arXiv subjects

M. Medarde

Publications and source records attributed to M. Medarde.

At least 19 recordsLinked to original sources

arXiv2025

Tailoring the normal and superconducting state properties of ternary scandium tellurides, Sc$_6M$Te$_2$ ($M = $ Fe, Ru and Ir) through chemical substitution

The pursuit of a unifying theory for non-BCS superconductivity has faced significant challenges. One approach to overcome such challenges is to perform systematic investigations into superconductors containing \textit{d}-electron metals in order to elucidate their underlying mechanisms. Recently, the Sc$_6M$Te$_2$ ($M$ = d-electron metal) family has emerged as a unique series of isostructural compounds exhibiting superconductivity across a range of $3d$, $4d$, and $5d$ electron systems. In this study, we employ muon spin rotation, neutron diffraction, and magnetisation techniques to probe the normal and superconducting states at a microscopic level. Our findings reveal extremely dilute superfluid densities that correlate with the critical temperature ($T_\mathrm{c}$). Additionally, we identify high-temperature normal-state transitions that are inversely correlated with $T_\mathrm{c}$. Notably, in Sc$_6$FeTe$_2$, the superconducting pairing symmetry is most likely characterised by two nodeless gaps, one of which closes as electron correlations diminish in the Ru and Ir Sc$_6M$Te$_2$ compounds. These results classify the Sc$_6M$Te$_2$ compounds ($M$ = Fe, Ru, Ir) as unconventional bulk superconductors, where the normal-state transitions and superconducting properties are governed by the interplay between electron correlations and spin-orbit coupling of the d-electron metal.

cond-mat.supr-con↗

arXiv2024

(C$_5$H$_9$NH$_3$)$_2$CuBr$_4$: a metal-organic two-ladder quantum magnet

Low-dimensional quantum magnets are a versatile materials platform for studying the emergent many-body physics and collective excitations that can arise even in systems with only short-range interactions. Understanding their low-temperature structure and spin Hamiltonian is key to explaining their magnetic properties, including unconventional quantum phases, phase transitions, and excited states. We study the metal-organic coordination compound (C$_5$H$_9$NH$_3$)$_2$CuBr$_4$ and its deuterated counterpart, which upon its discovery was identified as a candidate two-leg quantum ($S = 1/2$) spin ladder in the strong-leg coupling regime. By growing large single crystals and probing them with both bulk and microscopic techniques, we deduce that two previously unknown structural phase transitions take place between 136 K and 113 K. The low-temperature structure has a monoclinic unit cell giving rise to two inequivalent spin ladders. We further confirm the absence of long-range magnetic order down to 30 mK and discuss the implications of this two-ladder structure for the magnetic properties of (C$_5$H$_9$NH$_3$)$_2$CuBr$_4$.

cond-mat.str-el↗

arXiv2024

Charge orders with distinct magnetic response in a prototypical kagome superconductor LaRu$_{3}$Si$_{2}$

The kagome lattice has emerged as a promising platform for hosting unconventional chiral charge order at high temperatures. Notably, in LaRu$_{3}$Si$_{2}$, a room-temperature charge-ordered state with a propagation vector of ($\frac{1}{4}$,~0,~0) has been recently identified. However, understanding the interplay between this charge order and superconductivity, particularly with respect to time-reversal-symmetry breaking, remains elusive. In this study, we employ single crystal X-ray diffraction, magnetotransport, and muon-spin rotation experiments to investigate the charge order and its electronic and magnetic responses in LaRu$_{3}$Si$_{2}$ across a wide temperature range down to the superconducting state. Our findings reveal the emergence of a charge order with a propagation vector of ($\frac{1}{6}$,~0,~0) below $T_{\rm CO,2}$ ${\simeq}$ 80 K, coexisting with the previously identified room-temperature primary charge order ($\frac{1}{4}$,~0,~0). The primary charge-ordered state exhibits zero magnetoresistance. In contrast, the appearance of the secondary charge order at $T_{\rm CO,2}$ is accompanied by a notable magnetoresistance response and a pronounced temperature-dependent Hall effect, which experiences a sign reversal, switching from positive to negative below $T^{*}$ ${\simeq}$ 35 K. Intriguingly, we observe an enhancement in the internal field width sensed by the muon ensemble below $T^{*}$ ${\simeq}$ 35 K. Moreover, the muon spin relaxation rate exhibits a substantial increase upon the application of an external magnetic field below $T_{\rm CO,2}$ ${\simeq}$ 80 K. Our results highlight the coexistence of two distinct types of charge order in LaRu$_{3}$Si$_{2}$ within the correlated kagome lattice, namely a non-magnetic charge order ($\frac{1}{4}$,~0,~0) below $T_{\rm co,1}$ ${\simeq}$ 400 K and a time-reversal-symmetry-breaking charge order below $T_{\rm CO,2}$.

