X-ray spectroscopy study of ThO2 and ThF4

The structure of the X-ray photoelectron, X-ray O(F)Ka-emission spectra from ThO2 and ThF4 as well as the Auger OKLL spectra from ThO2 was studied. The spectral structure was analyzed by using fully relativistic cluster discrete variational calculations of the electronic structure of the ThO8 D4h) and ThF8 (C2) clusters reflecting thorium close environment in solid ThO2 and ThF4. As a result it was theoretically found and experimentally confirmed that during the chemical bond formation the filled O(F)2p electronic states are distributed mainly in the binding energy range of the outer valence molecular orbitals from 0-13 eV, while the filled O(F)2s electronic states - in the binding energy range of the inner valence molecular orbitals from 13-35 eV. It was shown that the Auger OKLL spectral structure from ThO2 characterizes not only the O2p electronic state density distribution, but also the O2s electronic state density distribution. It agrees with the suggestion that O2s electrons participate in formation of the inner valence molecular orbitals, in the binding energy range of 13-35 eV. The relative Auger OKL2-3L2-3 peak intensity was shown to reflect quantitatively the O2p electronic state density of the oxygen ion in ThO2.

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Valence electronic state density in thorium dioxide

Nuclear Technology and Radiation Protection ◽

10.2298/ntrp0802034t ◽

2008 ◽

Vol 23 (2) ◽

pp. 34-42 ◽

Cited By ~ 9

Author(s):

Anton Teterin ◽

Mikhail Ryzhkov ◽

Yury Teterin ◽

Labud Vukcevic ◽

Vladimir Terekhov ◽

...

Keyword(s):

Electronic State ◽

State Density ◽

Molecular Orbitals ◽

Photoelectron Spectra ◽

Spectral Structure ◽

Discrete Variation ◽

Thorium Dioxide ◽

X Ray ◽

Electronic State Density ◽

First Time

This work analyses the fine low energy (0-40 eV) X-ray photoelectron spectra of ThO2, taking into account relativistic X?-discrete variation electronic structure calculations for the ThO8 (D4h) cluster reflecting thorium's close environment in ThO2. As a result, it was theoretically shown and experimentally confirmed that Th5f electrons in ThO2 can participate directly (~0.6 Th5f electrons) in chemical bond formation.Th6p electrons were shown to be a significant part (~0.44 Th6p electrons) not only of inner valence molecular orbitals, but to play a significant role in outer valence molecular orbitals formation, as well. Inner valence molecular orbitals composition and sequent order were established to belong to the binding energy range of 13 eV to 40 eV. The valence electronic state density in the range of 0-40 eV in ThO2 was also calculated. For the first time, these data allowed an interpretation of the fine X-ray photoelectron spectra (0-40 eV) and high resolution O4,5(Th) X-ray emition spectral structure (~60 - ~85 eV) of ThO2.

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X-ray photoelectron spectra structure and chemical bonding in AmO2

Nuclear Technology and Radiation Protection ◽

10.2298/ntrp1502083t ◽

2015 ◽

Vol 30 (2) ◽

pp. 83-98 ◽

Cited By ~ 4

Author(s):

Yury Teterin ◽

Konstantin Maslakov ◽

Mikhail Ryzhkov ◽

Anton Teterin ◽

Kirill Ivanov ◽

...

Keyword(s):

Binding Energy ◽

Energy Range ◽

Chemical Bond ◽

Theoretical Data ◽

Molecular Orbitals ◽

Binding Energies ◽

Photoelectron Spectra ◽

Spectral Structure ◽

Discrete Variation ◽

X Ray

Quantitative analysis was done of the X-ray photoelectron spectra structure in the binding energy range of 0 eV to ~35 eV for americium dioxide (AmO2) valence electrons. The binding energies and structure of the core electronic shells (~35 eV-1250 eV), as well as the relativistic discrete variation calculation results for the Am63O216 and AmO8 (D4h) cluster reflecting Am close environment in AmO2 were taken into account. The experimental data show that the many-body effects and the multiplet splitting contribute to the spectral structure much less than the effects of formation of the outer (0-~15 eV binding energy) and the inner (~15 eV-~35 eV binding energy) valence molecular orbitals. The filled Am 5f electronic states were shown to form in the AmO2 valence band. The Am 6p electrons participate in formation of both the inner and the outer valence molecular orbitals (bands). The filled Am 6p3/2 and the O 2s electronic shells were found to make the largest contributions to the formation of the inner valence molecular orbitals. Contributions of electrons from different molecular orbitals to the chemical bond in the AmO8 cluster were evaluated. Composition and sequence order of molecular orbitals in the binding energy range 0-~35 eV in AmO2 were established. The experimental and theoretical data allowed a quantitative scheme of molecular orbitals for AmO2, which is fundamental for both understanding the chemical bond nature in americium dioxide and the interpretation of other X-ray spectra of AmO2.

