Angular distributions in two-colour two-photon ionization of He

We present R-Matrix with time dependence (RMT) calculations for the photoionization of helium irradiated by an EUV laser pulse and an overlapping IR pulse with an emphasis on the anisotropy parameters of the sidebands generated by the dressing laser field. We investigate how these parameters depend on the amount of atomic structure included in the theoretical model for two-photon ionization. To verify the accuracy of the RMT approach, our theoretical results are compared with experiment.

Time-dependent R -matrix theory for ultrafast atomic processes

We describe an ab initio nonperturbative time-dependent R-matrix theory for ultrafast atomic processes. This theory enables investigations of the interaction of few-femtosecond and -attosecond pulse lasers with complex multielectron atoms and atomic ions. A derivation and analysis of the basic equations are given, which propagate the atomic wave function in the presence of the laser field forward in time in the internal and external R-matrix regions. To verify the accuracy of the approach, we investigate two-photon ionization of Ne irradiated by an intense laser pulse and compare current results with those obtained using the R-matrix Floquet method and an alternative time-dependent method. We also verify the capability of the current approach by applying it to the study of two-dimensional momentum distributions of electrons ejected from Ne due to irradiation by a sequence of 2 as light pulses in the presence of a 780 nm laser field.

R-matrix Floquet theory of multiphoton processes:VI. The negative halide ions

The R-matrix Floquet approach is applied to study the negative F and Cl ions in a light field. Detachment rates are obtained for detachment processes involving up to three photons. The results obtained in the present approach are compared to other experimental and theoretical results. For two- and three-photon processes reasonable agreement with other calculations has been found, while for two-photon detachment the results agree with the experimental cross sections. The three-photon results are in less good agreement with experiment although the larger error bars make accurate comparisons more difficult. The changes in the detachment behaviour for these ions are compared to each other as well as to the detachment behaviour of H.

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.

Relaxation processes in room temperature ionic liquids: The case of 1-butyl-3-methyl imidazolium hexafluorophosphate

A detailed investigation on the nature of the relaxation processes occurring in a typical room temperature ionic liquid (RTIL), namely, 1-butyl-3-methyl imidazolium hexafluorophosphate ([bmim][PF6]), is reported. The study was conducted using both elastic and inelastic neutron scattering over a wide temperature range from 10 to 400 K, accessing the dynamic features of both the liquid and glassy amorphous states. In this study, the inelastic fixed energy scan technique has been applied for the first time to this class of materials. Using this technique, the existence of two relaxation processes below the glass transition and a further diffusive process occurring above the glass-liquid transition are observed. The low temperature processes are associated with methyl group rotation and butyl chain relaxation in the glassy state and have been modeled in terms of two Debye-like, Arrhenius activated processes. The high temperature process has been modeled in terms of a Kohlraush-Williams-Watts relaxation, with a distinct Vogel-Fulcher-Tamman temperature dependence. These results provide novel information that will be useful in rationalizing the observed structural and dynamical behavior of RTILs in the amorphous state.

An experiment for two-color photoionization using high intensity extreme-UNT free electron and near-IR laser pulses

We describe an experimental system designed for single-shot photoelectron spectroscopy on free atoms and molecules at the Free Electron Laser in Hamburg (FLASH at DESY). The combination of the extreme ultra-violet (EUV) Free Electron Laser and a temporally synchronized optical fs laser (Ti:Sapphire) enables a variety of two-color pump-probe experiments. The spectral, temporal and spatial characteristics of both the EUV FEL and the optical laser pulses, the experimental procedure to control their overlap as well as the performance of an electron spectrometer used to obtain single-shot photoelectron spectra are discussed. As an illustration of the capabilities of this set-up, some results on two-photon two-color ionization of rare gases are presented. (c) 2007 Elsevier B.V. All rights reserved.

