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Vladimir Falko

Publications and source records attributed to Vladimir Falko.

15 recordsLinked to original sources
arXiv2026

Up/down-conversion of infrared light by few-layer graphene polytypes

Optical nonlinearity of materials with broken inversion symmetry enables two-photon processes where an incoming pair of photons can generate an up-converted photon with the combined frequency, or a high-energy photon can be split into a correlated pair of down-converted photons. Here, we identify few-layer graphene films that offer up/down-conversion capability in the infrared spectral range. For mixed stacking tetralayers (ABCB), which are non-centrosymmetric 2D crystals, we find highly efficient nearly resonant up/down-conversion of [$ω_1,ω_2$] photon pairs into/from a photon with $0.7$eV$<Ω=ω_1+ω_2<1.1$eV. We also note that a pronounced second-order nonlinearity in the spectral range of $0.7$eV$<Ω<0.9$eV can be promoted in rhombohedral tri- and tetralayers by asymmetrical encapsulation. Potentially, for fibers coated with few-layer graphene, this opens the door for ``in fiber" production of photon pairs with correlated polarizations.

cond-mat.mes-hall↗
arXiv2026

Moiré-induced lattice reconstruction at buried atomic interfaces

Atomic reconstruction at twisted two-dimensional interfaces governs many of their emergent optical, electronic, and mechanical properties, including sliding ferroelectricity. Despite recent progress in understanding lattice reconstruction in suspended twisted bilayers, structural changes at van der Waals heterointerfaces between multilayer crystals remain largely unexplored. Here we use multi-slice electron ptychography to non-invasively recover the three-dimensional atomic structure at marginally twisted rhombohedral interfaces between thick transition-metal dichalcogenide crystals. With a position precision of ~3 pm and a depth resolution ~1 nm, we resolve the twist-induced lattice reconstruction field per layer, and the resulting dislocation network at the buried interface. Despite the bulk nature, we observe markedly strong in-plane interfacial reconstruction due to suppression of the out-of-plane bending by outer layers, exceeding predictions from our three-dimensional modelling. Furthermore, we extract the strain tensor evolution during the decay of the reconstruction into the bulk, providing a structural foundation for understanding multi-layer moiré systems.

cond-mat.mes-hall↗
arXiv2026

Locally resolved electronic textures of reconstruction domains in marginally twisted monolayer-bilayer graphene

Controlling the stacking and rotational registry of graphene layers provides a powerful handle on atomic-scale structural reconstructions that alter the electronic landscape at the nanoscale. In particular, this governs how massless and massive Dirac fermions coexist and interact at the monolayer-bilayer graphene interface. In the limit of marginal twist, the system reconstructs into domains of distinct vertical stacking order, introducing characteristic electronic properties and new electronic length scales, a regime that, despite its structural richness, remains largely unexplored. Here, using scanning tunnelling microscopy and spectroscopy, we demonstrate that at very low rotation angles the monolayer-bilayer graphene system relaxes into a network of three distinct stacking domains with individual electronic textures revealed through spatially resolved spectroscopic mapping and corroborated by computed local density of states. We report switching of the hierarchy of the tunnelling characteristics between Bernal and rhombohedral domains as a function of bias voltage. Furthermore, the measured spectroscopic maps exhibit theoretically anticipated domain wall 'twirling' around energetically unfavorable AAB stacking nodes, promoted by out-of-plane deformations. Our results shed light on fundamental structure-property relationships underpinning moiré-driven phenomena, opening new avenues for harnessing structural degrees of freedom in van der Waals heterostructures.

cond-mat.mes-hall↗
arXiv2026

Continuous correlated states and dual-flatness in a moiré heterostructure

Many-body effects in condensed matter yield novel quantum states when the electronic density of states is enhanced. A vivid example is flat bands, which suppress kinetic energy and let interactions dominate, when they are filled with an integer number of electrons in moire systems. Yet flat bands and commensurate fillings are not the only conditions for correlated phenomena. Situations may occur where the band structure develops locally enhanced density of states, leading to strong correlations even at non-integer fillings, although such cases often yield pseudogaps that make detection elusive. Here we demonstrate that small-angle twisted monolayer-bilayer graphene combines moire-induced global flat band and additional local band flattening. Their coexistence allows direct comparison of correlated effects. The global route stabilizes commensurate states, while the local mechanism produces nearly flat bands, lifting degeneracy and generating symmetry breaking at non-integer fillings, yet without opening a global gap. Because there is no global gapped signature, the system remains metallic, but the effect reveals itself in anomalous Hall responses, signaling time-reversal symmetry breaking and valley polarization. Our results demonstrate dual-flatness as a guiding principle, extending moire physics beyond commensurate fillings and identifying topological transport as a probe of gapless correlated metals.

