arXiv subjects

S. Agrestini

Publications and source records attributed to S. Agrestini.

At least 37 records · Page 2Linked to original sources

arXiv2017

The $c$-axis dimer and its electronic break-up: the insulator-to-metal transition in Ti$_2$O$_3$

We report on our investigation of the electronic structure of Ti$_2$O$_3$ using (hard) x-ray photoelectron and soft x-ray absorption spectroscopy. From the distinct satellite structures in the spectra we have been able to establish unambiguously that the Ti-Ti $c$-axis dimer in the corundum crystal structure is electronically present and forms an $a_{1g}a_{1g}$ molecular singlet in the low temperature insulating phase. Upon heating we observed a considerable spectral weight transfer to lower energies with orbital reconstruction. The insulator-metal transition may be viewed as a transition from a solid of isolated Ti-Ti molecules into a solid of electronically partially broken dimers where the Ti ions acquire additional hopping in the $a$-$b$ plane via the $e_g^π$ channel, the opening of which requires the consideration of the multiplet structure of the on-site Coulomb interaction.

cond-mat.str-el↗

arXiv2017

Bulk and surface electronic properties of SmB6: a hard x-ray photoelectron spectroscopy study

We have carried out bulk-sensitive hard x-ray photoelectron spectroscopy (HAXPES) measurements on in-situ cleaved and ex-situ polished SmB6 single crystals. Using the multiplet-structure in the Sm 3d core level spectra, we determined reliably that the valence of Sm in bulk SmB6 is close to 2.55 at ~5 K. Temperature dependent measurements revealed that the Sm valence gradually increases to 2.64 at 300 K. From a detailed line shape analysis we can clearly observe that not only the J=0 but also the J=1 state of the Sm 4f 6 configuration becomes occupied at elevated temperatures. Making use of the polarization dependence, we were able to identify and extract the Sm 4f spectral weight of the bulk material. Finally, we revealed that the oxidized or chemically damaged surface region of the ex-situ polished SmB6 single crystal is surprisingly thin, about 1 nm only.

cond-mat.mtrl-sci↗

arXiv2017

Intricacies of the Co$^{3+}$ spin state in Sr$_2$Co$_{0.5}$Ir$_{0.5}$O$_4$: an x-ray absorption and magnetic circular dichroism study

We report on a combined soft x-ray absorption and magnetic circular dichroism (XMCD) study at the Co-$L_{3,2}$ on the hybrid 3$d$/5$d$ solid state oxide Sr$_2$Co$_{0.5}$Ir$_{0.5}$O$_4$ with the K$_2$NiF$_4$ structure. Our data indicate unambiguously a pure high spin state $(S=2)$ for the Co$^{3+}$ (3$d^6$) ions with a significant unquenched orbital moment $L_z/2S_z=0.25$ despite the sizeable elongation of the CoO$_6$ octahedra. Using quantitative model calculations based on parameters consistent with our spectra, we have investigated the stability of this high spin state with respect to the competing low spin and intermediate spin states.

cond-mat.str-el↗

arXiv2017

Electronically highly cubic conditions for Ru in alpha-RuCl3

We studied the local Ru 4d electronic structure of alpha-RuCl3 by means of polarization dependent x-ray absorption spectroscopy at the Ru-L2,3 edges. We observed a vanishingly small linear dichroism indicating that electronically the Ru 4d local symmetry is highly cubic. Using full multiplet cluster calculations we were able to reproduce the spectra excellently and to extract that the trigonal splitting of the t2g orbitals is -12 $\pm10$ meV, i.e. negligible as compared to the Ru 4d spin-orbit coupling constant. Consistent with our magnetic circular dichroism measurements, we found that the ratio of the orbital and spin moments is 2.0, the value expected for a Jeff = 1/2 ground state. We have thus shown that as far as the Ru 4d local properties are concerned, alpha-RuCl3 is an ideal candidate for the realization of Kitaev physics.