Partial and total multiphoton detachment rates for H- in a perturbative B-spline-based approach

An ab initio approach has been applied to study multiphoton detachment rates for the negative hydrogen ion in the lowest nonvanishing order of perturbation theory. The approach is based on the use of B splines allowing an accurate treatment of the electronic repulsion. Total detachment rates have been determined for two- to six-photon processes as well as partial rates for detachment into the different final symmetries. It is shown that B-spline expansions can yield accurate continuum and bound-state wave functions in a very simple manner. The calculated total rates for two- and three-photon detachment are in good agreement with other perturbative calculations. For more than three-photon detachment little information has been available before now. While the total cross sections show little structure, a fair amount of structure is predicted in the partial cross sections. In the two-photon process, it is shown that the detached electrons mainly have s character. For four- and six-photon processes, the contribution from the d channel is the most important. For three- and five-photon processes p electrons dominate the electron emission spectrum. Detachment rates for s and p electrons show minima as a function of photon energy. © 1994 The American Physical Society.

Direct Photodetachment of F‾ by mid-infrared few-cycle femtosecond laser pulses

The recent adiabatic saddle-point approach of Shearer et al. [ Phys. Rev. A 84 033409 (2011)] is extended to multiphoton detachment of negative ions with outer p-state electrons. This theory is applied to investigate the strong-field photodetachment dynamics of F- ions exposed to few-cycle femtosecond laser pulses, without taking into account the rescattering mechanism. Numerical calculations are considered for mid-infrared laser wavelengths of 1300 and 1800 nm at laser intensities of 7.7 × 1012, 1.1 × 1013, and 1.3 × 1013 W/cm2. Two-dimensional momenta saddle-point spectra exhibit a distinct distribution in the shape of a “smile” in the complex-time plane. Electron momentum distribution maps of direct electrons are investigated. These produce a distinct pattern of above-threshold detachment (ATD) concentric rings due to constructive and destructive quantum interference of electrons detached from their parent ions. Probability detachment distributions presented, capturing the influence of saturation effects that are found to become more significant with increasing laser intensity at a fixed wavelength. ATD photoangular distributions as functions of laser intensity and wavelength near channel closings are also investigated and found to be sensitive to initial-state symmetry. Nonmonotonic structures observed in the ejected photoelectron energy spectra are attributed to interference effects from coherent electronic wave packets. Additionally the profiles of all the photoelectron emission spectra show strong dependence on the carrier-envelope phase, indicating that it is a reliable parameter for characterizing the wave form of the pulse.

Effect of two different rice dehusking procedures on total arsenic concentration in rice

Pollution of subterranean water by arsenic (As) in Asia has resulted in the worst chemical disaster in human history. For populations living on subsistence rice diets, As contamination of rice grain contributes greatly to dietary As exposure. The main objectives of this study were to compare two dehusking processes: (a) wet process (soaking of rice, boiling and mechanical hulling) and (b) dry process (mechanical hulling), and recommend the method leading to a lower As content in commercial rice. In general, hulling of paddy rice (373 mu g As kg(-1)) significantly decreased As content in rice grain (311 mu g As kg(-1)). The final As concentrations in boiled rice (final product of the wet process) and atab rice (dry process) were 332 and 290 mu g kg(-1). Thus, the dry method is recommended for dehusking paddy rice if not As-free water is available. However, villagers can reduce the As content in the wet system by discarding the soaking water and using new water for the light boiling. Finally, it is not recommended to use rice husk for feeding animals because the As concentration is very high, approximately 1,000 mu g As kg(-1).

Multiphoton inner-shell ionization of the carbon atom

We apply time-dependent R-matrix theory to study inner-shell ionization of C atoms in ultra-short high-frequency light fields with a photon energy between 170 and 245 eV. At an intensity of 10¹⁷ W/cm², ionization is dominated by single-photon emission of a 2l electron, with two-photon emission of a 1s electron accounting for about 2-3% of all emission processes, and two-photon emission of 2l contributing about 0.5-1%. Three-photon emission of a 1s electron is estimated to contribute about 0.01-0.03%. Around a photon energy of 225 eV, two-photon emission of a 1s electron, leaving C⁺ in either 1s2s2p³ or 1s2p⁴ is resonantly enhanced by intermediate 1s2s²2p³ states. The results demonstrate the capability of time-dependent R-matrix theory to describe inner-shell ionization processes including rearrangement of the outer electrons.