cond-mat.str-el↗
arXiv2026

Atomic-resolution imaging of gold species at organic liquid-solid interfaces

Understanding solid-liquid interfaces at the atomic-scale is key to improved performance of heterogeneous catalysts, electrodes and membranes. Here we combine unique specimen design, record atomic resolution in situ electron microscopy, and artificial intelligence-enabled analysis to achieve a step change in quantitative understanding of interfacial atomic behaviour. We create the first graphene liquid cells with organic solvents and employ them to track over 106 gold adatoms and clusters at a graphene surface immersed in acetone and cyclohexanone. We reveal dynamic correlated behaviour of gold adatom monomers, dimers, trimers and clusters, strongly influenced by each other, the solvent properties, and the atomic lattice of the substrate, in good agreement with theoretical calculations. We use the results to interpret differences in catalytic activity towards the industrially important acetylene hydrochlorination reaction. This new capability for exploration of atomic scale chemistry could enable rational design of future catalysts, membranes and electrodes with improved functionality.

cond-mat.mtrl-sci↗
arXiv2024

Electron Channelling Contrast SEM Imaging of Twist Domains in Transition Metal Dichalcogenide Heterostructures

Twisted 2D material heterostructures provide an exciting platform for investigating new fundamental physical phenomena. Many of the most interesting behaviours emerge at small twist angles, where the materials reconstruct to form areas of perfectly stacked crystal separated by partial dislocations. However, understanding the properties of these systems is often impossible without correlative imaging of their local reconstructed domain architecture, which exhibits random variations due to disorder and contamination. Here we demonstrate a simple and widely accessible route to visualise domains in as-produced twisted transition metal dichalcogenide (TMD) heterostructures using electron channelling contrast imaging (ECCI) in the scanning electron microscope (SEM). This non-destructive approach is compatible with conventional substrates and allows domains to be visualised even when sealed beneath an encapsulation layer. Complementary theoretical calculations reveal how a combination of elastic and inelastic scattering leads to contrast inversions at specified detector scattering angles and sample tilts. We demonstrate that optimal domain contrast is therefore achieved by maximising signal collection while avoiding contrast inversion conditions.

cond-mat.mtrl-sci↗
arXiv2024

In-plane staging in lithium-ion intercalation of bilayer graphene

The ongoing efforts to optimize Li-ion batteries led to the interest in intercalation of nanoscale layered compounds, including bilayer graphene. Its lithium intercalation has been demonstrated recently but the mechanisms underpinning the storage capacity remain poorly understood. Here, using magnetotransport measurements, we report in-operando intercalation dynamics of bilayer graphene. Unexpectedly, we find four distinct intercalation stages that correspond to well-defined Li-ion densities. We refer to these stages as 'in-plane', with no in-plane analogues in bulk graphite. The fully intercalated bilayers represent a stoichiometric compound C14LiC14 with a Li density of 2.7x10^{14} cm^{-2}, notably lower than fully intercalated graphite. Combining the experimental findings and DFT calculations, we show that the critical step in bilayer intercalation is a transition from AB to AA stacking which occurs at a density of 0.9x10^{14} cm^{-2}. Our findings reveal the mechanism and limits for electrochemical intercalation of bilayer graphene and suggest possible avenues for increasing the Li storage capacity.

cond-mat.mtrl-sci↗
arXiv2023

Valley-hybridized gate-tunable 1D exciton confinement in MoSe2

Controlling excitons at the nanoscale in semiconductor materials represents a formidable challenge in the fields of quantum photonics and optoelectronics. Achieving this control holds great potential for unlocking strong exciton-exciton interaction regimes, enabling exciton-based logic operations, exploring exotic quantum phases of matter, facilitating deterministic positioning and tuning of quantum emitters, and designing advanced optoelectronic devices. Monolayers of transition metal dichalcogenides (TMDs) offer inherent two-dimensional confinement and possess significant binding energies, making them particularly promising candidates for achieving electric-field-based confinement of excitons without dissociation. While previous exciton engineering strategies have predominantly focused on local strain gradients, the recent emergence of electrically confined states in TMDs has paved the way for novel approaches. Exploiting the valley degree of freedom associated with these confined states further broadens the prospects for exciton engineering. Here, we show electric control of light polarization emitted from one-dimensional (1D) quantum confined states in MoSe2. By employing non-uniform in-plane electric fields, we demonstrate the in-situ tuning of the trapping potential and reveal how gate-tunable valley-hybridization gives rise to linearly polarized emission from these localized states. Remarkably, the polarization of the localized states can be entirely engineered through either the spatial geometry of the 1D confinement potential or the application of an out-of-plane magnetic field.

