characterize the temporal phase and amplitude of isolated attosecond pulses produced by high-order harmonic generation. This approach, however, does not provide any information about the carrier-envelope phase of the attosecond pulses. We demonstrate that the photoelectron spectra generated by an attosecond waveform and an intense synchronized infrared field are sensitive to the electric field of the attosecond pulse. The dependence on the carrier-envelope phase of the attosecond pulse is understood in terms of the coherent superposition of two photoelectron wave packets. This effect suggests an experimentally feasible method for complete reconstruction of attosecond waveforms.
We demonstrate a simple and robust single-shot interferometric technique that allows the in situ measurement of intensity-dependent phase changes experienced by ultrashort laser pulses upon nonlinear propagation. The technique is applied to the characterization of carrier-envelope phase noise in hollow fiber compressors both in the pressure gradient and in the static cell configuration. Measurements performed simultaneously with conventional f-to-2f interferometers before and after compression indicate that the noise emerging in the waveguide adds up arithmetically to the phase noise of the amplifier, thus being strongly correlated to the phase noise of the pulses coupled into the compressor.
We have developed a novel attosecond beamline designed for attosecond-pump/attosecond probe experiments. Microfocusing of the Extreme-ultraviolet (XUV) radiation is obtained by using a coma-compensated optical configuration based on the use of three toroidal mirrors controlled by a genetic algorithm. Trains of attosecond pulses are generated with a measured peak intensity of about 3 × 10(11) W/cm(2).
The design of optical systems for micro-focusing of extreme-ultraviolet (XUV) attosecond pulses through grazing-incidence toroidal mirrors is presented. Aim of the proposed configuration is to provide a micro-focused image through a high demagnification of the XUV source with the following characteristics: i) almost negligible aberrations; ii) long exit arm to easily accommodate at the output the experimental setups required for the applications of the focused attosecond pulses; iii) possibility to have an intermediate region where the XUV beam is collimated, in order to insert a plane split-mirror for the generation of two XUV pulse replicas to be used in a XUV-pump/XUV-probe setup. We present the analytical and numerical study of two optical configurations characterized by two sections based on the use of toroidal mirrors. The first section provides a demagnified image of the source in an intermediate focus that is free from defocusing but has a large coma aberration. The second section consists of a relay mirror that is mounted in Z-shaped geometry with respect to the previous one, in order to give a stigmatic image with a coma that is opposite to that provided by the first section. An example is provided to demonstrate the capability to achieve spot sizes in the 5-15 μm range with a demagnification higher than 10 in a compact envelope.
We experimentally studied the dependence of high harmonic generation in argon and molecular hydrogen on pressure changes in a gas jet that cause variations of the phase matching conditions and absorption. The study was performed at a peak laser intensity of ∼1.5 × 10(14) W/cm(2). To enable measurements over a wide range of pressures, we employed differential pumping with an additional cell (∼20 cm(3) volume) enclosing the gas jet. By increasing the pressure in the gas jet up to a maximum of 1.5 bars with argon or 0.5 bars with hydrogen, we observed an increase in the high harmonic (HH) yield until an optimum pressure of 0.2 bars was reached for Ar, beyond which the output began decreasing. For H2, we observed an increase of the HH output up to the maximum pressure of 0.5 bars. This pressure-dependence study allowed us to achieve a tenfold enhancement in the high harmonic yield at the optimum pressure.
We investigated molecular alignment wakes of femtosecond laser pulses. Evolution of nonadiabatic molecular alignment in nitrogen gas has been measured via its nonlinear interaction effects with a variably delayed probe pulse. The induced rotational wave packet was mapped as a function of the angular difference between polarization directions of femtosecond pump and probe pulses as well as their relative delay and the plot of the variations of the rotational wave packet, i.e. "quantum carpet", was found to be in good agreement with the calculated angular and temporal dependencies of molecular alignment parameter.
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