cond-mat.str-el↗

arXiv2016

Long-range interactions in the effective low energy Hamiltonian of Sr2IrO4: a core level resonant inelastic x-ray scattering study

We have investigated the electronic structure of Sr2IrO4 using core level resonant inelastic x-ray scattering. The experimental spectra can be well reproduced using ab initio density functional theory based multiplet ligand field theory calculations, thereby validating these calculations. We found that the low-energy, effective Ir t2g orbitals are practically degenerate in energy. We uncovered that covalency in Sr2IrO4, and generally in iridates, is very large with substantial oxygen ligand hole character in the Ir t2g Wannier orbitals. This has far reaching consequences, as not only the onsite crystal-field energies are determined by the long range crystal-structure, but, more significantly, magnetic exchange interactions will have long range distance dependent anisotropies in the spin direction. These findings set constraints and show pathways for the design of d^5 materials that can host compass-like magnetic interactions.

cond-mat.str-el↗

arXiv2016

Termination control of magnetic coupling at a complex oxide interface

Atomically flat interfaces between ternary oxides have chemically different variants, depending on the terminating lattice planes of both oxides. Electronic properties change with the interface termination which affects, for instance, charge accumulation and magnetic interactions at the interface. Well-defined terminations have yet rarely been achieved for oxides of ABO3 type (with metals A, B). Here, we report on a strategy of thin film growth and interface characterization applied to fabricate the La0.7Sr0.3MnO3-SrRuO3 interface with controlled termination. Ultra-strong antiferromagnetic coupling between the ferromagnets occurs at the MnO2-SrO interface, but not for the other termination, in agreement with density functional calculations. X-ray magnetic circular dichroism measurements reveal coupled reversal of Mn and Ru magnetic moments at the MnO2-SrO interface. Our results demonstrate termination control of magnetic coupling across a complex oxide interface and provide a pathway for theoretical and experimental explorations of novel electronic interface states with engineered magnetic properties.

cond-mat.mtrl-sci↗

arXiv2015

Electronic and Spin States of SrRuO3 Thin Films: an X-ray Magnetic Circular Dichroism Study

We report a study of the local magnetism in thin films of SrRuO3 grown on (111) and (001) oriented SrTiO3 substrates using x-ray magnetic circular dichroism spectroscopy (XMCD) at the Ru-L2,3 edges. The application of the sum rules to the XMCD data gives an almost quenched orbital moment and a spin moment close to the value expected for the low spin state S = 1 . Full-multiplet cluster calculations indicate that the low spin state is quite stable and suggest that the occurrence of a transition to the high spin state S = 2 in strained thin films of SrRuO3 is unlikely as it would be too expensive in energy.

cond-mat.str-el↗

arXiv2013

Soft x-rays absorption and high-resolution powder x-ray diffraction study of superconducting CaxLa(1-x)Ba(1.75-x)La(0.25+x)Cu3Oy system

We have studied the electronic structure of unoccupied states measured by O K-edge and Cu L-edge x-ray absorption spectroscopy (XAS), combined with crystal structure studied by high resolution powder x-ray diffraction (HRPXRD), of charge-compensated layered superconducting CaxLa(1-x)Ba(1.75-x)La(0.25+x)Cu3Oy (0<x<0.4, 6.4<y<7.3) cuprate. A detailed analysis shows that, apart from hole doping, chemical pressure on the electronically active CuO2 plane due to the lattice mismatch with the spacer layers greatly influences the superconducting properties of this system. The results suggest chemical pressure to be the most plausible parameter to control the maximum critical temperatures (Tcmax) in different cuprate families at optimum hole density.

cond-mat.supr-con↗

arXiv2013

Spectroscopic evidence for giant orbital moment and magnetic anisotropy induced by local distortions in alpha-CoV2O6

