3D Simulations of Surface Harmonic Generation with few-cycle laser pulses

The mechanism of harmonic generation in the interaction of short laser pulses with solid targets holds the promise for the production of intense attosecond pulses. Using the three dimensional code ILLUMINATION we have performed simulations pertaining to an experimentally realizable parameter range by high power laser systems to become available in the near future. The emphasis of the investigation is on the coherent nature of the emission. We studied the influence of the plasma scale length on the harmonic efficiency, angular distribution and the focusability using a post processing scheme in which the far-field of the emission is calculated. It is found that the presence of an extended density profile reduces significantly the transverse coherence length of the emitted XUV light. The different stages of the interaction for two particular cases can be followed with the help of movies.

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.

Controlled redistribution of vibrational population by few-cycle strong-field laser pulses

The use of strong-field (i.e. intensities in excess of 10(13) Wcm(-2)) few-cycle ultrafast (durations of 10 femtoseconds or less) laser pulses to create, manipulate and image vibrational wavepackets is investigated. Quasi-classical modelling of the initial superposition through tunnel ionization, wavepacket modification by nonadiabatically altering the nuclear environment via the transition dipole and the Stark effect, and measuring the control outcome by fragmenting the molecule is detailed. The influence of the laser intensity on strong-field ultrafast wavepacket control is discussed in detail: by modifying the distribution of laser intensities imaged, we show that focal conditions can be created that give preference to this three-pulse technique above processes induced by the pulses alone. An experimental demonstration is presented, and the nuclear dynamics inferred by the quasi-classical model discussed. Finally, we present the results of a systematic investigation of a dual-control pulse scheme, indicating that single vibrational states should be observable with high fidelity, and the populated state defined by varying the arrival time of the two control pulses. The relevance of such strong-field coherent control methods to the manipulation of electron localization and attosecond science is discussed.

Strong-field photodetachment of H- by few-cycle laser pulses

The recent adiabatic saddle-point method of Shearer et al. [ Phys. Rev. A 84 033409 (2011)] is applied to study strong-field photodetachment of H- by few-cycle linearly polarized laser pulses of frequencies near the two-photon detachment threshold. The behavior of the saddle points in the complex-time plane for a range of laser parameters is explored. A detailed analysis of the influence of laser intensities [(2×1011)–(6.5 × 1011) W/cm2], midinfrared laser wavelengths (1800–2700 nm), and various values of the carrier envelope phase (CEP) on (i) three-dimensional probability detachment distributions, (ii) photoangular distributions (PADs), (iii) energy spectra, and (iv) momentum distributions are presented. Examination of the probability distributions and PADs reveal main lobes and jetlike structures. Bifurcation phenomena in the probability distributions and PADs are also observed as the wavelength and intensity increase. Our simulations show that the (i) probability distributions, (ii) PADs, and (iii) energy spectra are extremely sensitive to the CEP and thus measuring such distributions provides a useful tool for determining this phase. The symmetrical properties of the electron momentum distributions are also found to be strongly correlated with the CEP and this provides an additional robust method for measuring the CEP of a laser pulse. Our calculations further show that for a three-cycle pulse inclusion of all eight saddle points is required in the evaluation of the transition amplitude to yield an accurate description of the photodetachment process. This is in contrast to recent results for a five-cycle pulse.

Methods of generating carrier-envelope-phase stabilized, intense, few-cycle laser pulses

Ultrafast laser pulses have become an integral part of the toolbox of countless laboratories doing physics, chemistry, and biological research. The work presented here is motivated by a section in the ever-growing, interdisciplinary research towards understanding the fundamental workings of light-matter interactions. Specifically, attosecond pulses can be useful tools to obtain the desired insight. However access to, and the utility of, such pulses is dependent on the generation of intense, few-cycle, carrier-envelope-phase stabilized laser pulses. The presented work can be thought of as a sort of roadmap towards the latter. From the oscillator which provides the broadband seed to amplification methods, the integral pieces necessary for the generation of attosecond pulses are discussed. A range of topics from the fundamentals to design challenges is presented, outfitting the way towards the practical implementation of an intense few-cycle carrier-envelope-phase stabilized laser source.

Asymmetry of the photoionization rate of H atoms by a sequence of one-cycle laser pulses

Using an unperturbed scattering theory, the characteristics of H atom photoionization are studied respectively by a linearly- and by a circularly- polarized one-cycle laser pulse sequence. The asymmetry for photoelectrons in two directions opposite to each other is investigated. It is found that the asymmetry degree varies with the carrier-envelope (CE) phase, laser intensity, as well as the kinetic energy of photoelectrons. For the linear polarization, the maximal ionization rate varies with the CE phase, and the asymmetry degree varies with the CE phase in a sine-like pattern. For the circular polarization, the maximal ionization rate keeps constant for various CE phases, but the variation of asymmetry degree is still in a sine-like pattern.

Propagation of a few-cycle laser pulse in a V-type three-level system

Propagation of a few-cycle laser pulse in a V-type three-level system (fine structure levels of rubidium) is investigated numerically. The full three-level Maxwell-Bloch equations without the rotating wave approximation and the standing slowly varying envelope approximation are solved by using a finite-difference time-domain method. It is shown that, when the usual unequal oscillator strengths are considered, self-induced transparency cannot be recovered and higher spectral components can be produced even for small-area pulses. (c) 2005 Pleiades Publishing, Inc.

Optimization of high-order harmonic by genetic algorithm for the chirp and phase of few-cycle pulses

The brightness of a particular harmonic order is optimized for the chirp and initial phase of the laser pulse by genetic algorithm. The influences of the chirp and initial phase of the excitation pulse on the harmonic spectra are discussed in terms of the semi-classical model including the propagation effects. The results indicate that the harmonic intensity and cutoff have strong dependence on the chirp of the laser pulse, but slightly on its initial phase. The high-order harmonics can be enhanced by the optimal laser pulse and its cutoff can be tuned by optimization of the chirp and initial phase of the laser pulse.

Redistribution of vibrational population in a molecular ion with nonresonant strong-field laser pulses

We present an experimental demonstration of nonresonant manipulation of vibrational states in a molecule by an intense ultrashort laser pulse. A vibrational wave packet is generated in D-2(+) through tunnel ionization of D-2 by a few-cycle pump pulse. A similar control pulse is applied as the wave packet begins to dephase so that the dynamic Stark effect distorts the electronic environment of the nuclei, transferring vibrational population. The time evolution of the modified wave packet is probed via the D-2(+) photodissociation yield that results from the application of an intense probe pulse. Comparing the measured yield with a quasiclassical trajectory model allows us to determine the redistribution of vibrational population caused by the control pulse. ©

Few-cycle driven relativistically oscillating plasma mirrors:A source of intense isolated attosecond pulses

The conditions required for the production of isolated attosecond pulses from relativistically oscillating mirrors (ROM) are investigated numerically and experimentally. In simulations, carrier-envelope-phase-stabilized three-cycle pulses are found to be sufficient to produce isolated attosecond pulses, while two-cycle pulses will predominantly lead to isolated attosecond pulses even in the absence of carrier-envelope stabilization. Using a state-of-the-art laser system delivering three-cycle pulses at multiple-terawatt level, we have generated higher harmonics up to 70 eV photon energy via the ROM mechanism. The observed spectra are in agreement with theoretical expectations and highlight the potential of few-cycle-driven ROM harmonics for intense isolated attosecond pulse generation for performing extreme ultraviolet-pump extreme ultraviolet-probe experiments. © 2012 American Physical Society.