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Vladimir I. Fal'ko

Publications and source records attributed to Vladimir I. Fal'ko.

At least 19 recordsLinked to original sources

Lifshitz transitions and isospin polarization in twist-decoupled monolayer-bilayer graphene

Bernal-stacked bilayer graphene (BLG) hosts correlated electronic phases tied to low-energy Lifshitz transitions at saddle points in its valence band. To access this regime, ultralow charge disorder and control over a vertical electric field are simultaneously required. Here, we employ a twist-decoupled monolayer (MLG) to bias a proximal BLG in the absence of an external displacement field (D). We thereby reveal three-fold degenerate quantum Hall states at D = 0, with multiple transitions driven by doping, magnetic and electric field. Spontaneous broken symmetry in the vicinity of the valence band edge is signaled by the emergence of quantum oscillations with anomalous frequencies and large quasiparticle mass. These results indicate that electronic interactions in BLG are preserved in presence of an atomically close MLG, while showcasing the potential of CVD-grown graphene multilayers for the exploration of correlated phases of matter.

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Charge distribution across dislocation networks induced by a strained top layer in hexagonal boron nitride substrates

Hexagonal boron nitride (hBN) flakes are key building blocks for encapsulating two-dimensional (2D) materials, providing atomically flat surfaces and an excellent dielectric environment for high-mobility field-effect transistors and tunnelling devices. However, strain induced during mechanical exfoliation and assembly of van der Waals heterostructures may lead to plastic deformations of the hBN surface, injecting dislocation lines between the topmost layer and the underlying film. Since a monolayer of hBN is non-centrosymmetric and exhibits a piezoelectric response to deformation, individual dislocations and, in particular their networks, can generate electrostatic potential modulations in the encapsulated 2D material. Here, we examine scenarios in which the top hBN layer is uniaxially strained and/or twisted, and show how lattice reconstruction into dislocation networks leads to the formation of piezoelectric charge hotspots that effectively behave as charged defects.

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Tunable Kondo effect in a bilayer graphene quantum channel

The interaction between itinerant electrons and localized spins is key to a wide range of electronic phenomena. Of particular interest is the regime where the interacting electrons exhibit both spin and valley degeneracy, resulting in SU(4) Kondo physics. However, this regime is challenging to realize in typical mesoscopic systems because it requires a strong interaction between electrons, resulting in a Kondo temperature ($T_\mathrm{K}$) significantly larger than the spin and valley splittings. Here, we present conductance measurements of a quantum point contact (QPC) in bilayer graphene (BLG). Beyond the expected quantized conductance plateaus, which reflect spin and valley degeneracy, we observe an additional subband, known as `0.7 anomaly' exhibiting signatures of Kondo physics and a $T_\mathrm{K}$ ranging from approximately 0.5 up to 2.4 K at zero magnetic field, corresponding to Kondo energies between 40 and 200 $μ$eV. Given that the spin-orbit splitting in BLG is between 40 and 80 $μ$eV, we argue that these results are consistent with a transition between four-fold degenerate SU(4) and two-fold degenerate spin-valley locked SU(2) Kondo effects. Furthermore, we break the valley degeneracy of the lowest subband by an out-of-plane magnetic field and show that Kondo signatures remain present, indicating a transition from SU(4) to a valley-polarized SU(2) Kondo effect, and showing the versatility of BLG QPCs for exploring many-body effects.

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Tunable spin-orbit splitting in bilayer graphene/WSe$_2$ quantum devices

Bilayer graphene (BLG)-based quantum devices represent a promising platform for emerging technologies, such as quantum computing and spintronics. However, their intrinsically weak spin-orbit coupling (SOC) complicates spin and valley manipulation. Integrating BLG with transition metal dichalcogenides (TMDs) enhances the SOC via proximity effects. While this enhancement has been demonstrated in 2D-layered structures, 1D and 0D nanostructures in BLG/TMD remain unrealized, with open questions regarding SOC strength and tunability. Here, we investigate quantum point contacts and quantum dots in two BLG/WSe$_2$ heterostructures with different stacking orders. Across multiple devices, we reproducibly demonstrate spin-orbit splitting up to 1.5 meV - more than 1 order of magnitude higher than in pristine BLG. Furthermore, we show that the induced SOC can be tuned in situ from its maximum value to near-complete suppression via the perpendicular electric field. This enhancement and in situ tunability establish the SOC as a control mechanism for dynamic spin and valley manipulation.