Inner-shell photodetachment of excited 4S° and 6S° metastable bound states of Be-

The total cross sections for photodetachment of the metastable 1s ²2p^{3 4}S° and 1s2s2p^{3 6}S° excited bound states of the negative ion of beryllium are presented for a range of initial photon energies across and beyond the 1s detachment threshold. A multichannel close-coupling R-matrix approximation is used to compute the cross sections, with sophisticated configuration-interaction wavefunctions being used to represent the initial and final states. At present there are no other theoretical or experimental data available with which to compare the cross sections for these two photodetachment processes.

Single- and multiphoton detachment of K

Single- and multiphoton detachment rates have been calculated for K- using the R-matrix Floquet approach. Single-photon detachment rates, obtained at a laser field peak intensity of 10(9) W cm(-2), are discussed and compared with other theoretical work. Two-photon detachment rates at the same intensity have also been obtained, and similarities with results from earlier calculations for Li- and Na- are discussed. Three-photon rates are also presented at this laser intensity, and are compared and contrasted with those arising in the single-photon case, since both involve resonance structure with P-1(o) symmetry. The influence of resonances such as the 5s(2) S-1(e) doubly excited state and excitations of the residual atom are also considered.

Diagnostics on an atmospheric pressure plasma jet

The atmospheric pressure plasma jet (APPJ) is a homogeneous non-equilibrium discharge at ambient pressure. It operates with a noble base gas and a percentage-volume admixture of a molecular gas. Applications of the discharge are mainly based on reactive species in the effluent. The effluent region of a discharge operated in helium with an oxygen admixture has been investigated. The optical emission from atomic oxygen decreases with distance from the discharge but can still be observed several centimetres in the effluent. Ground state atomic oxygen, measured using absolutely calibrated two-photon laser induced fluorescence spectroscopy, shows a similar behaviour. Detailed understanding of energy transport mechanisms requires investigations of the discharge volume and the effluent region. An atmospheric pressure plasma jet has been designed providing excellent diagnostics access and a simple geometry ideally suited for modelling and simulation. Laser spectroscopy and optical emission spectroscopy can be applied in the discharge volume and the effluent region.

Spatially resolved diagnostics on a micro atmospheric pressure plasma jet

Despite enormous potential for technological applications, fundamentals of stable non-equilibrium micro-plasmas at ambient pressure are still only partly understood. Micro-plasma jets are one sub-group of these plasma sources. For an understanding it is particularly important to analyse transport phenomena of energy and particles within and between the core and effluent of the discharge. The complexity of the problem requires the combination and correlation of various highly sophisticated diagnostics yielding different information with an extremely high temporal and spatial resolution. A specially designed rf microscale atmospheric pressure plasma jet (µ-APPJ) provides excellent access for optical diagnostics to the discharge volume and the effluent region. This allows detailed investigations of the discharge dynamics and energy transport mechanisms from the discharge to the effluent. Here we present examples for diagnostics applicable to different regions and combine the results. The diagnostics applied are optical emission spectroscopy (OES) in the visible and ultraviolet and two-photon absorption laser-induced fluorescence spectroscopy. By the latter spatially resolved absolutely calibrated density maps of atomic oxygen have been determined for the effluent. OES yields an insight into energy transport mechanisms from the core into the effluent. The first results of spatially and phase-resolved OES measurements of the discharge dynamics of the core are presented.

CO dissociation and O removal on Co(0001): a density functional theory study

CO dissociation and O removal (water formation) are two important processes in the Fischer-Tropsch synthesis. In this study, both processes are studied on the flat and stepped Co(0 0 0 1) using density functional theory. It is found that (i) it is difficult for CO to dissociate on the flat Co(0 0 0 1) due to the high barrier of 1.04 eV relative to the CO molecule in the gas phase; (ii) the stepped Co(0 0 0 1) is much more favoured for CO dissociation; (iii) the first step in water formation, O + H --> OH, is unlikely to occur on the flat Co(0 0 0 1) due to the high barrier of 1.72 eV, however, this reaction can become feasible on steps where the barrier is reduced to 0.73 eV; and (iv) the barrier in the second step, OH + H --> H2O, on steps is higher than that on the flat surface. (C) 2004 Elsevier B.V. All rights reserved.