L. Poletto

Ultrafast Electron Dynamics in Phenylalanine Initiated by Attosecond Pulses

In the past 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-femtosecond 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 toward the investigation of more and more complex systems. Electronic dynamics in a complex polyatomic molecule are tracked faster than the time scale for vibrational motion. A very quick look at phenylalanine Over the past decade, laser technology has pushed back the fastest directly observable time scale from femtoseconds (quadrillionths of a second) to attoseconds (quintillionths of a second). For the most part, attosecond studies so far have probed very simple molecules such as H2 and O2. Calegari et al. now look at a more elaborate molecule—the amino acid phenylalanine. They tracked changes in the electronic structure of the compound after absorption of an ultrafast pulse, before the onset of conventional vibrational motion. Science, this issue p. 336

Cluster effects in high-order harmonics generated by ultrashort light pulses

High-order harmonic generation in argon driven by 25-fs-light pulses is investigated from the gaseous to the cluster regime. The harmonic cutoff observed in presence of clusters shows a considerable extension with respect to the gaseous phase. Harmonic spectra are investigated as a function of cluster size, showing the existence of an optimal cluster dimension, which maximizes the harmonic photon yield.

Efficient continuum generation exceeding 200 eV by intense ultrashort two-color driver

A temporal gating on the high-order harmonic emission process is achieved using an intense 20 fs, 1.45 microm pulse (IR) in combination with an intense 13 fs, 800 nm pulse [visible (VIS)]. Exploiting this two-color gating scheme, a coherent continuous emission extending up to 160 eV using Ar gas and 200 eV using Ne gas is efficiently generated. The IR pulse contributes to significantly extending the harmonic emission to higher photon energies, whereas the VIS pulse improves the conversion efficiency of the process. These results indicate the possibility to produce bright attosecond pulses approaching the soft X spectral region.

Gratings in a conical diffraction mounting for an extreme-ultraviolet time-delay-compensated monochromator

The conical diffraction mounting in which the direction of incident light belongs to a plane parallel to the direction of the grooves has the unique property of maintaining high diffraction efficiency, even in the extreme-ultraviolet (EUV) region. This property is useful for designing high-throughput time-delay-compensated monochromators for the spectral selection of ultrashort EUV pulses as the high-order harmonics generated by the interaction between an ultrashort laser pulse and a gas jet. The time compensation allows one to exploit the femtosecond scale duration of the harmonics both to have high intensity and to reach an unprecedented temporal resolution for pump and probe experiments. Because two gratings have to be used for time compensation, the high diffraction efficiency becomes an essential requirement, which can be fulfilled by the conical diffraction mounting. Measurements recently accomplished at the Bending Magnet for Emission Absorption and Reflectivity (BEAR) beam line (ELETTRA Synchrotron, Trieste, Italy) for three gratings in the 10-90 nm region are reported here that show a peak efficiency of as much as 0.7 in the first order. A model computing the electromagnetic propagation and the grating efficiency, implemented and tested with the experimental data, permits the study and design of rather complex systems operating in the conical mounting. Basic physical principles and mathematical aspects of the model are discussed here.

Instrumentation for analysis and utilization of extreme-ultraviolet and soft x-ray high-order harmonics

The design and the performances of an extreme ultraviolet (EUV)spectrometer/monochromator for generation and diagnostics of high-order harmonics of an ultrashort (<30 fs) pulsed laser focused onto a gas jet are presented. The harmonic generation is optimized using an adaptive mirror before the laser focusing stage. A toroidal mirror is used to focus the XUV radiation in an intermediate stage for pump/probe experiments. A grazing-incidence flat-field spectrometer for the 5–75 nm spectral region has been designed: it adopts a stigmatic toroidal mirror and a varied line-space flat grating mounted in converging light. The almost flat stigmatic spectrum is acquired by a 40-mm-diameter microchannel plate intensifier; the whole detector can be moved to scan various portions of the spectrum. Different detectors allow one to acquire both integrated and single shot spectra at 1 kHz repetition rate. The absolute calibration of the spectrometer is provided. The same optical scheme can be applied to the design of a co...

High harmonic generation spectroscopy of hydrocarbons

We have demonstrated the ability of few-cycle midinfrared intense laser pulses to produce extended harmonic spectra (≥45 eV) suitable for high harmonic spectroscopy in aligned hydrocarbons with ionization potentials in the range 9.07–11.52 eV. Modulations in the spectra measured with different alignment angles show signatures of the molecular structure. These results pave the way for the extension of high harmonic spectroscopy to complex biomolecules.

Spectroscopic characterization of vacuum ultraviolet free electron laser pulses

Because of the stochastic nature of self-amplified spontaneous emission (SASE), it is crucial to measure for single pulses the spectral characteristics of ultrashort pulses from the vacuum ultraviolet free electron laser (FLASH) at DESY, Germany. To meet this particular challenge, we have employed both photon and photoelectron spectroscopy. Each FEL pulse is composed of an intense and spectrally complex fundamental, centered at a photon energy of about 38.5 eV, with a bandwidth of 0.5% accompanied by higher harmonics, each carrying an intensity of typically 0.3 to 0.6% of that of the fundamental. The correlation between the harmonics and the fundamental is in remarkable agreement with a simple statistical model of SASE FEL radiation.

Wave front active control by a digital-signal-processor-driven deformable membrane mirror

The correction of the beam wave front degradations, introduced by optical aberrations or by medium inhomogeneities, has a widespread relevance in several areas of optics. We describe here an adaptive optics system aimed to the optical optimization of the beam wave front in few seconds using an electrostatic deformable mirror and a controller based on a fixed-point digital signal processor. The correction system acts the wave front modification by a deformable mirror in closed loop with a genetic algorithm. We also studied the dynamics of the mirror for its use in beam wander correction due to atmospheric turbulence in free space classical and quantum optical communications.

CITIUS: an infrared-extreme ultraviolet light source for fundamental and applied ultrafast science.

We present the main features of CITIUS, a new light source for ultrafast science, generating tunable, intense, femtosecond pulses in the spectral range from infrared to extreme ultraviolet (XUV). The XUV pulses (about 10(5)-10(8) photons/pulse in the range 14-80 eV) are produced by laser-induced high-order harmonic generation in gas. This radiation is monochromatized by a time-preserving monochromator, also allowing one to work with high-resolution bandwidth selection. The tunable IR-UV pulses (10(12)-10(15) photons/pulse in the range 0.4-5.6 eV) are generated by an optical parametric amplifier, which is driven by a fraction of the same laser pulse that generates high order harmonics. The IR-UV and XUV pulses follow different optical paths and are eventually recombined on the sample for pump-probe experiments. We also present the results of two pump-probe experiments: with the first one, we fully characterized the temporal duration of harmonic pulses in the time-preserving configuration; with the second one, we demonstrated the possibility of using CITIUS for selective investigation of the ultra-fast dynamics of different elements in a magnetic compound.

Elemental sensitivity in soft x-ray imaging with a laser-plasma source and a color center detector

Elemental sensitivity in soft x-ray imaging of thin foils with known thickness is observed using an ultrafast laser-plasma source and a LiF crystal as detector. Measurements are well reproduced by a simple theoretical model. This technique can be exploited for high spatial resolution, wide field of view imaging in the soft x-ray region, and it is suitable for the characterization of thin objects with thicknesses ranging from hundreds down to tens of nanometers.