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Proximity screening greatly enhances electronic quality of graphene

The electronic quality of two-dimensional systems is crucial when exploring quantum transport phenomena. In semiconductor heterostructures, decades of optimization have yielded record-quality two-dimensional gases with transport and quantum mobilities reaching close to 10$^8$ and 10$^6$ cm$^2$/Vs, respectively. Although the quality of graphene devices has also been improving, it remains comparatively lower. Here we report a transformative improvement in the electronic quality of graphene by employing graphite gates placed in its immediate proximity, at 1 nm separation. The resulting screening reduces charge inhomogeneity by two orders of magnitude, bringing it down to a few 10$^7$ cm$^-2$ and limiting potential fluctuations to less than 1 meV. Quantum mobilities reach 10$^7$ cm$^2$/Vs, surpassing those in the highest-quality semiconductor heterostructures by an order of magnitude, and the transport mobilities match their record. This quality enables Shubnikov-de Haas oscillations in fields as low as 1 mT and quantum Hall plateaus below 5 mT. Although proximity screening predictably suppresses electron-electron interactions, fractional quantum Hall states remain observable with their energy gaps reduced only by a factor of 3-5 compared to unscreened devices, demonstrating that many-body phenomena at spatial scales shorter than 10 nm remain robust. Our results offer a reliable route to improving electronic quality in graphene and other two-dimensional systems, which should facilitate the exploration of new physics previously obscured by disorder.

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Adhesion and Reconstruction of Graphene/Hexagonal Boron Nitride Heterostructures: A Quantum Monte Carlo Study

We investigate interlayer adhesion and relaxation at interfaces between graphene and hexagonal boron nitride (hBN) monolayers in van der Waals heterostructures. The adhesion potential between graphene and hBN is calculated as a function of local lattice offset using diffusion quantum Monte Carlo methods, which provide an accurate treatment of van der Waals interactions. Combining the adhesion potential with elasticity theory, we determine the relaxed structures of graphene and hBN layers at interfaces, finding no metastable structures. The adhesion potential is well described by simple Lennard-Jones pair potentials that we parameterize using our quantum Monte Carlo data. Encapsulation of graphene between near-aligned crystals of hBN gives rise to a moiré pattern whose period is determined by the misalignment angle between the hBN crystals superimposed over the moiré superlattice previously studied in graphene on an hBN substrate. We model minibands in such supermoiré superlattices and find them to be sensitive to a 180$^\circ$ rotation of one of the encapsulating hBN crystals. We find that monolayer and bilayer graphene placed on a bulk hBN substrate and bulk hBN/graphene/bulk hBN systems do not relax to adopt a common lattice constant. The energetic balance is much closer for free-standing monolayer graphene/hBN bilayers and hBN/graphene/hBN trilayers. The layers in an alternating stack of graphene and hBN are predicted to strain to adopt a common lattice constant and hence we obtain a new, stable three-dimensional crystal with a unique electronic structure.

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Built-in Bernal gap in large-angle-twisted monolayer-bilayer graphene

Atomically thin materials offer multiple opportunities for layer-by-layer control of their electronic properties. While monolayer graphene (MLG) is a zero-gap system, Bernal-stacked bilayer graphene (BLG) acquires a finite band gap when the symmetry between the layers' potential energy is broken, usually, via a displacement electric field applied in double-gate devices. Here, we introduce a twistronic stack comprising both MLG and BLG, synthesized via chemical vapor deposition, showing a Bernal gap in the absence of external fields. Although a large ($\sim30^{\circ}$) twist angle decouples the MLG and BLG electronic bands near Fermi level, proximity-induced energy shifts in the outermost layers result in a built-in asymmetry, which requires a displacement field of $0.14$ V/nm to be compensated. The latter corresponds to a $\sim10$ meV intrinsic BLG gap, a value confirmed by our thermal-activation measurements. The present results highlight the role of structural asymmetry and encapsulating environment, expanding the engineering toolbox for monolithically-grown graphene multilayers.

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Interlayer dislocations in multilayer and bulk MoS${}_2$

Dislocations in van der Waals materials are linear defects confined to the interfaces between consecutive stoichiometric monolayers of a bulk layered crystal. Here, we present a mesoscale model for the description of interlayer dislocations in thin films of transition metal dichalcogenides. Taking 2H-MoS${}_2$ as a representative material, we compute the dependence of the dislocation energy on the film thickness, from few-layer MoS$_2$ to the bulk crystal, and analyse the strain field in the layers surrounding a dislocation. We also analyse the influence of strain field on the band edge profiles for electrons and holes, and conclude that the resulting energy profiles are incapable of localising charge carriers, in particular at room temperature.