We present a combined experimental and theoretical study on the local magnetism of the Co ions in the spin-chain compound CoV2O6, which crystallizes in two different allotropic phases, alpha- and gamma-CoV2O6. Using x-ray magnetic circular dichroism, we have found a very large and a moderate orbital contribution to the magnetism in alpha- and gamma-CoV2O6, respectively. Full-multiplet calculations indicate that the differences in the magnetic behavior of alpha- and gamma-CoV2O6 phases originate from different local distortions of the CoO6 octahedra. In particular, the strong compression of the CoO6 octahedra in alpha-CoV2O6 lead to a strong mixture of t2g and eg orbitals which, via the local atomic Coulomb and exchange interactions, results in an exceptionally large orbital moment.

cond-mat.str-el↗

arXiv2012

Crystal-field ground state of the orthorhombic Kondo insulator CeRu2Al10

We have succeeded in establishing the crystal-field ground state of CeRu2Al10, an orthorhombic intermetallic compound recently identified as a Kondo insulator. Using polarization dependent soft x-ray absorption spectroscopy at the Ce M4,5 edges, together with input from inelastic neutron and magnetic susceptibility experiments, we were able to determine unambiguously the orbital occupation of the 4f shell and to explain quantitatively both the measured magnetic moment along the easy a axis and the small ordered moment along the c-axis. The results provide not only a platform for a realistic modeling of the spin and charge gap of CeRu2Al10, but demonstrate also the potential of soft x-ray absorption spectroscopy to obtain information not easily accessible by neutron techniques for the study of Kondo insulators in general.

cond-mat.str-el↗

arXiv2011

Slow Magnetic Order-Order Transition in the Spin Chain Antiferromagnet Ca3Co2O6

Using powder neutron diffraction we have discovered an unusual magnetic order-order transition in the Ising spin chain compound Ca3Co2O6. On lowering the temperature an antiferromagnetic phase with propagation vector k=(0.5,-0.5,1) emerges from a higher temperature spin density wave structure with k=(0, 0, 1.01). This transition occurs over an unprecedented time-scale of several hours and is never complete.

cond-mat.str-el↗

arXiv2011

Magnetic order, metamagnetic transitions, and low-temperature spin freezing in Ca3Co2O6: an NMR study

We report on a 59Co NMR investigation of the trigonal cobaltate Ca3Co2O6 carried out on a single crystal, providing precise determinations of the electric field gradient and chemical shift tensors, and of the internal magnetic fields at the non-magnetic Co I sites, unavailable from former studies on powders. The magnetic field-induced ferri- and ferromagnetic phases at intermediate temperature (e.g. 10 K) are identified by distinct internal fields, well accounted for by purely dipolar interactions. The vanishing transferred hyperfine field at the Co I site indicates that the Co3+(I) orbitals do not participate in the intra-chain superexchange, in disagreement with a previous theoretical model. The strong Ising character of the system is confirmed experimentally by the field dependence of the resonance lines, indicating that local moments are saturated even at the phase boundaries. In the vicinity of the critical fields, nuclear spin-spin relaxations detect the spin reversal dynamics of large magnetic assemblies, either Ising chain fragments or finite size domains, which drive the metamagnetic transitions. Such collective excitations exhibit a glassy behavior, slowing down to subacoustic frequencies and freezing at low temperature. The relevance of such slow fluctuation modes for the low-temperature multi-step behavior reported in the magnetization is discussed.

cond-mat.str-el↗

arXiv2010

Field-driven magnetisation steps in Ca3Co2O6: A single-crystal neutron-diffraction study

We present single-crystal neutron-diffraction data for the spin-chain compound Ca3Co2O6. The intensity and line shapes of the two families of Bragg peaks characterising both the antiferromagnetic and the ferromagnetic components of the magnetic order present in this material have been measured as a function of temperature and applied magnetic fields of up to 5 T. We have studied the microscopic nature of the magnetic order at each step seen in the bulk magnetisation and investigated the evolution of the long and short-range components of the magnetic order in Ca3Co2O6.

