arXiv subjects

Sergio O. Valenzuela

Publications and source records attributed to Sergio O. Valenzuela.

At least 19 recordsLinked to original sources

arXiv2026

Strain-Mediated Lattice Reconstruction Enhances Ferromagnetism in Cr2Ge2Te6/WTe2 van der Waals Heterobilayers

Van der Waals (vdW) heterostructures enable tailored electronic and magnetic phases by stacking atomically thin layers with pristine interfaces. Here, we investigate fully 2D Cr2Ge2Te6/WTe2 heterostructures and identify a strong enhancement of ferromagnetism in Cr2Ge2Te6 (CGT). Magnetotransport measurements across multiple devices with WTe2 thicknesses ranging from monolayer to bulk reveal a robust anomalous Hall effect together with a more than twofold increase of the Curie temperature and substantially enhanced coercive fields. Interface microscopy confirms chemically abrupt vdW interfaces with no detectable interdiffusion, while control experiments rule out processing- or stray-field-induced artifacts. Our experiments and theoretical calculations demonstrate that interfacial charge transfer renders CGT conductive and that proximity-induced lattice distortions in CGT enhance exchange and magnetocrystalline anisotropy. These results establish strain-mediated lattice reconstruction as a strategy for engineering high-temperature magnetic order in 2D heterostructures and clarify that modifications within the magnetic layer itself can govern proximity effects in vdW stacks.

cond-mat.mtrl-sci↗

arXiv2026

Hanle lineshapes and spin-rotation signatures from in-plane anisotropic spin relaxation in heterogeneous spin devices

Spin precession experiments in lateral spin devices are a powerful tool for probing the spin transport properties of materials. These experiments can be quantitatively described using the Bloch diffusion equation, which offers a practical framework for modeling spin-related phenomena. In this work, we present calculations of the spin density across heterogeneous, diffusive spintronic devices. The modeled devices feature spin transport channels that include both isotropic and in-plane anisotropic spin relaxation regions. We analyze how different geometric configurations and spin transport parameters influence the lineshape of spin precession signals under magnetic fields applied in different orientations and compare with experimental observations. Our results introduce a theoretical framework for interpreting spin transport measurements in lateral graphene spin devices. The framework is especially relevant when the graphene is partially proximitized by other two-dimensional materials, where proximity-induced spin-orbit coupling leads to anisotropic spin relaxation.

cond-mat.mes-hall↗

arXiv2025

Room-temperature anisotropic in-plane spin dynamics in graphene induced by PdSe$_2$ proximity

Van der Waals heterostructures offer a versatile platform for tailoring electrical, magnetic, optical, and spin transport properties of materials through proximity effects. Notably, hexagonal transition metal dichalcogenides have been shown to induce valley-Zeeman spin-orbit coupling (SOC) in graphene, resulting in significant spin lifetime anisotropy between in-plane and out-of-plane spin orientations. However, in-plane lifetimes remain isotropic due to the inherent threefold symmetry of the heterostructure. Here, we demonstrate that pentagonal PdSe$_2$, characterised by unique in-plane anisotropy, induces an unprecedented gate-tunable SOC in graphene. Our measurements reveal a remarkable 10-fold modulation of the spin lifetime for spins oriented within the graphene plane at room temperature. Moreover, the directional dependence of the spin lifetimes, along the three spatial directions, suggests the existence of a persistent in-plane spin texture component that dominates the spin dynamics. These findings deepen our understanding of spin dynamics in van der Waals heterostructures and open avenues for designing and engineering novel topological phases in graphene-based heterostructures within the strong SOC regime.

