Above Threshold Dissociation of Vibrationally Cold HD+ Molecules

The experimental study of molecular dissociation of H2+ by intense laser pulses is complicated by the fact that the ions are initially produced in a wide range of vibrational states, each of which responds differently to the laser field. An electrostatic storage device has been used to radiatively cool HD+ ions enabling the observation of above threshold dissociation from the ground vibrational state by 40 fs laser pulses at 800 nm. At the highest intensities used, dissociation through the absorption of at least four photons is found to be the dominant process.

Mapping the evolution of optically generated rotational wave packets in a room-temperature ensemble of D2

A coherent superposition of rotational states in D2 has been excited by nonresonant, ultrafast (12 fs), intense (2×1014 W cm-2) 800 nm laser pulses, leading to impulsive dynamic alignment. Field-free evolution of this rotational wave packet 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, . The detailed fractional revivals of the neutral D2 wave packet as a function of and evolution time have been observed and modeled theoretically.

Impulsive electric fields driven by high-intensity interactions

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 experiments 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 channeling 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. Laser-driven impulsive fields at the surface of solid targets can be applied for energy-selective ion beam focusing.

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.

On the recollision-free excitation of krypton during ultrafast multi-electron tunnel ionization

The probability of multiple ionization of krypton by 50 femtosecond circularly polarized laser pulses, independent of the optical focal geometry, has been obtained for the first time. The excellent agreement over the intensity range 100 TW cm-2 to 100 PW cm-2 with the recent predictions of Kornev et al (2003 Phys. Rev. A 68 043414) provides the first experimental confirmation that non-recollisional electronic excitation can occur in strong-field ionization. This is particularly true for higher stages of ionization, when the laser intensity exceeds 10 PW cm-2 as the energetic departure of the ionized electron(s) diabatically distorts the wavefunctions of the bound electrons. By scaling the probability of ionization by the focal volume, we discuss why this mechanism was not apparent in previous studies.

Short pulse pumped X-ray lasers

Double laser pulses of duration similar to 75 ps and short laser pulses similar to 1 ps superimposed on longer duration background pulses have been shown to efficiently pump lasing in Ne-like and Ni-like ions. For the 75 ps pumping, X-ray laser output without travelling wave pumping is shown to be well-described by a model of ASE output. With I ps pumping, the X-ray laser output with different velocity travelling wave pumping is well-fitted with an extension to the ASE model allowing for travelling wave excitation of the gain along the plasma line. The model is used to investigate the production of short (<1 ps) x-ray laser pulses and the effects of non-ideal travelling wave velocities on the X-ray laser output. Resonance line spectra of emission perpendicular to the plasma line are measured and simulated. It is shown that an accurate opacity model for the more intense Ne-like ions is needed to correctly simulate the spectra.

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.

Time-resolved studies of ultrafast wavepacket dynamics in hydrogen molecules

Recent advances in the study of quantum vibrations and rotations in the fundamental hydrogen molecules are reported. Using the deuterium molecules (D-2(+) and D-2) as exemplars, the application of ultrafast femtosecond pump-probe experiments to study the creation and time-resolved imaging of coherent nuclear wavepackets is discussed. The ability to study the motion of these fundamental molecules in the time-domain is a notable milestone, made possible through the advent of ultrashort intense laser pulses with durations on sub-vibrational (and sub-rotational) timescales. Quantum wavepacket revivals are characterised for both vibrational and rotational degrees of freedom and quantum models are used to provide a detailed discussion of the underlying ultrafast physical dynamics for the specialist and non-specialist alike. (C) 2009 Elsevier B.V. All rights reserved.

Radiation-Pressure Acceleration of Ion Beams from Nanofoil Targets: The Leaky Light-Sail Regime

A new ion radiation-pressure acceleration regime, the "leaky light sail," is proposed which uses sub-skin-depth nanometer foils irradiated by circularly polarized laser pulses. In the regime, the foil is partially transparent, continuously leaking electrons out along with the transmitted laser field. This feature can be exploited by a multispecies nanofoil configuration to stabilize the acceleration of the light ion component, supplementing the latter with an excess of electrons leaked from those associated with the heavy ions to avoid Coulomb explosion. It is shown by 2D particle-in-cell simulations that a monoenergetic proton beam with energy 18 MeV is produced by circularly polarized lasers at intensities of just 10(19) W/cm(2). 100 MeV proton beams are obtained by increasing the intensities to 2 x 10(20) W/cm(2).

Effect of self-generated magnetic fields on fast-electron beam divergence in solid targets

The collimating effect of self-generated magnetic fields on fast-electron transport in solid aluminium targets irradiated by ultra-intense, picosecond laser pulses is investigated in this study. As the target thickness is varied in the range of 25 mu m to 1.4 mm, the maximum energies of protons accelerated from the rear surface are measured to infer changes in the fast-electron density and therefore the divergence of the fast-electron beam transported through the target. Purely ballistic spreading of the fast-electrons would result in a much faster decrease in the maximum proton energy with increasing target thickness than that measured. This implies that some degree of 'global' magnetic pinching of the fast-electrons occurs, particularly for thick (>400 mu m) targets. Numerical simulations of electron transport are in good agreement with the experimental data and show that the pinching effect of the magnetic field in thin targets is significantly reduced due to disruption of the field growth by refluxing fast-electrons.

