| 1. |
- Baev, A., et al.
(författare)
-
Doppler interference in dissociative resonant photoemission
- 2002
-
Ingår i: Physical Review A. Atomic, Molecular, and Optical Physics. - 1050-2947 .- 1094-1622. ; 66:2
-
Tidskriftsartikel (refereegranskat)abstract
- Resonant photoemission involving dissociative core excited states has been the subject of a great number of experimental and theoretical investigations in recent time. The resonant decay of such dissociating systems has been shown to lead to semiatomic Auger electron emission spectra, with particular angular behavior. In the present paper a detailed theoretical analysis of dissociative resonant photoemission spectra of homonuclear diatomic molecules is presented. The theory addresses both fixed in space and randomly oriented homonuclear molecules and emphasizes the Doppler effect and the role of the interference between channels referring to the Doppler split atomic fragments. It is shown that peaks originating from decay in the atomic fragments can be asymmetric and structured due to the Doppler interference effect. The predicted strong non-Lorentzian behavior of the substructure on the top of the Doppler broadened atomiclike contribution is traced to the interplay between decay channels leading to gerade and ungerade final states. Simulations based on wave-packet theory are compared with experimental data for molecular oxygen. Our numerical simulations of the atomiclike resonance of fixed in space molecules show that the spectral profile is very sensitive to the shape of interatomic potentials of core excited and final states. It is shown that the Doppler effect in the decay spectra depends upon the symmetry of the core excited state.
|
|
| 2. |
- Baev, A., et al.
(författare)
-
Geometrical information on core-excited states obtained from interference quenching of vibrational states in resonant x-ray photoemission
- 2003
-
Ingår i: Physical Review A. Atomic, Molecular, and Optical Physics. - 1050-2947 .- 1094-1622. ; 67:2
-
Tidskriftsartikel (refereegranskat)abstract
- An interference quenching of the m=1 final state vibrational line in the resonant Auger decay of N 1s-->pi(*) core-excited N-2 is observed and analyzed. The intensity ratio between the m=1 and m=0 vibrational levels of the X (2)Sigma(g)(+) final state shows a surprising nonmonotonic variation as a function of frequency detuning, going through a minimum with a complete suppression of m=1. We have developed a simple model which indicates a linear relation between the value of the detuning frequency for this minimum and the equilibrium bond distance of the core-excited state. This implies the possibility of determining the equilibrium bond distances for core-excited states to a high degree of accuracy. Simultaneously with the simple model we present a strict theory of the studied effect. This strict theory allows us to explore the accuracy of determining the bond length of the core-excited state from resonant Auger spectra. We obtain a weak influence of the core-hole lifetime on the determined bond length, whereas the number of intermediate vibrational states accounted for in the numerical simulations seems to be quite important.
|
|
| 3. |
- Barillot, T., et al.
(författare)
-
Angular asymmetry and attosecond time delay from the giant plasmon resonance in C60 photoionization
- 2015
-
Ingår i: Physical Review A. Atomic, Molecular, and Optical Physics. - 1050-2947 .- 1094-1622. ; 91
-
Tidskriftsartikel (refereegranskat)abstract
- This combined experimental and theoretical study demonstrates that the surface plasmon resonance in C 60 alters the valence photoemission quantum phase, resulting in strong effects in the photoelectron angular distribution and emission time delay. Electron momentum imaging spectroscopy is used to measure the photoelectron angular distribution asymmetry parameter that agrees well with our calculations from the time-dependent local density approximation (TDLDA). Significant structure in the valence photoemission time delay is simultaneously calculated by TDLDA over the plasmon active energies. Results reveal a unified spatial and temporal asymmetry pattern driven by the plasmon resonance and offer a sensitive probe of electron correlation. A semiclassical approach facilitates further insights into this link that can be generalized and applied to other molecular systems and nanometer-sized metallic materials exhibiting plasmon resonances.
|
|
| 4. |
- Feifel, R., et al.
(författare)
-
Profile of resonant photoelectron spectra versus the spectral function width and photon frequency detuning
- 2004
-
Ingår i: Physical Review A. Atomic, Molecular, and Optical Physics. - 1050-2947 .- 1094-1622. ; 70:3
-
Tidskriftsartikel (refereegranskat)abstract
- The outermost, singly ionized valence state of N-2, the X (2)Sigma(g)(+) state, is investigated in detail as a function of the photon frequency bandwidth for core excitation to the N 1s-->pi(*) resonance, where the photon frequency is tuned in between the first two vibrational levels of this bound intermediate electronic state. We find a strong, nontrivial dependence of the resulting resonant photoemission spectral profile on the monochromator function width and the frequency of its peak position. For narrow bandwidth excitation we observe a well resolved vibrational fine structure in the final electron spectrum, which for somewhat broader bandwidths gets smeared out into a continuous structure. For even broader monochromator bandwidths, it converts again into a well resolved vibrational progression. In addition, spectral features appearing below the adiabatic transition energy of the ground state of N-2(+) are observed for broadband excitation. A model taking into account the interplay of the partial scattering cross section with the spectral function is presented and applied to the X (2)Sigma(g)(+) final state of N-2(+).
|
|
| 5. |
- Kitajima, M., et al.
