| 1. |
- Butorin, Sergei, et al.
(författare)
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Effect of Ag Doping on Electronic Structure of Cluster Compounds AgxMo9Se11 (x = 3.4, 3.9)
- 2018
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Ingår i: ACS Applied Energy Materials. - : American Chemical Society (ACS). - 2574-0962. ; 1:8, s. 4032-4039
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Tidskriftsartikel (refereegranskat)abstract
- The electronic structure of AgxMo9Se11 as a potential material for thermoelectric applications was studied using high-energy-resolution fluorescence-detection X-ray absorption spectroscopy (HERFD-XAS) and the resonant inelastic X-ray scattering (RIXS) technique. The experiments were supported by first-principle calculations using density functional theory (DFT). The analysis of obtained spectra indicate the presence of subvalent (less than 1+) Ag in AgxMo9Se11. The advanced HERFD-XAS measurements allowed us to resolve the contribution of the electronic states at the Fermi level of AgxMo9Se11 and to monitor its dependence on the x value. A comparison of the experimental data with the results of the DFT calculations suggests the importance of the Ag2-type sites with the shortest Ag–Se distance for affecting the properties of AgxMo9Se11.
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| 2. |
- Kapaklis, Vassilios, et al.
(författare)
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Temperature dependence of the electrical resistivity and electronic structure of amorphous Fe100-xZrx films and multilayers
- 2012
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Ingår i: Journal of Physics. - : IOP Publishing. - 0953-8984 .- 1361-648X. ; 24:49, s. 495402-
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Tidskriftsartikel (refereegranskat)abstract
- The electrical resistivity of amorphous Fe100-xZrx metal alloy films and multilayers has been investigated in a wide temperature and composition range. The overall behavior of the resistivity is consistent with bulk measurements, exhibiting prominent semiconductor-like changes at low temperatures. The transition from positive (metallic) to negative temperature coefficient of resistivity behavior is accompanied by minute changes in magnetoresistance and we can therefore rule out magnetic phase changes as being the cause for the observed changes in the resistivity. Using x-ray absorption and emission spectroscopies we are able to probe the unoccupied and occupied electronic densities of states. The corresponding spectra are found to significantly overlap, as expected for a metallic-like electronic structure and the absence of a band gap. Besides a broadening of the x-ray emission lines expected from an amorphous material, remarkably small differences are observed in the electronic structures when changing the amount of Zr. The resistivity data were modeled and agreement with the Mott variable range hopping model was found, indicating localized electronic states due the disordered structure of the Fe100-xZrx alloys.
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| 3. |
- Kokkonen, E., et al.
(författare)
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Formation of stable HCl+ following resonant Auger decay in CH3Cl
- 2016
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Ingår i: PHYSICAL REVIEW A. - : American Physical Society. - 2469-9926. ; 94:3
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Tidskriftsartikel (refereegranskat)abstract
- Photoinduced reformation of chemical bonds is investigated in the CH3Cl molecule experimentally and computationally. The observation of stable HCl+ fragment formation after resonant Cl 2p photoexcitation is confirmed by an electron-ion coincidence experiment, and its possible creation mechanism is reported. We attribute the formation of HCl+ to specific final states populated by the resonant Auger decay. Quantum chemical computations support this attribution and suggest that in at least one of those states the system is placed on a potential energy surface which favors creation of HCl+ by moving one hydrogen atom to a closer proximity of the chlorine atom. This work demonstrates the effect of targeted core-shell excitation on the chemical bond breaking and reformation process, often called photoinduced chemistry.
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| 4. |
- Mailhiot, M., et al.
(författare)
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Multielectron coincidence spectroscopy of the Ar2+(2p-2) double-core-hole decay
- 2023
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Ingår i: Physical Review A. - 2469-9926. ; 107:6
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Tidskriftsartikel (refereegranskat)abstract
- The dominant decay pathways of argon 2p-2 double-core-hole states have been investigated using synchrotron radiation and a magnetic-bottle-type spectrometer coupled with an ion time-of-flight spectrometer. This experiment allows for efficient multi-electron-ion coincidence measurements, and thus for following the Auger cascade step by step in detail. Dominant decay pathways leading to Ar4+ final states via Ar3+ intermediate states have been assigned with the help of theoretical ab initio calculations. The weak correlated decay of the two core holes by emission of a single Auger electron, leading to Ar3+ final states, has been observed at 458.5-eV kinetic energy. Compared to the total decay of the 2p-2 double core vacancies, this two-electron-one-electron process was measured to have a branching ratio of 1.9 x 10-3 & PLUSMN; 1.0 x 10-3. Furthermore, the remaining decay paths of the Ar1+ (1s-1) core hole to higher charge states and their respective contributions to the total yield have been analyzed and show very good agreement with theoretical results.
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| 5. |
- Marchenko, T., et al.
(författare)
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Potential Energy Surface Reconstruction and Lifetime Determination of Molecular Double-Core-Hole States in the Hard X-Ray Regime
- 2017
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Ingår i: Physical Review Letters. - : AMER PHYSICAL SOC. - 0031-9007 .- 1079-7114. ; 119:13
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Tidskriftsartikel (refereegranskat)abstract
- A combination of resonant inelastic x-ray scattering and resonant Auger spectroscopy provides complementary information on the dynamic response of resonantly excited molecules. This is exemplified for CH3I, for which we reconstruct the potential energy surface of the dissociative I 3d(-2) double-core-hole state and determine its lifetime. The proposed method holds a strong potential for monitoring the hard x-ray induced electron and nuclear dynamic response of core-excited molecules containing heavy elements, where ab initio calculations of potential energy surfaces and lifetimes remain challenging.
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| 6. |
- Žitnik, M., et al.
