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.

Intense-field dissociation dynamics of D2+ molecular ions using ultrafast laser pulses

The dynamics of dissociation of pre-ionized D2+ molecules using intense (10^12–10^15 W cm-2), ultrashort (50 fs), infrared (? = 790 nm) laser pulses are examined. Use of an intensity selective scan technique has allowed the deuterium energy spectrum to be measured over a broad range of intensity. It is found that the dominant emission shifts to lower energies as intensity is increased, in good agreement with corresponding wavepacket simulations. The results are consistent with an interpretation in terms of bond softening, which at high intensity (approximately >3 × 10^14 W cm-2) becomes dominated by dissociative ionization. Angular distribution measurements reveal the presence of slow molecular dissociation, an indication that vibrational trapping mechanisms occur in this molecule.

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.

Carbon ion acceleration from thin foil targets irradiated by ultrahigh-contrast, ultraintense laser pulses

In this study, ion acceleration from thin planar target foils irradiated by ultrahigh-contrast (10(10)), ultrashort (50 fs) laser pulses focused to intensities of 7 x 10(20) W cm(-2) is investigated experimentally. Target normal sheath acceleration (TNSA) is found to be the dominant ion acceleration mechanism when the target thickness is >= 50 nm and laser pulses are linearly polarized. Under these conditions, irradiation at normal incidence is found to produce higher energy ions than oblique incidence at 35 degrees with respect to the target normal. Simulations using one-dimensional (1D) boosted and 2D particle-in-cell codes support the result, showing increased energy coupling efficiency to fast electrons for normal incidence. The effects of target composition and thickness on the acceleration of carbon ions are reported and compared to calculations using analytical models of ion acceleration.

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. ©

Production of ultracollimated bunches of multi-MeV electrons by 35 fs laser pulses propagating in exploding-foil plasmas

Very collimated bunches of high energy electrons have been produced by focusing super-intense femtosecond laser pulses in submillimeter under-dense plasmas. The density of the plasma, preformed with the laser exploding-foil technique, was mapped using Nomarski interferometry. The electron beam was fully characterized: up to 10(9) electrons per shot were accelerated, most of which in a beam of aperture below 10(-3) sterad, with energies up to 40 MeV. These measurements, which are well modeled by three-dimensional numerical simulations, validate a reliable method to generate ultrashort and ultracollimated electron bunches. (C) 2002 American Institute of Physics.

Control of ionization and dissociation of H2+ by elliptically polarized ultra-short VUV laser pulses

Resonance-enhanced multiphoton ionization of H₂ ⁺ exposed to elliptically polarized VUV laser pulses is investigated. Differential cross sections for nuclei and electron are obtained using numerical solutions of the time-dependent Schrödinger equation. In this work in progress, we explore the dependence of the dissociative ionization observables with the polarization of the light.

Ultrafast charge dynamics initiated by high-intensity, ultrashort laser-matter interaction

The interaction of high‐intensity laser pulses with matter releases instantaneously ultra‐large currents of highly energetic electrons, leading to the generation of highly‐transient, large‐amplitude electric and magnetic fields. We report results of recent experiment in which such charge dynamics have been studied by using proton probing techniques able to provide maps of the electrostatic fields with high spatial and temporal resolution. The dynamics of ponderomotive channelling in underdense plasmas have been studied in this way, as also the processes of Debye sheath formation and MeV ion front expansion at the rear of laser‐irradiated thin metallic foils. An application employing laser‐driven impulsive fields for energy‐selective ion beam focusing is also presented.

Electrically tunable delay for trains of optical pulses

A technique to implement an electrically tunable delay line with high bandwidth for trains of ultrashort optical pulses is presented. The system is based on the temporal self-imaging effect in fiber gratings and electrooptic modulation.

Ion acceleration in underdense plasmas by ultra-short laser pulses

We report on the ion acceleration mechanisms that occur during the interaction of an intense and ultrashort laser pulse ( λ > μ I 2 1018 W cm−2 m2) with an underdense helium plasma produced from an ionized gas jet target. In this unexplored regime, where the laser pulse duration is comparable to the inverse of the electron plasma frequency ωpe, reproducible non-thermal ion bunches have been measured in the radial direction. The two He ion charge states present energy distributions with cutoff energies between 150 and 200 keV, and a striking energy gap around 50 keV appearing consistently for all the shots in a given density range. Fully electromagnetic particle-in-cell simulations explain the experimental behaviors. The acceleration results from a combination of target normal sheath acceleration and Coulomb explosion of a filament formed around the laser pulse propagation axis

