Generation and control of ultrafast pulse trains for quasi-phase-matching high-harmonic generation

Two techniques are demonstrated to produce ultrashort pulse trains capable of quasi-phase-matching high-harmonic generation. The first technique makes use of an array of birefringent crystals and is shown to generate high-contrast pulse trains with constant pulse spacing. The second technique employs a grating-pair stretcher, a multiple-order wave plate, and a linear polarizer. Trains of up to 100 pulses are demonstrated with this technique, with almost constant inter-pulse separation. It is shown that arbitrary pulse separation can be achieved by introducing the appropriate dispersion. This principle is demonstrated by using an acousto-optic programmable dispersive filter to introduce third-and fourth-order dispersions leading to a linear and quadratic variation of the separation of pulses through the train. Chirped-pulse trains of this type may be used to quasi-phase-match high-harmonic generation in situations where the coherence length varies through the medium. (C) 2010 Optical Society of America

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.

Low pressure carbon dioxide solubility in pure electrolyte solvents for lithium-ion batteries as a function of temperature. Measurement and prediction

Experimental values for the carbon dioxide solubility in eight pure electrolyte solvents for lithium ion batteries – such as ethylene carbonate (EC), propylene carbonate (PC), dimethyl carbonate (DMC), ethyl methyl carbonate (EMC), diethyl carbonate (DEC), ?-butyrolactone (?BL), ethyl acetate (EA) and methyl propionate (MP) – are reported as a function of temperature from (283 to 353) K and atmospheric pressure. Based on experimental solubility data, the Henry’s law constant of the carbon dioxide in these solvents was then deduced and compared with reported values from the literature, as well as with those predicted by using COSMO-RS methodology within COSMOthermX software and those calculated by the Peng–Robinson equation of state implemented into Aspen plus. From this work, it appears that the CO2 solubility is higher in linear carbonates (such as DMC, EMC, DEC) than in cyclic ones (EC, PC, ?BL). Furthermore, the highest CO2 solubility was obtained in MP and EA solvents, which are comparable to the solubility values reported in classical ionicliquids. The precision and accuracy of the experimental values, considered as the per cent of the relative average absolute deviations of the Henry’s law constants from appropriate smoothing equations and from literature values, are close to (1% and 15%), respectively. From the variation of the Henry’s law constants with temperature, the partial molar thermodynamic functions of dissolution such as the standard Gibbs free energy, the enthalpy, and the entropy are calculated, as well as the mixing enthalpy of the solvent with CO2 in its hypothetical liquid state.

DNA damage induction in dry and hydrated DNA by synchrotron radiation

Radiation biophysics has sought to understand at a molecular level, the mechanisms through which ionizing radiations damage DNA, and other molecules within living cells. The complexity of lesions produced in the DNA by ionizing radiations is thought to depend on the amount of energy deposited at the site of each lesion. To study the relationship between the energy deposited and the damage produced, we have developed novel techniques for irradiating dry prasmid DNA, partially re-hydrated DNA and DNA in solution using monochromatic vacuum-UV synchrotron radiation. We have used photons in the energy range 7-150 eV, corresponding to the range of energies typically involved in the efficient production of DNA single-strand (SSB), and double-strand breaks (DSB) by ionizing radiation. The data show that both types of breaks are produced at all energies investigated (with, or without water present). Also, the energy dependence for DSB induction follows a similar trend to SSB induction but at a 20-30-fold reduced incidence, suggesting a common precursor for both types of damage. Preliminary studies where DNA has been irradiated in solution indicate a change in the shape of the dose-effect curve (from linear, to linear-quadratic for double-strand break induction) and a large increase in sensitivity due to the presence of water.

