arXiv subjects

Nicolae Atodiresei

Publications and source records attributed to Nicolae Atodiresei.

18 recordsLinked to original sources

arXiv2026

Emergence of a non-bulk hexagonal Fe$_2$S$_2$ single layer via phase transformation

Two-dimensional materials can stabilize crystal structures that are absent from their bulk counterparts, offering opportunities for materials design. Here, we report the synthesis of a previously unknown hexagonal Fe$_2$S$_2$ single layer with $\beta$-CuI structure, a buckled layer of two vertically stacked FeS honeycomb lattices, realized by thermally induced transformation of single layer mackinawite grown on graphene/Ir(111). In situ scanning tunneling microscopy and low-energy electron diffraction reveal a transition from a tetragonal to a hexagonal lattice accompanied by distinct morphological and electronic signatures. The hexagonal Fe$_2$S$_2$ forms reproducibly upon annealing and represents a new structural motif within the Fe-S material family. First-principles calculations identify the $\beta$-CuI structure as most consistent with experiment. The calculations suggest that on-site Coulomb interactions and magnetic order are relevant to understanding the stability of the new 2D Fe-S compound. The preferred nucleation of single-layer mackinawite, despite being energetically disfavored, is speculated to result from its low edge energy, analogous to the 3D case. Our results establish Fe$_2$S$_2$ as a platform for exploring structural polymorphism in two dimensions and demonstrate that reduced dimensionality can stabilize crystal structures not accessible in bulk materials.

cond-mat.mtrl-sci↗

arXiv2025

MnBr$_2$ on the graphene on Ir(110) substrate: growth, structure, and super-moirè

Single-layer MnBr$_2$ is grown on graphene (Gr) supported by Ir(110) and investigated using low-energy electron diffraction, scanning tunneling microscopy, and spectroscopy. The structure and epitaxial relationship with the substrate are systematically characterized. The structure and epitaxial relationship with the substrate are systematically characterized. The growth morphology strongly depends on the growth temperature, evolving from fractal to dendritic and eventually to compact dendritic skeletal islands, reflecting changes in the underlying surface diffusion processes. The pronounced variation in the apparent height with tunneling conditions for the magnetic insulator is explained based on the measured electronic density of states. MnBr$_2$ on Gr/Ir(110) constitutes a three-lattice system, giving rise to a super-moiré pattern -- a moiré of moirés. The super-moiré of MnBr$_2$/Gr/Ir(110) is unique, as it involves a virtual moiré of MnBr$_2$ with the Ir(110) surface lattice -- two lattices not in contact with each other. Using a careful Fourier analysis, the known properties of Gr/Ir(110), and the results of ab initio calculations, the origin of the virtual moiré is uncovered and related to the inhomogeneous binding of Gr to Ir(110). Comparative experiments with MnBr$_2$ on Gr/Ir(111) show similar growth and structure, but highlight the unique properties of the MnBr$_2$/Gr/Ir(110) super-moiré.

cond-mat.mtrl-sci↗

arXiv2025

Rare-earth atoms on Nb(110) as a platform to engineer topological superconductivity

Helical spin textures in one-dimensional magnetic chains on superconductors can enable topological superconductivity and host Majorana zero modes, independent of the presence of intrinsic spin-orbit coupling. Here, we show that gadolinium (Gd) adatoms, possessing large 4f magnetic moments when placed on a Nb(110) surface, establish indirect exchange interactions mediated by valence electrons, manifesting as Yu-Shiba-Rusinov states. By combining scanning tunneling microscopy and spectroscopy with density functional theory, we analyze the emergence of the Yu-Shiba-Rusinov states in single Gd atoms and Gd dimers and uncover the underlying magnetic interaction mechanisms, on the basis of which we predict by means of spin-dynamics simulations the formation of stable chiral Néel-type spin-spiral configurations in Gd chains. These findings highlight rare-earth magnets as a promising platform for precisely tuning spin-spiral ground states, an essential prerequisite for the realization of topological superconductivity.

