arXiv subjects

P. Giraldo-Gallo

Publications and source records attributed to P. Giraldo-Gallo.

At least 19 recordsLinked to original sources

arXiv2026

Defect-induced multiferroicity in bulk solid solutions of WSe$_2$ and WTe$_2$

Transition metal dichalcogenides provide a versatile platform for tunable ferroic phenomena at the atomic scale owing to their reduced dimensionality. Here we investigate the structural, magnetic, and ferroelectric properties of bulk solid solution W(Se1-xTex)2(1-delta) single crystals synthesized by chemical vapor transport. The room temperature behavior is analyzed as a function of tellurium concentration (x) and chalcogen defect fraction (delta). X ray diffraction and Raman spectroscopy reveal lattice expansion and symmetry reduction with increasing x, consistent with a 2H to 1Td structural transition above a critical composition xc about 18 percent. Piezoresponse force microscopy identifies piezoelectricity near stoichiometric compositions (delta less than 5 percent) and switchable ferroelectricity in the chalcogen deficient regime (delta greater than 20 percent). Magnetometry measurements show a corresponding evolution from paramagnetic to ferromagnetic behavior with increasing delta. Near stoichiometric Te poor samples exhibit piezoelectric and paramagnetic responses, whereas multiferroic states characterized by the coexistence of ferroelectric and ferromagnetic responses emerge at high vacancy concentrations. The performed characterizations indicate that x primarily governs structural symmetry, while delta controls the emergence of both ferromagnetic and ferroelectric responses. These trends are summarized in a configurational phase diagram highlighting the cooperative influence of dopants and defects on ferroic behavior. Overall, controlled stoichiometry and vacancy engineering offer an effective strategy to tailor ferroic responses in transition metal dichalcogenides.

cond-mat.mtrl-sci↗

arXiv2026

Lattice dynamics of the charge density wave compounds TaTe$_4$ and NbTe$_4$ and their evolution across solid solutions

Understanding lattice dynamics is central to elucidating the microscopic origin of charge density waves (CDWs), particularly in materials where electron-phonon coupling can play a dominant role. Raman spectroscopy, combined with first-principles calculations, offers a direct means to identify the vibrational modes involved and to monitor their evolution under controlled perturbations. In this work, we combine density functional theory calculations and Raman spectroscopy measurements to investigate the vibrational properties of the quasi-one-dimensional transition metal tetrachalcogenides TaTe$_4$ and NbTe$_4$, as well as their solid solutions Ta$_{1-x}$Nb$_{x}$Te$_4$ ($x$ = 0.0 - 1.0). For the stoichiometric compounds, first-principles calculations predict a phonon instability consistent with the trimerization associated with the CDW phase, providing theoretical evidence for the lattice distortion driving the transition. The calculated Raman-active modes show good agreement with room-temperature experimental spectra, enabling a systematic assignment of the observed peaks. Across the solid solution, most Raman modes evolve smoothly with composition. In contrast, the highest-frequency E$_{g}$ mode, dominated by transition-metal motion, exhibits a distinct behavior: its frequency remains close to that of the parent compounds while its intensity redistributes with stoichiometry. This evolution highlights the short-range character of this vibrational mode and suggests its relevance to the CDW-related lattice distortion in these materials.

cond-mat.mtrl-sci↗

arXiv2026

Universality of linear in temperature and linear in field Planckian scattering rate in high temperature cuprate superconductors

One of the long standing puzzles in strongly correlated materials is the microscopic origin of the quantum critical Planckian strange metal phase with universal linear in temperature scattering rate from which unconventional superconductivity directly emerges by lowering temperatures. Recently, the linear in temperature and linear in field resistivity have been simultaneously observed in high temperature cuprate superconductors, manifested by the universal field to temperature scaling in magnetoresistivity. To date, there has been a lack of coherent and unified understanding of these coexisting linear behaviors and their possible link to quantum criticality. In this work, we establish the universality in linear in temperature and linear in field Planckian behaviors in underdoped LSCO near optimal doping. Experimentally, we observe the linear in field Planckian scattering rate and its relation to its linear in temperature counterpart. Theoretically, we propose a spin based common microscopic mechanism based on Kondo-like charge fluctuations near local quantum criticality of heavy fermion formulated tJ model subject to a Zeeman term. Similar to frequency to temperature scaling near quantum criticality, we find the magnetic field here effectively introduces a Zeeman energy, reminiscent of an external energy in the quantum critical regime, leading to field to temperature scaling. Our analytically predicted universal field to temperature scaling in isotropic scattering rate and the relation between the linear in temperature and linear in field Planckian coefficients, unifies these two phenomena over an extended doping range, pointing toward a unified quantum-critical origin of Planckian transport in cuprates.

