Research highlights

Overview

Our research is about X-ray spectroscopy applied to quantum materials. Of course, if other spectroscopies are needed, we eagerly go after it.  We are mainly interested in i) frustrated magnets,  specially on how disorder and frustration interacts; ii) itinerant magnetism, specially on the local properties of itinerant magnets;  and iii) the interaction of magnetism and superconductivity, with focus on the pairing mechanism.  See below for our recent research highlights on each of these topics.

 High temperature superconductors 

Orbital hybridizations and the role of the 4p orbitals in the Iron based high temperature supercondutors

In this work, we investigated the pre-edge structure of the Fe K-edge absorption spectra. From previous works, this pre-edge  is known to  contain information about the hybridization  between Fe 3d and As  4p orbitals.  Our analysis added a new dimension to this problem: the pre-edge also contains a component from the local Fe3dFe4p hybridization. By investigating  how the pre-edge changes for Co and Mn "doped"  BaFe2As2, we suggested that the interplay between these two hybridizations  may be the mechanism which controls the strengh of the interactions in the Fe based materials.  This scenario agrees with the stand point that the BaFe2As2 is a Hund metal, wherein electronic correlations are controoled by the hybridizations of the Fe derived electronic states. 


References

A. G. de Figueiredo, M. R. Cantarino, W. R. da Silva Neto, K. R. Pakuszewski, R. Grossi, D. S. Christovam, J. C. Souza, M. M. Piva, G. S. Freitas, P. G. Pagliuso, C. Adriano, F. A. Garcia - "Orbital localization and the role of the Fe and As 4p orbitals in BaFe2As2  probed by XANES", Physical Review B 105, 045130 (2022)  (arXiv:2112.09980). (Are you interested in our data? Please, send us a message: fgarcia-at-if.usp.br)

Thermoelectric materials

Vibrational and elastic properties connected to chemical bonding

We have been exploring the RFe4Sb12 filled skutterudites in the past years, trying to understand the relation between chemical and physical properties in this interesting family of   thermoelectric materials.  In this work, we investigated  the interaction between the vibrations of R atoms (called the fillers) and the Fe4Sb12 atoms (called the cage), which have been a topic of intense discussion in this field. We performed x-ray absorption spectroscopy (XAS) and X-ray diffraction (XRD)  experiments  .We were able to characterize the role of the R atoms in the vibrational and elastic properties of the RFe4Sb12 materials. Moreover, our experimental results were connected with quantum chemistry calculations of the filler-cage bonding properties in skutterudites.  Our results suggest that in the case of the heavy fillers (Sr and Ba), the filler-cage bonding acquire a large degree of covalence, which is connected to their thermoelectric properties. 

References

Juliana G. de Abrantes, Marli R. Cantarino, Wagner R. da Silva Neto, Victória V. Freire, Alvaro G. Figueiredo, Tarsis M. Germano, Bassim Mounssef, Jr., Eduardo M. Bittar, Andreas Leithe-Jasper, and Fernando A. Garcia - “Vibrational and structural properties of the RFe4Sb12 ( R= Na, K ,Ca , Sr, Ba ) filled skutterudites”, Physical Review Materials 6, 085403 (2022) (arXiv:2203.14821).  (Are you interested in our data? Please, send us a message: fgarcia-at-if.usp.br)

Frustated magnets, the interaction of disorder and frustration at low temperatures.  

