arXiv subjects

J. R. L. Mardegan

Publications and source records attributed to J. R. L. Mardegan.

13 recordsLinked to original sources

arXiv2023

The Co$^{2+}$-Ir$^{5+}$ orbital hybridization in LaCaCoIrO$_6$ double perovskite

Here, we report on the structural, electronic, and magnetic properties of a polycrystalline sample of the LaCaCoIrO$_6$ double-perovskite investigated by means of synchrotron x-ray powder diffraction, x-ray absorption spectroscopy, and x-ray magnetic circular dichroism at the Co and Ir $L_{2,3}$ edges, magnetometry, and electrical transport. Our results indicate a configuration of nearly Co$^{2+}$/Ir$^{5+}$ configuration for the transition-metal ions, with spin canting within the Co antiferromagnetic superstructure responsible for the ferromagnetic-like behavior observed below 100 K. The highly insulating character of LaCaCoIrO$_6$ and its positive magnetoresistance further suggest that this antiferromagnetic superexchange interaction occurs through an indirect hybridization between the Co $e_g$ orbitals

cond-mat.str-el↗

arXiv2023

The 3d and 5d electronic structures and orbital hybridization in Ba- and Ca-doped La2CoIrO6 double perovskite

Here we present a detailed investigation of the Co and Ir local electronic structures in La1.5A0.5CoIrO6 (A = Ba, Ca) compounds in order to unravel the orbital hybridization mechanism in these CoIr-based double perovskites. Our results of x-ray powder diffraction, ac and dc magnetization, Co and Ir L2,3-edges and Co K-edge x-ray absorption spectroscopy and x-ray magnetic circular dichroism suggest a competition between magnetic interactions. A dominant antiferromagnetic coupling is found to be responsible for the ferrimagnetic behavior observed for A = Ca below approximately 96 K, the competing magnetic phases and the cationic disorder in this compound giving rise to a spin-glass state at low temperatures. For the A = Ba, on the other hand, there is no evidence of long range order down to its spin-glass transition temperature. The remarkably different magnetic properties observed between these two compounds is discussed in terms of the structural distortion that alters the strength of the Co - Ir couplings, with a relevant role played by the Co 3d eg - Ir 5d j = 1/2 hybridization.

cond-mat.mtrl-sci↗

arXiv2023

Element resolved evidence of superdiffusive terahertz spin current arising from ultrafast demagnetization process

Using element-specific measurements of the ultrafast demagnetization of Ru/Fe$_{65}$Co$_{35}$ heterostructures, we show that Ru can exhibit a significant magnetic contrast (3% asymmetry) resulting from ultrafast spin currents emanating from the demagnetization process of the FeCo layer. We use this magnetic contrast to investigate how superdiffusive spin currents are affected by the doping of heavy elements in the FeCo layer. We find that the spin currents are strongly suppressed, and that the recovery process in Ru slows down, by Re doping. This is in accordance with a change in interface reflectivity of spin currents as found by the superdiffusive spin transport model.

cond-mat.mtrl-sci↗

arXiv2021

Magnetic order of tetragonal CuO ultra-thin films

We present a detailed low-energy muon spin rotation and x-ray magnetic circular dichroism (XMCD) investigation of the magnetic structure in ultra-thin tetragonal (T)-CuO films. The measured muon-spin polarization decay indicates an antiferromagnetic (AFM) order with a transition temperature higher than 200K. The XMCD signal obtained around the Cu $L_{2,3}$ edges indicates the presence of pinned Cu$^{2+}$ moments that are parallel to the sample surface, and additionally, isotropic paramagnetic moments. The pinning of some of the Cu moments is caused by an AFM ordering consisting of moments that lie most likely in the plane of the film. Moreover, pinned moments show a larger orbital magnetic moment contribution with an approximate ratio of $m_{orb}/m_{spin} = 2$, indicating that these spins are located at sites with reduced symmetry. Some fractions of the pinned moments remain pinned from an AFM background even at 360K, indicating that $T_N >$ 360K. A simple model could explain qualitatively these experimental findings; however, it is in contrast to theoretical predictions, showing that the magnetic properties of ultra-thin T-CuO films differ from bulk expectations and is more complex.

cond-mat.mtrl-sci↗

arXiv2020

Unveiling charge density wave quantum phase transitions by x-ray diffraction

We investigate the thermal-driven charge density wave (CDW) transition of two cubic superconducting intermetallic systems Lu(Pt1-xPdx)2In and (Sr1-xCax)3Ir4Sn13 by means of x-ray diffraction technique. A detailed analysis of the CDW modulation superlattice peaks as function of temperature is performed for both systems as the CDW transition temperature T_CDW is suppressed to zero by an non-thermal control parameter. Our results indicate an interesting crossover of the classical thermal-driven CDW order parameter critical exponent from a three-dimensional universality class to a mean-field tendency, as T_CDW vanishes. Such behavior might be associated with presence of quantum fluctuations which influences the classical second-order phase transition, strongly suggesting the presence of a quantum critical point (QCP) at T_CDW = 0. This also provides experimental evidence that the effective dimensionality exceeds its upper critical dimension due to a quantum phase transition.