cond-mat.supr-con↗

arXiv2023

Charge order above room-temperature in a prototypical kagome superconductor La(Ru$_{1-x}$Fe$_{x}$)$_{3}$Si$_{2}$

The kagome lattice is an intriguing and rich platform for discovering, tuning and understanding the diverse phases of quantum matter, which is a necessary premise for utilizing quantum materials in all areas of modern and future electronics in a controlled and optimal way. The system LaRu$_{3}$Si$_{2}$ was shown to exhibit typical kagome band structure features near the Fermi energy formed by the Ru-$dz^{2}$ orbitals and the highest superconducting transition temperature $T_{\rm c}$ ${\simeq}$ 7K among the kagome-lattice materials. However, the effect of electronic correlations on the normal state properties remains elusive. Here, we report the discovery of charge order in La(Ru$_{1-x}$Fe$_{x}$)$_{3}$Si$_{2}$ ($x$ = 0, 0.01, 0.05) beyond room-temperature. Namely, single crystal X-ray diffraction reveals charge order with a propagation vector of ($\frac{1}{4}$,0,0) below $T_{\rm CO-I}$ ${\simeq}$ 400K in all three compounds. At lower temperatures, we see the appearance of a second set of charge order peaks with a propagation vector of ($\frac{1}{6}$,0,0). The introduction of Fe, which is known to quickly suppress superconductivity, does not drastically alter the onset temperature for charge order. Instead, it broadens the scattered intensity such that diffuse scattering appears at the same onset temperature, however does not coalesce into sharp Bragg diffraction peaks until much lower in temperature. Our results present the first example of a charge ordered state at or above room temperature in the correlated kagome lattice with bulk superconductivity.

cond-mat.supr-con↗

arXiv2023

Microscopic study of the impurity effect in the kagome superconductor La(Ru$_{1-x}$Fe$_{x}$)$_{3}$Si$_{2}$

We report on the effect of magnetic impurities on the microscopic superconducting (SC) properties of the kagome-lattice superconductor La(Ru$_{1-x}$Fe$_{x}$)$_{3}$Si$_{2}$ using muon spin relaxation/rotation. A strong suppression of the superconducting critical temperature $T_{\rm c}$, the SC volume fraction, and the superfluid density was observed. We further find a correlation between the superfluid density and $T_{\rm c}$ which is considered a hallmark feature of unconventional superconductivity. Most remarkably, measurements of the temperature-dependent magnetic penetration depth ${\lambda}$ reveal a change in the low-temperature behavior from exponential saturation to a linear increase, which indicates that Fe doping introduces nodes in the superconducting gap structure at concentrations as low as $x=$~0.015. Our results point to a rare example of unconventional superconductivity in the correlated kagome lattice and accessible tunability of the superconducting gap structure, offering new insights into the microscopic mechanisms involved in superconducting order.