cond-mat.mes-hall↗

arXiv2024

Terahertz Spin-Light Coupling in Proximitized Dirac Materials

The two-dimensional (2D) materials are highly susceptible to the influence of their neighbors, thereby enabling the design by proximity phenomena. We reveal a remarkable terahertz (THz) spin-light interaction in 2D Dirac materials that arises from magnetic and spin-orbital proximity effects. The dynamical realization of the spin-charge conversion, the electric dipole spin resonance (EDSR), of Dirac electrons displays distinctive THz features, upon emerging spin-pseudospin proximity terms in the Hamiltonian. To capture the effect of fast pseudospin dynamics on the electron spin, we develop a mean-field theory and complement it with a quantum-mechanical treatment. As a specific example, we investigate the THz response of a single graphene layer proximitized by a magnetic substrate. Our analysis demonstrates a strong enhancement and anomalous polarization structure of the THz-light absorption which can enable THz detection and efficient generation and control of spins in spin-based quantum devices. The identified coupled spin-pseudospin dynamics is not limited to EDSR and may influence a broad range of optical, transport, and ultrafast phenomena.

cond-mat.mes-hall↗

arXiv2023

Experimental demonstration of a magnetically induced warping transition in a topological insulator mediated by rare-earth surface dopants

Magnetic topological insulators (MTI) constitute a novel class of materials where the topologically protected band structure coexists with long-range ferromagnetic order, which can lead to the breaking of time-reversal symmetry (TRS), introducing a bandgap in the Dirac cone-shaped topological surface state (TSS). The gap opening in MITs has been predicted to be accompanied by a distortion in the TSS, evolving its warped shape from hexagonal to trigonal. In this work, we demonstrate such a transition by means of angle-resolved photoemission spectroscopy after the deposition of low concentrations of magnetic rare earths, namely Er and Dy, on the ternary three-dimensional prototypical topological insulator Bi$_2$Se$_2$Te. Signatures of the gap opening occurring as a consequence of the TRS breaking have also been observed, whose existence is supported by the observation of the aforementioned transition. Moreover, increasing the Er coverage results in a tunable p-type doping of the TSS. As a consequence, the Fermi level (E$_{\textrm{F}}$) of our Bi$_2$Se$_2$Te crystals can be gradually tuned towards the TSS Dirac point, and therefore to the magnetically induced bandgap; thus fulfilling two of the necessary prerequisites for the realization of the quantum anomalous Hall effect (QAHE) in this system. The experimental results are rationalized by a theoretical model where a magnetic Zeeman out-of-plane term is introduced in the hamiltonian governing the TSS band dispersion. Our results offer new strategies to control magnetic interactions with TSSs based on a simple approach and open up viable routes for the realization of the QAHE.

cond-mat.mes-hall↗

arXiv2023

Spin-orbit torque switching in 2D ferromagnet / topological insulator heterostructure grown by molecular beam epitaxy

Topological insulators (TIs) are a promising class of materials for manipulating the magnetization of an adjacent ferromagnet (FM) through the spin-orbit torque (SOT) mechanism. However, current studies combining TIs with conventional FMs present large device-to-device variations, resulting in a broad distribution of SOT magnitudes. It has been identified that the interfacial quality between the TI and the FM is of utmost importance in determining the nature and efficiency of the SOT. To optimize the SOT magnitude and enable ultra-low-power magnetization switching, an atomically smooth interface is necessary. To this end, we have developed the growth of a full van der Waals FM/TI heterostructure by molecular beam epitaxy. The compensated TI (Bi0.4Sb0.6)2Te3 and ferromagnetic Fe3GeTe2 (FGT) were chosen because of their exceptional crystalline quality, low carrier concentration in BST and relatively large Curie temperature and perpendicular magnetic anisotropy in FGT. We characterized the magnitude of the SOTs by using thorough harmonic magnetotransport measurements and showed that the magnetization of an ultrathin FGT film could be switched with a current density Jc < 10^10 A/m^2. In comparison to previous studies utilizing traditional FMs, our findings are highly reliable, displaying little to no variation between devices.

cond-mat.mes-hall↗

arXiv2022

Resolving spin currents and spin densities generated by charge-spin interconversion in systems with reduced crystal symmetry

The ability to control the generation of spins in arbitrary directions is a long-sought goal in spintronics. Charge-to-spin interconversion (CSI) phenomena depend strongly on symmetry. Systems with reduced crystal symmetry allow anisotropic CSI with unconventional components, where charge and spin currents and the spin polarization are not mutually perpendicular to each other. Here, we demonstrate experimentally that the CSI in graphene-WTe2 induces spins with components in all three spatial directions. By performing multi-terminal nonlocal spin precession experiments, with specific magnetic field orientations, we discuss how to disentangle the CSI from the spin Hall and inverse spin galvanic effects.

