arXiv subjects

I. D. Williams

Publications and source records attributed to I. D. Williams.

7 recordsLinked to original sources

arXiv2012

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.

physics.chem-ph↗

arXiv2010

Atomic excitation during recollision-free ultrafast multi-electron tunnel ionization

Modern intense ultrafast pulsed lasers generate an electric field of sufficient strength to permit tunnel ionization of the valence electrons in atoms. This process is usually treated as a rapid succession of isolated events, in which the states of the remaining electrons are neglected. Such electronic interactions are predicted to be weak, the exception being recollision excitation and ionization caused by linearly-polarized radiation. In contrast, it has recently been suggested that intense field ionization may be accompanied by a two-stage `shake-up' reaction. Here we report a unique combination of experimental techniques that enables us to accurately measure the tunnel ionization probability for argon exposed to 50 femtosecond laser pulses. Most significantly for the current study, this measurement is independent of the optical focal geometry, equivalent to a homogenous electric field. Furthermore, circularly-polarized radiation negates recollision. The present measurements indicate that tunnel ionization results in simultaneous excitation of one or more remaining electrons through shake-up. From an atomic physics standpoint, it may be possible to induce ionization from specific states, and will influence the development of coherent attosecond XUV radiation sources. Such pulses have vital scientific and economic potential in areas such as high-resolution imaging of in-vivo cells and nanoscale XUV lithography.

physics.atom-ph↗

arXiv2008

Quantum Chessboards in the Deuterium Molecular Ion

We present a new algorithm for vibrational control in deuterium molecules that is feasible with current experimental technology. A pump mechanism is used to create a coherent superposition of the D2+ vibrations. A short, intense infrared control pulse is applied after a chosen delay time to create selective interferences. A `chessboard' pattern of states can be realized in which a set of even- or odd-numbered vibrational states can be selectively annihilated or enhanced. A technique is proposed for experimental realization and observation of this effect using 5 fs pulses of 790 nm radiation, with intermediate intensity (5e13 W/cm2)

quant-ph↗

arXiv2007

Isolated vibrational wavepackets in D2+: Defining superposition conditions and wavepacket distinguishability

Tunnel ionization of room-temperature D$_2$ in an ultrashort (12 femtosecond) near infra-red (800 nm) pump laser pulse excites a vibrational wavepacket in the D2+ ions; a rotational wavepacket is also excited in residual D2 molecules. Both wavepacket types are collapsed a variable time later by an ultrashort probe pulse. We isolate the vibrational wavepacket and quantify its evolution dynamics through theoretical comparison. Requirements for quantum computation (initial coherence and quantum state retrieval) are studied using this well-defined (small number of initial states at room temperature, initial wavepacket spatially localized) single-electron molecular prototype by temporally stretching the pump and probe pulses.

physics.chem-ph↗

arXiv2007

Mapping the Evolution of Optically-Generated Rotational Wavepackets in a Room Temperature Ensemble of D$_2$

A coherent superposition of rotational states in D$_2$ has been excited by nonresonant ultrafast (12 femtosecond) intense (2 $\times$ 10$^{14}$ Wcm$^{-2}$) 800 nm laser pulses leading to impulsive dynamic alignment. Field-free evolution of this rotational wavepacket has been mapped to high temporal resolution by a time-delayed pulse, initiating rapid double ionization, which is highly sensitive to the angle of orientation of the molecular axis with respect to the polarization direction, $θ$. The detailed fractional revivals of the neutral D$_2$ wavepacket as a function of $θ$ and evolution time have been observed and modelled theoretically.

quant-ph↗

arXiv2005

Reconstruction of Atomic Ionization Probabilities in Intense Laser Fields

Application of a parallel-projection inversion technique to z-scan spectra of multiply charged xenon and krypton ions, obtained by non-resonant field ionization of neutral targets, has for the first time permitted the direct observation of intensity-dependent ionization probabilities. These ionization efficiency curves have highlighted the presence of structure in the tunnelling regime, previously unobserved under full-volume techniques.

physics.atom-ph↗

arXiv2005

Geometry- and diffraction-independent ionization probabilities in intense laser fields: probing atomic ionization mechanisms with effective intensity matching

We report a novel experimental technique for the comparison of ionization processes in ultrafast laser pulses irrespective of pulse ellipticity. Multiple ionization of xenon by 50 fs 790 nm, linearly and circularly polarized laser pulses is observed over the intensity range 10 TW/cm^2 to 10 PW/cm^2 using Effective Intensity Matching (EIM), which is coupled with Intensity Selective Scanning (ISS) to recover the geometry-independent probability of ionization. Such measurements, made possible by quantifying diffraction effects in the laser focus, are compared directly to theoretical predictions of multiphoton, tunnel and field ionization, and a remarkable agreement demonstrated. EIM-ISS allows the straightforward quantification of the probability of recollision ionization in a linearly polarized laser pulse. Furthermore, probability of ionization is discussed in terms of the Keldysh adiabaticity parameter, gamma, and the influence of the precursor ionic states present in recollision ionization is observed for the first time.

physics.atom-ph↗