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Cinthia Piamonteze

Publications and source records attributed to Cinthia Piamonteze.

At least 19 recordsLinked to original sources

Atomic Origins of Magnetic Anisotropy in Ru-substituted Manganite Films

Magnetic anisotropy in complex oxides often originates from the complex interplay of several factors, including crystal structure, spin-orbit coupling, and electronic interactions. Recent studies on Ru-substituted $La_{0.70}Sr_{0.30}MnO_3$ (Ru-LSMO) films demonstrate emerging magnetic and magneto-transport properties, where magnetic anisotropy plays a crucial role. However, the atomic origin and underlying mechanisms of the magnetic anisotropy of this material system remain elusive. This work sheds light on these aspects. Detailed element-specific X-ray magnetic dichroism analysis suggests that Ru single ion anisotropy governs the overall magnetic anisotropy. Furthermore, the magnetic property of Mn ions changes dramatically due to strong antiferromagnetic coupling between Ru and Mn ions. Our findings clarify the role of Ru single ion anisotropy behind magnetic anisotropy in Ru-LSMO, offering a promising avenue for designing advanced materials with tailored magnetic properties for next generation magnetic and spintronic technologies. As the Curie temperature of these materials is close to room temperature, such tunable magnetic anisotropy holds prospects for functional room-temperature magnetic devices.

cond-mat.mtrl-sci

Electronic and magnetic properties of (NdNiO$_3$)/(La$_{2/3}$Sr$_{1/3}$MnO$_3$) superlattices: a DFT+U perspective

The electronic and magnetic properties of NdNiO$_3$ (NNO) thin films are very sensitive to epitaxial strain and to the proximity to ferromagnetic oxides. In this work, we investigate the structural, electronic, and magnetic properties of NdNiO$_3$/La$_{2/3}$Sr$_{1/3}$MnO$_3$ (NNO/LSMO) superlattices under the epitaxial strain of NdGaO$_3$ (NGO) using density functional theory with Hubbard U correction (DFT+U) calculations. Our findings reveal that LSMO induces insignificant structural distortions on the NiO$_6$ octahedra, and that there is a negligible charge transfer between LSMO and NNO. More importantly, we find an intricate magnetic order regarding the interfacial Ni local moments, where we observe a coexistence of ferromagnetic interactions between interfacial Ni and Mn atoms, and antiferromagnetic interactions between inner Ni ions, which results in an overall ferromagnetic coupling across the interface. We also observe the metallization of NNO through the emergence of a half-metallic density of states in the same spin channel as LSMO, which becomes suppressed the further we move away from the interface. Our theoretical findings agrees well with recent experimental data, shedding light on the complex interplay between the induced magnetic order and the electronic properties of NNO.

cond-mat.mtrl-sci

Engineering the Magnetic Transition Temperatures and the Rare Earth Exchange Interaction in Oxide Heterostructures

The properties of functional oxide heterostructures are strongly influenced by the physics governing their interfaces. Modern deposition techniques allow us to accurately engineer the interface physics through the growth of atomically precise heterostructures. This enables minute control over the electronic, magnetic, and structural characteristics. Here, we investigate the magnetic properties of tailor-made superlattices employing the ferromagnetic and insulating double perovskites RE$_2$NiMnO$_6$ (RE = La, Nd), featuring distinct Curie temperatures. Adjusting the superlattice periodicity at the unit cell level allows us to engineer their magnetic phase diagram. Large periodicity superlattices conserve the individual para- to ferromagnetic transitions of the La$_2$NiMnO$_6$ and Nd$_2$NiMnO$_6$ parent compounds. As the superlattice periodicity is reduced, the Curie temperatures of the superlattice constituents converge and, finally, collapse into one single transition for the lowest period samples. This is a consequence of the magnetic order parameter propagating across the superlattice interfaces, as supported by a minimal Landau theory model. Further, we find that the Nd-Ni/Mn exchange interaction can be enhanced by the superlattice interfaces. This leads to a field-induced reversal of the Nd magnetic moments, as confirmed by synchrotron X-ray magnetic circular dichroism measurements and supported by first-principles calculations. Our work demonstrates how superlattice engineering can be employed to fine-tune the magnetic properties in oxide heterostructures and broadens our understanding of magnetic interfacial effects.

