arXiv subjects

Samuel Mañas-Valero

Publications and source records attributed to Samuel Mañas-Valero.

At least 19 recordsLinked to original sources

arXiv2026

Layered spin-crossover metal-organic frameworks for light-induced control of two-dimensional quantum materials

Metal-organic frameworks (MOFs) are widely explored for gas separation, catalysis or energy storage, yet their integration with other electronically functional materials remains largely unexplored. Here, we integrate the layered Hofmann-type spin-crossover (SCO) MOF {FeII(pyS2Et)2[PtII(CN)4]} into electrical nanodevices to control the properties of two-dimensional (2D) quantum materials. Our molecular approach exploits the stimuli-responsive nature of SCO layered materials as switchable building blocks. We demonstrate selective modulation of the electronic transport in van der Waals heterostructures interfacing SCO with 2D quantum materials (few-layer graphene, magnetic CrSBr, superconducting NbSe2) through the strain induced via thermal and light-induced spin transitions. In graphene, the conductivity is selectively switched by light. In spin-valves based on CrSBr bilayers, the MOF triggers magnetic hysteresis (absent in pristine CrSBr) and enables tunable non-volatile zero-field memory. In NbSe2, light modulates the superconducting critical current and transition temperature. These results establish layered stimuli-responsive SCO MOFs as active molecular control elements for 2D quantum materials, providing a route to strain-mediated control of electronic, magnetic, and superconducting functionalities and extending MOF-based architectures beyond traditional porous-matter applications towards multifunctional electronics and spintronics.

cond-mat.mtrl-sci↗

arXiv2026

Stacking-tuned superconductivity and competing charge-density-wave states in NbSe$_2$

Layer stacking provides a powerful yet underexplored route for reshaping collective quantum order in van der Waals materials. Here we use high-resolution scanning tunneling microscopy and spectroscopy to show that the stacking sequence alone can qualitatively transform the charge density and superconducting orders in NbSe$_2$, while preserving the same in-plane atomic structure. Comparing the 4Ha and 2H polytypes, we find that, unlike the ubiquitous triangular incommensurate $3Q^\mathrm{I}$ order of 2H-NbSe$_2$, 4Ha-NbSe$_2$ hosts two competing CDW states with no measurable correlation with local strain: a unidirectional commensurate $1Q^\mathrm{C}$ phase and a triangular incommensurate $3Q^\mathrm{I}$ phase, with $Q^\mathrm{I}=Q^\mathrm{C}+δ$. We introduce a phase-resolved analysis that directly maps the gradient of the CDW phases and reveals vortices bound to the $1Q^\mathrm{C}$ - $3Q^\mathrm{I}$ phase boundaries. These vortices accommodate the momentum mismatch $δ$ through abrupt $2π$ phase slips, providing a mechanism by which distinct charge orders coexist. Superconductivity is also reshaped by stacking, while both polytypes exhibit multiband pairing.

cond-mat.supr-con↗

arXiv2026

Reversible nanoscale patterning of WTe$_2$ with a scanning tunneling microscope

Manipulating the lattice structure of ferroelectric quantum materials enables their use in low-power electronic devices, including field-effect transistors. WTe$_2$ is a Weyl-semimetal candidate and ferroelectric, both properties arising from the reduced crystal symmetry of its T$_\mathrm{d}$ ground state. The T$_\mathrm{d}$ crystal phase results from a Peierls distortion of the 1T parent structure and an interlayer shift. While experiments in WTe$_2$ have established ferroelectric switching and transient control of the predicted topological phase via ultrafast excitations, persistent electronic changes on the nanometer scale remain elusive. Here, we demonstrate that current pulses applied via scanning tunneling microscopy can both write and erase persistent nanometer-scale patterns on the surface of WTe$_2$. These patterns consist of apparent picometer in-plane and out-of-plane atomic displacements, accompanied by changes to the local density of states. The out-of-plane displacements further modulate the Peierls-like distortion present in WTe$_2$, while the in-plane displacements are indicative of ferroelectric switching. The induced patterns can be repositioned and erased, suggesting a nanoscale handle on the ferroelectric properties of WTe$_2$.

