arXiv subjects

Jose Martinez-Castro

Publications and source records attributed to Jose Martinez-Castro.

14 recordsLinked to original sources

arXiv2026

Tailoring spontaneous symmetry breaking in engineered van der Waals superlattices

Superlattice engineering in van der Waals heterostructures (e.\,g.\ by moiré engineering) provides a powerful platform for designing electronic bands and realising correlated and topological quantum phenomena. Here, we pioneer a scheme to tailor superpotentials based on intrinsic substrate electronic orders. We show that this establishes a robust, self-aligned, and highly versatile route to band-structure control as we demonstrate in graphene by engineering two distinct, nearly commensurate superlattices using the charge density waves of 1T-NbSe$_2$. In these superlattices the graphene's Dirac cones are folded either to the $Γ$-point or to the K-points of the mini-Brillouin zone. Using scanning tunnelling microscopy, we observe that the $Γ$-folded system preserves C$_3$ symmetry, while the K-folded system exhibits spontaneous symmetry breaking. Combining density functional theory with an interlayer interaction model, we reveal that this difference is not electronically driven but originates from a structural instability. Our work establishes superlattice engineering for designer quantum states and unveils a structural mechanism for controlled emergent symmetry breaking.

cond-mat.mes-hall↗

arXiv2025

Giant orbital Zeeman effects in a magnetic topological van der Waals interphase

Van der Waals (vdW) heterostructures allow the engineering of electronic and magnetic properties by the stacking different two-dimensional vdW materials. For example, orbital hybridisation and charge transfer at a vdW interface may result in electric fields across the interface that give rise to Rashba spin-orbit coupling. In magnetic vdW heterostructures, this in turn can drive the Dzyaloshinskii-Moriya interaction which leads to a canting of local magnetic moments at the vdW interface and may thus stabilise novel 2D magnetic phases. While such emergent magnetic "interphases" offer a promising platform for spin-based electronics, direct spectroscopic evidence for them is still lacking. Here, we report Zeeman effects with Landé $g$-factors up to $\approx230$ at the interface of graphene and the vdW ferromagnet Fe$_3$GeTe$_2$. They arise from a magnetic interphase in which local-moment canting and itinerant orbital moments generated by the non-trivial band topology of Fe$_3$GeTe$_2$ conspire to cause a giant asymmetric level splitting when a magnetic field is applied. Exploiting the inelastic phonon gap of graphene, we can directly access the buried vdW interface to the Fe$_3$GeTe$_2$ by scanning tunnelling spectroscopy. Systematically analyzing the Faraday-like screening of the tip electric field by the graphene, we demonstrate the tunability of the constitutional interface dipole, as well as the Zeeman effect, by tip gating. Our findings are supported by density functional theory and electrostatic modelling.

cond-mat.mes-hall↗

arXiv2025

Bond-resolved STM with density-based methods

Bond-resolved STM (BRSTM) is a recent technique that combines the advantages of scanning tunneling microscopy (STM) with the outstanding intramolecular resolution provided by non-contact atomic force microscopy (ncAFM) using a CO-functionalized tips, offering unique insights into molecular interactions at surfaces. In this work, we present a novel and easily implementable approach for simulating BRSTM images, which we have applied to reproduce new experimental BRSTM data of Perylene-3,4,9,10-tetracarboxylic dianhydride (PTCDA) on Ag(111), obtained with unprecedented control of tip-sample separation ($\sim$10~pm). Our method integrates the Full-Density-Based Model (FDBM) developed for High-Resolution Atomic Force Microscopy (HRAFM) with Chen's derivative approximation for tunneling channels, effectively capturing the contributions of both $σ$ and $π$ channels, while accounting for the CO-tip deflection induced by probe-sample interactions. This approach accurately reproduces the experimental results for both PTCDA/Ag(111) and 1,5,9-trioxo-13-azatriangulene (TOAT)/Cu(111) systems, including intricate tip-sample distance-dependent features. Furthermore, we also demonstrate the important role of substrate-induced effects, which can modify molecular orbital occupation and the relaxation of the CO probe, resulting in distinct BRSTM image characteristics.