cond-mat.supr-con↗

arXiv2024

Engineering two-dimensional materials from single-layer NbS$_2$

Starting from a single layer of NbS$_2$ grown on graphene by molecular beam epitaxy, the single unit cell thick 2D materials Nb$_{5/3}$S$_3$-2D and Nb$_2$S$_3$-2D are created using two different pathways. Either annealing under sulfur-deficient conditions at progressively higher temperatures or deposition of increasing amounts of Nb at elevated temperature result in phase-pure Nb$_{5/3}$S$_3$-2D followed by Nb$_2$S$_3$-2D. The materials are characterized by scanning tunneling microscopy, scanning tunneling spectroscopy and X-ray photoemission spectroscopy. The experimental assessment combined with systematic density functional theory calculations reveals their structure. The 2D materials are covalently bound without any van der Waals gap. Their stacking sequence and structure are at variance with expectations based on corresponding bulk materials highlighting the importance of surface and interface effects in structure formation.

cond-mat.mtrl-sci↗

arXiv2024

Molecular order induced charge transfer in a C$_{60}$-topological insulator moiré heterostructure

We synthesize and spectroscopically investigate monolayer C$_{60}$ on the topological insulator (TI) Bi$_4$Te$_3$. This C$_{60}$/Bi$_4$Te$_3$ heterostructure is characterized by excellent translational order in a novel (4 x 4) C$_{60}$ superstructure on a (9 x 9) unit of Bi$_4$Te$_3$. We measure the full two-dimensional energy band structure of C$_{60}$/Bi$_4$Te$_3$ using angle-resolved photoemission spectroscopy (ARPES). We find that C$_{60}$ accepts electrons from the TI at room temperature but no charge transfer occurs at low temperatures. We unravel this peculiar behaviour by Raman spectroscopy of C$_{60}$/Bi$_4$Te$_3$ and density functional theory (DFT) calculations of the electronegativity of C$_{60}$. Both methods are sensitive to orientational order of C$_{60}$. At low temperatures, Raman spectroscopy shows a dramatic intensity increase of the C$_{60}$ Raman signal, evidencing a transition to a rotationally ordered state. DFT reveals that the orientational order of C$_{60}$ at low temperatures has a higher electron affinity than at high temperatures. These results neatly explain the temperature-dependent charge transfer observed in ARPES. Our conclusions are supported by the appearance of a strong photoluminescence from C$_{60}$/Bi$_4$Te$_3$ at low temperatures.

cond-mat.mtrl-sci↗

arXiv2024

Novel 2D vanadium sulphides: synthesis, atomic structure engineering and charge density waves

Two new ultimately thin vanadium rich 2D materials based on VS2 are created via molecular beam epitaxy and investigated using scanning tunneling microscopy, X-ray photoemission spectroscopy and density-functional theory calculations. The controlled synthesis of stoichiometric single-layer VS2 or either of the two vanadium-rich materials is achieved by varying the sample coverage and the sulphur pressure during annealing. Through annealing of small stoichiometric single-layer VS2 islands without S pressure, S-vacancies spontaneously order in 1D arrays, giving rise to patterned adsorption. Via the comparison of density-functional theory calculations with scanning tunneling microscopy data, the atomic structure of the S-depleted phase, with a stoichiometry of V4S7, is determined. By depositing larger amounts of vanadium and sulphur, which are subsequently annealed in a S-rich atmosphere, self-intercalated ultimately thin V5S8-derived layers are obtained, which host 2x2 V-layers between sheets of VS2. We provide atomic models for the thinnest V5S8-derived structures. Finally, we use scanning tunneling spectroscopy to investigate the charge density wave observed in the 2D V5S8-derived islands.

cond-mat.mtrl-sci↗

arXiv2023

Enantioselective adsorption on magnetic surfaces

From the beginning of molecular theory, the interplay of chirality and magnetism has intrigued scientists. There is still the question if enantiospecific adsorption of chiral molecules occurs on magnetic surfaces. Enantiomer discrimination was conjectured to arise from chirality-induced spin separation within the molecules and exchange interaction with the substrate's magnetization. Here we show that single helical aromatic hydrocarbons undergo enantioselective adsorption on ferromagnetic cobalt surfaces. Spin and chirality sensitive scanning tunneling microscopy reveals that molecules of opposite handedness prefer adsorption onto cobalt islands with opposite out-of-plane magnetization. As mobility ceases in the final chemisorbed state, it is concluded that enantioselection must occur in a physisorbed transient precursor state. State-of-the-art spin-resolved ab initio simulations support this scenario by refuting enantio-dependent chemisorption energies. These findings demonstrate that van der Waals interaction should also include spin-fluctuations which are crucial for molecular magnetochiral processes.