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X-Ray photoelectron study of actinide (Th, U, Pu, Am) nitrates

Nuclear Technology and Radiation Protection ◽

10.2298/ntrp0302031t ◽

2003 ◽

Vol 18 (2) ◽

pp. 31-35 ◽

Cited By ~ 7

Author(s):

Yury Teterin ◽

Anton Teterin ◽

Nikolay Yakovlev ◽

Igor Utkin ◽

Kirill Ivanov ◽

...

Keyword(s):

Binding Energy ◽

Energy Range ◽

Photoelectron Spectroscopy ◽

Molecular Orbitals ◽

Spectral Structure ◽

X Ray ◽

Atomic Orbitals ◽

Photoelectron Study ◽

Actinide Ions ◽

Outer Valence

In this work an X-ray photoelectron spectroscopy study of nitrates Th(NO3)4.4H2O UO2(NO3)2-nH2O, Pu(NO3)4-nH2O, and Am(NO3)2.nH2O was done in the binding energy range from 0 to 1000 eV in order to draw a correlation of the fine spectral structure parameters with the actinide ions oxidation states close environment structure, and chemical bond nature. The linearity of the dependence of the An5fn line intensity on the number n5f of the An5f electrons was proven to remain up to the Am3+ ion with the electron configu5fra-tion{Rn 5f6. The spectral structure in the binding energy range from 0 to ~ 15 eV was associated with the formation of the outer valence molecular orbitals due to the interaction of the An6d-, 7s, 5f - O2p electrons, and the fine spectral structure in the binding energy range from ~ 15 to ~50 eV - with the formation of the inner valence molecular orbitals due to the interaction of the An6p - O2s electrons from the filled neighboring atomic orbitals of actinide and oxygen in the studied compounds. The fine structure of the core level electron spectra in the binding energy range from ~50 to 1000 eV was shown to correlate with the actinide ion oxidation state.

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Electronic structure and chemical bond nature in Cs2PuO2Cl4

Nuclear Technology and Radiation Protection ◽

10.2298/ntrp1502099t ◽

2015 ◽

Vol 30 (2) ◽

pp. 99-112 ◽

Cited By ~ 1

Author(s):

Yury Teterin ◽

Konstantin Maslakov ◽

Mikhail Ryzhkov ◽

Anton Teterin ◽

Kirill Ivanov ◽

...

Keyword(s):

Binding Energy ◽

Energy Range ◽

Chemical Bond ◽

Theoretical Data ◽

Molecular Orbitals ◽

Binding Energies ◽

Spectral Structure ◽

Discrete Variation ◽

X Ray ◽

Outer Valence

X-ray photoelectron spectral analysis of dicaesiumtetrachlorodioxoplutonate (Cs2PuO2Cl4) single crystal was done in the binding energy range 0-~35 eV on the basis of binding energies and structure of the core electronic shells (~35 eV-1250 eV), as well as the relativistic discrete variation calculation results for the PuO2Cl4 (D4h). This cluster reflects Pu close environment in Cs2PuO2Cl4 containing the plutonyl group PuO2. The many-body effects due to the presence of cesium and chlorine were shown to contribute to the outer valence (0-~15 eV binding energy) spectral structure much less than to the inner valence (~15 eV- ~35 eV binding energy) one. The filled Pu 5f electronic states were theoretically calculated and experimentally con- firmed to present in the valence band of Cs2PuO2Cl4. It corroborates the suggestion on the direct participation of the Pu 5f electrons in the chemical bond. The Pu 6p atomic orbitals were shown to participate in formation of both the inner and the outer valence molecular orbitals (bands), while the filled Pu 6p and O 2s, Cl 3s electronic shells were found to take the largest part in formation of the inner valence molecular orbitals. The composition of molecular orbitals and the sequence order in the binding energy range 0-~35 eV in Cs2PuO2Cl4 were established. The quantitative scheme of molecular orbitals for Cs2PuO2Cl4 in the binding energy range 0-~15 eV was built on the basis of the experimental and theoretical data. It is fundamental for both understanding the chemical bond nature in Cs2PuO2Cl4 and the interpretation of other X-ray spectra of Cs2PuO2Cl4. The contributions to the chemical binding for the PuO2Cl4 cluster were evaluated to be: the contribution of the outer valence molecular orbitals -66 %, the contribution of the inner valence molecular orbitals -34 %.

