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

Collisions Strengths and Effective Collision Strengths for transitions within the ground state configuration of S III

We have carried out a 29-state R-matrix calculation in order to calculate collision strengths and effective collision strengths for the electron impact excitation of S III. The recently developed parallel RMATRX II suite of codes have been used, which perform the calculation in intermediate coupling. Collision strengths have been generated over an electron energy range of 0-12 Ryd, and effective collision strength data have been calculated from these at electron temperatures in the range 1000-100,000 K. Results are here presented for the fine-structure transitions between the ground-state configurations of 3s(2)3p(2) P-3(0,1,2), D-1(2), and S-1(0), and the values given resolve a discrepancy between two previous R-matrix calculations.

Hyperfine interaction in the ground state of the negatively charged nitrogen vacancy center in diamond

The N-14, N-15, and C-13 hyperfine interactions in the ground state of the negatively charged nitrogen vacancy (NV-) center have been investigated using electron-paramagnetic-resonance spectroscopy. The previously published parameters for the N-14 hyperfine interaction do not produce a satisfactory fit to the experimental NV- electron-paramagnetic-resonance data. The small anisotropic component of the NV- hyperfine interaction can be explained from dipolar interaction between the nitrogen nucleus and the unpaired-electron probability density localized on the three carbon atoms neighboring the vacancy. Optical spin polarization of the NV- ground state was used to enhance the electron-paramagnetic-resonance sensitivity enabling detailed study of the hyperfine interaction with C-13 neighbors. The data confirmed the identification of three equivalent carbon nearest neighbors but indicated the next largest C-13 interaction is with six, rather than as previously assumed three, equivalent neighboring carbon atoms.

Monogamy and ground-state entanglement in highly connected systems

We consider the ground-state entanglement in highly connected many-body systems consisting of harmonic oscillators and spin-1/2 systems. Varying their degree of connectivity, we investigate the interplay between the enhancement of entanglement, due to connections, and its frustration, due to monogamy constraints. Remarkably, we see that in many situations the degree of entanglement in a highly connected system is essentially of the same order as in a low connected one. We also identify instances in which the entanglement decreases as the degree of connectivity increases.

Experimental linear-optics simulation of multipartite non-locality in the ground state of a quantum Ising ring

Critical phenomena involve structural changes in the correlations of its constituents. Such changes can be reproduced and characterized in quantum simulators able to tackle medium-to-large-size systems. We demonstrate these concepts by engineering the ground state of a three-spin Ising ring by using a pair of entangled photons. The effect of a simulated magnetic field, leading to a critical modification of the correlations within the ring, is analysed by studying two- and three-spin entanglement. In particular, we connect the violation of a multipartite Bell inequality with the amount of tripartite entanglement in our ring.

The scattering of low-energy electrons by argon atoms

Phaseshifts, differential, total and momentum transfer cross sections are calculated using an R-matrix approach for the elastic scattering of electrons by argon atoms in the impact energy range 0-19 eV. The coupled-state calculation is based upon a single-configuration atomic ground-state wavefunction coupled to a P pseudostate. A critical assessment of earlier theoretical and experimental data is made and the conclusion is reached that the present results are the most satisfactory over the entire energy range considered.

Diagnostic based modeling for determining absolute atomic oxygen densities in atmospheric pressure helium-oxygen plasmas

Absolute atomic oxygen ground state densities in a radio-frequency driven atmospheric pressure plasma jet, operated in a helium-oxygen mixture, are determined using diagnostic based modeling. One-dimensional numerical simulations of the electron dynamics are combined with time integrated optical emission spectroscopy. The population dynamics of the upper O 3p 3P (l=844 nm) atomic oxygen state is governed by direct electron impact excitation, dissociative excitation, radiation losses, and collisional induced quenching. Absolute values for atomic oxygen densities are obtained through comparison with the upper Ar 2p1 (l=750.4 nm) state. Results for spatial profiles and power variations are presented and show excellent quantitative agreement with independent two-photon laser-induced fluorescence measurements.

Fully differential cross sections for transfer ionization - a sensitive probe of high level correlation effects in atoms

The transfer ionization process offers a unique opportunity to study radial and angular electron correlations in the helium atom. We report calculations for the multiple differential cross sections of the transfer ionization process p + He --> H + He++ + e(-). The results of these calculations demonstrate the strong sensitivity of the fully differential cross sections to fine details of electron correlation in the target atom. Specifically, angular electron correlation in the ground state of helium results in a broad peak in the electron emission spectra in the backward direction, relative to the incoming beam. Our model explains some of the key effects observed in measurements of multiple differential cross sections using the COLTRIMS technique.

Phase-resolved emission spectroscopy of a hydrogen rf discharge for the determination of quenching coefficients

Collisional effects can have strong influences on the population densities of excited states in gas discharges at elevated pressure. The knowledge of the pertinent collisional coefficient describing the depopulation of a specific level (quenching coefficient) is, therefore, important for plasma diagnostics and simulations. Phase resolved optical emission spectroscopy (PROES) applied to a capacitively coupled rf discharge excited with a frequency of 13.56 MHz in hydrogen allows the measurement of quenching coefficients for emitting states of various species, particularly of noble gases, with molecular hydrogen as a collision partner. Quenching coefficients can be determined subsequent to electron-impact excitation during the short field reversal phase within the sheath region from the time behavior of the fluorescence. The PROES technique based on electron-impact excitation is not limited â?? in contrast to laser techniques â?? by optical selection rules and the energy gap between the ground state and the upper level of the observed transition. Measurements of quenching coefficients and natural fluorescence lifetimes are presented for several helium (3 1S,4 1S,3 3S,3 3P,4 3S), neon (2p1 ,2p2 ,2p4 ,2p6), argon (3d2 ,3d4 ,3d18 and 3d3), and krypton (2p1 ,2p5) states as well as for some states of the triplet system of molecular hydrogen.