cond-mat.mtrl-sci↗

arXiv2025

Multi-Orbital Charge Transfer into Nonplanar Cycloarenes Revealed with CO-Functionalized Tips

On-surface synthesis has allowed for the tuneable preparation of numerous molecular systems with variable properties. Recently, we demonstrated the highly selective synthesis of kekulene (>99%) on Cu(111) and isokekulene (92%) on Cu(110) from the same molecular precursor (Ruan et al., Angew. Chem. Int. Ed. 2025, e202509932). Scanning tunneling microscopy with CO-functionalized tips can identify the single molecules on the basis of their geometric structure at a low coverage on Cu(110), but it also detects complex features due to electronic contributions close to the Fermi energy. Here, we investigate the origin of these features by simulating STM images based on a weighted sum of multiple molecular orbitals, for which we employ weights based on the calculated molecular-orbital projected density of states. This allows for an experimental confirmation of charge transfer from the surface into multiple formerly unoccupied molecular orbitals for single molecules of kekulene as well as isokekulene in its two nonplanar adsorption configurations. In comparison, the area-integrating photoemission orbital tomography technique confirms the charge transfer as well as the high selectivity for the formation of a full monolayer of mainly isokekulene on Cu(110). Our STM-based approach is applicable to a wide range of adsorbed molecular systems and specifically also suited for strongly interacting surfaces, nonplanar molecules, and such molecules which can only be prepared at extremely low yields.

physics.chem-ph↗

arXiv2025

Systematic Modulation of Charge and Spin in Graphene Nanoribbons on MgO

Graphene nanostructures can be engineered with atomic precision to display customized electronic states with application in spintronics or quantum technologies. In order to take advantage of their full potential, their charge and spin state must be precisely controlled. Graphene systems exchange charge to reach thermodynamic equilibrium with their environment, requiring external gating potentials to tune their ground state. Alternative strategies like intrinsic doping or substrate modifications provided small variations of their equilibrium charge and poor control over their spin. Here, we show systematic manipulation of the electron occupation in graphene nanoribbons (GNRs) laying on MgO layers grown on Ag(001). Owing to the extraordinary decoupling properties of MgO, and the electropositive character of the substrate, GNRs are found to host an integer number of electron charges that depend on their length and shape. This results in the alternation between a non-magnetic closed-shell state and an open-shell paramagnetic system for even and odd electron occupations respectively. For the odd case, we found the spectral fingerprint of a narrow Coulomb correlation gap, which is the smoking gun of its spin 1/2 paramagnetic state. Comparisons of scanning tunnelling microscopy (STM) data with mean-field Hubbard (MFH) simulations confirm the practical discretization of the GNR electronic states and point to charge excess of up to 19 electrons in a single ribbon. We anticipate that GNRs supported by MgO ultra-thin insulating films can open the door to customized devices for quantum sensing and quantum processing applications..

cond-mat.mes-hall↗

arXiv2024

Scattering makes a difference in circular dichroic angle-resolved photoemission

Recent years have witnessed a steady progress towards blending 2D quantum materials into technology, with future applications often rooted in the electronic structure. Since crossings and inversions of electronic bands with different orbital characters determine intrinsic quantum transport properties, knowledge of the orbital character is essential. Here, we benchmark angle-resolved photoelectron emission spectroscopy (ARPES) as a tool to experimentally derive orbital characters. For this purpose we study the valence electronic structure of two technologically relevant quantum materials, graphene and WSe$_2$, and focus on circular dichroism that is believed to provide sensitivity to the orbital angular momentum. We analyze the contributions related to angular atomic photoionization profiles, interatomic interference, and multiple scattering. Regimes in which initial-state properties could be disentangled from the ARPES maps are critically discussed and the potential of using circular-dichroic ARPES as a tool to investigate the spin polarization of initial bands is explored. For the purpose of generalization, results from two additional materials, GdMn$_6$Sn$_6$ and PtTe$_2$ are presented in addition. This research demonstrates rich complexity of the underlying physics of circular-dichroic ARPES, providing new insights that will shape the interpretation of both past and future circular-dichroic ARPES studies.

cond-mat.mtrl-sci↗

arXiv2023

Induced Superconductivity in Hybrid Au/YBa2Cu3O7-x Electrodes on Vicinal Substrates