cond-mat.supr-con↗

arXiv2023

Hidden magnetism uncovered in charge ordered bilayer kagome material ScV_6Sn_6

Charge ordered kagome lattices have been demonstrated to be intriguing platforms for studying the intertwining of topology, correlation, and magnetism. The recently discovered charge ordered kagome material ScV_6Sn_6 does not feature a magnetic groundstate or excitations, thus it is often regarded as a conventional paramagnet. Here, using advanced muon-spin rotation spectroscopy, we uncover an unexpected hidden magnetism of the charge order. We observe a striking enhancement of the internal field width sensed by the muon ensemble, which takes place within the charge ordered state. More remarkably, the muon spin relaxation rate below the charge ordering temperature is substantially enhanced by applying an external magnetic field. Taken together with the hidden magnetism found in AV_3Sb_5 (A = K, Rb, Cs) and FeGe kagome systems, our results suggest ubiqitous time-reversal symmetry-breaking in charge ordered kagome lattices.

cond-mat.str-el↗

arXiv2022

Local spectroscopic evidence for a nodeless magnetic kagome superconductor CeRu$_2$

We report muon spin rotation (${\mu}$SR) experiments on the microscopic properties of superconductivity and magnetism in the kagome superconductor CeRu$_{2}$ with $T_{\rm c}$~${\simeq}$~5~K. From the measurements of the temperature-dependent magnetic penetration depth ${\lambda}$, the superconducting order parameter exhibits nodeless pairing, which fits best to an anisotropic $s$-wave gap symmetry. We further show that the $T_{\rm c}$/$\lambda^{-2}$ ratio is comparable to that of unconventional superconductors. Furthermore, the powerful combination of zero-field (ZF)-${\mu}$SR and high-field ${\mu}$SR has been used to uncover magnetic responses across three characteristic temperatures, identified as $T_1^*$~${\simeq}$~110~K, $T_2^*$~${\simeq}$~65~K, and $T_3^*$~${\simeq}$~40~K. Our experiments classify CeRu$_{2}$ as an exceedingly rare nodeless magnetic kagome superconductor.

cond-mat.supr-con↗

arXiv2022

Magnetic order and exchange couplings in the frustrated diamond lattice antiferromagnet MnSc$_2$Se$_4$

We report the magnetic properties of $A$-site spinel compound MnSc$_2$Se$_4$. The macroscopic magnetic measurements uncovers successive magnetic transitions at $T_{\rm{N1}}$= 2.04 K, followed by two further transitions at $T_{\rm{N2}}$=1.8 K and $T_{\rm{N3}}$=1.6 K. Neutron powder diffraction reveals that both, $T_{\rm{N2}} < T < T_{\rm{N1}}$ and $T <T_{\rm{N3}}$, orders are associated with the propagation vector $k$=(3/4 3/4 0), while the magnetic structures are collinear amplitude modulated and helical, respectively. Using neutron powder spectroscopy we demonstrated the effect of substitution of S by Se on the magnetic exchange. The energy range of the spin-wave excitations is supressed due to the chemical pressure of the $X$- ion in MnSc$_2X_4$ ($X$=S, Se) spinels.

cond-mat.str-el↗

arXiv2022

Weak ferromagnetism linked to the high-temperature spiral phase of YBaCuFeO5

The layered perovskite YBaCuFeO5 is a rare example of cycloidal spiral magnet whose ordering temperature Tspiral can be tuned far beyond room temperature by adjusting the degree of Cu2+/Fe3+ chemical disorder in the structure. This unusual property qualifies this material as one of the most promising spin-driven multiferroic candidates. However, very little is known about the response of the spiral to magnetic fields, crucial for magnetoelectric cross-control applications. Using bulk magnetization and neutron powder diffraction measurements under magnetic fields up to 9 T we report here the first temperature-magnetic field phase diagram of this material. Besides revealing a strong stability of the spiral state, our data uncover the presence of weak ferromagnetism coexisting with the spiral modulation. Since ferromagnets can be easily manipulated with magnetic fields, this observation opens new perspectives for the control of the spiral orientation, directly linked to the polarization direction, as well as for a possible future use of this material in technological applications.

