arXiv subjects

M. R. Cantarino

Publications and source records attributed to M. R. Cantarino.

5 recordsLinked to original sources

arXiv2026

From perovskite to infinite-layer nickelates: hole concentration from x-ray absorption

The difficulty of determining cation concentrations and oxygen stoichiometry in infinite-layer nickelate thin films has so far prevented clear experimental identification of the nickel electron configuration in the superconducting phase. We used soft x-ray absorption spectroscopy to study the successive changes in PrNiO$_x$ thin films at various intermediate stages of topotactic reduction with $x=2-3$. By comparing the Ni-$L$ edge spectra to single and double cluster ligand-field calculations, we find that none of our samples exhibit a pure $d^9$ configuration. Our quantitative analysis using the charge sum rule shows that even when films are maximally reduced, the averaged number of nickel $3d$ holes is 1.35. Superconducting samples have even higher values, calling into question the previously assumed limit of hole doping. Concomitant changes in the oxygen $K$-edge absorption spectra upon reduction indicate the presence of oxygen $2p$ holes, even in the most reduced films. Overall, our results suggest a complex interplay of hole doping mechanisms resulting from self-doping effects and oxygen non-stoichiometry.

cond-mat.supr-con↗

arXiv2025

Orbital-Selective Band Structure Evolution in BaFe$_{2-x}$M$_x$As$_2$ (M = Cr, Co, Cu, Ru and Mn) Probed by Polarization-Dependent ARPES

We present a systematic study of the evolution of the band structure in the Fe-based superconductor family BaFe$_{2-x}$M$_x$As$_2$ (M = Cr, Co, Cu, Ru and Mn) using polarization-dependent angle-resolved photoemission spectroscopy (ARPES). Low-substituted samples, with comparable spin-density wave transition temperatures ($T_\text{SDW}$), were chosen to facilitate controlled comparisons. The sizes of the central hole pockets ($α$, $β$, and $γ$) remain largely unchanged across different substitutions, showing no clear correlation with either $T_\text{SDW}$ or the As height relative to the Fe planes. However, subtle trends are observed: a modest increase in the size of the $η_\text{X}$ electron pocket correlates with the suppression of $T_\text{SDW}$. Furthermore, the contraction of the $η_\text{X}$ pocket appears to be linked to an increase in the As height relative to the Fe planes. Our results suggest that the suppression of $T_\text{SDW}$ is primarily driven by changes in the Fe-As bond length, with the effect being more pronounced in electronic states with planar character. These findings provide insight into the electronic structure of BaFe$_{2-x}$M$_x$As$_2$.

cond-mat.supr-con↗

arXiv2022

Orbital localization and the role of the Fe and As $4p$ orbitals in BaFe$_{2}$As$_{2}$ probed by XANES

The polarization dependence of the near edge x-ray absorption spectroscopy (XANES) is an element specific probe to the real-space distribution of the density of unoccupied states in solid-state materials. In this paper, we present Fe and As $K$-edge experiments of Ba(Fe$_{1-x}$$M_{x}$)$_{2}$As$_{2}$ ($M=$ Mn, Co and $x=0.0$ and $0.08$). The experiments reveal a strong polarization dependence of the probed XANES spectra, which concerns mainly an increase of the intensity of electronic transitions when the beam polarization is set out of the sample's $ab$ crystallographic plane. The results show that states with $p_{z}$-orbital character dominate the density of unoccupied states close to the Fermi level. Partial substitution of Fe by Co is shown to decrease the intensity anisotropy, suggesting that Co promotes electronic transfer preferentially to states with $p_{z}$-orbital character. On the other hand, Mn substitution causes the increase of the spectra $p_{z}$-orbital anisotropy, which is proposed to take place by means of an enhanced local Fe $3d4p$ mixing, unveiling the role of Fe $4p$ states in the localization of the Fe $3d$ orbitals. Moreover, by comparing our results to previous experiments, we identify the relative mixing between Fe and the pnictide $4p_{x,y,z}$ orbitals as a clear divide between the electronic properties of iron arsenides and selenides. Our conclusions are supported by multiple-scattering theory calculations of the XANES spectra and by quantum chemistry calculations of Fe coordination electronic structure.

cond-mat.str-el↗

arXiv2019

Dynamic magnetism in the disordered hexagonal double perovskite BaTi$_{1/2}$Mn$_{1/2}$O$_{3}$

Magnetic frustration and disorder are key ingredients to prevent the onset of magnetic order. In the disordered hexagonal double perovskite BaTi$_{1/2}$Mn$_{1/2}$O$_{3}$, Mn$^{4+}$ cations, with $S=3/2$ spins, can either form highly correlated states of magnetic trimers or dimers or remain as weakly interacting orphan spins. At low temperature ($T$), the dimer response is negligible, and magnetism is dominated by the trimers and orphans. To explore the role of magnetic frustration, disorder and possibly of quantum fluctuations, the low-$T$ magnetic properties of the remaining magnetic degrees of freedom of BaTi$_{1/2}$Mn$_{1/2}$O$_{3}$ are investigated. Heat-capacity data and magnetic susceptibility display no evidence for a phase transition to a magnetically ordered phase but indicate the formation of a correlated spin state. The low-temperature spin dynamics of this state is then explored by $μ$SR experiments. The zero field $μ^{+}$ relaxation rate data show no static magnetism down to $T=19$ mK and longitudinal field experiments support as well that dynamic magnetism persists at low $T$. Our results are interpreted in terms of a spin glass state which stems from a disordered lattice of orphans spins and trimers. A spin liquid state in BaTi$_{1/2}$Mn$_{1/2}$O$_{3}$, however, is not excluded and is also discussed.

cond-mat.str-el↗

arXiv2019

Hard X-ray spectroscopy of the itinerant magnets $R$Fe$_{4}$Sb$_{12}$ ($R=$Na, K, Ca, Sr, Ba)

Ordered states in itinerant magnets may be related to magnetic moments displaying some weak local moment characteristics, as in intermetallic compounds hosting transition metal coordination complexes. In this paper, we report on the Fe $K$-edge X-ray absorption spectroscopy (XAS) of the itinerant magnets $R$Fe$_{4}$Sb$_{12}$ ($R=$ Na, K, Ca, Sr, Ba), aiming at exploring the electronic and structural properties of the octahedral building block formed by Fe and the Sb ligands. We find evidence for strong hybridization between the Fe $3d$ and Sb $5p$ states at the Fermi level, giving experimental support to previous electronic structure calculations of the $R$Fe$_{4}$Sb$_{12}$ skutterudites. The electronic states derived from Fe 3$d$ Sb $5p$ mixing are shown to be either more occupied and/or less localized in the cases of the magnetically ordered systems, for which $R=$ Na or K, connecting the local Fe electronic structure to the itinerant magnetic properties. Moreover, the analysis of the extended region of the XAS spectra (EXAFS) suggests that bond disorder may be a more relevant parameter to explain the suppression of the ferromagnetic ordered state in CaFe$_{4}$Sb$_{12}$ than the decrease of the density of states.

cond-mat.str-el↗