cond-mat.mtrl-sci↗

arXiv2022

Elastic properties of moiré lattices in epitaxial two-dimensional materials

Unlike conventional two-dimensional (2D) semiconductor superlattices, moiré patterns in 2D materials are flexible and their electronic, magnetic, optical, and mechanical properties depend on their topography. Within a continuous+atomistic theory treating 2D materials as crystalline elastic membranes, we abandon the flat-membrane scenario usually assumed for these materials and address out-of-plane deformations. We confront our predictions to experimental analyses on model systems, epitaxial graphene, and MoS$_2$ on metals and reveal that compression/expansion and bending energies stored in the membrane can compete with adhesion energy, leading to a subtle moiré wavelength selection and the formation of wrinkles.

cond-mat.mes-hall↗

arXiv2021

Single-crystal graphene on Ir(110)

A single-crystal sheet of graphene is synthesized on the low-symmetry substrate Ir(110) by thermal decomposition of C$_2$H$_4$ at 1500 K. Using scanning tunneling microscopy, low-energy electron diffraction, angle-resolved photoemission spectroscopy, and ab initio density functional theory the structure and electronic properties of the adsorbed graphene sheet and its moiré with the substrate are uncovered. The adsorbed graphene layer forms a wave pattern of nm wave length with a corresponding modulation of its electronic properties. This wave pattern is demonstrated to enable the templated adsorption of aromatic molecules and the uniaxial growth of organometallic wires. Not limited to this, graphene on Ir(110) is also a versatile substrate for 2D-layer growth and makes it possible to grow epitaxial layers on ureconstructed Ir(110).

cond-mat.mtrl-sci↗

arXiv2019

Tomonaga-Luttinger liquid in a box: electrons confined within MoS$_2$ mirror twin boundaries

Two- or three-dimensional metals are usually well described by weakly interacting, fermionic quasiparticles. This concept breaks down in one dimension due to strong Coulomb interactions. There, low-energy electronic excitations are expected to be bosonic collective modes, which fractionalize into independent spin and charge density waves. Experimental research on one-dimensional metals is still hampered by their difficult realization, their limited accessibility to measurements, and by competing or obscuring effects such as Peierls distortions or zero bias anomalies. Here we overcome these difficulties by constructing a well-isolated, one-dimensional metal of finite length present in MoS$_2$ mirror twin boundaries. Using scanning tunneling spectroscopy we measure the single-particle density of the interacting electron system as a function of energy and position in the 1D box. Comparison to theoretical modeling provides unambiguous evidence that we are observing spin-charge separation in real space.

cond-mat.str-el↗

arXiv2018

One-dimensional Si chains embedded in Pt(111)and protected by a hexagonal boron-nitride monolayer

Using scanning tunneling microscopy, we show that Si deposition on Pt(111) at 300K leads to a network of one-dimensional Si chains. On the bare Pt(111) surface, the chains, embedded into the Pt surface, are orientated along the <112>-direction. They disappear within a few hours in ultrahigh vacuum due to the presence of residual gas. Exposing the chains to different gases deliberately reveals that CO is largely responsible for the disappearance of the chains. The chains can be stabilized by a monolayer of hexagonal boron nitride, which is deposited prior to the Si deposition. The resulting Si chains are rotated by 30° with respect to the chains on the bare Pt(111) surface and survive even an exposure to air for 10 minutes.

cond-mat.mes-hall↗

arXiv2016

Sub-molecular modulation of a 4f driven Kondo resonance by surface-induced asymmetry

Coupling between a magnetic impurity and an external bath can give rise to many-body quantum phenomena, including Kondo and Hund's impurity states in metals, and Yu-Shiba-Rusinov states in superconductors. While advances have been made in probing the magnetic properties of d-shell impurities on surfaces, the confinement of f orbitals makes them difficult to access directly. Here we show that a 4f driven Kondo resonance can be modulated spatially by asymmetric coupling between a metallic surface and a molecule containing a 4f-like moment. Strong hybridisation of dysprosium double-decker phthalocyanine with Cu(001) induces Kondo screening of the central magnetic moment. Misalignment between the symmetry axes of the molecule and the surface induces asymmetry in the molecule's electronic structure, spatially mediating electronic access to the magnetic moment through the Kondo resonance. This work demonstrates the important role that molecular ligands play in mediating electronic and magnetic coupling and in accessing many-body quantum states.