physics.app-ph↗

arXiv2021

Time-reversal symmetry-breaking charge order in a kagome superconductor

The kagome lattice, the most prominent structural motif in quantum physics, benefits from inherent nontrivial geometry to host diverse quantum phases, ranging from spin-liquid phases, topological matter to intertwined orders, and most rarely unconventional superconductivity. Recently, charge sensitive probes have suggested that the kagome superconductors AV_3Sb_5 (A = K, Rb, Cs) (A = K, Rb, Cs) exhibit unconventional chiral charge order, which is analogous to the long-sought-after quantum order in the Haldane model or Varma model. However, direct evidence for the time-reversal symmetry-breaking of the charge order remains elusive. Here we utilize muon spin relaxation to probe the kagome charge order and superconductivity in KV_3Sb_5. We observe a striking enhancement of the internal field width sensed by the muon ensemble, which takes place just below the charge ordering temperature and persists into the superconducting state. Remarkably, the muon spin relaxation rate below the charge ordering temperature is substantially enhanced by applying an external magnetic field. We further show the multigap nature of superconductivity in KV_3Sb_5 and that the T_c/lambda_{ab}^{-2} ratio is comparable to those of unconventional high-temperature superconductors. Our results point to time-reversal symmetry breaking charge order intertwining with unconventional superconductivity in the correlated kagome lattice.

cond-mat.mtrl-sci↗

arXiv2021

Raman spectroscopic evidence for multiferroicity in rare earth nickelate single crystals

The rare earth nickelates RNiO3 are metallic at high temperatures and insulating and magnetically ordered at low temperatures. The low temperature phase has been predicted to be type II multiferroic, i.e. ferroelectric and magnetic order are coupled and occur simultaneously. Confirmation of those ideas has been inhibited by the absence of experimental data on single crystals. Here we report on Raman spectroscopic data of RNiO3 single crystals (R = Y, Er, Ho, Dy, Sm, Nd) for temperatures between 10 K and 1000 K. Entering the magnetically ordered phase we observe the appearance of a large number of additional vibrational modes, implying a breaking of inversion symmetry expected for multiferroic order.

cond-mat.str-el↗

arXiv2021

Nodeless superconductivity in the centro- and noncentrosymmetric rhenium-boron superconductors

We report a comprehensive study of the centrosymmetric Re$_3$B and noncentrosymmetric Re$_7$B$_3$ superconductors. At a macroscopic level, their bulk superconductivity (SC), with $T_c$ = 5.1 K (Re$_3$B) and 3.3 K (Re$_7$B$_3$), was characterized via electrical-resistivity, magnetization, and heat-capacity measurements, while their microscopic superconducting properties were investigated by means of muon-spin rotation/relaxation ($\mu$SR). In both Re$_3$B and Re$_7$B$_3$ the low-$T$ zero-field electronic specific heat and the superfluid density (determined via tranverse-field $\mu$SR) suggest a nodeless SC. Both compounds exhibit some features of multigap SC, as evidenced by temperature-dependent upper critical fields $H_\mathrm{c2}(T)$, as well as by electronic band-structure calculations. The absence of spontaneous magnetic fields below the onset of SC, as determined from zero-field $\mu$SR measurements, indicates a preserved time-reversal symmetry in the superconducting state of both Re$_3$B and Re$_7$B$_3$. Our results suggest that a lack of inversion symmetry and the accompanying antisymmetric spin-orbit coupling effects are not essential for the occurrence of multigap SC in these rhenium-boron compounds.