cond-mat.mtrl-sci

Octahedral and polar phase transitions in freestanding films of SrTiO3

From extreme strain to bending, the possibilities in the manipulation of freestanding films of oxide perovskites bring a novel landscape to their properties and brings them one step closer to their application. It is therefore of great importance to fully understand the inherent properties of such films, in which dimensionality and surface effects can play a major role in defining the properties of the materials ground state. This paper reports the properties of freestanding (FS) films of the canonical oxide, SrTiO3 (STO) with thicknesses 20, 30, 40 and 80 nm. We show that the relaxed ultrathin STO FS films become polar at temperatures as high as 85 K, in contrast to the quantum paraelectric behavior of bulk. Our findings are based on the softening of the ferroelectric mode towards the ferroelectric transition temperature Tc and its consecutive hardening below Tc with further decreasing temperature, probed with THz time domain spectroscopy in transmission mode. We find almost no thickness dependence in Tc. Moreover, we characterize the antiferrodistortive (AFD) phase transition in STO FS by X-ray diffraction (XRD) probing superlattice reflections characteristic for the rotation of the TiO6 octahedra. Our results point to a higher phase transition temperature in comparison to bulk STO, as well as an unbalanced domain population favoring the rotation axis to be in plane. X-ray linear dichroism results further show a preferential Ti xz/yz orbital occupancy at the surface, but with a complete degeneracy in the t2g states in the inner part of the film indicating that the AFD distortion does not strongly affect the t2g splitting. These findings demonstrate that STO FS films have clearly different properties than bulk.

cond-mat.mtrl-sci

The impact of the near-surface region on the interpretation of x-ray absorption spectroscopy

Transition metal oxides (TMOs) exhibit a broad spectrum of electronic, magnetic, and optical properties, making them intriguing materials for various technological applications. Soft x-ray absorption spectroscopy (XAS) is widely used to study TMOs, shedding light on their chemical state, electronic structure, orbital polarization, element-specific magnetism, and more. Different XAS acquisition modes feature different information depth regimes in the sample. Here, we employ two XAS acquisition modes, having surface-sensitive versus bulk probing depths, on the prototypical TMO SrVO3. We illustrate and elucidate a strong apparent discrepancy between the different modes, emphasizing the impact of the near-surface region on the interpretation of XAS data. These findings highlight the importance of the acquisition mode selection in XAS analysis. Moreover, the results highlight the role of the near-surface region not only in the characterization of TMOs, but also in the design of future nanoscale oxide electronics.

cond-mat.mtrl-sci

Charge fluctuations in the intermediate-valence ground state of SmCoIn$_5$

The microscopic mechanism of heavy band formation, relevant for unconventional superconductivity in CeCoIn$_5$ and other Ce-based heavy fermion materials, depends strongly on the efficiency with which $f$ electrons are delocalized from the rare earth sites and participate in a Kondo lattice. Replacing Ce$^{3+}$ ($4f^1$, $J=5/2$) with Sm$^{3+}$ ($4f^5$, $J=5/2$), we show that a combination of crystal field and on-site Coulomb repulsion causes SmCoIn$_5$ to exhibit a $Γ_7$ ground state similar to CeCoIn$_5$ with multiple $f$ electrons. Remarkably, we also find that with this ground state, SmCoIn$_5$ exhibits a temperature-induced valence crossover consistent with a Kondo scenario, leading to increased delocalization of $f$ holes below a temperature scale set by the crystal field, $T_v$ $\approx$ 60 K. Our result provides evidence that in the case of many $f$ electrons, the crystal field remains the most important tuning knob in controlling the efficiency of delocalization near a heavy fermion quantum critical point, and additionally clarifies that charge fluctuations play a general role in the ground state of "115" materials.

cond-mat.str-el

Bandwidth Control and Symmetry Breaking in a Mott-Hubbard Correlated Metal

In Mott materials strong electron correlation yields a spectrum of complex electronic structures. Recent synthesis advancements open realistic opportunities for harnessing Mott physics to design transformative devices. However, a major bottleneck in realizing such devices remains the lack of control over the electron correlation strength. This stems from the complexity of the electronic structure, which often veils the basic mechanisms underlying the correlation strength. Here, we present control of the correlation strength by tuning the degree of orbital overlap using picometer-scale lattice engineering. We illustrate how bandwidth control and concurrent symmetry breaking can govern the electronic structure of a correlated $SrVO_3$ model system. We show how tensile and compressive biaxial strain oppositely affect the $SrVO_3$ in-plane and out-of-plane orbital occupancy, resulting in the partial alleviation of the orbital degeneracy. We derive and explain the spectral weight redistribution under strain and illustrate how high tensile strain drives the system towards a Mott insulating state. Implementation of such concepts will drive correlated electron phenomena closer towards new solid state devices and circuits. These findings therefore pave the way for understanding and controlling electron correlation in a broad range of functional materials, driving this powerful resource for novel electronics closer towards practical realization.

