arXiv subjects

Shawulienu Kezilebieke

Publications and source records attributed to Shawulienu Kezilebieke.

At least 19 recordsLinked to original sources

arXiv2026

Multiferroic Quantum Dot in an Artificial van der Waals Heterostructure

Quantum dots (QDs) provide a versatile platform for engineering quantum-confined electronic states with functionalities relevant for optoelectronics, spintronics, and quantum technologies. While substantial progress has been achieved in coupling confined states to spin, valley, topological, or ferroelectric degrees of freedom, the realization of a multiferroic QD in which quantum confinement simultaneously intertwines with magnetism and ferroelectricity remains elusive. Here, we engineer a multiferroic QD in an artificial van der Waals heterostructure grown by molecular beam epitaxy under ultra-high-vacuum conditions. The heterostructure consists of ferroelectric SnTe nanoislands deposited on the layered magnet CrBr$_2$ supported on highly oriented pyrolytic graphite. Combining scanning tunneling microscopy and spectroscopy with ab initio calculations and low-energy tight-binding models, we demonstrate the emergence of spin-polarized discretized electronic states confined within the SnTe islands. Remarkably, the spectroscopic response of the QD strongly depends on the ferroelectric domain configuration of the SnTe nanoislands, demonstrating an interplay between quantum confinement, magnetic exchange, and ferroelectric order at the atomic scale. Our results establish engineered van der Waals heterostructures as a platform for multiferroic quantum confinement and open new routes toward electrically tunable quantum spintronic devices.

cond-mat.mes-hall↗

arXiv2026

Observation of electromagnons in a monolayer multiferroic

Van der Waals multiferroics have emerged as a promising platform to explore novel magnetoelectric phenomena. Recently, it has been shown that monolayer NiI$_2$ hosts robust type-II multiferroicity down to the two-dimensional limit, a giant dynamical magnetoelectric coupling at terahertz frequencies, and an electrically switchable spin polarization. These developments present the possibility of engineering ultrafast, low-energy-consumption, and electrically-tunable spintronic devices based on the collective excitations of the multiferroic order, electromagnons. However, the direct visualization of these bosonic modes in real space and within the monolayer limit remains elusive. Here, we report the atomic-scale observation of electromagnons in monolayer NiI$_2$ using low-temperature scanning tunneling microscopy. By tracking the thermal evolution of the multiferroic phase, we establish the energy scale and resolve coherent in-gap excitations of the symmetry-broken multiferroic state. Comparison with first-principles and spin-model calculations reveals that the low-energy modes originate from electromagnon excitations. Spatially resolved inelastic tunneling spectroscopy maps show a stripe-like modulation of the local spectral function at electromagnon energies, matching theoretical predictions. These results provide direct evidence of the internal structure of electromagnons and establish a methodology to probe these modes at the atomic scale, opening avenues for electrically tunable spintronics.

cond-mat.mtrl-sci↗

arXiv2026

Lattice Reconstruction and Orbital Hybridization Suppress Magnetism in TaCo$_2$Te$_2$

Structural reconstruction in low-dimensional quantum materials can strongly modify electronic symmetry and magnetic stability through orbital hybridization. Here, we investigate the interplay between lattice reconstruction, electronic structure, and magnetic instability in the layered van der Waals compound TaCo$_2$Te$_2$ using scanning tunneling microscopy and spectroscopy (STM/STS), non-contact atomic force microscopy (nc-AFM), angle-resolved photoemission spectroscopy (ARPES), and density functional theory (DFT). While nc-AFM resolves a distorted hexagonal Te surface lattice, STM/STS reveal a pronounced square-like electronic symmetry that does not directly follow the atomic structure. ARPES further shows a strongly anisotropic Fermi surface and reconstructed low-energy states. Spatially resolved spectroscopy and orbital-projected DFT demonstrate that the bias-dependent STM contrast does not arise from a simple reversal between occupied and unoccupied states, but from the energy-integrated local density of states dominated by electronic states exhibiting opposite spatial contrast at selected energies. DFT calculations further show that reconstruction suppresses the magnetic instability present in the undistorted structure, stabilizing a nonmagnetic ground state through enhanced orbital hybridization. These results establish TaCo$_2$Te$_2$ as a model system in which lattice reconstruction reorganizes electronic symmetry and suppresses magnetism, highlighting structural reconstruction as a route for controlling correlated and magnetic phases in low-dimensional quantum materials.