cond-mat.supr-con↗

arXiv2025

Fermi Surface Reconstruction and Anisotropic Linear Magnetoresistance in the Charge Density Wave Topological Semimetal TaTe4

Understanding the interplay between topology and correlated electron states is central to the study of quantum materials. TaTe$_4$ is a quasi-one-dimensional charge density wave (CDW) compound predicted to host topological phases, which makes it a model platform to explore this interplay. Here, we combine high-field magnetotransport measurements with density functional theory calculations to provide a comprehensive mapping of the Fermi surface (FS) of TaTe$_4$ in its CDW phase. Using multiple current-field geometries, we resolve the four largest of six pockets of the FS predicted by theory and find no evidence of non-CDW bands, highlighting the full reconstruction of the FS in the bulk. We identify a previously unobserved quasi-cylindrical pocket and uncover a large size orbit consistent with magnetic breakdown between reconstructed FS sheets, from which we estimate a CDW gap of $\sim$0.29~eV. Moreover, we observe a robust linear magnetoresistance that persists across all field directions when current flows perpendicular to the 1D chains along which the CDW is formed, with a distinct high-field linear regime emerging when field is along the chains. These findings establish TaTe$_4$ as a prototypical material to study the coexistence of correlation-driven reconstruction and topological electronic states.

cond-mat.mtrl-sci↗

arXiv2023

Experimental observation of metallic states with different dimensionality in a quasi-1D charge density wave compound

TaTe$_4$ is a quasi-1D tetrachalcogenide that exhibits a CDW instability caused by a periodic lattice distortion. Recently, pressure-induced superconductivity has been achieved in this compound, revealing a competition between these different ground states and making TaTe$_4$ very interesting for fundamental studies. Although TaTe$_4$ exhibits CDW ordering below 475 K, transport experiments have reported metallic behavior with a resistivity plateau at temperatures lower than 10 K. In this paper, we study the electronic structure of TaTe$_4$ using a combination of high-resolution angle-resolved photoemission spectroscopy and density functional calculations. Our results reveal the existence of the long-sought metallic states. These states exhibit mixed dimensionality, while some of them might have potential topological properties.

cond-mat.str-el↗

arXiv2023

Room temperature multiferroicity in a transition metal dichalcogenide

The coexistence of multiple ferroic orders, i.e. multiferroicity, is a scarce property to be found in materials. Historically, this state has been found mainly in 3-dimensional complex oxides, but so far this state has still been elusive for the most widely studied and characterized family of 2-dimensional compounds, the transition metal dichalcogenides. In this study we report the experimental realization of multiferroic states in this family of materials, at room temperature, in bulk single crystals of Te-doped WSe2. We observe the coexistence of ferromagnetism and ferroelectricity, evidenced in the presence of magnetization and piezoresponse force microscopy hysteresis loops. These findings open the possibility of widening the use and study of van der Waals-based multifunctional devices for new nanoelectronics and spintronics applications.

cond-mat.mtrl-sci↗

arXiv2022

Direct observation of discommensurate charge density wave modulation in the quasi-1D Weyl semimetal candidate NbTe$_4$

The transition-metal tetrachalcogenides are a model system to explore the conjunction of correlated electronic states such as charge density waves (CDW), with topological phases of matter. Understanding the connection between these phases requires a thorough understanding of the individual states, which for the case of the CDW in this system, is still missing. In this paper we combine phonon-structure calculations and scanning tunneling microscopy measurements of NbTe$_4$ in order to provide a full characterization of the CDW state. We find that, at short range, the superstructure formed by the CDW is fully commensurate with the lattice parameters. Moreover, our data reveals the presence of phase-slip domain-walls separating regions of commensurate-CDW in the nanoscale, indicating that the CDW in this compound is discommensurate at long-range. Our results solve a long-standing discussion about the nature of the CDW in these materials, and provide a strong basis for the study of the interplay between this state and other novel quantum electronic states.