cond-mat.mes-hall↗

arXiv2022

Milliwatt terahertz harmonic generation from topological insulator metamaterials

Achieving efficient, high-power harmonic generation in the terahertz spectral domain has technological applications, for example in sixth generation (6G) communication networks. Massless Dirac fermions possess extremely large terahertz nonlinear susceptibilities and harmonic conversion efficiencies. However, the observed maximum generated harmonic power is limited, because of saturation effects at increasing incident powers, as shown recently for graphene. Here, we demonstrate room-temperature terahertz harmonic generation in a Bi$_2$Se$_3$ topological insulator and topological-insulator-grating metamaterial structures with surface-selective terahertz field enhancement. We obtain a third-harmonic power approaching the milliwatt range for an incident power of 75 mW - an improvement by two orders of magnitude compared to a benchmarked graphene sample. We establish a framework in which this exceptional performance is the result of thermodynamic harmonic generation by the massless topological surface states, benefiting from ultrafast dissipation of electronic heat via surface-bulk Coulomb interactions. These results are an important step towards on-chip terahertz (opto)electronic applications.

physics.optics↗

arXiv2021

Van der Waals heterostructures for spintronics and opto-spintronics

The large variety of 2D materials and their co-integration in van der Waals (vdW) heterostructures enable innovative device engineering. In addition, their atomically-thin nature promotes the design of artificial materials by proximity effects that originate from short-range interactions. Such a designer approach is particularly compelling for spintronics, which typically harnesses functionalities from thin layers of magnetic and non-magnetic materials and the interfaces between them. Here, we overview recent progress on 2D spintronics and opto-spintronics using vdW heterostructures. After an introduction to the forefront of spin transport research, we highlight the unique spin-related phenomena arising from spin-orbit and magnetic proximity effects. We further describe the ability to create multi-functional hybrid heterostructures based on vdW materials, combining spin, valley and excitonic degrees of freedom. We end with an outlook on perspectives and challenges for the design and production of ultra-compact all-2D spin devices and their potential applications in conventional and quantum technologies.

cond-mat.mes-hall↗

arXiv2021

Heat dissipation in few-layer MoS2 and MoS2/hBN heterostructure

State-of-the-art fabrication and characterization techniques have been employed to measure the thermal conductivity of suspended, single-crystalline MoS2 and MoS2/hBN heterostructures. Two-laser Raman scattering thermometry was used combined with real time measurements of the absorbed laser power, which allowed us to determine the thermal conductivities without any assumptions. Measurements on MoS2 layers with thicknesses of 5 and 14 exhibit thermal conductivity in the range between 12 and 24 Wm-1K-1. Additionally, after determining the thermal conductivity of a selected MoS2 sample, an hBN flake was transferred onto it and the effective thermal conductivity of the heterostructure was subsequently measured. Remarkably, despite that the thickness of the hBN layer was less than a third of the thickness of the MoS2 layer, the heterostructure showed an almost eight-fold increase in the thermal conductivity, being able to dissipate more than 10 times the laser power without any visible sign of damage. These results are consistent with a high thermal interface conductance between MoS2 and hBN and an efficient in-plane heat spreading driven by hBN. Indeed, we estimate G 70 MWm-2K-1 which is significantly higher than previously reported values. Our work therefore demonstrates that the insertion of hBN layers in potential MoS2 based devices holds the promise for efficient thermal management.

cond-mat.mes-hall↗

arXiv2021

Large-area van der Waals epitaxy and magnetic characterization of Fe$_3$GeTe$_2$ films on graphene