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.

Absolute atomic oxygen density profiles in the discharge core of a microscale atmospheric pressure plasma jet

The micro atmospheric pressure plasma jet is an rf driven (13.56 MHz, ~20 W) capacitively coupled discharge producing a homogeneous plasma at ambient pressure when fed with a gas flow of helium (1.4 slm) containing small admixtures of oxygen (~0.5%). The design provides excellent optical access to the plasma core. Ground state atomic oxygen densities up to 3x1016 cm-3 are measured spatially resolved in the discharge core by absolutely calibrated two-photon absorption laser-induced fluorescence spectroscopy. The atomic oxygen density builds up over the first 8 mm of the discharge channel before saturating at a maximum level. The absolute value increases linearly with applied power.

Generation of Atomic Oxygen in the Effluent of an Atmospheric Pressure Plasma Jet

The planar 13.56MHz RF-excited low temperature atmospheric pressure plasma jet (APPJ) investigated in this study is operated with helium feed gas and a small molecular oxygen admixture. The effluent leaving the discharge through the jet’s nozzle contains very few charged particles and a high reactive oxygen species’ density. As its main reactive radical, essential for numerous applications, the ground state atomic oxygen density in the APPJ’s effluent is measured spatially resolved with two-photon absorption laser induced fluorescence spectroscopy. The atomic oxygen density at the nozzle reaches a value of ~1016 cm-3. Even at several centimetres distance still 1% of this initial atomic oxygen density can be detected. Optical emission spectroscopy (OES) reveals the presence of short living excited oxygen atoms up to 10 cm distance from the jet’s nozzle. The measured high ground state atomic oxygen density and the unaccounted for presence of excited atomic oxygen require further investigations on a possible energy transfer from the APPJ’s discharge region into the effluent: energetic vacuum ultraviolet radiation, measured by OES down to 110 nm, reaches far into the effluent where it is presumed to be responsible for the generation of atomic oxygen.

Three-photon detachment of electrons from the fluorine negative ion

Absolute three-photon detachment cross sections are calculated for the fluorine negative ion within the lowest-order perturbation theory. The Dyson equation of the atomic many-body theory is used to obtain the ground-state 2p wavefunction with correct asymptotic behaviour, corresponding to the true (experimental) binding energy. We show that in accordance with the adiabatic theory this is crucial for obtaining absolute values of the multiphoton cross sections. Comparisons with other calculations and experimental data are presented.

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.

TIME-RESOLVED ABSORPTION, INFRARED, AND RESONANCE RAMAN-SPECTRA OF THE COMPLEXES [RU(X)(R)(CO)(2)(ALPHA-DIIMINE)] (X=HALIDE R=ALKYL) - INFLUENCE OF X ON THE CHARGE-TRANSFER CHARACTER OF THE LOWEST EXCITED-STATE

Nanosecond time-resolved absorption (TA), resonance Raman (TR(3)), and infrared (TRIR) spectra are reported for several complexes [Ru(X)(R)(CO)(2)(alpha-diimine)] (X = Cl, Br, I; R = Me, Et; alpha-diimine = N,N'-diisopropyl-1,4-diaza-1,3-butadiene (iPr-DAB), pyridine-2-carbaldehyde-N-isopropylimine (iPr-PyCa), 2,2'-bipyridine (bpy)). This is the first instance in which the TA, TR(3), and TRIR techniques have been used to probe excited states in the same series of complexes. The TA spectra of the iodide complexes show a transient absorption between 550 and 700 nm, which does not depend on the solvent but shifts to lower energy in the order iPr-DAB > bpy > iPr-PyCa. This band is assigned to an intraligand transition. For the corresponding chloride and bromide complexes this band occurs at higher energy, most probably because of a change of character of the lowest excited state from XLCT to MLCT. The TRIR spectra show an increase in v(CO) (and k(CO)) on promotion to the excited state; however, the shifts Delta v(CO) show a decrease in the order Cl- > Br- > I-. The TR(3) spectra of the excited complexes [Ru(X)(R)(Co)(2)(iPr-DAB)] show v(s)(CN) of the iPr-DAB ligand 50-80 cm(-1) lower in frequency than for the complexes in their ground state. This frequency shift decreases in the order Cl- > Br- > I-, indicating a decrease of CT character of the lowest excited state in this order. However, going from X = Br to I, the effect on Delta v(CO) is much larger than the decrease of Delta v(s)(CN). This different effect on the CO- and CN-stretching frequencies is assigned to a gradual change in character of the lowest excited state from MLCT to XLCT when Cl- is replaced by Br- and I-. This result confirms a similar conclusion derived from previous resonance Raman and emission experiments on these complexes.