arXiv subjects

G. Allodi

Publications and source records attributed to G. Allodi.

At least 19 recordsLinked to original sources

arXiv2025

Molecular spin qudits to test generalized Bell inequalities

We show that Yb(trensal) molecular nanomagnet, embedding an electronic spin qubit coupled to a nuclear spin qudit, provides an ideal platform to probe entanglement in a qubit-qudit system.This is demonstrated by developing an optimized pulse sequence to show violation of generalized Bell inequalities and by performing realistic numerical simulations including experimentally measured decoherence. We find that the inequalities are safely violated in a wide range of parameters, proving the robustness of entanglement in the investigated system. Furthermore, we propose a scheme to study qudit-qudit entanglement on a molecular spin trimer, in which two spins 3/2 are linked via an interposed switch to turn on and off their mutual interaction.

quant-ph↗

arXiv2025

Magnetic properties of Ge, Re and Cr substituted Fe$_5$SiB$_2$

One of the possible approaches to decrease the demand for critical elements such as rare earths is to develop new sustainable magnets. Iron-based materials are suitable for gap magnets applications since iron is the most abundant ferromagnetic element on Earth. Fe$_5$SiB$_2$ is a candidate as gap magnet thanks to its high Curie temperature (T$_{\text{C}} \sim$ 800 K) and saturation magnetization (M$_{\text{S}}\sim$ 140 Am$^2$kg$^{-1}$). However its anisotropy field is too low for applications (H$_{\text{A}} \sim$ 0.8 T). In order to increase the anisotropy value, we synthesized a series of Ge, Re and Cr substituted Fe$_5$SiB$_2$ samples and studied their magnetic properties. They all crystallize in the Cr$_5$B$_3$-type tetragonal structure with the $I4/mcm$ space group. Curie temperature (T$_{\text{C}}$ = 803 K) and saturation magnetization (M$_{\text{S}}$ = 138 Am$^2$kg$^{-1}$) are slightly decreased by elemental substitution with Re having the largest effect. Despite being reduced, T$_{\text{C}}$ and M$_{\text{S}}$ still maintain significant values (T$_{\text{C}}>$ 750 K and M$_{\text{S}}$ = 118 Am$^2$kg$^{-1}$). The room temperature anisotropy field has been measured by Singular Point Detection (SPD) and increases by about 15% upon Re substitution, reaching 0.92 T for Fe$_{4.75}$Re$_{0.25}$SiB$_2$. We have also used Nuclear Magnetic Resonance and SPD measurements to study the spin reorientation transition which takes place at 172 K and we have found that it is partially suppressed by substitution of Ge from 172 K to 140 K and completely suppressed upon Cr and Re substitution.

cond-mat.mtrl-sci↗

arXiv2024

Ubiquitous order-disorder transition in the Mn antisite sublattice of the (MnBi$_2$Te$_4$)(Bi$_2$Te$_3$)$_n$ magnetic topological insulators

Magnetic topological insulators (TIs) herald a wealth of applications in spin-based technologies, relying on the novel quantum phenomena provided by their topological properties. Particularly promising is the (MnBi$_2$Te$_4$)(Bi$_2$Te$_3$)$_n$ layered family of established intrinsic magnetic TIs that can flexibly realize various magnetic orders and topological states. High tunability of this material platform is enabled by manganese-pnictogen intermixing, whose amounts and distribution patterns are controlled by synthetic conditions. Positive implication of the strong intermixing in MnSb$_2$Te$_4$ is the interlayer exchange coupling switching from antiferromagnetic to ferromagnetic, and the increasing magnetic critical temperature. On the other side, intermixing also implies atomic disorder which may be detrimental for applications. Here, we employ nuclear magnetic resonance and muon spin spectroscopy, sensitive local probe techniques, to scrutinize the impact of the intermixing on the magnetic properties of (MnBi$_2$Te$_4$)(Bi$_2$Te$_3$)$_n$ and MnSb$_2$Te$_4$. Our measurements not only confirm the opposite alignment between the Mn magnetic moments on native sites and antisites in the ground state of MnSb$_2$Te$_4$, but for the first time directly show the same alignment in (MnBi$_2$Te$_4$)(Bi$_2$Te$_3$)$_n$ with n = 0, 1 and 2. Moreover, for all compounds, we find the static magnetic moment of the Mn antisite sublattice to disappear well below the intrinsic magnetic transition temperature, leaving a homogeneous magnetic structure undisturbed by the intermixing. Our findings provide a microscopic understanding of the crucial role played by Mn-Bi intermixing in (MnBi$_2$Te$_4$)(Bi$_2$Te$_3$)$_n$ and offer pathways to optimizing the magnetic gap in its surface states.

