Time delay between singly and doubly ionizing wavepackets in laser-driven helium

We present calculations of the time delay between single and double ionization of helium, obtained from full-dimensionality numerical integrations of the helium-laser Schroedinger equation. The notion of a quantum mechanical time delay is defined in terms of the interval between correlated bursts of single and double ionization. Calculations are performed at 390 and 780 nm in laser intensities that range from 2 X 10^14 to 14 X 10^14 W /cm^2. We find results consistent with the rescattering model of double ionization but supporting its classical interpretation only at 780 nm.

Observing time-dependent vibrational quantum dynamics in deuterium hydride molecular ions

Few-cycle laser pulses are used to "pump and probe" image the vibrational wavepacket dynamics of a HD+ molecular ion. The quantum dephasing and revival structure of the wavepacket are mapped experimentally with time-resolved photodissociation imaging. The motion of the molecule is simulated using a quantum-mechanical model predicting the observed structure. The coherence of the wavepacket is controlled by varying the duration of the intense laser pulses. By means of a Fourier transform analysis both the periodicity and relative population of the vibrational states of the excited molecular ion have been characterized.

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.

Imaging quantum vibrations on an ultrashort timescale: the deuterium molecular ion

The vibrational wavepacket revival of a basic quantum system is demonstrated experimentally. Using few-cycle laser pulse technology, pump and probe imaging of the vibrational motion of D+2 molecules is conducted, and together with a quantum-mechanical simulation of the excited wavepacket motion, the vibrational revival phenomenon has been characterised. The simulation shows good correlation with the temporal motion and structural features obtained from the data, relaying fundamental information on this diatomic system.

Quantum revivals in ultrashort intense field dissociation of molecular ions

Ultrashort (<15 fs) high intensity (1014-1016 W cm-2) laser pulses have provided novel methods for investigation of the dynamics of simple molecular ions such as H2+ and D2+. In this paper we report on simulations carried out for the D2+ molecular ion, within the Born- Oppenheimer and two-state approximations. These simulations allow one to investigate the dissociation dynamics of the D2+ molecular ion when subjected to such ultrashort, intense laser pulses. In particular, these simulations are compared to the results from recent pump-probe experiments, in which, the nuclear vibrational motion of D2+ has been imaged. Simulations suggest that the nature of the dissociation process, be it 1- or 2-photon, may be influenced by the tuning of the pump-probe delay time.

Theory of laser-driven double-ionization of atoms at Ti : sapphire laser wavelengths

Progress in the theoretical understanding of non-sequential double-ionization of atoms is reviewed from its beginnings with Kuchiev's work in the late 1980s and Corkum's work in the early 1990s to the present day. The crucial role of laboratory experiment as a persistent stimulus to theoretical endeavour is underlined but the predictive roles of simple, yet fundamental, theory and also of a full quantum mechanical description are not forgotten. A theoretical forward look is provided.

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.

Electromagnetic pulse compression and energy localization in quantum plasmas

The evolution of the intensity of a relativistic laser beam propagating through a dense quantum plasma is investigated, by considering different plasma regimes. A cold quantum fluid plasma and then a thermal quantum description(s) is (are) adopted, in comparison with the classical case of reference. Considering a Gaussian beam cross-section, we investigate both the longitudinal compression and lateral/longitudinal localization of the intensity of a finite-radius electromagnetic pulse. By employing a quantum plasma fluid model in combination with Maxwell's equations, we rely on earlier results on the quantum dielectric response, to model beam-plasma interaction. We present an extensive parametric investigation of the dependence of the longitudinal pulse compression mechanism on the electron density in cold quantum plasmas, and also study the role of the Fermi temperature in thermal quantum plasmas. Our numerical results show pulse localization through a series of successive compression cycles, as the pulse propagates through the plasma. A pulse of 100 fs propagating through cold quantum plasma is compressed to a temporal size of approximate to 1.35 attosecond and a spatial size of approximate to 1.08 10(-3) cm. Incorporating Fermi pressure via a thermal quantum plasma model is shown to enhance localization effects. A 100 fs pulse propagating through quantum plasma with a Fermi temperature of 350 K is compressed to a temporal size of approximate to 0.6 attosecond and a spatial size of approximate to 2.4 10(-3) cm. (c) 2010 Elsevier B.V. All rights reserved.

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.

Quantum ground state of self-organized atomic crystals in optical resonators

Cold atoms, driven by a laser and simultaneously coupled to the quantum field of an optical resonator, may self-organize in periodic structures. These structures are supported by the optical lattice, which emerges from the laser light they scatter into the cavity mode and form when the laser intensity exceeds a threshold value. We study theoretically the quantum ground state of these structures above the pump threshold of self-organization by mapping the atomic dynamics of the self-organized crystal to a Bose-Hubbard model. We find that the quantum ground state of the self-organized structure can be the one of a Mott insulator, depending on the pump strength of the driving laser. For very large pump strengths, where the intracavity-field intensity is maximum and one would expect a Mott-insulator state, we find intervals of parameters where the phase is compressible. These states could be realized in existing experimental setups.

Prospects for ultracold carbon via charge exchange reactions and laser cooled carbides

Strategies to produce an ultracold sample of carbon atoms are explored and assessed with the help of quantum chemistry. After a brief discussion of the experimental difficulties using conventional methods, two strategies are investigated. The first attempts to exploit charge exchange reactions between ultracold metal atoms and sympathetically cooled C+ ions. Ab initio calculations including electron correlation have been conducted on the molecular ions [LiC]+ and [BeC]+ to determine whether alkali or alkaline earth metals are a suitable buffer gas for the formation of C atoms but strong spontaneous radiative charge exchange ensure they are not ideal. The second technique involves the stimulated production of ultracold C atoms from a gas of laser cooled carbides. Calculations on LiC suggest that the alkali carbides are not suitable but the CH radical is a possible laser cooling candidate thanks to very favourable Frank-Condon factors. A scheme based on a four pulse STIRAP excitation pathway to a Feshbach resonance is outlined for the production of atomic fragments with near zero centre of mass velocity.

Development of XUV lasers at the RAL central laser facility

Recent progress in the development of XUV lasers by research teams using high-power and ultrashort-pulse Nd:glass and KrF laser facilities at the Rutherford Appleton Laboratory is reviewed. Injector-amplifier operation and prepulse enhanced output of the Ge XXIII collisional laser driven by a kilojoule glass laser, enhanced gain in CVI recombination with picosecond CPA drive pulses from a glass laser, and optical field ionization and XUV harmonic generation with a KrF CPA laser are described.

Efficient control of quantum paths via dual-gas high harmonic generation

The accurate control of the relative phase of multiple distinct sources of radiation produced by high harmonic generation is of central importance in the continued development of coherent extreme UV (XUV) and attosecond sources. Here, we present a novel approach which allows extremely accurate phase control between multiple sources of high harmonic radiation generated within the Rayleigh range of a single-femtosecond laser pulse using a dualgas, multi-jet array. Fully ionized hydrogen acts as a purely passive medium and allows highly accurate control of the relative phase between each harmonic source. Consequently, this method allows quantum path selection and rapid signal growth via the full coherent superposition of multiple HHG sources (the so-called quasi-phase-matching). Numerical simulations elucidate the complex interplay between the distinct quantum paths observed in our proof-of-principle experiments.