cond-mat.mtrl-sci↗

arXiv2026

Atomically Reconfigurable Single-Molecule Optoelectronics

Deterministic control of excitonic properties is key to advancing nanoscale optoelectronic and quantum technologies and to understanding diverse physical, optical, chemical, and biological phenomena. At the molecular scale, these properties can be tuned through chemical modification, local-environment influence or charge-state manipulation. Yet, direct control of a molecule's transition dipole moment and its resulting light emission via atomic-scale structural modification has remained elusive. Here, using scanning tunnelling microscopy-induced luminescence, we show that a single structural parameter-the vertical displacement of the central metal atom in a planar phthalocyanine molecule on a decoupling layer-enables active tuning of the transition dipole, allowing either suppression or enhancement of emission. Exploiting this control, we realized a tunable homodimer switchable among three optical states: non-emissive, single-molecule-like emissive, and coupled states exhibiting subradiant and superradiant modes, directly revealing intermolecular dipole-dipole coupling. We further demonstrate a heterodimer in which resonant energy transfer can be turned on or off simply by controlling the acceptor's transition dipole moment. These findings not only establish atomic-scale displacement as a general strategy for optical molecular switching, but also demonstrate the reconfigurable engineering of excitonic interactions within molecular assemblies.

cond-mat.mtrl-sci↗

arXiv2025

Atomic-scale probe of molecular magneto-electric coupling

Van der Waals heterostructures are a core tool in quantum material design. The recent addition of monolayer ferroelectrics expands the possibilities of designer materials. Ferroelectric domains can be manipulated using electric fields, thus opening a route for external control over material properties. In this paper we explore the possibility of engineering magneto-electric coupling in ferroelectric heterostructures by studying the interface of bilayer SnTe with iron phthalocyanine molecules as a model system. The molecules act as sensor spins, allowing us to sample the magneto-electric coupling with nanometer precision through scanning tunneling microscopy. Our measurements uncover a structural, and therefore material-independent and intrinsic, mechanism to couple electric and magnetic degrees of freedom at the nanoscale.

cond-mat.mes-hall↗

arXiv2024

Emergence of Exotic Spin Texture in Supramolecular Metal Complexes on a 2D Superconductor

Designer heterostructures, where the desired physics emerges from the controlled interactions between different components, represent one of the most powerful strategies to realize unconventional electronic states. This approach has been particularly fruitful in combining magnetism and superconductivity to create exotic superconducting states. In this work, we use a heterostructure platform combining supramolecular metal complexes (SMCs) with a quasi-2D van der Waals (vdW) superconductor NbSe$_2$. Our scanning tunneling microscopy (STM) measurements demonstrate the emergence of Yu-Shiba-Rusinov (YSR) bands arising from the interaction between the SMC magnetism and the NbSe$_2$ superconductivity. Using X-ray absorption spectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD) measurements, we show the presence of antiferromagnetic coupling between the SMC units. These result in the emergence of an unconventional $3\times3$ reconstruction in the magnetic ground state that is directly reflected in real space modulation of the YSR bands. The combination of flexible molecular building blocks, frustrated magnetic textures, and superconductivity in heterostructures establishes a fertile starting point to fabricating tunable quantum materials, including unconventional superconductors and quantum spin liquids.