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Direct Visualization of Relativistic Quantum Scars

Quantum scars refer to eigenstates with enhanced probability density along unstable classical periodic orbits (POs). First predicted 40 years ago, scars are special eigenstates that counterintuitively defy ergodicity in quantum systems whose classical counterpart is chaotic. Despite the importance and long history of scars, their direct visualization in quantum systems remains an open field. Here we demonstrate that, by using an in-situ graphene quantum dot (GQD) creation and wavefunction mapping technique, quantum scars are imaged for Dirac electrons with nanometer spatial resolution and meV energy resolution with a scanning tunneling microscope. Specifically, we find enhanced probability densities in the form of lemniscate-shaped and streak-like patterns within our stadium-shaped GQDs. Both features show equal energy interval recurrence, consistent with predictions for relativistic quantum scars. By combining classical and quantum simulations, we demonstrate that the observed patterns correspond to two unstable POs that exist in our stadium-shaped GQD, thus proving they are both quantum scars. In addition to providing the first unequivocal visual evidence of quantum scarring, our work offers insight into the quantum-classical correspondence in relativistic chaotic quantum systems and paves the way to experimental investigation of other recently proposed scarring species such as perturbation-induced scars, chiral scars, and antiscarring.

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Substrate, temperature and magnetic field dependence of electric polarisation in mixed-stacking tetralayer graphenes

Polytypes of tetralayer graphene (TLG: Bernal, rhombohedral and mixed stacking) are crystalline structures with different symmetries. Among those, mixed-stacking tetralayers lack inversion symmetry, which allows for intrinsic spontaneous out-of-plane electrical polarisation, inverted in the mirror-image pair, ABCB and ABAC stackings. Here, we compare the intrinsic polarisation of such TLGs with the symmetry-breaking effect of a substrate, which can also generate out-of-plane electric dipole moments with different sizes in all four polytypes, including ABCB and ABAC twins. We analyse their temperature and magnetic field dependence, in view of understanding the origin of the recently measured Kelvin probe force microscopy maps of tetralayer flakes, and notice that the intrinsic contribution could be singled out based on magnetic field dependence of polarisation measured at low temperatures.

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Two-dimensional electrons at mirror and twistronic twin boundaries in van der Waals ferroelectrics

Semiconducting transition metal dichalcogenides (MX$_2$) occur in 2H and rhombohedral (3R) polytypes, respectively distinguished by anti-parallel and parallel orientation of consecutive monolayer lattices. In its bulk form, 3R-MX$_2$ is ferroelectric, hosting an out-of-plane electric polarisation, the direction of which is dictated by stacking. Here, we predict that twin boundaries, separating adjacent polarization domains with reversed built-in electric fields, are able to host two-dimensional electrons and holes with an areal density reaching $\sim 10^{13} {\rm cm}^{-2}$. Our modelling suggests that n-doped twin boundaries have a more promising binding energy than p-doped ones, whereas hole accumulation is stable at external surfaces of a twinned film. We also propose that assembling pairs of mono-twin films with a `magic' twist angle $θ^*$ that provides commensurability between the moiré pattern at the interface and the accumulated carrier density, should promote a regime of strongly correlated states of electrons, such as Wigner crystals, and we specify the values of $θ^*$ for homo- and heterostructures of various TMDs.

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Ultimate charge transport regimes in doping-controlled graphene laminates: phonon-assisted processes revealed by the linear magnetoresistance

Understanding and controlling the electrical properties of solution-processed 2D materials is key to further printed electronics progress. Here we demonstrate that the thermolysis of the aromatic intercalants utilized in nanosheet exfoliation for graphene laminates opens the route to achieving high intrinsic mobility and simultaneously controlling doping type ($n$- and $p$-) and concentration over a wide range. We establish that the intra-flake mobility is high by observing a linear magnetoresistance of such solution-processed graphene laminates and using it to devolve the inter-flake tunneling and intra-layer magnetotransport. Consequently, we determine the temperature dependences of the inter- and intra-layer characteristics, which both appear to be dominated by phonon-assisted processes at temperature $T>$20 Kelvin. In particular, we identify the efficiency of phonon-assisted tunneling as the main limiting factor for electrical conductivity in graphene laminates at room temperature. We also demonstrate a thermoelectric sensitivity of around 50 $μ$V K$^{-1}$ in a solution-processed metal-free graphene-based thermocouple.

