Bulk-sensitive Mo 4d electronic structure of Sr₂FeMoO₆probed by high-energy Mo L₃resonant photoemission

Abstract

We studied the Mo 4d electronic structure of Sr2FeMoO6 using high-energy Mo L3 resonant photoemission. The experimental spectra are in good agreement with modified Becke-Johnson (mBJ) band structure calculations. The energy dependence of the spectra can be explained by the changes in the photoemission cross-sections. The Mo L3 resonant spectrum shows Mo 4d character below the Fermi level and mixed Mo 4d-O 2p character around 8.0 eV. The Mo 4d weight in the resonant spectrum is in good agreement with the calculated interference between the direct and decay terms. The high photon energy used in this study (about 2520 eV) provides a bulk-sensitive determination of the Mo 4d electronic structure.

Charge screening effects in the resonant photoemission of Rh2O3, RuO2 , and MoO2Stoeberl1, Guedes2, Abbate3 et al. 2020Phys. Rev. BSelf Cite1000View full textAdd to dashboardCite

“…In MoO 2 , the large value for T is due to the dimerization that occurs between neighboring Mo 4+ ions. Overall, the parameters for RuO 2 and MoO 2 are in good agreement with those reported in similar materials [8,21], but no previous cluster model studies were found for the Rh 2 O 3 compound. Table II presents the main contributions to the ground state of Rh 2 O 3 , RuO 2 , and MoO 2 .…”

“…In principle, it allows one to identify and decompose the O 2p and transition-metal (TM) d partial contributions to the valence band (VB) of a given system, which are usually heavily mixed. The use of high photon energies also gives this method bulk sensitivity, which can be applied to interpret with an excellent agreement several physical properties of these TMO materials [5][6][7][8].…”

“…Here, we aim to study the photon energy dependence of the intensities in the valence-band structure of 4d TMO's, as well as to reproduce the effect of the interference between direct and indirect photoemission processes illustrated by Fano line-shape curves. Since cluster model calculations have produced reliable results in the description of several TMO compound spectra [8,[18][19][20][21], we propose to combine Davis and Feldkamp's extension of Fano's theory [14] with an extended cluster model to describe 4d TMO resonance within the L 3 (2p 3/2 ) absorption edge. To do so, we choose three TM 4d compounds with the following crystal structures and ionic fillings: Rh 2 O 3 (a regular d 6 semiconductor), RuO 2 (a regular d 4 metal), and MoO 2 (a distorted d 2 metal).…”

Many-body effects and non-local charge fluctuations in the double perovskite Sr2FeMoO6

“…The core level Fe 2p and Mo 3p spectra presented here are new, whereas the valence band spectrum was already presented in a previous study. 21…”

“…The energy position and relative intensity of these Mo 4d structures are in agreement with those observed in a recent Mo L 3 resonant photoemission experiment. 21 Although the single cluster model results reproduce the overall shape of the valence band, they fail to explain the magnetic order and the electrical conductivity of the compound. The double cluster model gives an anti-parallel ordering of the Fe 3d 5 and Mo 4d 1 magnetic moments, which is in agreement with the observed ferrimagnetic ordering in Sr 2 FeMoO 6 , whereas the single cluster model produces an independent alignment of the magnetic moments yielding a paramagnetic state.…”