Ultrashort pulse generation from diode laser devices

This thesis presents a detailed, experiment-based study of generation of ultrashort optical pulses from diode lasers. Simple and cost-effective techniques were used to generate high power, high quality optical short pulses at various wavelength windows. The major achievements presented in the thesis is summarised as follows. High power pulses generation is one of the major topics discussed in the thesis. Although gain switching is the simplest way for ultrashort pulse generation, it proves to be quite effective to deliver high energy pulses on condition that the pumping pulses with extremely fast rising time and high enough amplitude are applied on specially designed pulse generators. In the experiment on a grating-coupled surface emitting laser (GCSEL), peak power as high as 1W was achieved even when its spectral bandwidth was controlled within 0.2nm. Another experiment shows violet picosecond pulses with peak power as high as 7W was achieved when the intensive electrical pulses were applied on optimised DC bias to pump on InGaN violet diode laser. The physical mechanism of this phenomenon, as we considered, may attributed to the self-organised quantum dots structure in the laser. Control of pulse quality, including spectral quality and temporal profile, is an important issue for high power pulse generation. The ways to control pulse quality described in the thesis are also based on simple and effective techniques. For instance, GCSEL used in our experiment has a specially designed air-grating structure for out-coupling of optical signals; hence, a tiny flat aluminium mirror was placed closed to the grating section and resulted in a wavelength tuning range over 100nm and the best side band suppression ratio of 40dB. Self-seeding, as an effective technique for spectral control of pulsed lasers, was demonstrated for the first time in a violet diode laser. In addition, control of temporal profile of the pulse is demonstrated in an overdriven DFB laser. Wavelength tuneable fibre Bragg gratings were used to tailor the huge energy tail of the high power pulse. The whole system was compact and robust. The ultimate purpose of our study is to design a new family of compact ultrafast diode lasers. Some practical ideas of laser design based on gain-switched and Q-switched devices are also provided in the end.

Thermal tweezers for manipulation of adatoms and nanoparticles on surfaces heated by interfering laser pulses

We conduct the detailed numerical investigation of a nanomanipulation and nanofabrication technique—thermal tweezers with dynamic evolution of surface temperature, caused by absorption of interfering laser pulses in a thin metalfilm or any other absorbing surface. This technique uses random Brownian forces in the presence of strong temperature modulation (surfacethermophoresis) for effective manipulation of particles/adatoms with nanoscale resolution. Substantial redistribution of particles on the surface is shown to occur with the typical size of the obtained pattern elements of ∼100 nm, which is significantly smaller than the wavelength of the incident pulses used (532 nm). It is also demonstrated that thermal tweezers based on surfacethermophoresis of particles/adatoms are much more effective in achieving permanent high maximum-to-minimum concentration ratios than bulk thermophoresis, which is explained by the interaction of diffusing particles with the periodic lattice potential on the surface. Typically required pulse regimes including pulse lengths and energies are also determined. The approach is applicable for reproducing any holographically achievable surfacepatterns, and can thus be used for engineering properties of surfaces including nanopatterning and design of surface metamaterials.

From short pulses to short breaks : exotic plasma bullets via residual electron control

Plasma plumes with exotically segmented channel structure and plasma bullet propagation are produced in atmospheric plasma jets. This is achieved by tailoring interruptions of a continuous DC power supply over the time scales of lifetimes of residual electrons produced by the preceding discharge phase. These phenomena are explained by studying the plasma dynamics using nanosecond-precision imaging. One of the plumes is produced using 2-10μs interruptions in the 8kV DC voltage and features a still bright channel from which a propagating bullet detaches. A shorter interruption of 900ns produces a plume with the additional long conducting dark channel between the jet nozzle and the bright area. The bullet size, formation dynamics, and propagation speed and distance can be effectively controlled. This may lead to micrometer-and nanosecond-precision delivery of quantized plasma bits, warranted for next-generation health, materials, and device technologies.

Solitary filamentary structures and nanosecond dynamics in atmospheric-pressure plasmas driven by tailored dc pulses

Nanosecond dynamics of two separated discharge cycles in an asymmetric dielectric barrier discharge is studied using time-resolved current and voltage measurements synchronized with high-speed (∼5 ns) optical imaging. Nanosecond dc pulses with tailored raise and fall times are used to generate solitary filamentary structures (SFSs) during the first cycle and a uniform glow during the second. The SFSs feature ∼1.5 mm thickness, ∼1.9 A peak current, and a lifetime of several hundred nanoseconds, at least an order of magnitude larger than in common microdischarges. This can be used in alternating localized and uniform high-current plasma treatments in various applications.