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Levente Tapasztó

Publications and source records attributed to Levente Tapasztó.

16 recordsLinked to original sources

Ultrastrong Au-Te bonding drives disorder in monolayer ZrTe$_5$ on gold

Monolayer ZrTe$_5$ is predicted to host a large-gap quantum spin Hall phase, motivating efforts to isolate single layers of the material. Gold-assisted exfoliation produces clean monolayers of many chalcogen-terminated van der Waals crystals, but the strong Te-Au bond may compete with the bonding network of the ZrTe$_5$ layer itself. Across tens of samples, low-temperature scanning tunneling microscopy on gold-exfoliated flakes shows a disordered monolayer surface in the overwhelming majority of cases, while thicker flakes preserve the characteristic quasi-one-dimensional chain structure. \emph{Ab initio} calculations of the ZrTe$_5$/Au(111) interface reproduce this asymmetry and resolve its mechanism: the Te atoms facing the gold chemisorb, rupturing the weak zigzag Te-Te bonds that cross-link the ZrTe$_3$ chains, turning the discrete bond-length spectrum of the crystal into a continuous one, while the chains persist as distorted units. Charge analysis shows the signature of covalent Te-Au bonding with a modest transfer that hole-dopes the monolayer; in the bilayer, the distortion and the doping stay confined to the layer contacting the gold, and the chemisorption and disorder each preclude the predicted quantum spin Hall phase. The same quasi-covalent Te-Au bond may perturb the contact layer of other gold-exfoliated Te-terminated crystals, particularly those with weakly connected intralayer networks.

cond-mat.mtrl-sci↗

Enrichment of rhombohedral stacking by mechanical exfoliation of graphite

Rhombohedral (ABC) graphite hosts a surface-localized flat band that supports correlated and topological electronic phases, but its experimental study is limited by the scarcity of ABC stacking in natural graphite, which is dominated by Bernal (AB) stacking. Here we show that the routine mechanical exfoliation step itself enriches the rhombohedral content of graphite flakes, and that a simple blade-assisted exfoliation step, which introduces additional shear, amplifies the effect further. Using large-area Raman 2D-band skewness mapping we measure ABC content at area fractions of 3\% in the pristine source crystal, 16\% after conventional exfoliation, and 26\% after blade-assisted exfoliation for thick flakes. In thin flakes ($<20$ layers) the per-flake area fraction reaches 75\% in the upper tail of the distribution. Tracking individual flakes before and after blade-assisted exfoliation shows that wrinkles seed AB-ABC domain walls, and uniaxial strain can move these walls. Blade-assisted mechanical exfoliation therefore removes one of the bottlenecks to the preparation of ABC-rich graphite samples for studies of correlated and topological phases in rhombohedral graphite.

cond-mat.mtrl-sci↗

Identification of graphite with perfect rhombohedral stacking by electronic Raman scattering

Rhombohedral graphite (RG) shows strong correlations in its topological flat band and is pivotal for exploring emergent, correlated electronic phenomena. One key advantage is the enhancement of electronic interactions with the increase in the number of rhombohedrally stacked graphene layers. Increasing thickness also leads to an exponential increase in the number of stacking faults, necessitating a precise method to identify flawless rhombohedral stacking. Overcoming this challenge is difficult because the established technique for stacking sequence identification, based on the Raman 2D peak, fails in thick RG samples. We demonstrate that the strong layer dependence of the band structure can be harnessed to identify RG without stacking faults, or alternatively, to detect their presence. For thicknesses ranging from 3 to 12 layers, we show that each perfect RG structure presents distinctive peak positions in electronic Raman scattering (ERS). This measurement can be carried out using a conventional confocal Raman spectrometer at room temperature, using visible excitation wavelengths. Consequently, this overcomes the identification challenge by providing a simple and fast optical measurement technique, thereby helping to establish RG as a platform for studying strong correlations in one of the simplest crystals possible.

cond-mat.mes-hall↗

Revealing the impact of ambient molecular contamination on scanning tunneling microscopy and spectroscopy of layered materials