cond-mat.str-el

Collective topological spin dynamics in a correlated spin glass

The interplay between spin-orbit interaction (SOI) and magnetic order is currently one of the most active research fields in condensed matter physics and leading the search for materials with novel and tunable magnetic and spin properties. Here we report on a variety of unexpected and unique observations in thin multiferroic \Ge$_{1-x}$Mn$_x$Te films. The ferrimagnetic order in this ferroelectric semiconductor is found to reverse with current pulses six orders of magnitude lower as for typical spin-orbit torque systems. Upon a switching event, the magnetic order spreads coherently and collectively over macroscopic distances through a correlated spin-glass state. Lastly, we present a novel methodology to controllably harness this stochastic magnetization dynamics, allowing us to detect spatiotemporal nucleation of topological spin textures we term ``skyrmiverres''.

cond-mat.mtrl-sci

Large orbital magnetic moment in VI3

The existence of the V3+ ion orbital moment is the open issue of the nature of magnetism in the van der Waals ferromagnet VI3. The huge magnetocrystalline anisotropy in conjunction with the significantly reduced ordered magnetic moment compared to the spin-only value provides strong but indirect evidence of a significant V orbital moment. We used the unique capability of X-ray magnetic circular dichroism to determine the orbital component of the total magnetic moment and provide for the first time a direct proof of an exceptionally sizable orbital moment of the V3+ ion in VI3. Our ligand field multiplet simulations of the XMCD spectra in synergy with the results of DFT calculations agree with the existence of two V sites with different orbital occupations and therefore different OM magnitudes in the ground state.

cond-mat.mtrl-sci

Unusual ferrimagnetism in CaFe2O4

Incomplete cancellation of collinear antiparallel spins gives rise to ferrimagnetism. Even if the oppositely polarized spins are owing to the equal number of a single magnetic element having the same valence state, in principle, a ferrimagnetic state can still arise from the crystallographic inequivalence of the host ions. However, experimental identification of such a state as ferrimagnetic is not straightforward because of the tiny magnitude expected for M and the requirement for a sophisticated technique to differentiate similar magnetic sites. We report a synchrotron-based resonant x-ray investigation at the Fe L2,3 edges on an epitaxial film of CaFe2O4, which exhibits two magnetic phases with similar energies. We find that while one phase of CaFe2O4 is antiferromagnetic, the other one is ferrimagnetic with an antiparallel arrangement of an equal number of spins between two distinct crystallographic sites with very similar local coordination environments. Our results further indicate two distinct origins of an overall minute M; one is intrinsic, from distinct Fe3+ sites, and the other one is extrinsic, arising from defective Fe2+ likely forming weakly-coupled ferrimagnetic clusters. These two origins are uncorrelated and have very different coercive fields. Hence, this work provides a direct experimental demonstration of ferrimagnetism solely due to crystallographic inequivalence of the Fe3+ as the origin of the weak M of CaFe2O4.

cond-mat.mtrl-sci

A multiferroic two-dimensional electron gas

Multiferroics are compounds in which at least two ferroic orders coexist - typically (anti)ferromagnetism and ferroelectricity. While magnetic order can arise in both insulating and conducting compounds, ferroelectricity is in principle not allowed in metals although a few two-dimensional (semi)metals were reported to behave as ferroelectrics. Yet, the combination with magnetic order to realize multiferroic metals remains elusive. Here, by combining x-ray spectroscopy and magnetotransport, we show the coexistence of ferroelectricity and magnetism in an oxide-based two-dimensional electron gas (2DEG). The data evidence a non-volatile switching of the polar displacements and of the anomalous Hall effect by the polarization direction, demonstrating a magnetoelectric coupling. Our findings provide new opportunities in quantum matter stemming from the interplay between ferroelectricity, ferromagnetism and Rashba spin-orbit coupling in a 2DEG.

