Ultrafast coherent control and quantum encoding of molecular vibrations in D2+ using intense laser pulses

Intense, few-femtosecond pulse technology has enabled studies of the fastest vibrational relaxation processes. The hydrogen group vibrations can be imaged and manipulated using intense infrared pulses. Through numerical simulation, we demonstrate an example of ultrafast coherent control that could be effected with current experimental facilities, and observed using high-resolution time-of-flight spectroscopy. The proposal is a pump-probe-type technique to manipulate the D2+ ion with ultrashort pulse sequences. The simulations presented show that vibrational selection can be achieved through pulse delay. We find that the vibrational system can be purified to a two-level system thus realizing a vibrational qubit. A novel scheme for the selective transfer of population between these two levels, based on a Raman process and conditioned upon the delay time of a second control-pulse is outlined, and may enable quantum encoding with this system.

Coherent Control of High Harmonic Generation via Dual-Gas Multijet Arrays

High harmonic generation (HHG) is a central driver of the rapidly growing field of ultrafast science. We present a novel quasiphase-matching (QPM) concept with a dual-gas multijet target leading, for the first time, to remarkable phase control between multiple HHG sources (> 2) within the Rayleigh range. The alternating jet structure with driving and matching zones shows perfect coherent buildup for up to six QPM periods. Although not in the focus of the proof-of-principle studies presented here, we achieved competitive conversion efficiencies already in this early stage of development.

Pathways to state-selective control of vibrational wavepackets in the deuterium molecular ion

The capability of intense ultrashort laser pulses to initiate, control and image vibrational wavepacket dynamics in the deuterium molecular ion has been simulated with a view to inform and direct future femtosecond pump-control-probe experiments. The intense-field coherent control of the vibrational superposition has been studied as a function of pulse intensity and delay time, to provide an indication of key constraints for experimental studies. For selected cases of the control mechanism, probing of the subsequent vibrational wavepacket dynamics has been simulated via the photodissociation (PD) channel. Such PD probing is shown to elucidate the modified wavepacket dynamics where the position of the quantum revival is sensitive to the control process. Through Fourier transform analysis the PD yield is also shown to provide a characterisation of the vibrational distribution. It has been shown that a simple 'critical R cut-off' approximation can be used to reproduce the effect of a probe pulse interaction, providing a convenient and efficient alternative to intensive computer simulations of the PD mechanism in the deuterium molecular ion.

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.

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.

Controlling the divergence of high harmonics from solid targets: a route toward coherent harmonic focusing

Harmonic generation from relativistically oscillating plasma surfaces formed during the interaction of high contrast lasers with solid-density targets has been shown to be an efficient source of extreme ultraviolet (XUV) and X-ray radiation. Recent work has demonstrated that the exceptional coherence properties of the driving laser can be mirrored in the emitted radiation, permitting diffraction limited performance and attosecond phase locking of the harmonic radiation. These unique properties may allow the coherent harmonic focusing (CHF) of high harmonics generated from solid density targets to intensities on the order of the Schwinger limit of 10(29) W cm(-2) with laser systems available in the near future [Phys. Rev. Lett. 93, 115002 (2004)] and thus pave the way for unique experiments exploring the nonlinear properties of vacuum on ultra-fast timescales. In this paper we investigate experimentally as well as numerically the prospect of focusing high harmonics under realistic experimental conditions and demonstrate, using particle in cell (PIC) simulations, that precise control of the wavefronts and thus the focusability of the generated harmonics is possible with pre-shaped targets.

Conundrums in Conservation: Complexity in Control

The departure point for this investigation is to highlight the centrality of regulation theory as a praxis in planning enforcement. The value of the conceptual framework is demonstrated by application in the problematic arena of conservation regulatory compliance, where there is currently a dearth of investigation. It is evidenced that this thematic approach provides a lens to scrutinise problematic areas of control and provides a deeper understanding of the difficulties faced by planning enforcement operational practice generally and heritage regimes specifically. The utility of the proposed mechanism is that it remedies the current well documented pitfalls of disjointed, piecemeal strategies by providing a framework for robust, coherent decision making not only in planning but in the wider regulatory arena.

Possibilistic Information Fusion Using Maximal Coherent Subsets

When multiple sources provide information about the same unknown quantity, their fusion into a synthetic interpretable message is often a tedious problem, especially when sources are conicting. In this paper, we propose to use possibility theory and the notion of maximal coherent subsets, often used in logic-based representations, to build a fuzzy belief structure that will be instrumental both for extracting useful information about various features of the information conveyed by the sources and for compressing this information into a unique possibility distribution. Extensions and properties of the basic fusion rule are also studied.

Beyond Criminal Justice: An anthology of abolitionist papers presented to conferences of the European Group for the Study of Deviance and Social Control over the past decade

Beyond Criminal Justice presents a vision of a future without brutal, authoritarian and repressive penal regimes. Many of the papers brought together here have been unavailable for more than two decades. Their republication indicates not only their continuing theoretical importance to abolitionist studies but also how they provide important insights into the nature and legitimacy of criminal processes in the here and now. Contributors highlight the human consequences of the harms of imprisonment, evidencing the hurt, injury and damage of penal incarceration across a number of different countries in Europe. Focusing on penal power and prisoner contestation to such power, the moral and political crises of imprisonment are laid bare. The contributors to Beyond Criminal Justice explore the urgent need for a coherent, rational and morally and politically sophisticated theoretical basis for penal abolitionism. Advocating a utopian imagination and at the same time practical solutions already implemented in countries around Europe - alongside grappling with controversial debates such as abolitionist responses to rape and sexual violence - the book steps outside of common sense assumptions regarding 'crime', punishment and 'criminal justice'. Beyond Criminal Justice will be of interest to students of criminology, zemiology, sociology, penology and critical legal studies as well as anyone interested in rethinking the problem of 'crime' and challenging the logic of the penal rationale.