cond-mat.supr-con↗

arXiv2024

Strain-induced two-dimensional topological crystalline insulator

Topological crystalline insulators (TCIs) host topological phases of matter protected by crystal symmetries. Topological surface states in three-dimensional TCIs have been predicted and observed in IV-VI SnTe-class semiconductors. Despite the prediction of a two-dimensional (2D) TCI characterized by two pairs of edge states inside the bulk gap, materials challenges have thus far prevented its experimental realization. Here we report the growth and characterization of bilayer SnTe on the 2$H$-NbSe$_2$ substrate by molecular beam epitaxy and scanning tunneling microscopy. We experimentally observe two anticorrelated, periodically modulated pairs of conducting edge states along the perimeters of the sample with a large band gap exceeding $0.2$ eV. We identify these states with a 2D TCI through first principles calculations. Finally, we probe the coupling of adjacent topological edge states and demonstrate the resulting energy shift driven by a combination of electrostatic interactions and tunneling coupling. Our work opens the door to investigations of tunable topological states in 2D TCIs, of potential impact for spintronics and nanoelectronics applications at room temperature.

cond-mat.mes-hall↗

arXiv2024

Atomically sharp 1D interfaces in 2D lateral heterostructures of VSe$_2$-NbSe$_2$ monolayers

Van der Waals heterostructures have emerged as an ideal platform for creating engineered artificial electronic states. While vertical heterostructures have been extensively studied, realizing high-quality lateral heterostructures with atomically sharp interfaces remains a major experimental challenge. Here, we advance a one-pot two-step molecular beam lateral epitaxy approach and successfully synthesize atomically well-defined 1T-VSe$_2$ -- 1H-NbSe$_2$ lateral heterostructures. We demonstrate the formation of defect-free lateral heterostructures and characterize their electronic structure using scanning tunnelling microscopy and spectroscopy together with density functional theory calculations. We find additional electronic states at the one-dimensional interface as well as signatures of Kondo resonances in a side-coupled geometry. Our experiments explore the full potential of lateral heterostructures for realizing exotic electronic states in low-dimensional systems for further studies of artificial designer quantum materials.

cond-mat.mes-hall↗

arXiv2024

Tuning spinaron and Kondo resonances via quantum confinement

Controlling zero bias anomalies in magnetic atoms provides a promising strategy to engineer tunable quantum many-body excitations. Here we show how two different quantum impurities featuring spinaron and Kondo excitations can be controlled via quantum confinement engineering by using circular quantum corrals on a Ag(111) surface. In corrals built from both Ag and Co adatoms, the width of the zero bias anomaly in the central Co adatom oscillates as a function of corral radius with a period of half of the Ag(111) surface state wavelength. Parameters extracted for Co/Ag(111) show only small differences in extracted spinaron zero-bias anomaly between corral walls built from Ag or Co adatoms. In quantum corrals occupied with metal-free phthalocyanine, a $S=1/2$ Kondo system, we observe notable changes in the zero bias anomaly lineshape as a function of corral radius. Our results offer insight into many-body Kondo and spinaron resonances where the electronic density is controlled by confinement engineering.

cond-mat.mes-hall↗

arXiv2023

Atomic-scale visualization of multiferroicity in monolayer NiI$_2$

Progress in layered van der Waals materials has resulted in the discovery of ferromagnetic and ferroelectric materials down to the monolayer limit. Recently, evidence of the first purely two-dimensional multiferroic material was reported in monolayer NiI$_2$. However, probing multiferroicity with scattering-based and optical bulk techniques is challenging on 2D materials, and experiments on the atomic scale are needed to fully characterize the multiferroic order at the monolayer limit. Here, we use scanning tunneling microscopy (STM) supported by theoretical calculations based on density functional theory (DFT) to probe and characterize the multiferroic order in monolayer NiI$_2$. We demonstrate that the type-II multiferroic order displayed by NiI$_2$, arising from the combination of a magnetic spin spiral order and a strong spin-orbit coupling, allows probing the multiferroic order in the STM experiments. Moreover, we directly probe the magnetoelectric coupling of NiI$_2$ by external electric field manipulation of the multiferroic domains. Our findings establish a novel point of view to analyse magnetoelectric effects at the microscopic level, paving the way towards engineering new multiferroic orders in van der Waals materials and their heterostructures.

