Multiphoton absorption in CsLiB6O10 with femtosecond infrared laser pulses

Nonlinear absorption and refraction characteristics of cesium lithium borate (CsLiB6O10) crystal have been studied using Z-scan technique. Ti:sapphire laser with 110 fs pulse width operating at 800 nm wavelength and pulse repetition rate of 1 kHz is used as the source of photons. Intensity of the laser pulse is varied from 0.541 to 1.283 T W/cm2 to estimate the intensity dependence of multiphoton absorption coefficients. Using the theory of multiphoton absorption proposed by Sutherland [ Handbook of Nonlinear Optics, in 2nd ed., edited by D. G. McLean and S. Kirkpatrick, Dekker, New York (2003) ], found that open aperture Z-scan data fit well for the five-photon absorption (5PA) process. 5PA coefficients are obtained by fitting the expressions into the open aperture experimental data for various peak intensities (I00). The nonlinear refractive index n2 estimated from closed aperture Z-scan experiment is 1.075×10−4 cm2/T W at an input peak intensity of 0.723 T W/cm2. The above experiment when repeated with a 532 nm, 6 ns pulsed laser led to an irreversible damage of the sample resulting in an asymmetric open aperture Z-scan profile. This indicates that it is not possible to observe multiphoton absorption in this regime of pulse width using 532 nm laser.

Single-shot characterisation of independent femtosecond extreme ultraviolet free electron andf infrared laser pulses

Two-color above threshold ionization of helium and xenon has been used to analyze the synchronization between individual pulses of the femtosecond extreme ultraviolet (XUV) free electron laser in Hamburg and an independent intense 120 fs mode-locked Ti:sapphire laser. Characteristic sidebands appear in the photoelectron spectra when the two pulses overlap spatially and temporally. The cross-correlation curve points to a 250 fs rms jitter between the two sources at the experiment. A more precise determination of the temporal fluctuation between the XUV and infrared pulses is obtained through the analysis of the single-shot sideband intensities. ©2007 American Institute of Physics

Controlling dissociation processes in the D-2(+) molecular ion using high-intensity, ultrashort laser pulses

A novel technique is proposed to control the dissociation mechanism of small diatomic molecules. This technique, relying upon the creation of a coherent nuclear wavepacket, uses intense (> 10(14) W cm(-2)), ultrashort (similar to 10 fs) infrared laser pulses in a pump and probe scheme. In applying this technique to D-2(+) good agreement has been observed between a quantum simulation and experiment. This represents a major step towards quantum state control in molecules, using optical fields.

Quasi-classical model of non-destructive wavepacket manipulation by intense ultrashort nonresonant laser pulses

A quasi-classical model (QCM) of nuclear wavepacket generation, modification and imaging by three intense ultrafast near-infrared laser pulses has been developed. Intensities in excess of 10(13) W cm(-2) are studied, the laser radiation is non-resonant and pulse durations are in the few-cycle regime, hence significantly removed from the conditions typical of coherent control and femtochemistry. The 1s sigma ground state of the D-2 precursor is projected onto the available electronic states in D-2(+) (1s sigma(g) ground and 2p sigma(u) dissociative) and D+ + D+ (Coulomb explosion) by tunnel ionization by an ultrashort 'pump' pulse, and relative populations are found numerically. A generalized non-adiabatic treatment allows the dependence of the initial vibrational population distribution on laser intensity to be calculated. The wavepacket is approximated as a classical ensemble of particles moving on the 1s sigma(g) potential energy surface (PES), and hence follow trajectories of different amplitudes and frequencies depending on the initial vibrational state. The 'control' pulse introduces a time-dependent polarization of the molecular orbital, causing the PES to be modified according to the dynamic Stark effect and the transition dipole. The trajectories adjust in amplitude, frequency and phase-offset as work is done on or by the resulting force; comparing the perturbed and unperturbed trajectories allows the final vibrational state populations and phases to be determined. The action of the 'probe' pulse is represented by a discrete internuclear boundary, such that elements of the ensemble at a larger internuclear separation are assumed to be photodissociated. The vibrational populations predicted by the QCM are compared to recent quantum simulations (Niederhausen and Thumm 2008 Phys. Rev. A 77 013404), and a remarkable agreement has been found. The applicability of this model to femtosecond and attosecond time-scale experiments is discussed and the relation to established femtochemistry and coherent control techniques are explored.

Strong-field approximation for Coulomb explosion of H-2(+) and D-2(+) by short intense laser pulses

We present a simple quantum mechanical model to describe Coulomb explosion of H-2(+) and D-2(+) by short, intense infrared laser pulses. The model is based on the length gauge version of the molecular strong-field approximation and is valid when the process of dissociation prior to ionization is negligible. The results are compared with recent experimental data for the proton kinetic energy spectrum [Th. Ergler , Phys. Rev. Lett. 95, 093001 (2005); D. S. Murphy , J. Phys. B 40, S359 (2007)]. Using a Franck-Condon distribution over initial vibrational states, the theory reproduces the overall shape of the spectrum with only a small overestimation of slow protons. The agreement between theory and experiment can be made perfect by using a non-Frank-Condon initial distribution characteristic for H-2(+) (D-2(+)) targets produced by strong-field ionization of H-2 (D-2). For comparison, we also present results obtained by two different tunneling models for this process.