cond-mat.mes-hall↗

arXiv2015

Tuning the van der Waals Interaction of Graphene with Molecules via Doping

We use scanning tunneling microscopy to visualize and thermal desorption spectroscopy to quantitatively measure that the binding of naphthalene molecules to graphene (Gr), a case of pure van der Waals (vdW) interaction, strengthens with $n$- and weakens with $p$-doping of Gr. Density functional theory calculations that include the vdW interaction in a seamless, ab initio way accurately reproduce the observed trend in binding energies. Based on a model calculation, we propose that the vdW interaction is modified by changing the spatial extent of Gr's $π$ orbitals via doping.

cond-mat.mes-hall↗

arXiv2013

Hybridisation at the organic-metal interface: a surface-scientific analogue of Hückel's rule?

We demonstrate that cyclooctatetraene (COT) can be stabilised in different conformations when adsorbed on different noble-metal surfaces due to varying molecule-substrate interaction. While at first glance the behaviour seems to be in accordance with Hückel's rule, a theoretical analysis reveals no significant charge transfer. The driving mechanism for the conformational change is hybridisation at the organic-metal interface and does not necessitate any charge transfer.

cond-mat.mes-hall↗

arXiv2011

Graphene on Ir(111): Physisorption with chemical modulation

The non-local van der Waals density functional (vdW-DF) approach is applied to calculate the binding of graphene to Ir(111). The precise agreement of the calculated mean height h = 3.41 Å of the C atoms with their mean height h = (3.38 \pm 0.04) Å as measured by the X-ray standing wave (XSW) technique provides a benchmark for the applicability of the non-local functional. We find bonding of graphene to Ir(111) to be due to the van der Waals interaction with an antibonding average contribution from chemical interaction. Despite its globally repulsive character, in certain areas of the large graphene moiré unit cell charge accumulation between Ir substrate and grapheneC atoms is observed, signaling a weak covalent bond formation.

cond-mat.mtrl-sci↗

arXiv2010

Real-space electronic-structure calculations with full-potential all-electron precision for transition-metals

We have developed an efficient computational scheme utilizing the real-space finite-difference formalism and the projector augmented-wave (PAW) method to perform precise first-principles electronic-structure simulations based on the density functional theory for systems containing transition metals with a modest computational effort. By combining the advantages of the time-saving double-grid technique and the Fourier filtering procedure for the projectors of pseudopotentials, we can overcome the egg box effect in the computations even for first-row elements and transition metals, which is a problem of the real-space finite-difference formalism. In order to demonstrate the potential power in terms of precision and applicability of the present scheme, we have carried out simulations to examine several bulk properties and structural energy differences between different bulk phases of transition metals, and have obtained excellent agreement with the results of other precise first-principles methods such as a plane wave based PAW method and an all-electron full-potential linearized augmented plane wave (FLAPW) method.

cond-mat.mtrl-sci↗

arXiv2010

Controlling the Local Spin-Polarization at the Organic-Ferromagnetic Interface

By means of ab initio calculations and spin-polarized scanning tunneling microscopy experiments we show how to manipulate the local spin-polarization of a ferromagnetic surface by creating a complex energy dependent magnetic structure. We demonstrate this novel effect by adsorbing organic molecules containing pi(pz)-electrons onto a ferromagnetic surface, in which the hybridization of the out-of-plane pz atomic type orbitals with the d-states of the metal leads to the inversion of the spin-polarization at the organic site due to a pz - d Zener exchange type mechanism. As a key result, we demonstrate that it is possible to selectively inject spin-up and spin-down electrons from the same ferromagnetic surface, an effect which can be exploited in future spintronic devices.

cond-mat.mtrl-sci↗

arXiv2010

Spin- and energy-dependent tunneling through a single molecule with intramolecular spatial resolution

We investigate the spin- and energy dependent tunneling through a single organic molecule (CoPc) adsorbed on a ferromagnetic Fe thin film, spatially resolved by low-temperature spin-polarized scanning tunneling microscopy. Interestingly, the metal ion as well as the organic ligand show a significant spin-dependence of tunneling current flow. State-of-the-art ab initio calculations including also van-der-Waals interactions reveal a strong hybridization of molecular orbitals and surface 3d states. The molecule is anionic due to a transfer of one electron, resulting in a non-magnetic (S= 0) state. Nevertheless, tunneling through the molecule exhibits a pronounced spin-dependence due to spin-split molecule-surface hybrid states.

cond-mat.mtrl-sci↗