Scalable fabrication of magnetic 2D materials and heterostructures constitutes a crucial step for scaling down current spintronic devices and the development of novel spintronic applications. Here, we report on van der Waals (vdW) epitaxy of the layered magnetic metal Fe$_3$GeTe$_2$ - a 2D crystal with highly tunable properties and a high prospect for room temperature ferromagnetism - directly on graphene by employing molecular beam epitaxy. Morphological and structural characterization confirmed the realization of large-area, continuous Fe$_3$GeTe$_2$/graphene heterostructure films with stable interfaces and good crystalline quality. Furthermore, magneto-transport and X-ray magnetic circular dichroism investigations confirmed a robust out-of-plane ferromagnetism in the layers, comparable to state-of-the-art exfoliated flakes from bulk crystals. These results are highly relevant for further research on wafer-scale growth of vdW heterostructures combining Fe$_3$GeTe$_2$ with other layered crystals such as transition metal dichalcogenides for the realization of multifunctional, atomically thin devices.

cond-mat.mtrl-sci↗

arXiv2021

The 2021 Quantum Materials Roadmap

In recent years, the notion of Quantum Materials has emerged as a powerful unifying concept across diverse fields of science and engineering, from condensed-matter and cold atom physics to materials science and quantum computing. Beyond traditional quantum materials such as unconventional superconductors, heavy fermions, and multiferroics, the field has significantly expanded to encompass topological quantum matter, two-dimensional materials and their van der Waals heterostructures, Moire materials, Floquet time crystals, as well as materials and devices for quantum computation with Majorana fermions. In this Roadmap collection we aim to capture a snapshot of the most recent developments in the field, and to identify outstanding challenges and emerging opportunities. The format of the Roadmap, whereby experts in each discipline share their viewpoint and articulate their vision for quantum materials, reflects the dynamic and multifaceted nature of this research area, and is meant to encourage exchanges and discussions across traditional disciplinary boundaries. It is our hope that this collective vision will contribute to sparking new fascinating questions and activities at the intersection of materials science, condensed matter physics, device engineering, and quantum information, and to shaping a clearer landscape of quantum materials science as a new frontier of interdisciplinary scientific inquiry.

cond-mat.mes-hall↗

arXiv2020

Control of spin-orbit torques by interface engineering in topological insulator heterostructures

(Bi$_{1-x}$Sb$_x$)$_2$Te$_3$ topological insulators (TIs) are gathering increasing attention owing to their large charge-to-spin conversion efficiency and the ensuing spin-orbit torques (SOTs) that can be used to manipulate the magnetization of a ferromagnet (FM). The origin of the torques, however, remains elusive, while the implications of hybridized states and the strong material intermixing at the TI/FM interface are essentially unexplored. By combining interface chemical analysis and spin-transfer ferromagnetic resonance (ST-FMR) measurements, we demonstrate that intermixing plays a critical role in the generation of SOTs. By inserting a suitable normal metal spacer, material intermixing is reduced and the TI properties at the interface are largely improved, resulting in strong variations in the nature of the SOTs. A dramatic enhancement of a field-like torque, opposing and surpassing the Oersted-field torque, is observed, which can be attributed to the non-equilibrium spin density in Rashba-split surface bands and to the suppression of spin memory loss.

cond-mat.mes-hall↗

arXiv2020

A Molecular Approach for Engineering Interfacial Interactions in Magnetic-Topological Insulator Heterostructures

Controlling interfacial interactions in magnetic/topological insulator heterostructures is a major challenge for the emergence of novel spin-dependent electronic phenomena. As for any rational design of heterostructures that rely on proximity effects, one should ideally retain the overall properties of each component while tuning interactions at the interface. However, in most inorganic interfaces interactions are too strong, consequently perturbing, and even quenching, both the magnetic moment and the topological surface states at each side of the interface. Here we show that these properties can be preserved by using ligand chemistry to tune the interaction of magnetic ions with the surface states. By depositing Co-based porphyrin and phthalocyanine monolayers on the surface of Bi$_2$Te$_3$ thin films, robust interfaces are formed that preserve undoped topological surface states as well as the pristine magnetic moment of the divalent Co ions. The selected ligands allow us to tune the interfacial hybridization within this weak interaction regime. These results, which are in stark contrast with the observed suppression of the surface state at the first quintuple layer of Bi$_2$Se$_3$ induced by the interaction with Co phthalocyanines, demonstrate the capability of planar metal-organic molecules to span interactions from the strong to the weak limit.