Hydrocarbon contamination is an ever-present factor to consider in surface science measurements. In the case of van der Waals material surfaces, the structure of this contamination has become known in recent years as a self-assembled layer of normal-alkanes, resulting from a few days' exposure to ambient air. Knowledge of its composition and structure enables systematic investigation of its influence on surface properties. Here, we investigate the effect of this contamination on scanning tunneling microscopy (STM) and spectroscopy measurements by comparing clean and ambient alkane-contaminated surfaces of graphite. Our results reveal that the ambient alkane layer suppresses the well-known phonon-induced gap near the Fermi energy, resolving a long-standing inconsistency in STM studies, where this feature is often absent. Furthermore, we show that the presence of the contamination layer alters the current-distance ($I(z)$) characteristics, flattening its exponential decay by a factor of 1.5 to 5 compared to the clean surface. This change arises from extra conductance channels through the alkane layer alongside the tunnel junction, as the tip penetrates the contaminant overlayer. Finally, based on the $I(z)$ characteristics, we provide a practical guide to detect the presence of surface contamination in STM measurements.

cond-mat.mes-hall↗

The composition and structure of the ubiquitous hydrocarbon contamination on van der Waals materials

The behavior of single layer van der Waals (vdW) materials is profoundly influenced by the immediate atomic environment at their surface, a prime example being the myriad of emergent properties in artificial heterostructures. Equally significant are adsorbates deposited onto their surface from ambient. While vdW interfaces are well understood, our knowledge regarding atmospheric contamination is severely limited. Here we show that the common ambient contamination on the surface of: graphene, graphite, hBN and MoS2 is composed of a self-organized molecular layer, which forms during a few days of ambient exposure. Using low-temperature STM measurements we image the atomic structure of this adlayer and in combination with infrared spectroscopy identify the contaminant molecules as normal alkanes with lengths of 20-26 carbon atoms. Through its ability to self-organize, the alkane layer displaces the manifold other airborne contaminant species, capping the surface of vdW materials and possibly dominating their interaction with the environment.

cond-mat.mes-hall↗

Observation of competing, correlated ground states in the flat band of rhombohedral graphite

In crystalline solids the interactions of charge and spin can result in a variety of emergent quantum ground states, especially in partially filled, topological flat bands such as Landau levels or in 'magic-angle' bilayer graphene. Much less explored is rhombohedral graphite (RG), perhaps the simplest and structurally most perfect condensed matter system to host a flat band protected by symmetry. By scanning tunneling microscopy we map the flat band charge density of 8, 10 and 17 layers and identify a domain structure emerging from a competition between a sublattice antiferromagnetic insulator and a gapless correlated paramagnet. Our density-matrix renormalization group calculations explain the observed features and demonstrate that the correlations are fundamentally different from graphene based magnetism identified until now, forming the ground state of a quantum magnet. Our work establishes RG as a new platform to study many-body interactions beyond the mean-field approach, where quantum fluctuations and entanglement dominate.

cond-mat.mes-hall↗

Revealing the topological phase diagram of ZrTe$_5$ using the complex strain fields of microbubbles

Topological materials host robust properties, unaffected by microscopic perturbations, owing to the global topological properties of the bulk electron system. Materials in which the topological invariant can be changed by easily tuning external parameters are especially sought after. Zirconium pentatelluride (ZrTe$_5$) is one of a few experimentally available materials that reside close to the boundary of a topological phase transition, allowing the switching of its invariant by mechanical strain. Here, we unambiguously identify a topological insulator - metal transition as a function of strain, by a combination of ab initio calculations and direct measurements of the local charge density. Our model quantitatively describes the response to complex strain patterns found in bubbles of few layer ZrTe$_5$ without fitting parameters, reproducing the mechanical deformation dependent closing of the band gap observed using scanning tunneling microscopy. We calculate the topological phase diagram of ZrTe$_5$ and identify the phase at equilibrium, enabling the design of device architectures which exploit the unique topological switching characteristics of the system.

cond-mat.mtrl-sci↗

Robust quantum point contact operation of narrow graphene constrictions patterned by AFM cleavage lithography