cond-mat.mtrl-sci↗

arXiv2023

Real-space imaging of dispersive triplon excitations in engineered quantum magnets

Quantum magnets provide a powerful platform to explore complex quantum many-body phenomena. One example is triplon excitations, exotic many-body modes emerging from deconfined singlet-triplet transitions with no single particle analog. Triplons are challenging to observe in conventional materials, as the energy scales of singlet-triplet transitions are associated with Hund's energy and are dramatically larger than the typical bandwidth of spin fluctuations. We engineer a minimal quantum magnet from organic molecules and demonstrate the emergence of dispersive triplon modes in one- and two-dimensional assemblies probed with scanning tunneling microscopy and spectroscopy. We show the variable bandwidth of triplon excitations in these two different geometries. Our results provide the first demonstration of dispersive triplon excitations from a real-space measurement, suggesting their potential engineering to realize exotic many-body phenomena in quantum magnets without breaking time-reversal symmetry.

cond-mat.str-el↗

arXiv2023

Control of molecular orbital ordering using a van der Waals monolayer ferroelectric

Two-dimensional (2D) ferroelectric materials provide a promising platform for the electrical control of quantum states. In particular, due to their 2D nature, they are suitable for influencing the quantum states of deposited molecules via the proximity effect. Here, we report electrically controllable molecular states in phthalocyanine molecules adsorbed on monolayer ferroelectric material SnTe. In particular, we demonstrate that the strain and ferroelectric order in SnTe creates a transition between two distinct orbital orders in the adsorbed phthalocyanine molecules. By controlling the polarization of the ferroelectric domain using scanning tunneling microscopy (STM), we have successfully demonstrated that orbital order can be manipulated electrically. Our results show how ferroelastic coupling in 2D systems allows control of molecular states, providing a starting point for ferroelectrically switchable molecular orbital ordering and ultimately, electrical control of molecular magnetism.

cond-mat.mtrl-sci↗

arXiv2023

Evidence of nodal superconductivity in monolayer 1H-TaS$_2$ with hidden order fluctuations

Unconventional superconductors represent one of the fundamental directions in modern quantum materials research. In particular, nodal superconductors are known to appear naturally in strongly correlated systems, including cuprate superconductors and heavy-fermion systems. Van der Waals materials hosting superconducting states are well known, yet nodal monolayer van der Waals superconductors have remained elusive. Here, using low-temperature scanning tunneling microscopy (STM) and spectroscopy (STS) experiments, we show that pristine monolayer 1H-TaS$_2$ realizes a nodal superconducting state. By including non-magnetic disorder, we drive the nodal superconducting state to a conventional gapped s-wave state. Furthermore, we observe the emergence of many-body excitations close to the gap edge, signalling a potential unconventional pairing mechanism. Our results demonstrate the emergence of nodal superconductivity in a van der Waals monolayer, providing a building block for van der Waals heterostructures exploiting unconventional superconducting states.

cond-mat.supr-con↗

arXiv2023

Visualization of moiré magnons in monolayer ferromagnet

Two-dimensional magnetic materials provide an ideal platform to explore collective many-body excitations associated with spin fluctuations. In particular, it should be feasible to explore, manipulate and ultimately design magnonic excitations in two-dimensional van der Waals magnets in a controllable way. Here we demonstrate the emergence of moiré magnon excitations, stemming from the interplay of spin-excitations in monolayer CrBr$_3$ and the moiré pattern stemming from the lattice mismatch with the underlying substrate. The existence of moiré magnons is further confirmed via inelastic quasiparticle interference, showing the appearance of a dispersion pattern correlated with the moiré length scale. Our results provide a direct visualization in real-space of the dispersion of moiré magnons, demonstrating the versatility of moiré patterns in creating emerging many-body excitations.

cond-mat.mes-hall↗

arXiv2022

Confinement-engineered superconductor to correlated-insulator transition in a van der Waals monolayer

