| 1. |
- Céolin, A, et al.
(author)
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Study of the Dissociation of Nitrous Oxide Following Resonant Excitation of the Nitrogen and Oxygen K-shells
- 2008
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In: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 128:2, s. 024306-
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Journal article (peer-reviewed)abstract
- A photochemistry study on nitrous oxide making use of site-selective excitation of terminal nitrogen, central nitrogen, and oxygen 1s -> 3 pi excitations is presented. The resonant Auger decay which takes place following excitation can lead to dissociation of the N2O+ ion. To elucidate the nuclear dynamics, energy-resolved Auger electrons were detected in coincidence with the ionic dissociation products, and a strong dependence of the fragmentation pathways on the core-hole site was observed in the binding energy region of the first satellite states. A description based on the molecular orbitals as well as the correlation between the thermodynamical thresholds of ion formation and the first electronic states of N2O+ has been used to qualitatively explain the observed fragmentation patterns.
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| 2. |
- Liu, X. J., et al.
(author)
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Young's double-slit experiment using core-level photoemission from N-2 : revisiting Cohen-Fano's two-centre interference phenomenon
- 2006
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In: Journal of Physics B. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 39:23, s. 4801-4817
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Journal article (peer-reviewed)abstract
- The core-level photoelectron spectra of N-2 molecules are observed at high energy resolution, resolving the 1 sigma(g) and 1 sigma(u) components as well as the vibrational components in the extended energy region from the threshold up to 1 keV. The sigma(g)/sigma(u) cross section ratios display modulation as a function of photoelectron momentum due to the two-centre interference, analogous to the classical Young's double-slit experiment, as predicted by Cohen and Fano a long time ago. The Cohen-Fano interference modulations display different phases depending on the vibrational excitations in the core-ionized state. Extensive ab initio calculations have been performed within the Hartree-Fock and random phase approximations in prolate spheroidal coordinates. The dependence of photoionization amplitudes on the vibrational states was taken into account using the Born-Oppenheimer approximation. The ab initio results are in reasonable agreement with the experimental data. The theoretical analysis allows the modulation to be connected with the onset of transitions to the states of increasing orbital angular momentum which occurs at increasing photon energies. Deviation from the Cohen-Fano formula is found for both the experimental and the ab initio results and is attributed to electron scattering by the neighbouring atom. A new formula for the interference modulation is derived within the framework of the multiple scattering technique. It differs from the classical Cohen-Fano formula by the addition of twice the scattering phase of the photoelectron by the neighbouring atom. We demonstrate that one can measure directly the scattering phase by fitting our formula to the experimental results.
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| 3. |
- Piancastelli, Maria Novella, et al.
(author)
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A High-resolution Study of Resonant Auger Decay Processes in N2O After Core Electron Excitation from Terminal Nitrogen, Central Nitrogen and Oxygen Atoms to the 3π LUMO
- 2007
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In: Journal of Physics B. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 40:17, s. 3357-3365
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Journal article (peer-reviewed)abstract
- Decay spectra of N2O following excitation to the N terminal (Nt) → π*, N central (Nc) → π* and O is → π* intermediate states are reported. The final states reached after participator decay show resonant enhancement consistent with a local-density-of-states analysis based on the Mulliken population of the valence molecular orbitals. In particular, the X-state is resonantly enhanced mostly after excitation from the Nt 1s and the O Is core levels to the π*, while the B-state is mostly enhanced following the excitation of the Nc Is → π* intermediate state. Below the Nt Is threshold, the lowest lying peak related to spectator decay falls at lower binding energy than the highest lying participator peak. This can be attributed to a particularly strong screening effect exerted by the excited electron in the LUMO.
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| 4. |
- Piancastelli, Maria Novella, et al.
(author)
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Electronic Structure of Core-excited and Core-ionized Methyl Oxirane
- 2007
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In: Journal of Electron Spectroscopy and Related Phenomena. - : Elsevier BV. - 0368-2048 .- 1873-2526. ; 156, s. 259-264
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Journal article (peer-reviewed)abstract
- We report a detailed analysis of the electronic structure of methyl oxirane, including core-level photoelectron spectroscopy, X-ray absorption at both C and O K-shells, resonant Auger and normal Auger spectroscopy. The X-ray absorption spectra (XAS) around the C K-edge can be easily interpreted on the ground of the chemical shift between the carbon atoms with different chemical environments. The X-ray absorption data around the O K-edge are quite structureless, hinting for a likely fragmentation process (possibly implying a ring-opening reaction). In resonant Auger spectra obtained after excitation below both the C 1s and O 1s ionization thresholds we notice a predominance of spectator decay implying a strong mixing between empty molecular orbitals and Rydberg states.
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| 5. |
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| 6. |
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| 7. |
- Thomas, T.D., et al.
(author)
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Photoelectron-recoil-induced rotational excitation of the B 2 state in N2
- 2009
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In: Physical Review A. Atomic, Molecular, and Optical Physics. - 1050-2947 .- 1094-1622. ; 79:022506
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Journal article (peer-reviewed)abstract
- In the photoelectron spectrum of N-2 the apparent ionization energy to form the B (2)Sigma(+)(u) state increases linearly with the photon energy. Rotationally resolved measurements of the fluorescent decay of this state show a linear increase of rotational heating with increasing photon energy. These results are in quantitative agreement with the prediction of the theory of recoil-induced rotational excitation, indicating that the rotational heating that has been observed previously arises primarily from such recoil-induced excitation. Together with other results that have been reported they show that recoil-induced internal excitation is significant in many situations, including near threshold.
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| 8. |
- Ueda, K., et al.