cond-mat.mtrl-sci↗

arXiv2022

Effects of charge doping on Mott insulator with strong spin-orbit coupling, Ba$_2$NaOsO$_6$

The effects of doping on the electronic evolution of the Mott insulating state have been extensively studied in efforts to understand mechanisms of emergent quantum phases of materials. The study of these effects becomes ever more intriguing in the presence of entanglement between spin and orbital degrees of freedom. Here, we present a comprehensive investigation of charge doping in the double perovskite Ba$_2$NaOsO$_6$, a a complex Mott insulator where such entanglement plays an important role. We establish that the insulating magnetic ground state evolves from canted antiferromagnet (cAF)to N\'eel order for dopant levels exceeding ~ 10 %. Furthermore, we determine that a broken local point symmetry (BLPS) phase, precursor to the magnetically ordered state, occupies an extended portion of the (H-T) phase diagram with increased doping. This finding reveals that the breaking of the local cubic symmetry is driven by a multipolar order, most-likely of the antiferro-quadrupolar type.

cond-mat.str-el↗

arXiv2022

Effective decoupling of ferromagnetic sublattices by frustration in Heusler alloys

Magnetic frustration in ferromagnetic metallic systems is unusual due to the long-range and symmetric nature of the exchange interactions. In this work we prove that it is possible to obtain a highly frustrated ferromagnetic phase in a multi-sublattices cubic structure through a fine tuning of the magnetic interactions. This peculiar state is achieved in Ni-Mn-(In, Sn) Heusler alloys and results in the effective decoupling of their two intertwined ferromagnetic sublattices. One sublattice is ferromagnetic long range ordered below the macroscopic Curie temperature (TC ) whereas the second one remains disordered until a crossover to a polarized state occurs at T << TC . This result points out that a fine engineering of the magnetic interactions in metallic systems can lead to interesting novel and emergent phenomena.

cond-mat.mtrl-sci↗

arXiv2021

Breaking the ring: $^{53}$Cr-NMR on the Cr$_{8}$Cd molecular nanomagnet

An accurate experimental characterization of finite antiferromagnetic (AF) spin chains is crucial for controlling and manipulating their magnetic properties and quantum states for potential applications in spintronics or quantum computation. In particular, finite AF chains are expected to show a different magnetic behaviour depending on their length and topology. Molecular AF rings are able to combine the quantum-magnetic behaviour of AF chains with a very remarkable tunability of their topological and geometrical properties. In this work we measure the $^{53}$Cr-NMR spectra of the Cr$_{8}$Cd ring to study the local spin densities on the Cr sites. Cr$_{8}$Cd can in fact be considered a model system of a finite AF open chain with an even number of spins. The NMR resonant frequencies are in good agreement with the theoretical local spin densities, by assuming a core polarization feld AC = -12.7 T/$μ_B$. Moreover, these NMR results confirm the theoretically predicted non-collinear spin arrangement along the Cr$_{8}$Cd ring, which is typical of an even-open AF spin chain.

cond-mat.mes-hall↗

arXiv2019

Mixed magnetism, nanoscale electronic segregation and ubiquitous first order transitions in giant magnetocaloric MnFeSiP alloys detected by $^{55}$Mn NMR