(författare)
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Atomic two-color XUV interferometer
- 2023
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Ingår i: 2023 Conference on Lasers and Electro-Optics Europe and European Quantum Electronics Conference, CLEO/Europe-EQEC 2023. - 9798350345995
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Konferensbidrag (refereegranskat)abstract
- We extend our recently published work which demonstrated the coherent control of population of 2s21S doubly excited state in helium by tuning the interference of ω1 + ω1 and ω3 − ω1 two-photon excitation paths [1]. The maximum yield of electrons from 2s2 autoionization was observed when the two-color phase difference matched phase difference of the atomic amplitudes describing the two alternative excitation paths. A displacement of position of the maximum yield in the same reference frame therefore signals the presence of an additional phase shifting agent along any of the two paths and also provides a measure of the corresponding phase shift. This constitutes the operational principle of an atomic XUV interferometer which is comparable to the well-known RABBITT method based on using a combination of XUV and IR light pulses [2]. The work was performed at LDM beamline at the free-electron-laser facility FERMI in Trieste (Italy). The phase difference of the two components of the light pulse was set by slightly delaying the ω3 emission from the last three undulators with respect to the ω1 emission produced by the first three undulators and this was achieved by delaying the generating electron bunch by properly adjusted magnetic chicane in between the two undulator sections.
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| 7. |
- Zitnik, M, et al.
(författare)
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High resolution multiphoton spectroscopy by a tunable free-electron-laser light.
- 2014
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Ingår i: Physical Review Letters. - 1079-7114 .- 0031-9007. ; 113:19
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Tidskriftsartikel (refereegranskat)abstract
- Seeded free electron lasers theoretically have the intensity, tunability, and resolution required for multiphoton spectroscopy of atomic and molecular species. Using the seeded free electron laser FERMI and a novel detection scheme, we have revealed the two-photon excitation spectra of dipole-forbidden doubly excited states in helium. The spectral profiles of the lowest (-1,0)^{+1} ^{1}S^{e} and (0,1)^{0} ^{1}D^{e} resonances display energy shifts in the meV range that depend on the pulse intensity. The results are explained by an effective two-level model based on calculated Rabi frequencies and decay rates.
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| 8. |
- Zitnik, M., et al.
(författare)
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Interference of two-photon transitions induced by XUV light
- 2022
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Ingår i: Optica. - : Optica Publishing Group. - 2334-2536. ; 9:7, s. 692-700
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Tidskriftsartikel (refereegranskat)abstract
- The relative phase of first (omega(1)) and third harmonics (omega(3)) extreme ultraviolet light pulses was varied to control the population of the 2s(2) state in helium through the interference of omega(1) + omega(1) and omega(3) - omega(1) two-photon excitation paths. The population was monitored by observing the total electron yield due to the 2s(2) autoionization decay. Maximum yield occurs when the relative phase of the two harmonics matches the phase difference of complex atomic amplitudes governing the two excitation paths. The calculated trend of atomic phase differences agrees well with the measured data in the spectral region of the resonance, provided that time-reversed -omega(1) + omega(3) path is also taken into account. These results open the way to accessing phase differences of two-photon ionization paths involving energetically distant intermediate states and to perform interferometry in the extreme ultraviolet range by monitoring final state populations. (c) 2022 Optica Publishing Group under the terms of the Optica Open Access Publishing Agreement
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| 9. |
- Iwayama, H., et al.
(författare)
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A local chemical environment effect in site-specific Auger spectra of ethyl trifluoroacetate
- 2013
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Ingår i: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 138:2, s. 024306-
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Tidskriftsartikel (refereegranskat)abstract
- We have investigated a local chemical environment effect on Auger spectra of ethyl trifluoroacetate (C4H5F3O2), using multi-electron coincidence spectroscopy and high-resolution electron spectroscopy. Site-specific KVV Auger spectra for each carbon atom, and for the fluorine and oxygen atoms are presented. The extent of hole localization in the final dicationic states was investigated with the help of theoretical calculations based on a two-hole population analysis. The Auger spectra have been simulated using a statistical approach. It is found that all Auger decays populate mainly localized dicationic states, with the two holes located either on the same fluorine atom or on adjacent fluorine atoms. While the decay of the F 1s hole populates exclusively the former states, the latter class of states is also populated by the decay of the C and O 1s holes.
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| 10. |
- Marchenko, T., et al.
(författare)
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Electron Dynamics in the Core-Excited CS2 Molecule Revealed through Resonant Inelastic X-Ray Scattering Spectroscopy
- 2015
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Ingår i: Physical Review X. - 2160-3308. ; 5:3
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Tidskriftsartikel (refereegranskat)abstract
- We present an experimental and theoretical study of resonant inelastic x-ray scattering (RIXS) in the carbon disulphide CS 2 molecule near the sulfur K-absorption edge. We observe a strong evolution of the RIXS spectral profile with the excitation energy tuned below the lowest unoccupied molecular orbital (LUMO) absorption resonance. The reason for this is twofold. Reducing the photon energy in the vicinity of the LUMO absorption resonance leads to a relative suppression of the LUMO contribution with respect to the emission signal from the higher unoccupied molecular orbitals, which results in the modulation of the total RIXS profile. At even larger negative photon-energy detuning from the resonance, the excitation-energy dependence of the RIXS profile is dominated by the onset of electron dynamics triggered by a coherent excitation of multiple electronic states. Furthermore, our study demonstrates that in the hard x-ray regime, localization of the S 1s core hole occurs in CS2 during the RIXS process because of the orientational dephasing of interference between the waves scattering on the two sulfur atoms. Core-hole localization leads to violation of the symmetry selection rules for the electron transitions observed in the spectra.
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