cond-mat.mtrl-sci↗

arXiv2022

Raman spectroscopy of few-layers TaS$_2$ and Mo-doped TaS$_2$ with enhanced superconductivity

The use of simple, fast and economic experimental tools to characterize low-dimensional materials is an important step in the process of democratizing the use of such materials in laboratories around the world. Raman spectroscopy has arisen as a way of indirectly determining the thickness of nanolayers of transition metal dichalcogenides (TMDs), avoiding the use of more expensive tools such as atomic force microscopy, and it is therefore a widely used technique in the study of semiconducting TMDs. However, the study of many metallic TMDs in the limit of few atomic layers is still behind when compared to their semiconducting counterparts, partly due to the lack of similar alternative characterization studies. In this work we present the characterization of the Raman spectrum, specifically of the E$^1_{2g}$- and A$_{1g}$-modes, of mechanically exfoliated crystals of Ta$_{1-x}$Mo$_x$S$_2$, a metallic TMD which exhibits charge density wave formation and superconductivity. The clear identification of contributions to the Raman spectrum coming from the SiO$_2$/Si substrate, which overlap with the peaks coming from the sample, and which dominate in intensity in the few-layer-samples limit, allowed the isolation of the individual E$^1_{2g}$- and A$_{1g}$-modes of the samples and, for the first time, the observation of a clear evolution of the Raman shifts of both modes as a function of sample thickness. The evolution of such peaks qualitatively resembles the evolution seen in other TMDs, and provide a way of indirectly determining sample thickness in the limit of few atomic layers at a low cost. In addition, we observe a softening (red-shift) of both E$^1_{2g}$- and A$_{1g}$-modes with Mo-doping in the nanolayers, possibly related to the increased out-of-plane lattice parameter with respect to the pure compound.

cond-mat.mes-hall↗

arXiv2020

Formation of buried domain walls in the ultrafast transition of SmTe$_3$

We study ultrafast x-ray diffraction on the charge density wave (CDW) of SmTe$_3$ using an x-ray free electron laser. The CDW peaks show that photoexcitation with near-infrared pump centered at 800 nm generates domain walls of the order parameter propagating perpendicular to the sample surface. These domain walls break the CDW long range order and suppress the diffraction intensity of the CDW for times much longer than the $\sim 1$~ps recovery of the local electronic gap. We reconstruct the spatial and temporal dependence of the order parameter using a simple Ginzburg-Landau model and find good agreement between the experimental and model fluence dependences. Based on the model we find that at long times, depending on the pump fluence, multiple domain walls remain at distances of few nm from the surface.

cond-mat.str-el↗

arXiv2020

Magnetic breakdown and charge density wave formation: a quantum oscillation study of the rare-earth tritellurides

The rare-earth tritellurides ($R$Te$_3$, where $R$ = La, Ce, Pr, Nd, Sm, Gd, Tb, Dy, Ho, Er, Tm, Y) form a charge density wave state consisting of a single unidirectional charge density wave for lighter $R$, with a second unidirectional charge density wave, perpendicular and in addition to the first, also present at low temperatures for heavier $R$. We present a quantum oscillation study in magnetic fields up to 65T that compares the single charge density wave state with the double charge density wave state both above and below the magnetic breakdown field of the second charge density wave. In the double charge density wave state it is observed that there remain several small, light pockets with the largest occupying around 0.5% of the Brillouin zone. By applying magnetic fields above the independently determined magnetic breakown field, the quantum oscillation frequencies of the single charge density wave state are recovered, as expected in a magnetic breakdown scenario. Measurements of the electronic effective mass do not show any divergence or significant increase on the pockets of Fermi surface observed here as the putative quantum phase transition between the single and double charge density wave states is approached.

cond-mat.str-el↗

arXiv2018

A sharp increase in the density of states in PbTe approaching a saddle point in the band structure

PbTe is a leading mid-range thermoelectric material with a $zT$ that has been enhanced by, amongst other methods, band engineering. Here we present an experimental study of the Hall effect, quantum oscillations, specific heat, and electron microprobe analysis that explores the evolution of the electronic structure of PbTe heavily doped with the `ideal' acceptor Na up to the solubility limit. We identify two phenomenological changes that onset as the electronic structure deviates from a Kane-type dispersion at around 180meV; a qualitative change in the field dependence of the Hall effect indicative of an increase in the high-field limit and a change in the Fermiology, and a sharp increase in the density of states as a function of energy. Following consideration of three possible origins for the observed phenomenology we conclude that the most likely source is non-ellipsoidicity of the $L$-pocket upon approach to a saddle point in the band structure, which is evidenced directly by our quantum oscillation measurements. Comparison to density functional theory calculations imply that this evolution of the electronic structure may be a key contributor to the large thermopower in PbTe.