cond-mat.mtrl-sci↗

arXiv2026

One-Dimensional Materials Supported in Two-Dimensional van der Waals Metal-Organic Frameworks with Optical Anisotropy Switching via Twist-Engineering

Van der Waals (vdW) materials provide a platform to study and control the physical properties of low-dimensional materials. While strategies developed for two-dimensional (2D) crystals are not directly transferable to one-dimensional (1D) systems, we can benefit from them by creating layers formed by interconnected chains. Here, we develop a molecular strategy to illustrate this concept consisting of assembling 1D materials in 2D metal-organic frameworks (MOFs). Crystals of [FeX(pzX)(bpy)] (X = Cl, F; pz = pyrazole; bpy = bipyridine) consist of iron chains along the b-axis, crosslinked via bpy ligands along the a-axis to form 2D layers, stacked along the c-axis via vdW forces. This structural anisotropy manifests itself in highly-anisotropic optical properties, as demonstrated by optical measurements in the visible and terahertz ranges, results which are supported by DFT calculations. Chemical substitution enables the tuning of the optical properties, as exemplified by the photoluminescence of the Cl-derivative, which is quenched for the F-derivative. Thin-layers are obtained by mechanical exfoliation, and their optical properties are further tuned through the fabrication of orthogonally-twisted vdW heterostructures, enabling to effectively switch-off the optical anisotropy. Our work highlights the chemical flexibility of vdW layered MOFs as a platform for designing and manipulating 1D architectures.

cond-mat.mtrl-sci↗

arXiv2026

Anomalous Nonlinear Magnetoconductivity in van der Waals Magnet CrSBr

Nonlinear magnetoconductivity (NLMC) is a nonreciprocal transport response arising in non-centrosymmetric materials. However, this ordinary NLMC signal vanishes at zero magnetic field, limiting its potential for applications. Here, we report the observation of an anomalous NLMC controlled by internal order parameters such as the magnetization or Néel vectors. We achieve this response by breaking both inversion and time-reversal symmetry in artificial van der Waals heterostructures based on the magnetic CrSBr and insulating hBN. The nonreciprocal signal can be tuned between two different states in ferromagnetic monolayer CrSBr and among four different states in antiferromagnetic bilayer CrSBr, thanks to its metamagnetic transition. Remarkably, this output signal in the ferromagnetic (antiferromagnetic) state of CrSBr is three (one) orders of magnitude higher than those previously measured. A conductivity scaling analysis reveals the Berry connection polarizability as the origin of the anomalous NLMC. Our results pave the way for high-frequency rectifiers with magnetically switchable output polarity as well as for an efficient electrical readout of the magnetic state of antiferromagnetic materials.

cond-mat.mes-hall↗

arXiv2026

Galvanic intercalation of molecular cations into van der Waals materials

The intercalation of molecular species between the layers of van der Waals (vdW) crystals is a powerful approach to combine the remarkable physical properties of vdW materials with the chemical versatility of organic molecules. However, the full transformative potential of molecular intercalation remains underexplored, largely due to the lack of simple, broadly applicable methods that preserve high crystalline quality down to the few-layer limit. Here, we introduce a simple galvanic approach to intercalate different molecules into various vdW materials under ambient conditions, leveraging the low reduction potential of selected metals. We employ our method, which is particularly well-suited for the in-situ intercalation of few-layer-thick crystals, to intercalate nine vdW materials, including magnets and superconductors, with molecules ranging from conventional alkylammonium ions to metallorganic and bio-inspired chiral cations. Notably, intercalation leads to an unprecedented transition from antiferromagnetic to ferrimagnetic ordering in α-RuCl3 and to a molecule-dependent enhancement of the superconducting transition in 2H-TaS2. These results establish our approach as a versatile technique for engineering atomically thin quantum materials and heterostructures, unlocking the transformative effects of molecular intercalation.