cond-mat.str-el↗

arXiv2009

Local structure of REFeAsO (RE=La, Pr, Nd, Sm) oxypnictides studied by Fe K-edge EXAFS

Local structure of REOFeAs (RE=La, Pr, Nd, Sm) system has been studied as a function of chemical pressure varied due to different rare-earth size. Fe K-edge extended X-ray absorption fine structure (EXAFS) measurements in the fluorescence mode has permitted to compare systematically the inter-atomic distances and their mean square relative displacements (MSRD). We find that the Fe-As bond length and the corresponding MSRD hardly show any change, suggesting the strongly covalent nature of this bond, while the Fe-Fe and Fe-RE bond lengths decrease with decreasing rare earth size. The results provide important information on the atomic correlations that could have direct implication on the superconductivity and magnetism of REOFeAs system, with the chemical pressure being a key ingredient.

cond-mat.supr-con↗

arXiv2009

Experimental evidence of chemical-pressure-controlled superconductivity in cuprates

X-ray absorption spectroscopy (XAS) and high resolution X-ray diffraction are combined to study the interplay between electronic and lattice structures in controlling the superconductivity in cuprates with a model charge-compensated CaxLa1-xBa1.75-xLa0.25+xCu3Oy (0<x<0.5, y=7.13) system. In spite of a large change in Tc, the doped holes, determined by the Cu L and O K XAS, hardly show any variation with the x. On the other hand, the CuO2 plaquette size shows a systematic change due to different size of substituted cations. The results provide a direct evidence for the chemical pressure being a key parameter for controlling the superconducting ground state of the cuprates.

cond-mat.supr-con↗

arXiv2008

Resonant X-ray scattering investigation of the multipolar ordering in Ca3Co2O6

We have performed a resonant x-ray scattering (RXS) study near the Co K edge on a single crystal of Ca3Co2O6. In the magnetically ordered phase a new class of weak reflections appears at the magnetic propagation vector tau (1/3,1/3,1/3). These new reflections allow direct access to the dipolar-quadrupolar E1E2 scattering channel. The theoretical possibility of observing isolated E1E2 electromagnetic multipoles has attracted a lot of interest in the recent years. Unfortunately in many system of interest, parity even and parity odd tensor contributions occur at the same positions in reciprocal space. We demonstrate that in Ca3Co2O6 it is possible to completely separate the parity even from the parity odd terms. The possibility of observing such terms even in globally centrosymmetric systems using RXS has been investigated theoretically; Ca3Co2O6 allows a symmetry based separation of this contribution.

cond-mat.str-el↗

arXiv2008

The nature of the magnetic order in Ca3Co2O6

We present a detailed powder and single crystal neutron diffraction study of the spin chain compound Ca3Co2O6. Below 25 K, the system orders magnetically with a modulated partially disordered antiferromagnetic structure. We give a description of the magnetic interactions in the system which is consistent with this magnetic structure. Our study also reveals that the long-range magnetic order co-exists with a shorter range order with a correlation length scale of 180 A in the ab plane. Remarkably, on cooling, the volume of material exhibiting short range order increases at the expense of the long-range order.

cond-mat.str-el↗

arXiv2008

Incommensurate magnetic ground state revealed by RXS in the frustrated spin system Ca3Co2O6

We have performed a resonant x-ray scattering study at the Co pre-K edge on a single crystal of Ca3Co2O6. The measurements reveal an abrupt transition to a magnetically ordered state immediately below T_N = 25 K, with a magnetic correlation length in excess of 5500 Å along the c-axis chains. There is no evidence for modifications to the Co$^{3+}$ spin state. A temperature dependent modulation in the magnetic order along the c-axis and an unusual decrease in the magnetic correlation lengths on cooling are observed. The results are compatible with the onset of a partially disordered antiferromagnetic structure in Ca3Co2O6.

cond-mat.other↗