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Valence XPS structure and chemical bond in Cs2UO2Cl4

Nuclear Technology and Radiation Protection ◽

10.2298/ntrp1601037t ◽

2016 ◽

Vol 31 (1) ◽

pp. 37-50 ◽

Cited By ~ 1

Author(s):

Yury Teterin ◽

Konstantin Maslakov ◽

Mikhail Ryzhkov ◽

Anton Teterin ◽

Kirill Ivanov ◽

...

Keyword(s):

Binding Energy ◽

Chemical Bond ◽

Theoretical Data ◽

Molecular Orbitals ◽

Photoelectron Spectra ◽

Spectral Structure ◽

Many Body ◽

Discrete Variation ◽

X Ray ◽

Calculation Results

Quantitative analysis was done of the valence electrons X-ray photoelectron spectra structure in the binding energy (BE) range of 0 eV to ~35 eV for crystalline dicaesium tetrachloro-dioxouranium (VI) (Cs2UO2Cl4). This compound contains the uranyl group UO2. The BE and structure of the core electronic shells (~35 eV-1250 eV), as well as the relativistic discrete variation calculation results for the UO2Cl4(D4h) cluster reflecting U close environment in Cs2UO2Cl4 were taken into account. The experimental data show that many-body effects due to the presence of cesium and chlorine contribute to the outer valence (0-~15 eV BE) spectral structure much less than to the inner valence (~15 eV-~35 eV BE) one. The filled U5f electronic states were theoretically calculated and experimentally confirmed to be present in the valence band of Cs2UO2Cl4. It corroborates the suggestion on the direct participation of the U5f electrons in the chemical bond. Electrons of the U6p atomic orbitals participate in formation of both the inner (IVMO) and the outer (OVMO) valence molecular orbitals (bands). The filled U6p and the O2s, Cl3s electronic shells were found to make the largest contributions to the IVMO formation. The molecular orbitals composition and the sequence order in the binding energy range 0 eV-~35 eV in the UO2Cl4 cluster were established. The experimental and theoretical data allowed a quantitative molecular orbitals scheme for the UO2Cl4 cluster in the BE range 0-~35 eV, which is fundamental for both understanding the chemical bond nature in Cs2UO2Cl4 and the interpretation of other X-ray spectra of Cs2UO2Cl4. The contributions to the chemical binding for the UO2Cl4 cluster were evaluated to be: the OVMO contribution - 76%, and the IVMO contribution - 24 %.

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Electronic structure and chemical bond nature in Cs2NpO2Cl4

Nuclear Technology and Radiation Protection ◽

10.2298/ntrp1701001t ◽

2017 ◽

Vol 32 (1) ◽

pp. 1-9 ◽

Cited By ~ 2

Author(s):

Yury Teterin ◽

Konstantin Maslakov ◽

Mikhail Ryzhkov ◽

Anton Teterin ◽

Kirill Ivanov ◽

...

Keyword(s):

Electronic Structure ◽

Binding Energy ◽

Energy Range ◽

Valence Band ◽

Chemical Bond ◽

Photoelectron Spectroscopy ◽

Theoretical Calculations ◽

Molecular Orbitals ◽

X Ray ◽

Outer Valence

On the basis of the X-ray photoelectron spectroscopy data and results of theoretical calculations for the NpO2Cl4 (D4h) cluster, the electronic structure and the chemical bond nature in , was done in the binding Cs2NpO2Cl4 single crystal, containing the neptunyl group NpO2 energy range of 0 eV to ~35 eV. The filled Np 5f electronic states were established to form in the valence band of Cs2NpO2Cl4. This was attributed to the direct participation of the Np 5f electrons in the chemical bonding. The Np 6p electrons were shown to participate in formation of both the inner valence band (~15 eV-~35 eV) and the outer valence band (0 eV-~15 eV). The filled Np 6p and the O 2s, Cl 3s electronic shells were found to make the largest contribution to the formation of the inner valence molecular orbitals. The molecular orbitals composition and the sequence order in the binding energy range 0 eV-~35 eV in Cs2NpO2Cl4, were established. For the first time the quantitative scheme of molecular orbitals for the NpO2Cl4 cluster in the binding energy range 0 eV-~35 eV, was built. This scheme reflects neptunium close environment in the studied compound and is fundamental for both understanding the chemical bond nature in Cs2NpO2Cl4 and the interpretation of other X-ray spectra of Cs2NpO2Cl4. The contributions to the chemical binding for the NpO2Cl4 cluster were evaluated to be: the outer valence molecular orbitals contribution - 73 %, and the inner valence molecular orbitals contribution - 27 %.