(author)
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Role of the recoil effect on two-center interference in x-ray photoionization
- 2006
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In: Chemical Physics. - : Elsevier BV. - 0301-0104 .- 1873-4421. ; 329:1-3, s. 329-337
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Journal article (peer-reviewed)abstract
- X-ray photoelectron spectra of the N-2 molecule are studied both experimentally and theoretically in the extended energy region up to 1 keV. The ratio of the photoionization cross sections for the gerade and ungerade core levels displays a modulation in the high energy region caused by the two-center interference, as predicted by Cohen and Fano (CF) in 1966. The physical background of this CF effect is the same as in Young's double-slit experiment. We have found that the interference pattern deviates significantly from the CF prediction. The origin of such a breakdown of the CF formula is the scattering of the photoelectron inside the molecule and the momentum transfer from the emitted fast photoelectron to the nuclei. Usually the recoil effect is small. We show that the electron recoil strongly affects the two-center interference pattern. Both stationary and dynamical aspects of the recoil effect shed light on the role of the momentum exchange in the two-center interference.
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| 9. |
- Baumjohann, W., et al.
(author)
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Dynamics of thin current sheets : Cluster observations
- 2007
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In: Annales Geophysicae. - : Copernicus GmbH. - 0992-7689 .- 1432-0576. ; 25:6, s. 1365-1389
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Research review (peer-reviewed)abstract
- The paper tries to sort out the specific signatures of the Near Earth Neutral Line (NENL) and the Current Disruption (CD) models. and looks for these signatures in Cluster data from two events. For both events transient magnetic si-natures are observed, together with fast ion flows. In the simplest form of NENL scenario, with a large-scale two-dimensional reconnection site, quasi-invariance along Y is expected. Thus the magnetic signatures in the S/C frame are interpreted as relative motions, along the X or Z direction, of a quasi-steady X-line, with respect to the S/C. In the simplest form of CD scenario an azimuthal modulation is expected. Hence the signatures in the S/C frame are interpreted as signatures of azimuthally (along Y) moving current system associated with low frequency fluctuations of J(y) and the corresponding field-aligned currents Event I covers a pseudo-breakup, developing only at high latitudes. First, a thin (H approximate to 2000Km approximate to 2 rho(i), with pi the ion gyroradius) Current Sheet (CS) is found to be quiet. A slightly thinner CS (H approximate to 1000-2000 km approximate to 1-2 rho(i)), crossed about 30 min later, is found to be active. with fast earthward ion flow bursts (300-600 km/s) and simultaneous large amplitude fluctuations (delta B/B similar to 1). In the quiet CS the current density J(y) is carried by ions. Conversely, in the active CS ions are moving eastward; the westward current is carried by electrons that move eastward, faster than ions. Similarly, the velocity of earthward flows (300-600 km/s), observed during the active period. maximizes near or at the CS center. During the active phase of Event I no signature of the crossing of an X-line is identified, but an X-line located beyond Cluster could account for the observed ion flows, provided that it is active for at least 20 min. Ion flow bursts can also be due to CD and to the corresponding dipolarizations which are associated with changes in the current density. Yet their durations are shorter than the duration of the active period. While the overall partial derivative Bz/partial derivative t is too weak to accelerate ions up to the observed velocities, short duration partial derivative B-z/partial derivative t can produce the azimuthal electric field requested to account for the observed ion flow bursts. The corresponding large amplitude perturbations are shown to move eastward. which suggests that the reduction in the tail current could be achieved via a series of eastward traveling partial dipolarisations/CD. The second event is much more active than the first one. The observed flapping of the CS corresponds to an azimuthally propagating wave. A reversal in the proton flow velocity, from 1000 to + 1000 km/s, is measured by CODIF. The overall flow reversal, the associated change in the sign of B-z and the relationship between B-x and B-y suggest that the spacecraft are moving with respect to an X-line and its associated Hall-structure. Yet, a simple tailward retreat of a large-scale X-line cannot account for all the observations, since several flow reversals are observed. These quasi-periodic flow reversals can also be associated with an azimuthal motion of the low frequency oscillations. Indeed, at the beginning of the interval B-y varies rapidly along the Y direction; the magnetic signature is three-dimensional and essentially corresponds to a structure of filamentary field-aligned current, moving eastward at similar to 200 km/s. The transverse size of the structure is similar to 1000 km. Similar structures are observed before and after. Thesefilamentary structures are consistent with an eastward propagation of an azimuthal modulation associated with a current system J(y), J(x). During Event 1, signatures of filamentary field-aligned current structures are also observed, in association with modulations of J(y). Hence, for both events the structure of the magnetic fields and currents is three-dimensional.
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| 10. |
- Gel'mukhanov, Faris, et al.
(author)
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Young's double-slit experiment using two-center core-level photoemission : Photoelectron recoil effects
- 2007
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In: Journal of Electron Spectroscopy and Related Phenomena. - : Elsevier BV. - 0368-2048 .- 1873-2526. ; 156, s. 265-269
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Journal article (peer-reviewed)abstract
- Core-level photoemission from N-2 can be considered an analogue of Young's double-slit experiment (YDSE) in which the double-slit is replaced by a pair of N 1s orbitals. The measured ratio between the 1 sigma(g) and 1 sigma(u) photoionization cross-sections oscillates as a function of photoelectron momentum, due to two-center YDSE interference, exhibiting a remarkable dependence on the vibrational sub-levels of the core ionized state. We theoretically demonstrate that the recoil of the photoelectron given to the ionized N atom strongly influences this interference pattern. The reason for this is that the momentum transfer affects the phases of the photoionization amplitudes.
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