Relativistic plasma surfaces as an efficient second harmonic generator

We report on the characterization of the specular reflection of 50 fs laser pulses in the intensity range 10(17)-10(21)Wcm(-2) obliquely incident with p-polarization onto solid density plasmas. These measurements show that the absorbed energy fraction remains approximately constant and that second harmonic generation (SHG) achieves efficiencies of 22 +/- 8% for intensities approaching 10(21)Wcm(-2). A simple model based on the relativistic oscillating mirror concept reproduces the observed intensity scaling, indicating that this is the dominant process involved for these conditions. This method may prove to be superior to SHG by sum frequency mixing in crystals as it is free from dispersion and retains high spatial coherence at high intensity.

Two-colour pulsed Raman studies of the lowest excited singlet state of tetraphenylporphyrin: band assignments and electronic structure

The resonance Raman spectra of the lowest lying singlet (S-1) state of free-base tetraphenylporphyrin and seven of its isotopomers were recorded under pump-and-probe conditions with a time delay of -2 ns between pump and probe laser pulses, In the S-1 spectra of the isotopomers, as in the ground state, there are dramatic splittings of what appear to be single bands in the natural isotopic abundance spectrum. The most structurally significant bands of the S-1 state were assigned on the basis of the isotope data, In some cases it was necessary to curve fit unresolved bands in the excited-state spectra in order to account for observed intensity ratios and to rationalize isotope shifts, The changes in band positions on excitation to the S-1 state were compared with those from earlier studies on the T-1 state. The changes in band positions were found to be similar For both excited states. Most notable was the similar shift in nu(2), the most widely used marker band for orbital character. The data are interpreted as implying that the lowest lying singlet state is a configuration interaction admixture of b(1u)b(2g) + a(u)b(3g) configurations with the coefficients weighted heavily in favour of b(1n)b(2g), which Is the configuration of the T-1 state. Copyright (C) 2000 John Wiley & Sons, Ltd.

RESONANCE RAMAN-SPECTRA OF THE TRIPLET-STATE OF FREE-BASE TETRAPHENYLPORPHYRIN AND 6 OF ITS ISOTOPOMERS

The resonance Raman spectra of the ground state and the lowest excited tripler state of free-base tetraphenylporphyrin and six of its isotopomers have been obtained using two-color time-resolved techniques. Ground-state spectra were recorded using low-energy 447 nm probe laser pulses, and triplet-state spectra were probed, with similar pulses, 30 ns after high-energy excitation with 532 nm pump pulses. Polarization data on both the ground and triplet states are also reported. The resonance Raman spectrum of the triplet is very different from that of the ground state but the combination of extensive isotope substitution with polarization data allows bands in the ground state to be assigned and corresponding bands in the tripler state to be located. Isotope shifts of the same bands in the S-0 and T-1 states are similar, implying that the compositions of the vibrational modes do not change significantly on excitation. Two of the strongest bands in the T-1 spectra are associated with phenyl ring substituents; these are shifted less than 5 cm(-1) between the S-0 and T-1 states so that bonding in the phenyl substituents is barely affected by excitation to the T-1 state. The changes in position of the porphyrin ring bands are larger, but still only tens of cm(-1) or less, the main changes in the spectra being due to differences in relative band intensities in the two states. The relatively small shifts in the porphyrin ring band positions which are observed show that the excitation energy is not localized on a single small region of the molecule but is delocalized over the entire porphyrin skeleton. This picture of an excited species with high chemical reactivity, but with individual bonds only slightly perturbed from the ground state, is contrasted with molecules, such as benzophenone, where excitation causes a large perturbation in the bonding within a single functional group.

Transient inversion soft X-ray lasers

The collisionally excited transient inversion scheme is shown to produce exceptionally high gain coefficients and gain-length products. Data are presented for the Ne-Like titanium and germanium and Ni-like silver X-ray lasers (XRL's) pumped using a combination of nanosecond and picosecond duration laser pulses. This method leads to a dramatic reduction of the required pump energy and makes down-sizing of XRL's possible, an important prerequisite if they are to become commonly used tools in the Long-term.

High contrast plasma mirror: spatial filtering and second harmonic generation at 10(19)Wcm(-2)

Recently, the use of plasma optics to improve temporal pulse contrast has had a remarkable impact on the field of high- power laser-solid density interaction physics. Opening an avenue to previously unachievable plasma density gradients in the high intensity focus, this advance has enabled researchers to investigate new regimes of harmonic generation and ion acceleration. Until now, however, plasma optics for fundamental laser reflection have been used in the sub-relativistic intensity regime (10(15) - 10(16)Wcm(-2)) showing high reflectivity (similar to 70%) and good focusability. Therefore, the question remains as to whether plasma optics can be used for such applications in the relativistic intensity regime (> 10(18)Wcm(-2)). Previous studies of plasma mirrors (PMs) indicate that, for 40 fs laser pulses, the reflectivity fluctuates by an order of magnitude and that focusability of the beam is lost as the intensity is increased above 5 x 10(16)Wcm(-2). However, these experiments were performed using laser pulses with a contrast ratio of similar to 10(7) to generate the reflecting surface. Here, we present results for PM operation using high contrast laser pulses resulting in a new regime of operation - the high contrast plasma mirror (HCPM). In this regime, pulses with contrast ratio > 10(10) are used to form the PM surface at > 10(19)Wcm(-2), displaying excellent spatial filtering, reflected near- field beam profile of the fundamental beam and reflectivities of 60 +/- 5%. Efficient second harmonic generation is also observed with exceptional beam quality suggesting that this may be a route to achieving the highest focusable harmonic intensities. Plasma optics therefore offer the opportunity to manipulate ultra-intense laser beams both spatially and temporally. They also allow for ultrafast frequency up-shifting without detrimental effects due to group velocity dispersion (GVD) or reduced focusability which frequently occur when nonlinear crystals are used for frequency conversion.