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Competition of moiré network sites to form electronic quantum dots in reconstructed MoX${}_2$/WX${}_2$ heterostructures

Twisted bilayers of two-dimensional semiconductors offer a versatile platform to engineer quantum states for charge carriers using moiré superlattice effects. Among the systems of recent interest are twistronic MoSe${}_{2}$/WSe${}_{2}$ and MoS${}_{2}$/WS${}_{2}$ heterostructures, which undergo reconstruction into preferential stacking domains and highly strained domain wall networks, determining the electron/hole localization across moiré superlattices. Here, we present a catalogue of options for the formation of self-organized quantum dots and wires in lattice-reconstructed marginally twisted MoSe${}_{2}$/WSe${}_{2}$ and MoS${}_{2}$/WS${}_{2}$ bilayers, fine tuned by the twist angle between the monolayers from perfect alignment to $θ\sim 1^{\circ}$, and by choosing parallel or anti-parallel orientation of their unit cells. The proposed scenarios of the quantum dots and wires formation are found using multi-scale modelling that takes into account the features of strain textures caused by twirling of domain wall networks.

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Mixed-Stacking Few-Layer Graphene as an Elemental Weak Ferroelectric Material

Ferroelectricity (Valasek, J. Phys. Rev. 1921, 17, 475) - a spontaneous formation of electric polarisation - is a solid state phenomenon, usually, associated with ionic compounds or complex materials. Here we show that, atypically for elemental solids, few-layer graphenes can host an equilibrium out-of-plane electric polarisation, switchable by sliding the constituent graphene sheets. The systems hosting such effect include mixed-stacking tetralayers and thicker (5-9 layers) rhombohedral graphitic films with a twin boundary in the middle of a flake. The predicted electric polarisation would also appear in marginally (small-angle) twisted few-layer flakes, where lattice reconstruction would give rise to networks of mesoscale domains with alternating value and sign of out-of-plane polarisation.

cond-mat.mtrl-sci↗

Semimetallic and semiconducting graphene-hBN multilayers with parallel or reverse stacking

We theoretically investigate 3D layered crystals of alternating graphene and hBN layers with different symmetries. Depending on the hopping parameters between the graphene layers, we find that these synthetic 3D materials can feature semimetallic, gapped, or Weyl semimetal phases. Our results demonstrate that 3D crystals stacked from individual 2D materials represent a synthetic materials class with emergent properties different from their constituents.

cond-mat.mtrl-sci↗

Mixing of surface and bulk electronic states at a graphite-hexagonal boron nitride interface

Van der Waals assembly enables exquisite design of electronic states in two-dimensional (2D) materials, often by superimposing a long-wavelength periodic potential on a crystal lattice using moiré superlattices. Here we show that electronic states in three-dimensional (3D) crystals such as graphite can also be tuned by the superlattice potential arising at the interface with another crystal, namely, crystallographically aligned hexagonal boron nitride. Such alignment is found to result in a multitude of Lifshitz transitions and Brown-Zak oscillations for near-surface 2D states whereas, in high magnetic fields, fractal states of Hofstadter's butterfly extend deep into graphite's bulk. Our work shows a venue to control 3D spectra by using the approach of 2D twistronics.

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Flat bands for electrons in rhombohedral graphene multilayers with a twin boundary

Topologically protected flat surface bands make thin films of rhombohedral graphite an appealing platform for searching for strongly correlated states of 2D electrons. In this work, we study rhombohedral graphite with a twin boundary stacking fault and analyse the semimetallic and topological properties of low-energy bands localised at the surfaces and at the twinned interface. We derive an effective 4-band low energy model, where we implement the full set of Slonczewski-Weiss-McClure (SWMcC) parameters, and find the conditions for the bands to be localised at the twin boundary, protected from the environment-induced disorder. This protection together with a high density of states at the charge neutrality point, in some cases -- due to a Lifshitz transition, makes this system a promising candidate for hosting strongly-correlated effects.

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Observation of Giant Orbital Magnetic Moments and Paramagnetic Shift in Artificial Relativistic Atoms and Molecules

Massless Dirac fermions have been observed in various materials such as graphene and topological insulators in recent years, thus offering a solid-state platform to study relativistic quantum phenomena. Single quantum dots (QDs) and coupled QDs formed with massless Dirac fermions can be viewed as artificial relativistic atoms and molecules, respectively. Such structures offer a unique platform to study atomic and molecular physics in the ultra-relativistic regime. Here, we use a scanning tunneling microscope to create and probe single and coupled electrostatically defined graphene QDs to unravel the unique magnetic field responses of artificial relativistic nanostructures. Giant orbital Zeeman splitting and orbital magnetic moment are observed in single graphene QDs. While for coupled graphene QDs, Aharonov Bohm oscillations and strong Van Vleck paramagnetic shift are observed. Such properties of artificial relativistic atoms and molecules can be leveraged for novel magnetic field sensing modalities.

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