cond-mat.mtrl-sci

Ferromagnetic order of ultra-thin La0.7Ba0.3MnO3 sandwiched between SrRuO3 layers

We demonstrate the stability of ferromagnetic order of one unit cell thick optimally doped manganite (La0.7Ba0.3MnO3, LBMO) epitaxially grown between two layers of SrRuO3 (SRO) by using x-ray magnetic circular dichroism. At low temperature LBMO shows an inverted hysteresis loop due to the strong antiferromagnetic coupling to SRO. Moreover, above SRO TC the manganite still exhibits magnetic remanence. Density Functional Theory calculations show that coherent interfaces of LBMO with SRO hinder electronic confinement and the strong magnetic coupling enables the increase of the LBMO TC. From the structural point of view, interfacing with SRO enables LBMO to have octahedral rotations similar to bulk. All these factors jointly contribute for stable ferromagnetism up to 130 K for a one unit cell LBMO film.

cond-mat.mtrl-sci

Disorder-induced time effect in the antiferromagnetic domain state of Fe1+yTe

We report on temperature-dependent soft X-ray absorption spectroscopy (XAS) measurements utilizing linearly polarized synchrotron radiation to probe magnetic phase transitions in iron-rich Fe1+yTe. X-ray magnetic linear dichroism (XMLD) signals, which sense magnetic ordering processes at surfaces, start to increase monotonically below the Néel temperature TN = 57 K. This increase is due to a progressive bicollinear antiferromagnetic (AFM) alignment of Fe spins of the monoclinic Fe1+yTe parent phase. This AFM alignment was achieved by a [100]-oriented biasing field favoring a single-domain state during cooling across TN. Our specific heat and magnetization measurements confirm the bulk character of this AFM phase transition. On longer time scales, however, we observe that the field-biased AFM state is highly unstable even at the lowest temperature of T = 3 K. After switching off the biasing field, the XMLD signal decays exponentially with a time constant τ = 1506 s. The initial XMLD signal is restored only upon repeating a cycle consisting of heating and field-cooling through TN. We explain the time effect by a gradual formation of a multi-domain state with 90 deg rotated AFM domains, promoted by structural disorder, facilitating the motion of twin-domains. Significant disorder in our Fe1+yTe sample is evident from our X-ray diffraction and specific heat data. The stability of magnetic phases in Fe-chalcogenides is an important material property, since the Fe(Te1-xSex) phase diagram shows magnetism intimately connected with superconductivity.

cond-mat.supr-con

Novel Cu-based dz2 order at a YBa2Cu3O7/ manganite interface

The interplay of nearly degenerate orders in quantum materials can lead to a myriad of emergent phases. A prominent case is that of the high-Tc cuprates for which the relationship between superconductivity and a short-ranged, incommensurate charge density wave in the CuO2 planes involving the dx2-y2 orbitals (Cu-CDW) is a subject of great current interest. Strong modifications of the strength and coherence of this Cu-CDW have been achieved by applying large magnetic fields, uniaxial pressure, or via the interfacial coupling in cuprate/manganite multilayers. However, such modifications do not alter the dominant orbital character. Here we investigate cuprate/manganite multilayers with resonant inelastic X-ray scattering (RIXS) and show that a new kind of Cu-based density wave order can be induced that has not been previously observed in the cuprates. This order has an unusually small wave vector of Q = 0.096 reciprocal lattice units (r.l.u.), a large correlation length of about 40 nm, and a predominant dz2 orbital character, instead of the typical dx2-y2 character. Its appearance is determined by the hole doping of the manganite which is a key parameter controlling the interfacial charge transfer and orbital reconstruction. We anticipate that the observation of a previously unknown type of density wave order at the YBCO interface will allow for fresh perspectives on the enigmatic relation between superconductivity and charge order (CO) in the cuprates.

cond-mat.str-el

Soft x-ray absorption of thin films detected using substrate luminescence: A performance analysis

X-ray absorption spectroscopy of thin films is central to a broad range of scientific fields, and is typically detected using indirect techniques. X-ray excited optical luminescence (XEOL) from the sample's substrate is one such detection method, in which the luminescence signal acts as an effective transmission measurement through the film. This detection method has several advantages that make it versatile compared to others, in particular for insulating samples or when a probing depth larger than 10nm is required. In this work we present a systematic performance analysis of this method with the aim of providing guidelines for its advantages and pitfalls, enabling a wider use of this method by the thin film community. We compare and quantify the efficiency of XEOL from a range of commonly used substrates. Our measurements demonstrate the equivalence between XEOL and x-ray transmission measurements for thin films. Moreover, we show the applicability of XEOL to magnetic studies by employing XMCD sum rules with XEOL-generated data. Lastly, we demonstrate that above a certain thickness XEOL shows a saturation-like effect, which can be modelled and corrected for.