cond-mat.supr-con↗

arXiv2021

Magnetic order in the quasi-one-dimensional Ising system RbCoCl$_3$

The dynamical properties of free and bound domain-wall excitations in Ising-chain materials have recently become the focus of intense research interest. New materials and spectrometers have made it possible to control the environment of coupled Ising chains by both effective internal and applied external fields, which can be both longitudinal and transverse, and thus to demonstrate how the resulting magnetic phase transitions and the nature of the associated excited states obey fundamental symmetry properties. In RbCoCl$_3$, the weakly coupled Ising chains form a triangular lattice whose frustrated geometry and magnetic ordering transitions at low temperature open new possibilities for the Ising-chain environment. We have investigated the structure and magnetism in RbCoCl$_3$ by high-resolution x-ray diffraction and neutron scattering measurements on powder and single crystal samples between 1.5 K and 300 K. Upon cooling, the Co$^{2+}$ spins develop one-dimensional antiferromagnetic correlations along the chain axis ($c$-axis) below 90 K. Below the first N\'eel temperature, $T_{N1}$ = 28 K, a partial 3D magnetic order sets in, with propagation vector ${\vec k}_1$ = (1/3,1/3,1), the moments aligned along the $c$-axis and every third chain uncorrelated from its neighbours. Only below a second magnetic phase transition at $T_{N2}$ = 13 K does the system achieve a fully ordered state, with two additional propagation vectors: ${\vec k}_2$ = (0,0,1) establishes a "honeycomb" $c$-axis order, in which 1/3 of the chains are subject to a strong effective mean field due to their neighbours whereas 2/3 experience no net field, while ${\vec k}_3$ = (1/2,0,1) governs a small, staggered in-plane ordered moment. We conclude that RbCoCl$_3$ is an excellent material to study the physics of Ising chains in a wide variety of temperature-controlled environments.

cond-mat.str-el↗

arXiv2021

Intriguing magnetism of the topological kagome magnet TbMn_6Sn_6

Magnetic topological phases of quantum matter are an emerging frontier in physics and material science. Along these lines, several kagome magnets have appeared as the most promising platforms. Here, we explore magnetic correlations in the transition-metal-based kagome magnet TbMn$_{6}$Sn$_{6}$ using muon spin rotation, combined with local field analysis and neutron diffraction. Our results show that the system exhibits an out-of-plane ferrimagnetic structure $P6/mm'm'$ (comprised by Tb and Mn moments) with slow magnetic fluctuations below $T_{\rm C2}$~=~320~K. These fluctuations exhibit a slowing down below $T_{\rm C1}^{*}$~${\simeq}$~120~K, and we see the formation of static patches with ideal out-of-plane order below $T_{\rm C1}$~${\simeq}$~20~K which grow in a volume with decreasing temperature. The appearance of the static patches has a similar onset to the interesting phenomenon such as spin-polarized Dirac dispersion with a large Chern gap and topological edge states. We further show that the temperature evolution of the anomalous Hall conductivity (AHC) is strongly influenced by the low temperature magnetic crossover. Our presented experimental results show that the onset of the topological electronic properties tied to the Dirac band is promoted only by true static out-of-plane ferrimagnetic order in TbMn$_{6}$Sn$_{6}$ and is washed out by the slow magnetic fluctuations above $T_{\rm C1}$~${\simeq}$~20~K. Remarkably, hydrostatic pressure of 2.1 GPa stabilises static out-of-plane topological ferrimagnetic ground state in the whole volume of the sample. Therefore the exciting perspective arises of a magnetic system in which the topological response can be controlled, and thus explored, over a wide range of parameters.

cond-mat.str-el↗

arXiv2020

Unconventional transverse transport above and below the magnetic transition temperature in Weyl semimetal EuCd$_2$As$_2$

As exemplified by the growing interest in the quantum anomalous Hall effect, the research on topology as an organizing principle of quantum matter is greatly enriched from the interplay with magnetism. In this vein, we present a combined electrical and thermoelectrical transport study on the magnetic Weyl semimetal EuCd$_2$As$_2$. Unconventional contribution to the anomalous Hall and anomalous Nernst effects were observed both above and below the magnetic transition temperature of EuCd$_2$As$_2$, indicating the existence of significant Berry curvature. EuCd$_2$As$_2$ represents a rare case in which this unconventional transverse transport emerges both above and below the magnetic transition temperature in the same material. The transport properties evolve with temperature and field in the antiferromagnetic phase in a different manner than in the paramagnetic phase, suggesting different mechanisms to their origin. Our results indicate EuCd$_2$As$_2$ is a fertile playground for investigating the interplay between magnetism and topology, and potentially a plethora of topologically nontrivial phases rooted in this interplay.