We report on a study on a representative set of Fe$_{2}$P-based MnFePSi samples by means of $^{55}$Mn NMR in both zero and applied magnetic field. The first-order nature of the magnetic transition is demonstrated by truncated order parameter curves with a large value of the local ordered moment at the Curie point, even at compositions where the transition appears second order from magnetic measurements. No weak ferromagnetic order could be detected at Si-poor compositions showing the kinetic arrest phenomenon, but rather the phase separation of fully ferromagnetic domains from volume fractions where Mn spins are fluctuating. The more pronounced decrease of the ordered moment at the $3f$ sites on approaching $T_C$, characteristic of the mixed magnetism of these materials, is demonstrated to be driven by a vanishing spin density rather than enhanced spin fluctuations at the $3f$ site. An upper limit of 0.03~$μ_B$ is set for the fluctuating Mn moment at the $3f$ site by the direct detection of a $^{55}$Mn NMR resonance peak in the Mn-rich samples above $T_C$, showing nearly temperature-independent frequency shifts. A sharper secondary peak observed at the same compositions reveals however the disproportionation of a significant $3f$-Mn fraction with negligible hyperfine couplings, which retains its diamagnetic character across the transition, down to the lowest available temperatures. Such a diamagnetic fraction qualitatively accounts for the reduced average $3f$ moment previously reported at large Mn concentrations.

cond-mat.str-el↗

arXiv2019

Singling out the effect of quenched disorder in the phase diagram of cuprates

We investigate the specific influence of structural disorder on the suppression of antiferromagnetic order and on the emergence of cuprate superconductivity. We single out pure disorder, by focusing on a series of Y$_{z}$Eu$_{1-z}$Ba$_2$Cu$_3$O$_{6+y}$ samples at fixed oxygen content $y=0.35$, in the range $0\le z\le 1$. The gradual Y/Eu isovalent substitution smoothly drives the system through the Mott-insulator to superconductor transition from a full antiferromagnet with Néel transition $T_N=320$ K at $z=0$ to a bulk superconductor with superconducting critical temperature $T_c=18$ K at $z=1$, YBa$_2$Cu$_3$O$_{6.35}$. The electronic properties are finely tuned by gradual lattice deformations induced by the different cationic radii of the two lanthanides, inducing a continuous change of the basal Cu(1)-O chain length, as well as a controlled amount of disorder in the active Cu(2)O$_2$ bilayers. We check that internal charge transfer from the basal to the active plane is entirely responsible for the doping of the latter and we show that superconductivity emerges with orthorhombicity. By comparing transition temperatures with those of the isoelectronic clean system we deterime the influence of pure structural disorder connected with the Y/Eu alloy.

cond-mat.supr-con↗

arXiv2018

Fast recovery of the pristine magnetic and structural phases in superconducting LaFeAsO$_{0.89}$F$_{0.11}$ by Mn/Fe substitution

We report on an experimental study of the effect of Mn impurities in the optimally doped LaFeAsO$_{0.89}$F$_{0.11}$ compound. The results show that a very tiny amount of Mn, of the order of 0.1\%, is enough to destroy superconductivity and to recover at low temperatures both the magnetic ground state and the orthorhombic structure of the pristine LaFeAsO parent compound. The results are discussed within a model where electron correlations enhance the Ruderman-Kittel-Kasuya-Yosida interaction among impurities.

cond-mat.supr-con↗

arXiv2017

Fast recovery of the stripe magnetic order by Mn/Fe substitution in F-doped LaFeAsO superconductors

$^{75}$As Nuclear Magnetic (NMR) and Quadrupolar (NQR) Resonance were used, together with Mössbauer spectroscopy, to investigate the magnetic state induced by Mn for Fe substitutions in F-doped LaFe$_{1-x}$Mn$_{x}$AsO superconductors. The results show that $0.5$% of Mn doping is enough to suppress the superconducting transition temperature $T_c$ from 27 K to zero and to recover the magnetic structure observed in the parent undoped LaFeAsO. Also the tetragonal to orthorhombic transition of the parent compound is recovered by introducing Mn, as evidenced by a sharp drop of the NQR frequency. The NQR spectra also show that a charge localization process is at play in the system. Theoretical calculations using a realistic five-band model show that correlation-enhanced RKKY exchange interactions between nearby Mn ions stabilize the observed magnetic order, dominated by $Q_1=(π,0)$ and $Q_2=(0,π)$ ordering vectors. These results give compelling evidence that F-doped LaFeAsO is a strongly correlated electron system at the verge of an electronic instability.