(författare)
-
Angle-resolved photoion yield and resonant Auger spectroscopy for the doubly excited Rydberg states above the C 1s threshold of CO
- 2008
-
Ingår i: Physical Review A. Atomic, Molecular, and Optical Physics. - 1050-2947 .- 1094-1622. ; 78:3, s. 033422-
-
Tidskriftsartikel (refereegranskat)abstract
- Doubly excited core-hole states of carbon monoxide in the photon energy region of 300-305 eV, i.e., directly above the C 1s ionization threshold, have been studied using both angle-resolved ion-yield and high-resolution resonant Auger spectroscopies. The leading configurations of the most prominent doubly excited Rydberg states are assigned by careful analysis of the ion-yield spectra and the final-state spectra to C 1s(-1) (5 sigma(-1)2 pi S-1=1) 3s sigma (v'=0,1,2), C 1s(-1) (5 sigma(-1)2 pi S-1=0) 3s sigma (v'=0,1,2), and C 1s(-1) (5 sigma(-1)2 pi S-1=1) 4s sigma (v'=0,1), which can only be populated via a conjugate shake-up process. Analysis of the resonant Auger spectra provides an assignment of several two-hole-one-electron (2h-1e) final states.
|
|
| 6. |
- Sorensen, S. L., et al.
(författare)
-
Electronic Doppler effect in resonant Auger decay of CO molecules upon excitation near a shake-up Pi resonance
- 2007
-
Ingår i: Physical Review A. Atomic, Molecular, and Optical Physics. - : APS. - 1050-2947 .- 1094-1622. ; 76:062704
-
Tidskriftsartikel (refereegranskat)abstract
- Wepresent an experimental observation of the electronic Doppler effect inresonant Auger spectra upon core excitation slightly above the carbonK edge of the CO molecule. Thus the electronic Dopplereffect has been identified in above-threshold excitation, and in atransition of symmetry. Ab initio calculations of the potentialenergy curves of the relevant states of CO and thewave packet technique have been employed to provide a theoreticalbackground to the experimental studies. The weak feature around 299.4 eVin the photoabsorption spectrum, whose decay has been investigated bythe present experiment, is assigned to double (core-valence) excitations toC 1s shake-up states |1s1−1*2 with a strong dissociative character,and the Doppler splitting of the atomic peak has beenreproduced by the simulation.
|
|
| 7. |
- Tanaka, T., et al.
(författare)
-
Symmetry-resolved x-ray absorption fine structure and resonant Auger-spectator-electron decay study of O 1s→Rydberg resonances in O2
- 2008
-
Ingår i: Physical Review A. Atomic, Molecular, and Optical Physics. - 1050-2947 .- 1094-1622. ; 78:2, s. 022516-
-
Tidskriftsartikel (refereegranskat)abstract
- A series of resonant Auger-electron spectra excited at selected photon energies across the O 1s -> Rydberg resonances in O-2 has been measured. Applying a spectator-electron shake relaxation model originally introduced for atomic resonant Auger-electron spectra, and using, to a large extent, the assignments for the core-excited resonances available from the literature, many of the observed spectator Auger-electron final states are assigned in terms of cationic Rydberg series. Vice versa the resonant Auger-electron spectra are used for consistency tests of the literature assignments for the core-excited intermediate Rydberg states. For some of the latter, alternative assignments are proposed for reasons discussed.
|
|
| 8. |
|
|
| 9. |
- Bueno, AM, et al.
(författare)
-
Influence of chemical bonds on the lifetime of the molecular-field-split 2p levels in H2S
- 2003
-
Ingår i: Physical Review A (Atomic, Molecular and Optical Physics). - 1050-2947. ; 67, s. 22714:1-7
-
Tidskriftsartikel (refereegranskat)abstract
- Different lifetime broadenings in molecular-field-split 2p core levels in H2S are predicted theoretically and are identified in an experimental investigation of the S 2p Auger electron spectrum. The measurements were performed for the transition to the vibrationally resolved X(1)A(1) ground state of H2S2+. The lifetimes of the 3e(1/2) and 5e(1/2) levels of the 2p ionized molecule are found to be 64 and 74 meV, respectively. This unambiguous determination of the lifetime difference of 10+/-1 meV is only possible as the 4e(1/2)-->X(1)A(1)(2b(1)(-2)) decay channel that overlaps the 5e(1/2)-->X(1)A(1)(2b(1)(-2)) channel is practically suppressed in Auger decay in H2S. The lifetime difference is confirmed by ab initio calculations. A theoretical analysis shows that it results from the mutual orientation of the core hole in the intermediate states and the valence electron density in the sulfur 3p orbitals. Both are strongly influenced by the chemical bond. Thus the observed effect is the direct result of a fundamental property of molecular electronic structure.
|
|
| 10. |
- Burmeister, F, et al.
(författare)
-
Nonadiabatic effects in photoelectron spectra of HCl and DCl. I. Experiment
- 2002
-
Ingår i: Physical Review A (Atomic, Molecular and Optical Physics). - 1050-2947. ; 65:1
-
Tidskriftsartikel (refereegranskat)abstract
- The HCl inner-valence photoelectron band at 26 eV binding energy has been recorded at high resolution. Discrete peaks arising from at least two separate vibrational progressions are superimposed on the broad continuum. Fano profiles are visible in one of the progressions. This indicates interference between superimposed electronic states, where weak avoided crossing allows two adiabatic states to couple. In the isotopic DCl molecular spectrum, the discrete lines are less pronounced, due to slower dissociation and therefore less coupling between the continuum and the bound state.
|
|