cond-mat.mtrl-sci↗

arXiv2026

Ferromagnetism above 200 K in organic-ion intercalated CrSBr

CrSBr is a van der Waals magnetic semiconductor exhibiting antiferromagnetic order below 140 K. It has emerged as a promising platform for engineering 2D magnetism because its intertwined electronic, optical, and magnetic properties can be profoundly modified via external stimuli such as electrical gating or magnetic fields. However, other strategies for tuning magnetism in layered materials, such as molecular intercalation, remain largely unexplored for CrSBr. Here, we demonstrate that the intercalation of tetramethylammonium (TMA) and tetrapropylammonium (TPA) ions into CrSBr induces a transition from antiferromagnetic to ferromagnetic order, while significantly enhancing the magnetic transition temperature to 190 K (TMA) and 230 K (TPA). The resulting intercalates are air-stable and exhibit large, hysteretic magnetoresistance exceeding 60% at 50 K in the TPA case. Besides, intercalation introduces symmetry-breaking structural changes in each CrSBr plane, revealed by Raman microscopy and corroborated by density functional theory (DFT) calculations. These findings highlight molecular intercalation as a powerful and versatile route to tailor the magnetic properties of CrSBr and unlock its potential to fabricate robust, high-temperature 2D magnetic devices.

cond-mat.mtrl-sci↗

arXiv2025

Isofrequency spin-wave imaging using color center magnetometry for magnon spintronics

Magnon spintronics aims to harness spin waves in magnetic films for information technologies. Color center magnetometry is a promising tool for imaging spin waves, using electronic spins associated with atomic defects in solid-state materials as sensors. However, two main limitations persist: the magnetic fields required for spin-wave control detune the sensor-spin detection frequency, and this frequency is further restricted by the color center nature. Here, we overcome these limitations by decoupling the sensor spins from the spin-wave control fields -selecting color centers with intrinsic anisotropy axes orthogonal to the film magnetization- and by using color centers in diamond and hexagonal boron nitride to operate at complementary frequencies. We demonstrate isofrequency imaging of field-controlled spin waves in a magnetic half-plane and show how intrinsic magnetic anisotropies trigger bistable spin textures that govern spin-wave transport at device edges. Our results establish color center magnetometry as a versatile tool for advancing spin-wave technologies.

cond-mat.mes-hall↗

arXiv2025

Gapless superconductivity from extremely dilute magnetic disorder in 2H-NbSe2-xSx

Most superconducting materials exhibit a vanishing density of states at the Fermi level and Anderson's theorem posits that the superconducting gap is robust against nonmagnetic disorder. Although dilute magnetic impurities lead to localized in-gap states, these states typically have no bearing on the material's bulk superconducting properties. However, numerous experiments reveal a finite density of states at the Fermi level in systems with an apparently negligible number of magnetic impurities. Here, using scanning tunneling microscopy and self-consistent Bogoliubov-de Gennes calculations, we find that gapless superconductivity emerges in 2H-NbSe2-xSx at remarkably low magnetic impurity concentrations. Furthermore, our density functional theory calculations and in-gap quasiparticle interference measurements demonstrate that the Se-S substitution significantly modifies the band structure. This modification favours nesting and dictates the in-gap scattering for x>0, in stark contrast to the dominant charge density wave interactions in pure 2H-NbSe2. Our findings reveal an unusual superconducting response to disorder and highlight the importance of incorporating material-specific band structures in the understanding of a superconductor's response to even very low concentrations of magnetic impurities.

cond-mat.supr-con↗

arXiv2025

Tunable magnons in a dual-gated 2D antiferromagnet

The layered antiferromagnet CrSBr features magnons coupled to other quasiparticles, including excitons and polaritons, enabling their easy optical accessibility. In this work, we investigate the tunability of magnons in few-layered devices in response to changes in carrier density and the application of a perpendicular electric field. We demonstrate an on-chip tunability of the in- and out-of-phase magnon frequencies by up to 2 GHz. While the frequencies of both modes increase with the electron density, we observe an asymmetric response with respect to the electric field in a dual-gated trilayer device. To understand the mechanism of this disparity, we develop a layer-resolved macrospin model describing the magnetic dynamics in thin, non-uniformly doped devices. Through this model we establish the doping- and electric-field-dependence of the exchange interaction, magnetic anisotropy, and magnetic moment of individual layers. Our results advance the applications of gate-tunable magnonic devices based on 2D materials.