cond-mat.str-el↗

arXiv2020

Multigap superconductivity in the Mo$_5$PB$_2$ boron-phosphorus compound

The tetragonal Mo$_5$PB$_2$ compound was recently reported to show superconductivity with a critical temperature up to 9.2 K. In search of evidence for multiple superconducting gaps in Mo$_5$PB$_2$, comprehensive measurements, including magnetic susceptibility, electrical resistivity, heat capacity, and muon-spin rotation and relaxation ($\mu$SR) measurements were carried out. Data from both low-temperature superfluid density and electronic specific heat suggest a nodeless superconducting ground state in Mo$_5$PB$_2$. Two superconducting energy gaps $\Delta_0$ = 1.02 meV (25%) and 1.49 meV (75%) are required to describe the low-$T$ electronic specific-heat data. The multigap features are clearly evidenced by the field dependence of the electronic specific-heat coefficient and the Gaussian relaxation rate in the superconducting state (i.e., superfluid density), as well as by the temperature dependence of the upper critical field. By combining our extensive experimental results with numerical band-structure calculations, we provide compelling evidence of multigap superconductivity in Mo$_5$PB$_2$.

cond-mat.supr-con↗

arXiv2020

Superconductivity and topological aspects of the rock-salt carbides NbC and TaC

Superconducting materials with a nontrivial band structure are potential candidates for topological superconductivity. Here, by combining muon-spin rotation and relaxation ($\mu$SR) methods with theoretical calculations, we investigate the superconducting and topological properties of the rock-salt-type compounds NbC and TaC (with$T_c$ = 11.5 and 10.3 K, respectively). At a macroscopic level, the magnetization and heat-capacity measurements under applied magnetic field provide an upper critical field of 1.93 and 0.65 T for NbC and TaC, respectively. The low-temperature superfluid density, determined by transverse-field $\mu$SR and electronic specific-heat data, suggest a fully-gapped superconducting state in both NbC and TaC, with a zero-temperature gap $\Delta_0 = 1.90$ and 1.45 meV, and a magnetic penetration depth $\lambda_0$ = 141 and 77 nm, respectively. Band-structure calculations suggest that the density of states at the Fermi level is dominated by the Nb $4d$- (or Ta $5d$-) orbitals, which are strongly hybridized with the C $p$-orbitals to produce large cylinder-like Fermi surfaces, similar to those of high-$T_c$ iron-based superconductors. Without considering the spin-orbit coupling (SOC) effect, the first Brillouin zone contains three closed node lines in the bulk band structure, protected by time-reversal and space-inversion symmetry. When considering SOC, its effects in the NbC case appear rather modest. Therefore, the node lines may be preserved in NbC, hence proposing it as a potential topological superconductor.

cond-mat.supr-con↗

arXiv2020

Simultaneous Nodal Superconductivity and Time-Reversal Symmetry Breaking in the Noncentrosymmetric Superconductor CaPtAs

By employing a series of experimental techniques, we provide clear evidence that CaPtAs represents a rare example of a noncentrosymmetric superconductor which simultaneously exhibits nodes in the superconducting gap and broken time-reversal symmetry (TRS) in its superconducting state (below $T_c$ $\approx$ 1.5 K). Unlike in fully-gapped superconductors, the magnetic penetration depth $\lambda(T)$ does not saturate at low temperatures, but instead it shows a $T^2$-dependence, characteristic of gap nodes. Both the superfluid density and the electronic specific heat are best described by a two-gap model comprising of a nodeless gap and a gap with nodes, rather than by single-band models. At the same time, zero-field muon-spin spectra exhibit increased relaxation rates below the onset of superconductivity, implying that TRS is broken in the superconducting state of CaPtAs, hence indicating its unconventional nature. Our observations suggest CaPtAs to be a new remarkable material which links two apparently disparate classes, that of TRS-breaking correlated magnetic superconductors with nodal gaps and the weakly-correlated noncentrosymmetric superconductors with broken TRS, normally exhibiting only a fully-gapped behavior.

cond-mat.supr-con↗