Disorder meets quantum fluctuations in a complex lattice

Frustrated magnets are systems displaying competing magnetic interactions. The interactions between electronic spins in a solid will usually create magnetic order below a characteristic transition temperature. Disorder, frustration and dimensionality may conspire to decrease this temperature, paving the way for another ingredient to come into play: quantum fluctuations. In a magnetic solid, electronic spins fluctuate in a rate that is determined by thermal energy. However, since spins interact, magnetic order emerges below the transition temperature. Disorder and frustration may cause magnetic solids to display, instead, a spin glass state, where the spins are frozen in a random configuration. In a low dimensional spin system, like spins distributed in layers, this glassy state may not be fully developed down to very low temperatures. Then, quantum fluctuations will compete with this frozen state, possibly giving rise to some exotic ground state. Our work explores the magnetic properties of an intrinsically disordered, frustrated and low dimensional magnet, in which the spins remain in a dynamic magnetic state down to very low temperatures. Our sample displays experimental signatures seen both in quantum spin liquid candidates and spin glasses, offering a very exciting playground to study the competition between these novel states of frustrated magnets.   

References

M.R. Cantarino, R.P. Amaral, R.S. Freitas, J.C.R. Araújo, R. Lora-Serrano, H. Luetkens, C. Baines, S. Bräuninger, V. Grinenko, R. Sarkar, H.H. Klauss, E. C. Andrade, F. A. Garcia - "Dynamic magnetism in the disordered hexagonal double Perovskite BaTi1/2Mn1/2O3", Physical Review B 2019, (arXiv:1802.09950).  (Are you interested in our data? Please, send us a message: fgarcia-at-if.usp.br)

F. A. Garcia, U. F. Kaneko, E. Granado, J. Sichelschmidt, M. Hoelzel, J. G. S. Duque, C. A. J. Nunes, R. P. Amaral, P. Marques-Ferreira, R. Lora-Serrano. “Magnetic dimers and trimmers in the disordered S = 3/2 spin system BaTi1/2Mn1/2O3 Physical Review B, 2015 (arXiv:1206.3813).

Local properties of itinerant magnets

Chemistry shows up at a traditional physical system

In solids, local moment magnetism originates from spins that are pinned down to specific sites in the system, like in insulators, while itinerant magnetism originates from spins that walk free throughout the solid, like the spins  of conduction electrons in a metal.  Local moment magnetism is strongly dependent on the chemical (or local) properties of the material and our work suggests that in certain instances this is also the case for itinerant magnets. In solids, electronic spins are the main source of magnetism.  The complexity of the magnetic properties emerges because of the interaction between nearby spins. In metals, conduction electrons are spread in the system and their density dictates the magnetic properties of the solid. However, some metallic magnets display a structural building block called a coordination structure, like insulators. In our work, we investigated the local structural and electronic properties of a series of itinerant magnets and we discovered that the probed local properties are relevant to understanding their itinerant magnetic properties. 

References

Magnetism and superconductivity

Spin excitations in the Iron based superconductors: necessary, but not sufficient. 

In superconducting materials, electrons are found in pairs that carry electric current without dissipation. For pairing up electrons, you need a glue and our work advance the understanding that in the iron based superconductors (IBS) this glue is provided by the iron spins. A number of distinct mechanisms may lead to the formation of electron pairs. In a solid, the flipping of electronic spins give rise to spin excitations possessing a wave-like character, that can transfer energy and momentum to electrons. This is believed to be the mechanism behind superconductivity in the IBS. To probe the spin excitations, one can apply a technique called resonant inelastic x-ray scattering (RIXS). Previous RIXS experiments of IBS found spin excitations that are weakly dependent on the fact that the material is a superconductor or not. Puzzled by these results, we investigated by RIXS the spin excitations of some close relatives of the IBS which, however, never become superconductors. We found that the spin excitations are strongly scattered along certain directions, suggesting that spin excitations are a necessary ingredient to superconductivity in the IBS, albeit not a sufficient one. 

Fernando A. Garcia, Oleh Ivashko , Daniel E. McNally, Lakshmi Das, Mario M. Piva, C. Adriano, Pascoal G. Pagliuso, Johan Chang, Thorsten Schmitt, Claude Monney - "Anisotropic magnetic excitations and incipient Néel order in Ba(Fe1-xMnx)2As2" Physical Review B 2019  (arXiv:1901.08543). (Are you interested in our data? Please, send us a message: fgarcia-at-if.usp.br)