cond-mat.mes-hall↗
arXiv2023

Spontaneous Electric Polarization in Graphene Polytypes

A crystalline solid is a periodic sequence of identical cells, each containing one or more atoms. If the constituting unit cell is not centrosymmetric, charge may distribute unevenly between the atoms, resulting in internal electric polarization. This effect serves as the basis for numerous ferroelectric, piezoelectric, and pyroelectric phenomena. In nearly all polar materials, including multilayered van der Waals stacks that were recently found to exhibit interfacial polarization, inversion symmetry is broken by having two or more atomic species within the unit cell. Here, we show that even elemental crystals, consisting of one type of atom, and composed of non-polar centrosymmetric layers, exhibit electric polarization if arranged in an appropriate three-dimensional architecture. This concept is demonstrated here for inversion and mirror asymmetric mixed-stacking tetra-layer polytypes of non-polar graphene sheets. Furthermore, we find that the room temperature out-of-plane electric polarization increases with external electrostatic doping, rather than decreases owing to screening. Using first-principles calculations, as well as tight-binding modeling, we unveil the origin of polytype-induced polarization and its dependence on doping. Extension of this idea to graphene multilayers suggests that solely by lateral shifts of constituent monolayers one can obtain multiple meta-stable interlayer stacking sequences that may allow for even larger electrical polarization.

cond-mat.mtrl-sci↗
arXiv2022

Ferroelectric switching at symmetry-broken interfaces by local control of dislocation networks

Semiconducting ferroelectric materials with low energy polarisation switching offer a platform for next-generation electronics such as ferroelectric field-effect transistors. Ferroelectric domains at symmetry-broken interfaces of transition metal dichalcogenide films provide an opportunity to combine the potential of semiconducting ferroelectrics with the design flexibility of two-dimensional material devices. Here, local control of ferroelectric domains in a marginally twisted WS2 bilayer is demonstrated with a scanning tunneling microscope at room temperature, and their observed reversible evolution understood using a string-like model of the domain wall network. We identify two characteristic regimes of domain evolution: (i) elastic bending of partial screw dislocations separating smaller domains with twin stacking and (ii) formation of perfect screw dislocations by merging pairs of primary domain walls. We also show that the latter act as the seeds for the reversible restoration of the inverted polarisation. These results open the possibility to achieve full control over atomically thin semiconducting ferroelectric domains using local electric fields, which is a critical step towards their technological use.

cond-mat.mes-hall↗
arXiv2018

Geometrically Enhanced Thermoelectric Effects in Graphene Nanoconstrictions

The influence of nanostructuring and quantum confinement on the thermoelectric properties of materials has been extensively studied. While this has made possible multiple breakthroughs in the achievable figure of merit, classical confinement, and its effect on the local Seebeck coefficient has mostly been neglected, as has the Peltier effect in general due to the complexity of measuring small temperature gradients locally. Here we report that reducing the width of a graphene channel to 100 nm changes the Seebeck coefficient by orders of magnitude. Using a scanning thermal microscope allows us to probe the local temperature of electrically contacted graphene two-terminal devices or to locally heat the sample. We show that constrictions in mono- and bilayer graphene facilitate a spatially correlated gradient in the Seebeck and Peltier coefficient, as evidenced by the pronounced thermovoltage $V_{th}$ and heating/cooling response $ΔT_{Peltier}$, respectively. This geometry dependent effect, which has not been reported previously in 2D materials, has important implications for measurements of patterned nanostructures in graphene and points to novel solutions for effective thermal management in electronic graphene devices or concepts for single material thermocouples.

cond-mat.mes-hall↗
arXiv2018

Nano-imaging of intersubband transitions in van der Waals quantum wells

The science and applications of electronics and optoelectronics have been driven for decades by progress in growth of semiconducting heterostructures. Many applications in the infrared and terahertz frequency range exploit transitions between quantized states in semiconductor quantum wells (intersubband transitions). However, current quantum well devices are limited in functionality and versatility by diffusive interfaces and the requirement of lattice-matched growth conditions. Here, we introduce the concept of intersubband transitions in van der Waals quantum wells and report their first experimental observation. Van der Waals quantum wells are naturally formed by two-dimensional (2D) materials and hold unexplored potential to overcome the aforementioned limitations: They form atomically sharp interfaces and can easily be combined into heterostructures without lattice-matching restrictions. We employ near-field local probing to spectrally resolve and electrostatically control the intersubband absorption with unprecedented nanometer-scale spatial resolution. This work enables exploiting intersubband transitions with unmatched design freedom and individual electronic and optical control suitable for photodetectors, LEDs and lasers.

cond-mat.mes-hall↗
arXiv2017

Superconductivity-induced features in electronic Raman spectrum of monolayer graphene

Using the continuum model, we investigate theoretically contribution of the low-energy electronic excitations to the Raman spectrum of superconducting monolayer graphene. We consider superconducting phases characterised by an isotropic order parameter in a single valley and find a Raman peak at a shift set by the size of the superconducting gap. The height of this peak is proportional to the square root of the gap and the third power of the Fermi level, and we estimate its quantum efficiency as $I\sim10^{-14}$.

cond-mat.mes-hall↗
arXiv2016

Rabi oscillations of two-photon states in nonlinear optical resonators

We demonstrate that four-wave mixing processes in high-quality non-linear resonators can lead to Rabi-like oscillations in photon occupation numbers and second-order correlation functions, being a characteristic feature of the presence of entangled photon pairs in the optical signal. In the case of a system driven by a continuous coherent pump, the oscillations occur in the transient regime. We show that driving the system with pulsed coherent pumping would generate strongly anti-bunched photon states.

quant-ph↗