cond-mat.mes-hall↗

arXiv2025

Nonvolatile Electric Control of Antiferromagnet CrSBr

van der Waals magnets are emerging as a promising material platform for electric field control of magnetism, offering a pathway towards the elimination of external magnetic fields from spintronic devices. A further step is the integration of such magnets with electrical gating components which would enable nonvolatile control of magnetic states. However, this approach remains unexplored for antiferromagnets, despite their growing significance in spintronics. Here, we demonstrate nonvolatile electric field control of magnetoelectric characteristics in van der Waals antiferromagnet CrSBr. We integrate a CrSBr channel in a flash-memory architecture featuring charge trapping graphene multilayers. The electrical gate operation triggers a nonvolatile 200 % change in the antiferromagnetic state of CrSBr resistance by manipulating electron accumulation/depletion. Moreover, the nonvolatile gate modulates the metamagnetic transition field of CrSBr and the magnitude of magnetoresistance. Our findings highlight the potential of manipulating magnetic properties of antiferromagnetic semiconductors in a nonvolatile way.

cond-mat.mes-hall↗

arXiv2025

Fundamentals and applications of Van der Waals magnets in magnon spintronics

Spintronics is concerned with replacing charge current with current of spin, the electron's intrinsic angular momentum. In magnetic insulators, spin currents are carried by magnons, the quanta of spin-wave excitations on top of the magnetically ordered state. Magnon spin currents are especially promising for information technology due to their low intrinsic damping, non-reciprocal transport, micrometer wavelengths at microwave frequencies, and strong interactions that enable signal transduction. In this perspective, we give our view on the progress and challenges towards realizing magnon spintronics based on atomically thin Van der Waals magnets, a recently discovered class of magnetic materials of which the tunability and versatility has attracted a great deal of ongoing research.

cond-mat.mes-hall↗

arXiv2025

Programmable Magnetic Hysteresis in Orthogonally-Twisted Two-Dimensional CrSBr Magnets via Stacking Engineering

Twisting two-dimensional van der Waals magnets allows the formation and control of different spin-textures, as skyrmions or magnetic domains. Beyond the rotation angle, different spin reversal processes can be engineered by increasing the number of magnetic layers forming the twisted van der Waals heterostructure. Here, we consider pristine monolayers and bilayers of the A-type antiferromagnet CrSBr as building blocks. By rotating 90 degrees these units, we fabricate symmetric (monolayer/monolayer and bilayer/bilayer) and asymmetric (monolayer/bilayer) heterostructures. The magneto-transport properties reveal the appearance of magnetic hysteresis, which is highly dependent upon the magnitude and direction of the applied magnetic field and is determined not only by the twist-angle but also by the number of layers forming the stack. This high tunability allows switching between volatile and non-volatile magnetic memory at zero-field and controlling the appearance of abrupt magnetic reversal processes at either negative or positive field values on demand. The phenomenology is rationalized based on the different spin-switching processes occurring in the layers, as supported by micromagnetic simulations. Our results highlight the combination between twist-angle and number of layers as key elements for engineering spin-switching reversals in twisted magnets, of interest towards the miniaturization of spintronic devices and realizing novel spin textures.

cond-mat.mes-hall↗

arXiv2024

Roadmap on Quantum Magnetic Materials

Fundamental research on two-dimensional (2D) magnetic systems based on van der Waals materials has been gaining traction rapidly since their recent discovery. With the increase of recent knowledge, it has become clear that such materials have also a strong potential for applications in devices that combine magnetism with electronics, optics, and nanomechanics. Nonetheless, many challenges still lay ahead. Several fundamental aspects of 2D magnetic materials are still unknown or poorly understood, such as their often-complicated electronic structure, optical properties, and magnetization dynamics, and their magnon spectrum. To elucidate their properties and facilitate integration in devices, advanced characterization techniques and theoretical frameworks need to be developed or adapted. Moreover, developing synthesis methods which increase critical temperatures and achieve large-scale, high-quality homogeneous thin films is crucial before these materials can be used for real-world applications. Therefore, the field of 2D magnetic materials provides many challenges and opportunities for the discovery and exploration of new phenomena, as well as the development of new applications. This Roadmap presents the background, challenges, and potential research directions for various relevant topics in the field on the fundamentals, synthesis, characterization, and applications. We hope that this work can provide a strong starting point for young researchers in the field and provide a general overview of the key challenges for more experienced researchers.