Detecting conductance quantization in graphene nanostructures turned out more challenging than expected. The observation of well-defined conductance plateaus through graphene nanoconstrictions so far has only been accessible in the highest quality suspended or h-BN encapsulated devices. However, reaching low conductance quanta in zero magnetic field, is a delicate task even with such ultra-high mobility devices. Here, we demonstrate a simple AFM-based nanopatterning technique for defining graphene constrictions with high precision (down to 10 nm width) and reduced edge-roughness (+/- 1 nm). The patterning process is based on the in-plane mechanical cleavage of graphene by the AFM tip, along its high symmetry crystallographic directions. As-defined, narrow graphene constrictions with improved edge quality enable an unprecedentedly robust QPC operation, allowing the observation of conductance quantization even on standard $SiO_2/Si$ substrates, down to low conductance quanta. Conductance plateaus, were observed at $ne^2/h$, evenly spaced by $2e^2/h$ (corresponding to n = 3, 5, 7, 9, 11) in the absence of an external magnetic field, while spaced by $e^2/h$ (n = 1, 2, 3, 4, 5, 6) in 8T magnetic field.

cond-mat.mes-hall↗

Signature of large-gap quantum spin Hall state in the layered mineral jacutingaite

Quantum spin Hall (QSH) insulators are materials that feature an insulating bulk and host edge states protected by time-reversal symmetry. The helical locking of spin and momentum in these states suppresses backscattering of charge carriers, promising applications from low-power electronics to quantum computing. A major challenge for applications is the identification of large gap QSH materials, which would enable room temperature dissipationless transport in their edge states. Here we show that the layered mineral jacutingaite (Pt$_2$HgSe$_3$) is a candidate QSH material, realizing the long sought after the Kane-Mele insulator. Using scanning tunneling microscopy, we measure a band gap of 110 meV, above room temperature, and identify the hallmark edge states. By calculating the $\mathbb{Z}_2$ invariant, we confirm the topological nature of the gap. Being a layered mineral, it is stable in air and can be thinned down to a few atomic layers by mechanical exfoliation. Furthermore, we demonstrate that it can be integrated into heterostructures with other two-dimensional materials. This adds a topological insulator to the 2D quantum material library, greatly expanding the possibilities for tuning 2D electron systems using stacks of layered materials.

cond-mat.mes-hall↗

Ultra-flat twisted superlattices in 2D heterostructures

Moiré-superlattices are ubiquitous in 2D heterostructures, strongly influencing their electronic properties. They give rise to new Dirac cones and are also at the origin of the superconductivity observed in magic-angle bilayer graphene. The modulation amplitude (corrugation) is an important yet largely unexplored parameter in defining the properties of 2D superlattices. The generally accepted view is that the corrugation monotonically decreases with increasing twist angle, while its effects on the electronic structure diminish as the layers become progressively decoupled. Here we found by lattice relaxation of around 8000 different Moiré-superstructures using high scale Classical Molecular Simulations combined with analytical calculations, that even a small amount of strain can substantially change this picture, giving rise to more complex behavior of superlattice corrugation as a function of twist angle. One of the most surprising findings is the emergence of an ultra-flat phase that can be present for arbitrary small twist angle having a much lower corrugation level than the decoupled phase at large angles. A possible experimental realization of the ultra-flat state is revealed by Scanning Tunneling Microscopy (STM) investigations of the graphene/graphite system.

cond-mat.mes-hall↗

Spontaneous doping of the basal plane of MoS2 single-layers through oxygen substitution under ambient conditions

The chemical inertness of the defect-free basal plane confers environmental stability to MoS2 single-layers, but it also limits their chemical versatility and catalytic activity. The stability of the pristine MoS2 basal plane against oxidation under ambient conditions is a widely accepted assumption in the interpretation of various studies and applications. However, single-atom level structural investigations reported here reveal that oxygen atoms spontaneously incorporate into the basal plane of MoS2 single layers during ambient exposure. Our scanning tunneling microscopy investigations reveal a slow oxygen substitution reaction, upon which individual sulfur atoms are one by one replaced by oxygen, giving rise to solid solution type 2D MoS2-xOx crystals. O substitution sites present all over the basal plane act as single-atomic active reaction centers, substantially increasing the catalytic activity of the entire MoS2 basal plane for the electrochemical H2 evolution reaction.