Superconducting electrodes are an integral part of hybrid Josephson junctions used in many applications including quantum technologies. We report on the fabrication and characterization of superconducting hybrid Au/YBa2Cu3O7-x (YBCO) electrodes on vicinal substrates. In these structures, superconducting CuO2-planes face the gold film, resulting in a higher value and smaller variation of the induced energy gap compared to the conventional Au/YBCO electrodes based on films with the c-axis normal to the substrate surface. Using scanning tunneling microscopy, we observe an energy gap of about 10-17 meV at the surface of the 15- nm-thick gold layer deposited in situ atop the YBCO film. To study the origin of this gap, we fabricate nanoconstrictions from the Au/YBCO heterostructure and measure their electrical transport characteristics. The conductance of the nanoconstrictions shows a series of dips due to multiple Andreev reflections in YBCO and gold providing clear evidence of the superconducting nature of the gap in gold. We consider the Au/YBCO electrodes to be a versatile platform for hybrid Josephson devices with a high operating temperature.

cond-mat.supr-con↗

arXiv2023

Suspended dry pick-up and flip-over assembly for van der Waals heterostructures with ultra-clean surfaces

Van der Waals heterostructures are an excellent platform for studying intriguing interface phenomena, such as moiré and proximity effects. Surface science techniques like scanning tunneling microscopy (STM) have proven a powerful tool to study such heterostructures but have so far been hampered because of their high sensitivity to surface contamination. Here, we report a dry polymer-based assembly technique to fabricate van der Waals heterostructures with atomically clean surfaces. The key features of our suspended dry pick-up and flip-over technique are 1) the heterostructure surface never comes into contact with polymers, 2) it is entirely solvent-free, 3) it is entirely performed in a glovebox, and 4) it only requires temperatures below 130$^{\circ}$. By performing ambient atomic force microscopy and atomically-resolved scanning tunneling microscopy on example heterostructures, we demonstrate that we can fabricate air-sensitive heterostructures with ultra-clean interfaces and surfaces. Due to the lack of polymer melting, the technique is further compatible with heterostructure assembly under ultra-high vacuum conditions, which promises ultimate heterostructure quality.

cond-mat.mes-hall↗

arXiv2023

One-dimensional topological superconductivity in a van der Waals heterostructure

One-dimensional (1D) topological superconductivity is a state of matter that is not found in nature. However, it can be realised, for example, by inducing superconductivity into the quantum spin Hall edge state of a two-dimensional topological insulator. Because topological superconductors are proposed to host Majorana zero modes, they have been suggested as a platform for topological quantum computing. Yet, conclusive proof of 1D topological superconductivity has remained elusive. Here, we employ low-temperature scanning tunnelling microscopy to show 1D topological superconductivity in a van der Waals heterostructure by directly probing its superconducting properties, instead of relying on the observation of Majorana zero modes at its boundary. We realise this by placing the two-dimensional topological insulator monolayer WTe$_2$ on the superconductor NbSe$_2$. We find that the superconducting topological edge state is robust against magnetic fields, a hallmark of its triplet pairing. Its topological protection is underpinned by a lateral self-proximity effect, which is resilient against disorder in the monolayer edge. By creating this exotic state in a van der Waals heterostructure, we provide an adaptable platform for the future realization of Majorana bound states. Finally, our results more generally demonstrate the power of Abrikosov vortices as effective experimental probes for superconductivity in nanostructures.

cond-mat.mes-hall↗

arXiv2023

Bistable electric field control of single-atom magnetocrystalline anisotropy

We reversibly switch the polar environment of an individual magnetic atom with an electric field to control the energy barrier for reversal of magnetization. By applying an electric field in the gap between the tip and sample of a scanning tunneling microscope, we induce bistable changes in the polarization of the region surrounding a chlorine vacancy in a monolayer of sodium chloride on copper terminated by a monolayer of copper nitride. The displacement of the sodium chloride ions alters the local electric polarization and modifies the magnetocrystalline anisotropy experienced by a single cobalt atom. When a cobalt atom is near a chlorine vacancy, spin-sensitive inelastic electron tunneling spectroscopy measurements can reveal the change in anisotropy. The demonstration of atomic-scale control of magnetic properties with electric fields opens new possibilities for probing the origins of magnetoelectric coupling and will stimulate the development of model artificial mutliferroic systems.