physics.app-ph

Magnetic properties of metal-organic coordination networks based on 3d transition metal atoms

The magnetic anisotropy and exchange coupling between spins localized at the positions of 3d transition metal atoms forming two-dimensional metal-organic coordination networks (MOCNs) grown on the Au(111) metal surface are studied. In particular, we consider MOCNs made of Ni or Mn metal centers linked by TCNQ (7,7,8,8-tetracyanoquinodimethane) organic ligands, which form rectangular networks with 1:1 stoichiometry. Based on the analysis of X-ray magnetic circular dichroism (XMCD) data taken at T= 2.5 K, we find that Ni atoms in the Ni-TCNQ MOCNs are coupled ferromagnetically and do not show any significant magnetic anisotropy, while Mn atoms in the Mn-TCNQ MOCNs are coupled antiferromagnetically and do show a weak magnetic anisotropy with in-planemagnetization. We explain these observations using both amodelHamiltonian based on mean-fieldWeiss theory and density functional theory calculations that include spin-orbit coupling. Our main conclusion is that the antiferromagnetic coupling between Mn spins and the in-plane magnetization of the Mn spins can be explained neglecting effects due to the presence of the Au(111) surface, while for Ni-TCNQ the metal surface plays a role in determining the absence of magnetic anisotropy in the system.

cond-mat.mes-hall

Strain-controlled responsiveness of slave half-doped manganite La0.5Sr0.5MnO3 layers inserted in BaTiO3 ferroelectric tunnel junctions

Insertion of layers displaying field-induced metal-to-insulator (M/I) transition in ferroelectric tunnel junctions (FTJs) has received attention as a potentially useful way to enlarge junction tunnel electroresistance (TER). Half-doped manganites being at the verge of metal-insulator character are thus good candidates to be slave layers in FTJs. However, the phase diagram of these oxides is extremely sensitive to strain and thus can be radically different when integrated in epitaxial FTJs. Here we report a systematic study of large-area (A = 4 to 100 um2) Pt/La0.5Sr0.5MnO3/BaTiO3/La0.7Sr0.3MnO3 (Pt/HD/BTO/LSMO) FTJs, having different thicknesses of the ferroelectric (2-3nm) and HD layers (1-2nm), grown on substrates imposing either tensile (SrTiO3) or compressive (LaAlO3) strains. Room-temperature electric characterization of the FTJs shows polarization-controlled ON/ OFF states. Clear evidences of field-induced M/I transition (difference between junction resistance in OFF and ON state is increased of more than one order of magnitude) are observed in junctions prepared on SrTiO3 but the HD layer is generally metallic on LaAlO3. Moreover, the M/I transition is only confined in an interfacial layer of the slave film thus entailing an overall reduction of TER. The orderly results reported here give some hints towards selection of HD materials and substrates for optimal FTJ responsiveness.

cond-mat.mtrl-sci

Evidence for Coexistence of Bulk Superconductivity and Itinerant Antiferromagnetism in the Heavy Fermion System CeCo(In$_{1-x}$Cd$_x$)$_5$

In the generic phase diagram of heavy fermion systems, tuning an external parameter such as hydrostatic or chemical pressure modifies the superconducting transition temperature. The superconducting phase forms a dome in the temperature-tuning parameter phase diagram, which is associated with a maximum of the superconducting pairing interaction. Proximity to antiferromagnetism suggests a relation between the disappearance of antiferromagnetic order and superconductivity. We combine muon spin rotation, neutron scattering, and x-ray absorption spectroscopy techniques to gain access to the magnetic and electronic structure of CeCo(In$_{1-x}$Cd$_x$)$_5$ at different time scales. Different magnetic structures are obtained that indicate a magnetic order of itinerant character, coexisting with bulk superconductivity. The suppression of the antiferromagnetic order appears to be driven by a modification of the bandwidth/carrier concentration, implying that the electronic structure and consequently the interplay of superconductivity and magnetism is strongly affected by hydrostatic and chemical pressure.

cond-mat.supr-con