Dielectronic recombination of ground-state and metastable Li+ ions

Dielectronic recombination has been investigated for Delta n = 1 resonances of ground-state Li+(1s(2)) and for Delta n = 0 resonances of metastable Li (+) (1s2s S-3). The ground-state spectrum shows three prominent transitions between 53 and 64 eV, while the metastable spectrum exhibits many transitions with energies

Time delay between photoemission from the 2p and 2s subshells of neon

The R-matrix incorporating time (RMT) method is a method developed recently for solving the time-dependent Schrödinger equation for multielectron atomic systems exposed to intense short-pulse laser light. We have employed the RMT method to investigate the time delay in the photoemission of an electron liberated from a 2p orbital in a neon atom with respect to one released from a 2s orbital following absorption of an attosecond xuv pulse. Time delays due to xuv pulses in the range 76-105 eV are presented. For an xuv pulse at the experimentally relevant energy of 105.2 eV, we calculate the time delay to be 10.2±1.3 attoseconds (as), somewhat larger than estimated by other theoretical calculations, but still a factor of 2 smaller than experiment. We repeated the calculation for a photon energy of 89.8 eV with a larger basis set capable of modeling correlated-electron dynamics within the neon atom and the residual Ne ion. A time delay of 14.5±1.5 as was observed, compared to a 16.7±1.5 as result using a single-configuration representation of the residual Ne⁺ ion. 

Measurement of absolute charge-exchange cross sections for He2+ collisions with He and H-2

Reported are total, absolute charge-exchange cross sections for collisions of 3He(2+) ions with He and H-2. Measurements are reported at fixed energies between 0.33 and 4.67 keV/amu. Both the present results and earlier results of others are analyzed in terms of available experimental small-angle differential cross sections as a function of collision energy, and hence the geometry of the exit aperture of the gas-collision cells used by the various experimental groups. In addition, the effective length of gas-collision cells is studied using fluid dynamic and molecular flow simulations to address the density patterns near the cell entrance and exit apertures. When small acceptance-angle corrections were applied, the results of present and previous measurements for the single electron capture in these systems were brought into good accord in the relevant energy ranges. Taken in their entirety, the present data for 3He(2+) with He and H-2 lend themselves to new theoretical calculations of the multichannel charge-exchange cross sections.

Phase Behaviour, Interactions, and Structural Studies of (Amines+Ionic Liquids) Binary Mixtures

We present a study on the phase equilibrium behaviour of binary mixtures containing two 1-alkyl-3-methylimidazolium bis{(trifluoromethyl)sulfonyl}imide-based ionic liquids, [Cnmim] [NTf2] (n=2 and 4), mixed with diethylamine or triethylamine as a function of temperature and composition using different experimental techniques. Based on this work, two systems showing an LCST and one system with a possible hourglass shape are measured. Their phase behaviours are then correlated and predicted by using Flory–Huggins equations and the UNIQUAC method implemented in Aspen. The potential of the COSMO-RS methodology to predict the phase equilibria was also tested for the binary systems studied. However, this methodology is unable to predict the trends obtained experimentally, limiting its use for systems involving amines in ionic liquids. The liquid-state structure of the binary mixture ([C2mim] [NTf2]+diethylamine) is also investigated by molecular dynamics simulation and neutron diffraction. Finally, the absorption of gaseous ethane by the ([C2mim][NTf2]+diethylamine) binary mixture is determined and compared with that observed in the pure solvents.

Configuration-interaction effects in and intensity dependence of F- multiphoton detachment

Two- and three-photon detachment rates have been obtained for F- using several expansions in the R-matrix Floquet approach. These rates are compared with other theoretical and experimental results. The use of Hartree-Fock wavefunctions for the ground state of F with addition of continuum electrons does not lead to agreement with experiment for two- and three-photon detachment. By adding correlation terms, agreement with experiment and other theoretical results is improved considerably, demonstrating the importance of electron correlation effects. However, convergence with respect to the wavefunction expansion cannot be established, we also study the intensity dependence of multiphoton detachment rates for F- at the Nd-YAG frequency. Due to the ponderomotive shift the three-photon detachment channel closes at an intensity of 8.5 x 10(11) W cm(-2) and the influence of this channel closure on the multiphoton detachment peaks is illustrated by determining the heights of the excess-photon peaks obtained using a Gaussian laser pulse.