cond-mat.supr-con↗

arXiv2015

Magnetic phase diagram of La$_{2-x}$Sr$_{x}$CoO$_{4}$ revised using muon-spin relaxation

We report the results of a muon-spin relaxation ($μ$SR) investigation of La$_{2-x}$Sr$_{x}$CoO$_{4}$, an antiferromagnetic insulating series which has been shown to support charge ordered and magnetic stripe phases and an hourglass magnetic excitation spectrum. We present a revised magnetic phase diagram, which shows that the suppression of the magnetic ordering temperature is highly sensitive to small concentrations of holes. Distinct behavior within an intermediate $x$ range ($0.2 \leq x \lesssim 0.6$) suggests that the putative stripe ordered phase extends to lower $x$ than previously thought. Further charge doping ($0.67 \leq x \leq 0.9$) prevents magnetic ordering for $T \gtrsim 1.5~{\rm K}$

cond-mat.str-el↗

arXiv2014

Electron localization and possible phase separation in the absence of a charge density wave in single-phase 1T-VS$_2$

We report on a systematic study of the structural, magnetic and transport properties of high-purity 1T-VS$_2$ powder samples prepared under high pressure. The results differ notably from those previously obtained by de-intercalating Li from LiVS$_2$. First, no Charge Density Wave (CDW) is found by transmission electron microscopy down to 94 K. Though, \textit{ab initio} phonon calculations unveil a latent CDW instability driven by an acoustic phonon softening at the wave vector ${\bf q}_{CDW} \approx$ (0.21,0.21,0) previously reported in de-intercalated samples. A further indication of latent lattice instability is given by an anomalous expansion of the V-S bond distance at low temperature. Second, infrared optical absorption and electrical resistivity measurements give evidence of non metallic properties, consistent with the observation of no CDW phase. On the other hand, magnetic susceptibility and NMR data suggest the coexistence of localized moments with metallic carriers, in agreement with \textit{ab initio} band structure calculations. This discrepancy is reconciled by a picture of electron localization induced by disorder or electronic correlations leading to a phase separation of metallic and non-metallic domains in the nm scale. We conclude that 1T-VS$_2$ is at the verge of a CDW transition and suggest that residual electronic doping in Li de-intercalated samples stabilizes a uniform CDW phase with metallic properties.

cond-mat.mtrl-sci↗

arXiv2014

Stripe disorder and dynamics in the hole-doped antiferromagnetic insulator La5/3Sr1/3CoO4

We report on an investigation into the dynamics of the stripe phase of La5/3Sr1/3CoO4, a material recently shown to have an hour-glass magnetic excitation spectrum. A combination of magnetic susceptibility, muon-spin relaxation and nuclear magnetic resonance measurements strongly suggest that the physics is determined by a disordered configuration of charge and spin stripes whose frustrated magnetic degrees of freedom are strongly dynamic at high temperature and which freeze out in a glassy manner as the temperature is lowered. Our results broadly confirm a recent theoretical prediction, but show that the charge quenching remains incomplete well below the charge ordering temperature and reveal, in detail, the manner in which the magnetic degrees of freedom are frozen.

cond-mat.str-el↗

arXiv2013

Band filling effect on polaron localization in La$_{1-x}($Ca$_y$Sr$_{1-y}$)$_{x}$MnO$_3$ manganites