cond-mat.str-el↗

arXiv2020

Possible quantum fluctuations in the vicinity of the quantum critical point of $\mathbf{(Sr, Ca)_3Ir_4Sn_{13}}$ revealed by high-energy X-ray diffraction study

We explore the evolution of the structural phase transition of $\rm{(Sr, Ca)_3Ir_4Sn_{13}}$, a model system to study the interplay between structural quantum criticality and superconductivity, by means of high-energy x-ray diffraction measurements at high pressures and low temperatures. Our results confirm a rapid suppression of the superlattice transition temperature $T^*$ against pressure, which extrapolates to zero at a critical pressure of $\approx 1.79(4)$ GPa. The temperature evolution of the superlattice Bragg peak in $\rm{Ca_3Ir_4Sn_{13}}$ reveals a drastic decrease of the intensity and an increase of the linewidth when $T \rightarrow 0$ K and $p \rightarrow p_c$. Such anomaly is likely associated to the emergence of quantum fluctuations that disrupt the formation of long-range superlattice modulation. The revisited temperature-pressure phase diagram of $\rm{(Sr, Ca)_3Ir_4Sn_{13}}$ thus highlights the intertwined nature of the distinct order parameters present in this system and demonstrates some similarities between this family and the unconventional superconductors.

cond-mat.str-el↗

arXiv2020

Possible quantum paramagnetism in compressed Sr$_2$IrO$_4$

The effect of compression on the magnetic ground state of Sr$_2$IrO$_4$ is studied with x-ray resonant techniques in the diamond anvil cell. The weak interlayer exchange coupling between square-planar 2D IrO$_2$ layers is readily modified upon compression, with a crossover between magnetic structures around 7 GPa mimicking the effect of an applied magnetic field at ambient pressure. Higher pressures drive an order-disorder magnetic phase transition with no magnetic order detected above 17-20 GPa. The persistence of strong exchange interactions between $\mathrm{J_{eff}}=1/2$ magnetic moments within the insulating IrO$_2$ layers up to at least 35 GPa points to a highly frustrated magnetic state in compressed Sr$_2$IrO$_4$ opening the door for realization of novel quantum paramagnetic phases driven by extended $5d$ orbitals with entangled spin and orbital degrees of freedom.

cond-mat.str-el↗

arXiv2019

Magnetic and electronic properties at the gamma-Al2O3/SrTiO3 interface

The magnetic and electronic nature of the gamma-Al2O3/SrTiO3 spinel/perovskite interface is explored by means of x-ray absorption spectroscopy. Polarized x-ray techniques combined with atomic multiplet calculations reveal localized magnetic moments assigned to Ti3+ at the interface with equivalent size for in- and out-of-plane magnetic field directions. Although magnetic fingerprints are revealed, the Ti3+ magnetism can be explained by a paramagnetic response at low temperature under applied magnetic fields. Modeling the x-ray linear dichroism results in a delta0 = 1.9 eV splitting between the t2g and eg states for the Ti4+ 3d0 orbitals. In addition these results indicate that the lowest energy states have the out-of-plane dxz/dyz symmetry. The isotropic magnetic moment behavior and the lowest energy dxz/dyz states are in contrast to the observations for the two-dimensional electron gas at the perovskite/perovskite interface of LaAlO3/SrTiO3, that exhibits an anisotropic magnetic dxy ground state.

cond-mat.str-el↗

arXiv2018

Pressure effects on the structural and superconducting transitions in La3Co4Sn13

La3Co4Sn13 is a superconducting material with transition temperature at Tc = 2.70 K, which presents a superlattice structural transition at T* ~ 150 K, a common feature for this class of compounds. However, for this material, it is not clear that at T* the lattice distortions arise from a charge density wave (CDW) or from a distinct microscopic origin. Interestingly, it has been suggested in isostructural non-magnetic intermetallic compounds that T* can be suppressed to zero temperature, by combining chemical and external pressure, and a quantum critical point is argued to be observed near these critical doping/pressure. Our study shows that application of pressure on single-crystalline La3Co4Sn13 enhances Tc and decreases T*. We observe thermal hysteresis loops for cooling/heating cycles around T* for P > 0.6 GPa, in electrical resistivity measurements, which are not seen in x-ray diffraction data. The hysteresis in electrical measurements may be due to the pinning of the CDW phase to impurities/defects, while the superlattice structural transition maintains its ambient pressure second-order transition nature under pressure. From our experiments we estimate that T* vanishes at around 5.5 GPa, though no quantum critical behavior is observed up to 2.53 GPa.

cond-mat.supr-con↗

arXiv2017

Pressure-tuning of bond-directional exchange interactions and magnetic frustration in hyperhoneycomb iridate $β$-$\mathrm{Li_2IrO_3}$