Transition metal dichalcogenides (TMDC) are a rich family of two-dimensional materials displaying a multitude of different quantum ground states. In particular, d$^3$ TMDCs are paradigmatic materials hosting a variety of symmetry broken states, including charge density waves, superconductivity, and magnetism. Among this family, NbSe$_2$ is one of the best-studied superconducting materials down to the monolayer limit. Despite its superconducting nature, a variety of results point towards strong electronic repulsions in NbSe$_2$. Here, we control the strength of the interactions experimentally via quantum confinement and use low-temperature scanning tunneling microscopy (STM) and spectroscopy (STS) to demonstrate that NbSe$_2$ is in close proximity to a correlated insulating state. This reveals the coexistence of competing interactions in NbSe$_2$, creating a transition from a superconducting to an insulating quantum correlated state by confinement-controlled interactions. Our results demonstrate the dramatic role of interactions in NbSe$_2$, establishing NbSe$_2$ as a correlated superconductor with competing interactions.

cond-mat.mes-hall↗

arXiv2022

Moiré-enabled topological superconductivity

The search for artificial topological superconductivity has been limited by the stringent conditions required for its emergence. As exemplified by the recent discoveries of various correlated electronic states in twisted van der Waals materials, moiré patterns can act as a powerful knob to create artificial electronic structures. Here, we demonstrate that a moiré pattern between a van der Waals superconductor and a monolayer ferromagnet creates a periodic potential modulation that enables the realization of a topological superconducting state that would not be accessible in the absence of the moiré. The magnetic moiré pattern gives rise to Yu-Shiba-Rusinov minibands and periodic modulation of the Majorana edge modes that we detect using low-temperature scanning tunneling microscopy (STM) and spectroscopy (STS). Moiré patterns and, more broadly, periodic potential modulations are powerful tools to overcome the conventional constrains for realizing and controlling topological superconductivity.

cond-mat.mes-hall↗

arXiv2021

A Two-Dimensional Metal-Organic Framework on Superconducting NbSe$_2$

The combination of two-dimensional (2D) materials into vertical heterostructures has emerged as a promising path to designer quantum materials with exotic properties. Here, we extend this concept from inorganic 2D materials to 2D metal-organic frameworks (MOFs) that offer additional flexibility in realizing designer heterostructures. We successfully fabricate a monolayer 2D Cu-dicyanoanthracene MOF on a 2D van der Waals NbSe$_2$ superconducting substrate. The structural and electronic properties of two different phases of the 2D MOF are characterized by low-temperature scanning tunneling microscopy (STM) and spectroscopy (STS), complemented by density-functional theory (DFT) calculations. These experiments allow us to follow the formation of the kagome bandstructure from Star of David -shaped building blocks. This work extends the synthesis and electronic tuneability of 2D MOFs beyond the electronically less relevant metal and semiconducting surfaces to superconducting substrates, which are needed for the development of emerging quantum materials such as topological superconductors.

cond-mat.mtrl-sci↗

arXiv2021

Electronic Characterization of a Charge-Transfer Complex Monolayer on Graphene

Organic charge-transfer complexes (CTCs) formed by strong electron acceptor and strong electron donor molecules are known to exhibit exotic effects such as superconductivity and charge density waves. We present a low-temperature scanning tunneling microscopy and spectroscopy (LT-STM/STS) study of a two-dimensional (2D) monolayer CTC of tetrathiafulvalene (TTF) and fluorinated tetracyanoquinodimethane (F4TCNQ), self-assembled on the surface of oxygen-intercalated epitaxial graphene on Ir(111) (G/O/Ir(111)). We confirm the formation of the charge-transfer complex by dI/dV spectroscopy and direct imaging of the singly-occupied molecular orbitals. High-resolution spectroscopy reveals a gap at zero bias, suggesting the formation of a correlated ground state at low temperatures. These results point to the possibility to realize and study correlated ground states in charge-transfer complex monolayers on weakly interacting surfaces.

cond-mat.mes-hall↗