Fine interference fringes formed in high-order harmonic spectra generated by infrared driving laser pulses

We experimentally investigate the high-order harmonic generation in argon gas using a driving laser pulse at a center wavelength of 1240 nm. High-contrast fine interference fringes could be observed in the harmonic spectra near the propagation axis, which is attributed to the interference between long and short quantum paths. We also systematically examine the variation of the interference fringe pattern with increasing energy of the driving pulse and with different phase-matching conditions.

Accurate measurement of carrier-envelope phase drift for infrared femtosecond laser pulses

A novel scheme to eliminate the artificial background phase jitter is proposed for measuring the carrier-envelope phase drift of tunable infrared femtosecond pulses from an OPA laser. Different from previous methods, a reference spectral interference measurement is performed, which reveals the artificial phase jitter in the measurement process, in addition to the normal f-to-2f interference measurement between the incident laser pulses and it second harmonic. By analyzing the interference fringes, the accurate CEP fluctuation of the incident pulses is obtained. (c) 2008 Optical Society of America

Direct Photodetachment of F‾ by mid-infrared few-cycle femtosecond laser pulses

The recent adiabatic saddle-point approach of Shearer et al. [ Phys. Rev. A 84 033409 (2011)] is extended to multiphoton detachment of negative ions with outer p-state electrons. This theory is applied to investigate the strong-field photodetachment dynamics of F- ions exposed to few-cycle femtosecond laser pulses, without taking into account the rescattering mechanism. Numerical calculations are considered for mid-infrared laser wavelengths of 1300 and 1800 nm at laser intensities of 7.7 × 1012, 1.1 × 1013, and 1.3 × 1013 W/cm2. Two-dimensional momenta saddle-point spectra exhibit a distinct distribution in the shape of a “smile” in the complex-time plane. Electron momentum distribution maps of direct electrons are investigated. These produce a distinct pattern of above-threshold detachment (ATD) concentric rings due to constructive and destructive quantum interference of electrons detached from their parent ions. Probability detachment distributions presented, capturing the influence of saturation effects that are found to become more significant with increasing laser intensity at a fixed wavelength. ATD photoangular distributions as functions of laser intensity and wavelength near channel closings are also investigated and found to be sensitive to initial-state symmetry. Nonmonotonic structures observed in the ejected photoelectron energy spectra are attributed to interference effects from coherent electronic wave packets. Additionally the profiles of all the photoelectron emission spectra show strong dependence on the carrier-envelope phase, indicating that it is a reliable parameter for characterizing the wave form of the pulse.

Effect of pulse repetition rate and number of pulses in the analysis of polypropylene and high density polyethylene by nanosecond infrared laser induced breakdown spectroscopy

Pulse repetition rates and the number of laser pulses are among the most important parameters that do affect the analysis of solid materials by laser induced breakdown spectroscopy, and the knowledge of their effects is of fundamental importance for suggesting analytical strategies when dealing with laser ablation processes of polymers. In this contribution, the influence of these parameters in the ablated mass and in the features of craters was evaluated in polypropylene and high density polyethylene plates containing pigment-based PbCrO4. Surface characterization and craters profile were carried out by perfilometry and scanning electron microscopy. Area, volume and profile of craters were obtained using Taylor Map software. A laser induced breakdown spectroscopy system consisted of a Q-Switched Nd:YAG laser (1064 nm, 5 ns) and an Echelle spectrometer equipped with ICCD detector were used. The evaluated operating conditions consisted of 10, 25 and 50 laser pulses at 1, 5 and 10 Hz, 250 mJ/pulse (85 J cm(-2)), 2 mu s delay time and 6 mu s integration time gate. Differences in the topographical features among craters of both polymers were observed. The decrease in the repetition rate resulted in irregular craters and formation of edges, especially in polypropylene sample. The differences in the topographical features and ablated masses were attributed to the influence of the degree of crystallinity, crystalline melting temperature and glass transition temperature in the ablation process of the high density polyethylene and polypropylene. It was also observed that the intensities of chromium and lead emission signals obtained at 10 Hz were two times higher than at 5 Hz by keeping the number of laser pulses constant. (C) 2011 Elsevier B. V. All rights reserved.

Tunable phase-stabilized infrared parametric laser source

This paper reports that the tunable self-phase-stabilized infrared laser pulses have been generated from a two-stage optical parametric amplifier. With an 800 nm pump source, the output idler pulses are tunable from 1.3 mu m to 2.3 mu m, and the maximum output energy of the idler pulses is higher than 1 mJ at 1.6 mu m by using 6 mJ pump laser. A carrier-envelope phase fluctuation of similar to 0.15 rad (rms) for the idler pulses is measured for longer than one hour by using a home build f-to-2f interferometer.

Optical breakdown of 6H SiC induced by wavelength-tunable femtosecond laser pulses

The damage mechanisms and micromachining of 6H SiC are studied by using femtosecond laser pulses at wavelengths between near infrared (NIR) and near ultraviolet (NUV) delivered from an optical parametric amplifier (OPA). Our experimental results indicate that high quality microstructures can be fabricated in SiC crystals. On the basis of the dependence of the ablated area and the laser pulse energy, the threshold fluence of SiC is found to increase with the incident laser wavelength in the visible region, while it remains almost constant for the NIR laser. For the NIR laser pulses, both photoionization and impact ionization play important roles in electronic excitation, while for visible lasers, photoionization plays a more important role.