cond-mat.mtrl-sci↗

arXiv2024

Quantum Spin Hall Effect in Magnetic Graphene

A promising approach to attain long-distance coherent spin propagation is accessing topological spin-polarized edge states in graphene. Achieving this without external magnetic fields necessitates engineering graphene band structure, obtainable through proximity effects in van der Waals heterostructures. In particular, proximity-induced staggered potentials and spin-orbit coupling are expected to form a topological bulk gap in graphene with gapless helical edge states that are robust against disorder. In this work, we detect the spin-polarized helical edge transport in graphene at zero external magnetic field, allowed by the proximity of an interlayer antiferromagnet, CrPS$_4$. We show the coexistence of the quantum spin Hall (QSH) states and magnetism in graphene, where the induced spin-orbit and exchange couplings also give rise to a large anomalous Hall (AH) effect. The detection of the QSH states at zero external magnetic field, together with the AH signal that persists up to room temperature, opens the route for practical applications of magnetic graphene in quantum spintronic circuitries.

cond-mat.mes-hall↗

arXiv2024

High harmonic spectroscopy reveals anisotropy of the Mott to Charge-Density-Wave phase transition in TiSe$_2$

This work explores the use of polarization-resolved high harmonic generation (HHG) spectroscopy to investigate the quantum phases and transitions in the correlated charge density wave (CDW) phase of TiSe$_2$. Unlike previous studies focusing on crystallographic changes, the research examines the reordering that occurs within the CDW phase as the material is cooled from room temperature to 14 K. By linking ultrafast field-driven dynamics to the material's potential landscape, the study demonstrates how HHG is sensitive to quantum phase transitions. The findings reveal an anisotropic component below the CDW transition temperature, providing new insights into the nature of this phase. The investigation highlights the interplay between linear and nonlinear optical responses and their departure from simple perturbative dynamics, offering a fresh perspective on correlated quantum phases in condensed matter systems.

cond-mat.str-el↗

arXiv2024

Probing Short-Range Correlations in the van der Waals Magnet CrSBr by Small-Angle Neutron Scattering

The layered metamagnet CrSBr offers a rich interplay between magnetic, optical and electrical properties that can be extended down to the two-dimensional (2D) limit. Despite the extensive research regarding the long-range magnetic order in magnetic van der Waals materials, short-range correlations have been loosely investigated. By using Small-Angle Neutron Scattering (SANS) we show the formation of short-range magnetic regions in CrSBr with correlation lengths that increase upon cooling up to ca. 3 nm at the antiferromagnetic ordering temperature (TN ~ 140 K). Interestingly, these ferromagnetic correlations start developing below 200 K, i.e., well above TN. Below TN, these correlations rapidly decrease and are negligible at low-temperatures. The experimental results are well-reproduced by an effective spin Hamiltonian, which pinpoints that the short-range correlations in CrSBr are intrinsic to the monolayer limit, and discard the appearance of any frustrated phase in CrSBr at low-temperatures within our experimental window between 2 and 200 nm. Overall, our results are compatible with a spin freezing scenario of the magnetic fluctuations in CrSBr and highlight SANS as a powerful technique for characterizing the rich physical phenomenology beyond the long-range order paradigm offered by van der Waals magnets.

cond-mat.str-el↗

arXiv2023

Multistep magnetization switching in orthogonally twisted ferromagnetic monolayers

The advent of twist-engineering in two-dimensional (2D) crystals enables the design of van der Waals (vdW) heterostructures exhibiting emergent properties. In the case of magnets, this approach can afford artificial antiferromagnets with tailored spin arrangements. Here, we fabricate an orthogonally-twisted bilayer by twisting 90 degrees two CrSBr ferromagnetic monolayers with an easy-axis in-plane anisotropy. The magneto-transport properties reveal multistep magnetization switching with a magnetic hysteresis opening, that is absent in the pristine case. By tuning the magnetic field, we modulate the remanent state and coercivity and select between hysteretic and non-hysteretic magneto-resistance scenarios. This complexity pinpoints spin anisotropy as a key aspect in twisted magnetic superlattices. Our results highlight the control over the magnetic properties in vdW heterostructures, leading to a variety of field-induced phenomena and opening a fruitful playground for creating desired magnetic symmetries and manipulating non-collinear magnetic configurations.

cond-mat.mes-hall↗