We explore the response of Ir $5d$ orbitals to pressure in $β$-$\mathrm{Li_2IrO_3}$, a hyperhoneycomb iridate in proximity to a Kitaev quantum spin liquid (QSL) ground state. X-ray absorption spectroscopy reveals a reconstruction of the electronic ground state below 2 GPa, the same pressure range where x-ray magnetic circular dichroism shows an apparent collapse of magnetic order. The electronic reconstruction, which manifests a reduction in the effective spin-orbit (SO) interaction in $5d$ orbitals, pushes $β$-$\mathrm{Li_2IrO_3}$ further away from the pure $J_{\rm eff}=1/2$ limit. Although lattice symmetry is preserved across the electronic transition, x-ray diffraction shows a highly anisotropic compression of the hyperhoneycomb lattice which affects the balance of bond-directional Ir-Ir exchange interactions driven by spin-orbit coupling at Ir sites. An enhancement of symmetric anisotropic exchange over Kitaev and Heisenberg exchange interactions seen in theoretical calculations that use precisely this anisotropic Ir-Ir bond compression provides one possible route to realization of a QSL state in this hyperhoneycomb iridate at high pressures.

cond-mat.str-el↗

arXiv2015

Magnetic properties of Gd$T_2$Zn$_{20}$ (T = Fe, Co) investigated by X-ray diffraction and spectroscopy

We investigate the magnetic and electronic properties of the Gd$T_2$Zn$_{20}$ ($T$ = Fe and Co) compounds using X-ray resonant magnetic scattering (XRMS), X-ray absorption near-edge structure (XANES) and X-ray magnetic circular dichroism (XMCD) techniques. The XRMS measurements reveal that the GdCo$_2$Zn$_{20}$ compound has a commensurate antiferromagnetic spin structure with a magnetic propagation vector $\vecτ$ = $(\frac{1}{2},\frac{1}{2},\frac{1}{2})$ below the Néel temperature ($T_N \sim$ 5.7 K). Only the Gd ions carry a magnetic moment forming an antiferromagnetic structure with magnetic representation $Γ_6$. For the ferromagnetic GdFe$_2$Zn$_{20}$ compound, an extensive investigation was performed at low temperature and under magnetic field using XANES and XMCD techniques. A strong XMCD signal of about 12.5 $\%$ and 9.7 $\%$ is observed below the Curie temperature ($T_C \sim$ 85 K) at the Gd-$L_2$ and $L_3$ edges, respectively. In addition, a small magnetic signal of about 0.06 $\%$ of the jump is recorded at the Zn $K$-edge suggesting that the Zn 4$p$ states are spin polarized by the Gd 5$d$ extended orbitals.

cond-mat.mtrl-sci↗

arXiv2013

Different routes to pressure-induced volume collapse transitions in gadolinium and terbium metals

The sudden decrease in molar volume exhibited by most lanthanides under high pressure is often attributed to changes in the degree of localization of their 4f-electrons. We give evidence, based on electrical resistivity measurements of dilute Y(Gd) and Y(Tb) alloys to 120 GPa, that the volume collapse transitions in Gd and Tb metals have different origins, despite their being neighbors in the periodic table. Remarkably, the change under pressure in the magnetic state of isolated Pr or Tb impurity ions in the nonmagnetic Y host appears to closely mirror corresponding changes in pure Pr or Tb metals. The collapse in Tb appears to be driven by an enhanced negative exchange interaction between 4f and conduction electrons under pressure (Kondo resonance) which, in the case of Y(Tb), dramatically alters the superconducting properties of the Y host, much like previously found for Y(Pr). In Gd our resistivity measurements suggest that a Kondo resonance is not the main driver for its volume collapse. X-ray absorption and emission spectroscopies clearly show that 4f local moments remain largely intact across both volume collapse transitions ruling out 4f band formation (delocalization) and valence transition models as possible drivers. The results highlight the richness of behavior behind the volume collapse transition in lanthanides and demonstrate the stability of the 4f level against band formation to extreme pressure.

cond-mat.str-el↗

arXiv2013

Pressure induced amorphization and collapse of magnetic order in type-I clathrate Eu8Ga16Ge30

We investigate the low temperature structural and electronic properties of the type-I clathrate Eu8Ga16Ge30 under pressure using x-ray powder diffraction (XRD), x-ray absorption near-edge structure (XANES) and x-ray magnetic circular dichroism (XMCD) techniques. The XRD measurements reveal a transition to an amorphous phase above 18 GPa. Unlike previous reports on other clathrate compounds, no volume-collapse is observed prior to the crystalline-amorphous phase transition which takes place when the unit cell volume is reduced to 81% of its ambient pressure value. Fits of the pressure-dependent relative volume to a Murnaghan equation of state (EOS) yield a bulk modulus B0 = 65+-3 GPa and a pressure derivative B'0 = 3.3+-0.5. The Eu L2-edge XMCD data shows quenching of the magnetic order at the crystalline-amorphous phase transition. The XANES spectra indicate the persistence of Eu2+ valency state up to 22 GPa, therefore the suppression of XMCD intensity is due to the loss of magnetic order as a result of frustrated exchange interactions in the amorphous phase, and not due to quenching of local moments. When compared with other clathrates, the results point to the importance of guest ion-cage interactions in determining the mechanical stability of the framework structure and the critical pressure for amorphization. Finally, the crystalline structure is not found to recover after pressure release, resulting in a novel amorphous material that is at least metastable at ambient pressure and temperature.

cond-mat.mtrl-sci↗