cond-mat.mtrl-sci↗

arXiv2018

Coherent order parameter dynamics in SmTe$_3$

We present a combined ultrafast optical pump-probe and ultrafast x-ray diffraction measurement of the CDW dynamics in SmTe$_3$ at 300 K. The ultrafast x-ray diffraction measurements, taken at the Linac Coherent Light Source reveal a $\sim 1.55$ THz mode that becomes overdamped with increasing fluence. We identify this oscillation with the lattice component of the amplitude mode. Furthermore, these data allow for a more clear identification of the frequencies present in the optical pump-probe data. In both, reflectivity and diffraction, we observe a crossover of the response from linear (for small displacements) to quadratic in the amplitude of the order parameter displacement. Finally, a time-dependent Ginzburg-Landau model captures the essential features of the experimental observations.

cond-mat.mtrl-sci↗

arXiv2018

Mass enhancement in multiple bands approaching optimal doping in a high-temperature superconductor

Pnictides provide an opportunity to study the effects of quantum criticality in a multi-band high temperature superconductor. Quasiparticle mass divergence near optimal doping, observed in two major classes of high-temperature superconductors, pnictides and cuprates, is a direct experimental indicator of enhanced electronic interactions that accompany quantum criticality. Whether quasiparticles on all Fermi surface pockets in BaFe2(As1-xPx)2 are affected by quantum criticality is an open question, which specific heat measurements at high magnetic fields can directly address. Here we report specific heat measurements up to 35T in BaFe2(As1-xPx)2 over a broad doping range, 0.44 <= x <= 0.6. We observe saturation of C/T in the normal state at all dopings where superconductivity is fully suppressed. Our measurements demonstrate that quasiparticle mass increases towards optimal doping in multiple pockets, some of which exhibit even stronger mass enhancement than previously reported from quantum oscillations of a single pocket.

cond-mat.supr-con↗

arXiv2018

Direct spectroscopic evidence for mixed-valence Tl in the low carrier-density superconductor Pb$_{1-x}$Tl$_x$Te

Upon doping with Tl the narrow band-gap semiconductor PbTe exhibits anomalously high temperature superconductivity despite a very low carrier density as well as signatures of the Kondo effect despite an absence of magnetic moments. These phenomena have been explained by invoking 2$e$ fluctuations of the valence of the Tl dopants but a direct measurement of the mixed-valency implied by such a mechanism has not been reported to date. In this work we present the unambiguous observation of multiple valences of Tl in Tl-doped PbTe via photo emission spectroscopy measurements. It is shown via our quantitative analysis that the suppression of the carrier density at compositions exhibiting superconductivity and Kondo-like behaviour is fully accounted for by mixed valency, thus arguing strongly against a self-compensation scenario proposed elsewhere for this material and strengthening the case for valence fluctuation models. In addition to the identification of Tl$^+$ and Tl$^{3+}$ a possible third intermediate local charge-density is tentatively suggested by full fits to the data, the implications of which are discussed in the context of the charge-Kondo effect.

cond-mat.supr-con↗

arXiv2018

Scale-invariant magnetoresistance in a cuprate superconductor

The anomalous metallic state in high-temperature superconducting cuprates is masked by the onset of superconductivity near a quantum critical point. Use of high magnetic fields to suppress superconductivity has enabled a detailed study of the ground state in these systems. Yet, the direct effect of strong magnetic fields on the metallic behavior at low temperatures is poorly understood, especially near critical doping, $x=0.19$. Here we report a high-field magnetoresistance study of thin films of \LSCO cuprates in close vicinity to critical doping, $0.161\leq x\leq0.190$. We find that the metallic state exposed by suppressing superconductivity is characterized by a magnetoresistance that is linear in magnetic field up to the highest measured fields of $80$T. The slope of the linear-in-field resistivity is temperature-independent at very high fields. It mirrors the magnitude and doping evolution of the linear-in-temperature resistivity that has been ascribed to Planckian dissipation near a quantum critical point. This establishes true scale-invariant conductivity as the signature of the strange metal state in the high-temperature superconducting cuprates.

