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.

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.

Comparison of parallel and perpendicular polarized counterpropagating light for suppressing high harmonic generation

The use of counterpropagating laser pulses to suppress high harmonic generation (HHG) is investigated experimentally for pulses polarized parallel or perpendicular to the driving laser pulse. It is shown for the first time that perpendicularly polarized pulses can suppress HHG. The intensity of the counterpropagating pulse required for harmonic suppression is found to be much larger for perpendicular polarization than for parallel polarization, in good agreement with simple models of the harmonic suppression. These results have applications to quasi-phase-matching of HHG with trains of counterpropagating pulses. (C) 2007 Optical Society of America.

Role of the plasma scale length in the harmonic generation from solid targets

We have investigated the generation of high harmonics from the interaction of 150 fsec, 790 nm, and 395 nm laser pulses with solid targets. Experiments are presented that demonstrate a strong dependence of the conversion efficiency on the temporal pulse shape and the resulting density scale length (L/lambda) of the preformed plasma. The highest conversion efficiencies are achieved for short density scale lengths (L/lambda less than or equal to 0.4), which result from high contrast ratio pulse interactions. [S1063-651X(98)50211-5].

Femtosecond lasers for mass spectrometry: Proposed application to catalytic hydrogenation of butadiene

Mass spectra from the interaction of intense, femtosecond laser pulses with 1,3-butadiene, 1-butene, and n-butane have been obtained. The proportion of the fragment ions produced as a function of intensity, pulse length, and wavelength was investigated. Potential mass spectrometry applications, for example in the analysis of catalytic reaction products, are discussed.

Imaging adiabatic control of charge transfer in molecules

Charge transfer is a subfemtosecond process in molecules that creates chemical and electronic structure changes. At the quantum level the process can be coherently controlled by ultrashort light pulses. We show how the charge transfer process can be manipulated using a combination of dynamic and static fields and predict how this can be observed experimentally by imaging with photoionization.

Experimental demonstration of particle energy, conversion efficiency and spectral shape required for ion-based fast ignition

Research on fusion fast ignition (FI) initiated by laser-driven ion beams has made substantial progress in the last years. Compared with electrons, FI based on a beam of quasi-monoenergetic ions has the advantage of a more localized energy deposition, and stiffer particle transport, bringing the required total beam energy close to the theoretical minimum. Due to short pulse laser drive, the ion beam can easily deliver the 200 TW power required to ignite the compressed D-T fuel. In integrated calculations we recently simulated ion-based FI targets with high fusion gain targets and a proof of principle experiment [1]. These simulations identify three key requirements for the success of ion-driven fast ignition (IFI): (1) the generation of a sufficiently high-energetic ion beam (approximate to 400-500 MeV for C), with (2) less than 20% energy spread at (3) more than 10% conversion efficiency of laser to beam energy. Here we present for the first time new experimental results, demonstrating all three parameters in separate experiments. Using diamond nanotargets and ultrahigh contrast laser pulses we were able to demonstrate >500 MeV carbon ions, as well as carbon pulses with Delta E/E

Dynamics of relativistic transparency and optical shuttering in expanding overdense plasmas

Overdense plasmas are usually opaque to laser light. However, when the light is of sufficient intensity to drive electrons in the plasma to near light speeds, the plasma becomes transparent. This process—known as relativistic transparency—takes just a tenth of a picosecond. Yet all studies of relativistic transparency so far have been restricted to measurements collected over timescales much longer than this, limiting our understanding of the dynamics of this process. Here we present time-resolved electric field measurements (with a temporal resolution of ~ 50 fs) of the light, initially reflected from, and subsequently transmitted through, an expanding overdense plasma. Our result provides insight into the dynamics of the transparent-overdense regime of relativistic plasmas, which should be useful in the development of laser-driven particle accelerators, X-ray sources and techniques for controlling the shape and contrast of intense laser pulses.