cond-mat.mes-hall↗

Large intravalley scattering due to pseudo-magnetic fields in crumpled graphene

The pseudo-magnetic field generated by mechanical strain in graphene can have dramatic consequences on the behavior of electrons and holes. Here we show that pseudo-magnetic field fluctuations present in crumpled graphene can induce significant intravalley scattering of charge carriers. We detect this by measuring the confocal Raman spectra of crumpled areas, where we observe an increase of the D'/D peak intensity ratio by up to a factor of 300. We reproduce our observations by numerical calculation of the double resonant Raman spectra and interpret the results as experimental evidence of the phase shift suffered by Dirac charge carriers in the presence of a pseudo-magnetic field. This lifts the restriction on complete intravalley backscattering of Dirac fermions.

cond-mat.mes-hall↗

Exfoliation of single layer BiTeI flakes

Spin orbit interaction can be strongly boosted when a heavy element is embedded into an inversion asymmetric crystal field. A simple structure to realize this concept in a 2D crystal contains three atomic layers, a middle one built up from heavy elements generating strong atomic spin-orbit interaction and two neighboring atomic layers with different electron negativity. BiTeI is a promising candidate for such a 2D crystal, since it contains heavy Bi layer between Te and I layers. Recently the bulk form of BiTeI attracted considerable attention due to its giant Rashba interaction, however, 2D form of this crystal was not yet created. In this work we report the first exfoliation of single layer BiTeI using a recently developed exfoliation technique on stripped gold. Our combined scanning probe studies and first principles calculations show that SL BiTeI flakes with sizes of 100 $μ$m were achieved which are stable at ambient conditions. The giant Rashba splitting and spin-momentum locking of this new member of 2D crystals open the way towards novel spintronic applications and synthetic topological heterostructures.

cond-mat.mes-hall↗

Novel graphene/Sn and graphene/SnOx hybrid nanostructures: Induced superconductivity and band gaps revealed by scanning probe measurements

The development of functional composite nanomaterials based on graphene and metal nanoparticles (NPs) is currently the subject of intense research interest. In this study we report the preparation of novel type of graphene/Sn and graphene/SnOx (1 < x < 2) hybrid nanostructures and their investigation by scanning probe methods. First, we prepare Sn NPs by evaporating 7 - 8 nm tin on highly oriented pyrolytic graphite substrates. Graphene/Sn nanostructures are obtained by transferring graphene on top of the tin NPs immediately after evaporation. We show by scanning tunnelling microscopy (STM) and spectroscopy (STS) that tin NPs reduce significantly the environmental p-type doping of graphene. Furthermore, we demonstrate by low-temperature STM and STS measurements that superconductivity is induced in graphene, either directly supported by Sn NPs or suspended between them. Additionally, we prepare SnOx NPs by annealing the evaporated tin at 500 ${^o}$C. STS measurements performed on hybrid graphene/SnOx nanostructures reveal the electronic band gap of SnOx NPs. The results can open new avenues for the fabrication of novel hybrid superconducting nanomaterials with designed structures and morphologies.

cond-mat.mes-hall↗

Preparing local strain patterns in graphene by atomic force microscope based indentation

Patterning graphene into various mesoscopic devices such as nanoribbons, quantum dots, etc. by lithographic techniques has enabled the guiding and manipulation of graphene's Dirac-type charge carriers. Graphene, with well-defined strain patterns, holds promise of similarly rich physics while avoiding the problems created by the hard to control edge configuration of lithographically prepared devices. To engineer the properties of graphene via mechanical deformation, versatile new techniques are needed to pattern strain profiles in a controlled manner. Here we present a process by which strain can be created in substrate supported graphene layers. Our atomic force microscope-based technique opens up new possibilities in tailoring the properties of graphene using mechanical strain.

cond-mat.mes-hall↗

Revealing the grain structure of graphene grown by chemical vapor deposition

The physical processes occurring in the presence of disorder: point defects, grain boundaries, etc. may have detrimental effects on the electronic properties of graphene. Here we present an approach to reveal the grain structure of graphene by the selective oxidation of defects and subsequent atomic force microscopy analysis. This technique offers a quick and easy alternative to different electron microscopy and diffraction methods and may be used to give quick feedback on the quality of graphene samples grown by chemical vapor deposition.

cond-mat.mes-hall↗