Energy levels, wavefunction compositions and electric dipole transitions in neutral Ca

A configuration-interaction approach, based on the use of B-spline basis sets combined with a model potential including monoelectronic and dielectronic core polarization effects, is employed to calculate term energies and wavefunctions for neutral Ca. Results are reported for singlet and triplet bound states, and some quasi-bound states above the lowest ionization limit, with angular momentum up to L = 4. Comparison with experiment and with other theoretical results shows that this method yields the most accurate energy values for neutral Ca obtained to date. Wavefunction compositions, necessary for labelling the levels, and the effects of semi-empirical polarization potentials on the wavefunctions are discussed, as are some recent identifications of doubly-excited states. It is shown that taking into account dielectronic core polarization changes the energies of the lowest terms in Ca significantly, in general by a few hundred cm(-1), the effect decreasing rapidly for the higher bound states. For Rydberg states with n approximate to 7 the accuracy of the results is often better than a few cm(-1). For series members (or perturbers) with a pronounced 3d character the error can reach 150 cm(-1). The wavefunctions are used to calculate oscillator strengths and lifetimes for a number of terms and these are compared with existing measurements. The agreement is good but points to a need for improved measurements.

Photon collisions with atoms and ions within an intermediate-energy R-matrix framework

Recent experimental advances in light technology necessitate the availability of sophisticated theoretical models which can incorporate an accurate treatment of double-electron continua. We describe here a new intermediate-energy R-matrix approach to photoionisation and photo-double-ionisation and illustrate its feasibilty by application to photoionisation and photo-double-ionisation of He, and photodetachment and photo-double-detachment of H^-. Results are shown to be in excellent agreement with previous theoretical and experimental studies. This work is a key step in the development of a multipurpose R-matrix code for multiple-electron ejection. © 2012 American Physical Society

Singly, doubly and triply resonant multiphoton processes involving autoionizing states in magnesium

Using the R-matrix Floquet theory we have carried out non-perturbative, ab initio one- and two-colour calculations of the multiphoton ionization of magnesium with the laser frequencies chosen such that the initial state of the atom is resonantly coupled with autoionizing resonances of the atom. Good agreement is obtained with previous calculations in the low-intensity regimes. The single-photon ionization from the 3s3p P excited state of magnesium has been studied in the vicinity of the 3p S autoionizing resonance at non-perturbative laser intensities. Laser-induced degenerate states (LIDS) are observed for modest laser intensities. By adding a second laser which resonantly couples the 3p S = and 3p3d P autoionizing levels, we show that, due to the small width of the 3p3d P state, LIDS occur between this state and the 3s3p P state at intensities of the first laser below 10 W cm . We next investigate the case in which the first laser induces a resonant two-photon coupling between the ground state and the 3p S autoionizing state, while the second laser again resonantly couples the respective 3p S and 3p3d P autoionizing states. At weak intensities, our calculations compare favourably with recent experimental data and calculations. We show that when the intensity of the first laser is increased, the effect of an additional autoionizing state, the 4s5s S state, becomes significant. This state is coupled to the 3p3d P autoionizing level by one photon, inducing a triply resonant processes. We show that LIDS occur among the three autoionizing levels and we discuss their effect on the decay rate of the ground state. We consider dressed two- and three-level atoms which can be used to model the results of our calculations.

Structure and interactions of ultracold Yb ions and Rb atoms

In order to study ultracold charge-transfer processes in hybrid atom-ion traps, we have mapped out the potential-energy curves and molecular parameters for several low-lying states of the Rb, Yb+ system. We employ both a multireference configuration interaction and a full configuration interaction (FCI) approach. Turning points, crossing points, potential minima, and spectroscopic molecular constants are obtained for the lowest five molecular states. Long-range parameters, including the dispersion coefficients, are estimated from our ab initio data. The separated-atom ionization potentials and atomic polarizability of the ytterbium atom (ad=128.4 atomic units) are in good agreement with experiment and previous calculations. We present some dynamical calculations for (adiabatic) scattering lengths for the two lowest (Yb, Rb+) channels that were carried out in our work. However, we find that the pseudopotential approximation is rather limited in validity and only applies to nK temperatures. The adiabatic scattering lengths for both the triplet and singlet channels indicate that both are large and negative in the FCI approximation.