cond-mat.mes-hall↗

arXiv2022

Determining spin-orbit coupling in graphene by quasiparticle interference imaging

Inducing and controlling spin-orbit coupling (SOC) in graphene is key to create topological states of matter, and for the realization of spintronic devices. Placing graphene onto a transition metal dichalcogenide is currently the most successful strategy to achieve this goal, but there is no consensus as to the nature and the magnitude of the induced SOC. Here, we show that the presence of backscattering in graphene-on-WSe$_2$ heterostructures can be used to probe SOC and to determine its strength quantitatively, by imaging quasiparticle interference with a scanning tunneling microscope. A detailed theoretical analysis of the Fourier transform of quasiparticle interference images reveals that the induced SOC consists of a valley-Zeeman ($λ_{\text{vZ}}\approx 2$ meV) and a Rashba ($λ_\text{R}\approx 15$ meV) term, one order of magnitude larger than what theory predicts, but in excellent agreement with earlier transport experiments. The validity of our analysis is confirmed by measurements on a 30 degree twist angle heterostructure that exhibits no backscattering, as expected from symmetry considerations. Our results demonstrate a viable strategy to determine SOC quantitatively by imaging quasiparticle interference.

cond-mat.mes-hall↗

arXiv2022

Tunable biaxial strain device for low dimensional materials

Strain is attracting much interest as a mean to tune the properties of thin exfoliated two-dimensional materials and their heterostructures. Numerous devices to apply tunable uniaxial strain are proposed in the literature, but only few for biaxial strain where there is often a trade-off between maximum strain and uniformity, reversibility and device size. We present a compact device that allows the controlled application of uniform in-plane biaxial strain, with maximum deformation and uniformity comparable to those found in much larger devices. Its performance and strain uniformity over the sample area are modeled using finite element analysis and demonstrated by measuring the response of exfoliated 2H-MoS$_2$ to strain by Raman spectroscopy.

cond-mat.mtrl-sci↗

arXiv2022

Disentangling the Complex Electronic Structure of an Adsorbed Nanographene: Cycloarene C108

We combine low-temperature scanning tunneling spectroscopy, CO functionalized tips and algorithmic data analysis to investigate the electronic structure of the molecular cycloarene C108 (graphene nanoring) adsorbed on a Au(111) surface. We demonstrate that CO functionalized tips enhance the visibility of molecular resonances, both in differential conductance spectra and in real-space topographic images without introducing spurious artifacts. Comparing our experimental data with ab-initio density functional theory reveals a remarkably precise agreement of the molecular orbitals and enables us to disentangle close-lying molecular states only separated by 50 meV at an energy of 2 eV below the Fermi level. We propose this combination of techniques as a promising new route for a precise characterization of complex molecules and other physical entities which have electronic resonances in the tip-sample junction.

cond-mat.mes-hall↗

arXiv2019

Scanning Tunneling Microscopy of an Air Sensitive Dichalcogenide Through an Encapsulating Layer

Many atomically thin exfoliated 2D materials degrade when exposed to ambient conditions. They can be protected and investigated by means of transport and optical measurements if they are encapsulated between chemically inert single layers in the controlled atmosphere of a glove box. Here, we demonstrate that the same encapsulation procedure is also compatible with scanning tunneling microscopy (STM) and spectroscopy (STS). To this end, we report a systematic STM/STS investigation of a model system consisting of an exfoliated 2H-NbSe2 crystal capped with a protective 2H-MoS2 monolayer. We observe different electronic coupling between MoS2 and NbSe2, from a strong coupling when their lattices are aligned within a few degrees to 2 essentially no coupling for 30° misaligned layers. We show that STM always probes intrinsic NbSe2 properties such as the superconducting gap and charge density wave at low temperature when setting the tunneling bias inside the MoS2 band gap, irrespective of the relative angle between the NbSe2 and MoS2 lattices. This study demonstrates that encapsulation is fully compatible with STM/STS investigations of 2D materials.

cond-mat.mes-hall↗