cond-mat.mtrl-sci↗

arXiv2019

Tunable room-temperature spin galvanic and spin Hall effects in van der Waals heterostructures

Spin-orbit coupling stands as a powerful tool to interconvert charge and spin currents and to manipulate the magnetization of magnetic materials through the spin torque phenomena. However, despite the diversity of existing bulk materials and the recent advent of interfacial and low-dimensional effects, control of the interconvertion at room-temperature remains elusive. Here, we unequivocally demonstrate strongly enhanced room-temperature spin-to-charge (StC) conversion in graphene driven by the proximity of a semiconducting transition metal dichalcogenide(WS2). By performing spin precession experiments in properly designed Hall bars, we separate the contributions of the spin Hall and the spin galvanic effects. Remarkably, their corresponding conversion effiencies can be tailored by electrostatic gating in magnitude and sign, peaking nearby the charge neutrality point with a magnitude that is comparable to the largest efficiencies reported to date. Such an unprecedented electric-field tunability provides a new building block for spin generation free from magnetic materials and for ultra-compact magnetic memory technologies.

cond-mat.mes-hall↗

arXiv2018

Pseudospin-driven spin relaxation mechanism in graphene

The possibility of transporting spin information over long distances in graphene, owing to its small intrinsic spin-orbit coupling (SOC) and the absence of hyperfine interaction, has led to intense research into spintronic applications. However, measured spin relaxation times are orders of magnitude smaller than initially predicted, while the main physical process for spin dephasing and its charge-density and disorder dependences remain unconvincingly described by conventional mechanisms. Here, we unravel a spin relaxation mechanism for nonmagnetic samples that follows from an entanglement between spin and pseudospin driven by random SOC, which makes it unique to graphene. The mixing between spin and pseudospin-related Berry's phases results in fast spin dephasing even when approaching the ballistic limit, with increasing relaxation times away from the Dirac point, as observed experimentally. The SOC can be caused by adatoms, ripples or even the substrate, suggesting novel spin manipulation strategies based on the pseudospin degree of freedom.

cond-mat.mes-hall↗

arXiv2018

Determination of the spin-lifetime anisotropy in graphene using oblique spin precession

We determine the spin-lifetime anisotropy of spin-polarized carriers in graphene. In contrast to prior approaches, our method does not require large out-of-plane magnetic fields and thus it is reliable for both low- and high-carrier densities. We first determine the in-plane spin lifetime by conventional spin precession measurements with magnetic fields perpendicular to the graphene plane. Then, to evaluate the out-of-plane spin lifetime, we implement spin precession measurements under oblique magnetic fields that generate an out-of-plane spin population. We find that the spin-lifetime anisotropy of graphene on silicon oxide is independent of carrier density and temperature down to 150 K, and much weaker than previously reported. Indeed, within the experimental uncertainty, the spin relaxation is isotropic. Altogether with the gate dependence of the spin lifetime, this indicates that the spin relaxation is driven by magnetic impurities or random spin-orbit or gauge fields.

cond-mat.mes-hall↗

arXiv2018

Thermoelectric spin voltage in graphene

In recent years, new spin-dependent thermal effects have been discovered in ferromagnets, stimulating a growing interest in spin caloritronics, a field that exploits the interaction between spin and heat currents. Amongst the most intriguing phenomena is the spin Seebeck effect, in which a thermal gradient gives rise to spin currents that are detected through the inverse spin Hall effect. Non-magnetic materials such as graphene are also relevant for spin caloritronics, thanks to efficient spin transport, energy-dependent carrier mobility and unique density of states. Here, we propose and demonstrate that a carrier thermal gradient in a graphene lateral spin valve can lead to a large increase of the spin voltage near to the graphene charge neutrality point. Such an increase results from a thermoelectric spin voltage, which is analogous to the voltage in a thermocouple and that can be enhanced by the presence of hot carriers generated by an applied current. These results could prove crucial to drive graphene spintronic devices and, in particular, to sustain pure spin signals with thermal gradients and to tune the remote spin accumulation by varying the spin-injection bias.

cond-mat.mes-hall↗