cond-mat.str-el↗

arXiv2018

Anomalous ^{125}Te Nuclear Spin Relaxation Coincident with Charge Kondo Behavior in Superconducting Pb_{1-x}Tl_{x}Te

We report a ^{125}Te-NMR study of single-crystalline Pb_{1-x}Tl_{x}Te for x= 0 (undoped non-superconducting "parent"), 0.35 at% (doped but on the borderline of superconductivity), and 1.0 at% (superconducting, with a critical temperature Tc ~ 1.0 K). The Knight shift in the normal state is enhanced as x increases, corresponding to an increase in the average density of states (DOS). The NMR line-width also increases significantly with increasing x, indicative of a strong spatial variation in the local DOS surrounding each Tl dopant. Remarkably, for the superconducting composition, the ^{125}Te nuclear spin relaxation rate (1/T1T) for Te ions that are close to the Tl dopants is unexpectedly enhanced in the normal state below a characteristic temperature of ~10 K. This temperature coincides with the temperature below which the normal state resistivity experiences an upturn. Such a simultaneous upturn in both the resistivity and (1/T1T) is highly anomalous, and puts Pb_{1-x}Tl_{x}Te in a distinct new class of doped semiconductors. These observations provide microscopic evidence for dynamical charge fluctuations in the absence of paramagnetism, and are consistent with expectations for charge Kondo behavior associated with the Tl dopant ions. In contrast, such anomalies were not detected in the non-superconducting samples (x=0 and 0.35 at%), suggesting a connection between dynamical valence fluctuations and the occurrence of superconductivity in Pb_{1-x}Tl_{x}Te.

cond-mat.supr-con↗

arXiv2017

Evidence of incoherent carriers associated with resonant impurity levels and their influence on superconductivity in the anomalous superconductor Pb$_{1-x}$Tl$_x$Te

We present a combined experimental and theoretical study of the evolution of the Fermi surface of the anomalous superconductor Pb$_{1-x}$Tl$_x$Te as a function of thallium concentration, drawing on a combination of magnetotransport measurements (Shubnikov de Haas oscillations and Hall coefficient), Angle Resolved Photoemission Spectroscopy (ARPES), and density functional theory (DFT) calculations of the electronic structure. Our results indicate that for Tl concentrations beyond a critical value the Fermi energy coincides with resonant impurity states in Pb$_{1-x}$Tl$_x$Te, and we rule out the presence of an additional valence band maximum at the Fermi energy. Through comparison to non-superconducting Pb$_{1-x}$Na$_x$Te we argue that the presence of these states at the Fermi energy provides the pairing interaction and thus also the anomalously high temperature superconductivity in this material.

cond-mat.supr-con↗

arXiv2017

Anomalous relaxation kinetics and charge density wave correlations in underdoped BaPb1-xBixO3

Superconductivity often emerges in proximity of other symmetry-breaking ground states, such as antiferromagnetism or charge-density-wave (CDW) order. However, the subtle inter-relation of these phases remains poorly understood, and in some cases even the existence of short-range correlations for superconducting compositions is uncertain. In such circumstances, ultrafast experiments can provide new insights, by tracking the relaxation kinetics following excitation at frequencies related to the broken symmetry state. Here, we investigate the transient terahertz conductivity of BaPb1-xBixO3 - a material for which superconductivity is adjacent to a competing CDW phase - after optical excitation tuned to the CDW absorption band. In insulating BaBiO3 we observed an increase in conductivity and a subsequent relaxation, which are consistent with quasiparticles injection across a rigid semiconducting gap. In the doped compound BaPb0.72Bi0.28O3 (superconducting below Tc=7K), a similar response was also found immediately above Tc. This observation evidences the presence of a robust gap up to T=40 K, which is presumably associated with short-range CDW correlations. A qualitatively different behaviour was observed in the same material fo T>40 K. Here, the photo-conductivity was dominated by an enhancement in carrier mobility at constant density, suggestive of melting of the CDW correlations rather than excitation across an optical gap. The relaxation displayed a temperature dependent, Arrhenius-like kinetics, suggestive of the crossing of a free-energy barrier between two phases. These results support the existence of short-range CDW correlations above Tc in underdoped BaPb1-xBixO3, and provide new information on the dynamical interplay between superconductivity and charge order.

cond-mat.supr-con↗