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X-ray spectral studies of the electronic structure of uranyl fluorite UO2F2

Nuclear Technology and Radiation Protection ◽

10.2298/ntrp0402015u ◽

2004 ◽

Vol 19 (2) ◽

pp. 15-23 ◽

Cited By ~ 3

Author(s):

Igor Utkin ◽

Yury Teterin ◽

Vladimir Terenov ◽

Mikhail Ryznkov ◽

Anton Teterin ◽

...

Keyword(s):

Binding Energy ◽

Axial Direction ◽

Molecular Orbitals ◽

Spectral Studies ◽

Spectral Structure ◽

Discrete Variation ◽

Uranyl Compounds ◽

X Ray ◽

Chemical Bond Formation ◽

Outer Valence

This work interpreted the fine X-ray photoelectron spectral structure of the low binding energy electrons (0-40 eV) and X-ray O4,5(U) emission spectral structure from UO2F2 taking into account the relativistic X? discrete variation (RX?-DV) calculation for the [(UO2)F6]4?(D6h) cluster reflecting an uranium close environment in UO2F2. The U5f electrons were shown to participate directly in the chemical bond formation. The U6p electrons were shown to participate not only information of the inner valence molecular orbitals, but also information of the outer valence molecular orbitals. The inner valence molecular orbitals sequence order in the binding energy range 12-40 eV was established. It is important for development of the technique of interatomic distance determination in the axial direction and equatorial plane of uranyl compounds on the X-ray photoelectron spectral basis.

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CORRELATION AMONG THE ELECTRONIC STATE IN Sn-DOPED YBCO SYSTEM

Modern Physics Letters B ◽

10.1142/s0217984991000691 ◽

1991 ◽

Vol 05 (08) ◽

pp. 581-585

Author(s):

H. ZHANG ◽

S.Q. FENG ◽

Q.R. FENG ◽

X. ZHU

Keyword(s):

Content Analysis ◽

Binding Energy ◽

Photoelectron Spectroscopy ◽

Strong Correlation ◽

Single Phase ◽

Vacuum Chamber ◽

High Vacuum ◽

Electronic States ◽

Ultra High Vacuum ◽

X Ray

We have performed an X-ray photoelectron spectroscopy investigation on single-phase samples of Sn -doped YBCO system, together with structure analysis, oxygen content analysis, and superconductivity measurements. The experiment gave evidence that there is a strong correlation between the electronic states of copper and oxygen. When the sample was heated to 600°C for 20 minutes in vacuum chamber, the oxygen escaped from the sample, the binding energy of Cu 2p was decreased, and the two indistinct components of O 1s became clear. Keeping the sample in ultra-high vacuum for 24 hours, a similar result was obtained.

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POLARIZATION DEPENDENCE OF RESONANT SOFT X-RAY EMISSION SPECTRA IN Ce COMPOUNDS

Surface Review and Letters ◽

10.1142/s0218625x02003184 ◽

2002 ◽

Vol 09 (02) ◽

pp. 983-987 ◽

Cited By ~ 8

Author(s):

M. WATANABE ◽

Y. HARADA ◽

M. NAKAZAWA ◽

Y. ISHIWATA ◽

R. EGUCHI ◽

...

Keyword(s):

Energy Range ◽

Electronic Structures ◽

Emission Spectroscopy ◽

Electronic States ◽

Emission Spectra ◽

Polarization Dependence ◽

Raman Peak ◽

Electron Hole ◽

Resonant Energy ◽

X Ray

The electronic structures of Ce compounds have been investigated by means of resonant soft X-ray emission spectroscopy (RXES) excited at resonant energy range of Ce 3d → 4f absorption. Polarization dependence of the RXES shows information on concerning electronic states. In CeO 2, the Ce 4f → 3d RXES spectra are interpreted as electronic structures hybridized between 4f0 and [Formula: see text] states. Peaks appearing in the spectra are attributed to bonding, nonbonding, and antibonding states between those states, while the spectra of CeRh 3 cannot be explained by only using the hybridization between 4f0 and [Formula: see text] states. The spectra have large broad Raman peak, especially when the excitation photon energy is set at satellite of Ce 3d → 4f absorption. We attribute the origin of the broad Raman peak to hybridization states involving electron–hole pairs.

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