We report on an a $μ$SR and $^{55}$Mn NMR investigation of the magnetic order parameter as a function of temperature in the optimally doped La$_{5/8}$(Ca$_y$Sr$_{1-y}$)$_{3/8}$MnO$_3$ and in the underdoped La$_{1-x}$Sr$_{x}$MnO$_3$ and La$_{1-x}$Ca$_{x}$MnO$_3$ metallic manganite families. The study is aimed at unraveling the effect of lattice distortions, implicitly controlled by the Ca-Sr isoelectronic substitution, from that of hole doping $x$ on the Curie temperature $T_c$ and the order of the magnetic transition. At optimal doping, the transitions are second order at all $y$ values, including the $y=1$ (La$_{5/8}$Ca$_{3/8}$MnO$_3$) end member. In contrast, they are first order in the underdoped samples, which show a finite (truncated) order parameter at the Curie point, including La$_{0.75}$Sr$_{0.25}$MnO$_3$ whose $T_c$ is much higher than that of La$_{5/8}$Ca$_{3/8}$MnO$_3$. The order parameter curves, on the other hand, exhibit a very minor dependence on $x$, if truncation is excepted. This suggests that the effective exchange interaction between Mn ions is essentially governed by local distortions, in agreement with the original double-exchange model, while truncation is primarily, if not entirely, an effect of under- or overdoping. A phase diagram, separating in the $x-y$ plane polaron-driven first order transitions from regular second order transitions governed by critical fluctuations, is proposed for the La$_{1-x}($Ca$_y$Sr$_{1-y}$)$_{x}$MnO$_3$ system.

cond-mat.str-el↗

arXiv2011

Correlated trends of coexisting magnetism and superconductivity in optimally electron-doped oxy-pnictides

We report on the recovery of the short-range static magnetic order and on the concomitant degradation of the superconducting state in optimally F-doped SmFe_(1-x)Ru_(x)AsO_0.85F_0.15 for 0.1< x<0.6. The two reduced order parameters coexist within nanometer-size domains in the FeAs layers and finally disappear around a common critical threshold x_c=0.6. Superconductivity and magnetism are shown to be closely related to two distinct well-defined local electronic environments of the FeAs layers. The two transition temperatures, controlled by the isoelectronic and diamagnetic Ru substitution, scale with the volume fraction of the corresponding environments. This fact indicates that superconductivity is assisted by magnetic fluctuations, which are frozen whenever a short-range static order appears, and totally vanish above the magnetic dilution threshold x_c.

cond-mat.supr-con↗

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↗

arXiv2008

Magnetic order in double-layer manganites (La(1-z)Pr(z))1.2Sr1.8Mn2O7: intrinsic properties and role of the intergrowths

We report on an investigation of the double-layer manganite series (La(1-z)Pr(z))1.2Sr1.8Mn2O7 (0 <= z <= 1), carried out on single crystals by means of both macroscopic magnetometry and local probes of magnetism (muSR, 55Mn NMR). Muons and NMR demonstrate an antiferromagnetically ordered ground state at non-ferromagnetic compositions (z >= 0.6), while more moderate Pr substitutions (0.2 <= z <= 0.4) induce a spin reorientation transition within the ferromagnetic phase. A large magnetic susceptibility is detected at {Tc,TN} < T < 250K at all compositions. From 55Mn NMR spectroscopy, such a response is unambiguously assigned to the intergrowth of a ferromagnetic pseudocubic phase (La(1-z)Pr(z))(1-x)Sr(x)MnO3, with an overall volume fraction estimated as 0.5-0.7% from magnetometry. Evidence is provided for the coupling of the magnetic moments of these inclusions with the magnetic moments of the surrounding (La(1-z)Pr(z))1.2Sr1.8Mn2O7 phase, as in the case of finely dispersed impurities. We argue that the ubiquitous intergrowth phase may play a role in the marked first-order character of the magnetic transition and the metamagnetic properties above Tc reported for double-layer manganites.

cond-mat.str-el↗

arXiv2008

Modification of magnetic and transport properties of manganite layers in Au/La_0.67Sr_0.33MnO_3/SrTiO_3 interfaces

The effect of gold capping on magnetic and transport properties of optimally doped manganite thin films is studied. An extraordinary suppression of conductivity and magnetic properties occurs in epitaxial (001) La_0.67Sr_0.33MnO_3 (LSMO) films grown on SrTiO_3 upon deposition of 2 nm of Au: in the case of ultrathin films of LSMO (4 nm thick) the resistivity increases by four orders of magnitude while the Curie temperature decreases by 180 K. Zero-field 55Mn nuclear magnetic resonance reveals a significant reduction of ferromagnetic double-exchange mechanism in manganite films upon the gold capping. We find evidence for the formation of a 1.9-nm thick magnetic "dead-layer" at the Au/LSMO interface, associated with the creation of interfacial non double-exchange insulating phases.

cond-mat.mtrl-sci↗