arXiv subjects

Vladimir I. Fal'ko

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

At least 37 records · Page 2Linked to original sources

arXiv2022

Moiré Modulation of Charge Density Waves

Here we investigate how charge density waves (CDW), inherent to a monolayer, are effected by creating twisted van der Waals structures. Homobilayers of metallic transition metal dichalcogenides (TMDs), at small twist angles where there is significant atomic reconstruction, are utilised as an example to investigate the interplay between the moiré domain structure and CDWs of different periods. For $\sqrt{3}\times\sqrt{3}$ CDWs, there is no geometric constraint to prevent the CDWs from propagating throughout the moiré structure. Whereas for $2\times2$ CDWs, to ensure the CDWs in each layer have the most favourable interactions in the domains, the CDW phase must be destroyed in the connecting domain walls. For $3\times3$ CDWs with twist angles close to 180 degree, moiré-scale triangular structures can form; while close to 0 degree, moiré-scale dimer domains occur. The star-of-David CDW ($\sqrt{13}\times\sqrt{13}$) is found to host CDWs in the domains only, since there is one low energy stacking configuration, similar to $2\times2$ CDWs. These predictions are offered for experimental verification in twisted bilayer metallic TMDs which host CDWs, and we hope this will stimulate further research on the interplay between the moiré supperlattice and CDW phases intrinsic to the comprising 2D materials.

cond-mat.mtrl-sci↗

arXiv2022

Band Gap Opening in Bilayer Graphene-CrCl$_3$/CrBr$_3$/CrI$_3$ van der Waals Interfaces

We report experimental investigations of transport through bilayer graphene (BLG)/chromium trihalide (CrX$_3$; X=Cl, Br, I) van der Waals interfaces. In all cases, a large charge transfer from BLG to CrX$_3$ takes place (reaching densities in excess of $10^{13}$ cm$^{-2}$), and generates an electric field perpendicular to the interface that opens a band gap in BLG. We determine the gap from the activation energy of the conductivity and find excellent agreement with the latest theory accounting for the contribution of the $σ$ bands to the BLG dielectric susceptibility. We further show that for BLG/CrCl$_3$ and BLG/CrBr$_3$ the band gap can be extracted from the gate voltage dependence of the low-temperature conductivity, and use this finding to refine the gap dependence on the magnetic field. Our results allow a quantitative comparison of the electronic properties of BLG with theoretical predictions and indicate that electrons occupying the CrX$_3$ conduction band are correlated.

cond-mat.mes-hall↗

arXiv2022

Light sources with bias tunable spectrum based on van der Waals interface transistors

Light-emitting electronic devices are ubiquitous in key areas of current technology, such as data communications, solid-state lighting, displays, and optical interconnects. Controlling the spectrum of the emitted light electrically, by simply acting on the device bias conditions, is an important goal with potential technological repercussions. However, identifying a material platform enabling broad electrical tuning of the spectrum of electroluminescent devices remains challenging. Here, we propose light-emitting field-effect transistors based on van der Waals interfaces of atomically thin semiconductors as a promising class of devices to achieve this goal. We demonstrate that large spectral changes in room-temperature electroluminescence can be controlled both at the device assembly stage -- by suitably selecting the material forming the interfaces -- and on-chip, by changing the bias to modify the device operation point. Even though the precise relation between device bias and kinetics of the radiative transitions remains to be understood, our experiments show that the physical mechanism responsible for light emission is robust, making these devices compatible with simple large areas device production methods.

cond-mat.mes-hall↗

arXiv2021

Multifaceted moiré superlattice physics in twisted WSe$_2$ bilayers

Lattice reconstruction in twisted transition-metal dichalcogenide (TMD) bilayers gives rise to piezo- and ferroelectric moiré potentials for electrons and holes, as well as a modulation of the hybridisation across the bilayer. Here, we develop hybrid $\mathbf{k}\cdot \mathbf{p}$ tight-binding models to describe electrons and holes in the relevant valleys of twisted TMD homobilayers with parallel (P) and anti-parallel (AP) orientations of the monolayer unit cells. We apply these models to describe moiré superlattice effects in twisted WSe${}_2$ bilayers, in conjunction with microscopic \emph{ab initio} calculations, and considering the influence of encapsulation, pressure and an electric displacement field. Our analysis takes into account mesoscale lattice relaxation, interlayer hybridisation, piezopotentials, and a weak ferroelectric charge transfer between the layers, and describes a multitude of possibilities offered by this system, depending on the choices of P or AP orientation, twist angle magnitude, and electron/hole valley.

cond-mat.mes-hall↗

arXiv2021

Control of Giant Topological Magnetic Moment and Valley Splitting in Trilayer Graphene

Bloch states of electrons in honeycomb two-dimensional crystals with multi-valley band structure and broken inversion symmetry have orbital magnetic moments of a topological nature. In crystals with two degenerate valleys, a perpendicular magnetic field lifts the valley degeneracy via a Zeeman effect due to these magnetic moments, leading to magnetoelectric effects which can be leveraged for creating valleytronic devices. In this work, we demonstrate that trilayer graphene with Bernal stacking, (ABA TLG) hosts topological magnetic moments with a large and widely tunable valley g-factor, reaching a value 1050 at the extreme of the studied parametric range. The reported experiment consists in sublattice-resolved scanning tunneling spectroscopy under perpendicular electric and magnetic fields that control the TLG bands. The tunneling spectra agree very well with the results of theoretical modeling that includes the full details of the TLG tight-binding model and accounts for a quantum-dot-like potential profile formed electrostatically under the scanning tunneling microscope tip.

cond-mat.mes-hall↗

arXiv2021

Interfacial ferroelectricity in marginally twisted 2D semiconductors

Twisted heterostructures of two-dimensional crystals offer almost unlimited scope for the design of novel metamaterials. Here we demonstrate a room-temperature ferroelectric semiconductor that is assembled using mono- or few- layer MoS2. These van der Waals heterostructures feature broken inversion symmetry, which, together with the asymmetry of atomic arrangement at the interface of two 2D crystals, enables ferroelectric domains with alternating out-of-plane polarisation arranged into a twist-controlled network. The latter can be moved by applying out-of-plane electrical fields, as visualized in situ using channelling contrast electron microscopy. The interfacial charge transfer for the observed ferroelectric domains is quantified using Kelvin probe force microscopy and agrees well with theoretical calculations. The movement of domain walls and their bending rigidity also agrees well with our modelling results. Furthermore, we demonstrate proof-of-principle field-effect transistors, where the channel resistance exhibits a pronounced hysteresis governed by pinning of ferroelectric domain walls. Our results show a potential venue towards room temperature electronic and optoelectronic semiconductor devices with built-in ferroelectric memory functions.

cond-mat.mes-hall↗

arXiv2021

Out-of-plane dielectric susceptibility of graphene in twistronic and Bernal bilayers

We describe how the out-of-plane dielectric polarizability of monolayer graphene influences the electrostatics of bilayer graphene -- both Bernal (BLG) and twisted (tBLG). We compare the polarizability value computed using density functional theory with the output from previously published experimental data on the electrostatically controlled interlayer asymmetry potential in BLG and data on the on-layer density distribution in tBLG. We show that monolayers in tBLG are described well by polarizability $α_{exp} = 10.8 \unicode{x212B}^3$ and effective out-of-plane dielectric susceptibility $ε_z = 2.5$, including their on-layer electron density distribution at zero magnetic field and the inter-layer Landau level pinning at quantizing magnetic fields.

cond-mat.mes-hall↗

arXiv2021

Full Slonczewski-Weiss-McClure parametrization of few-layer twistronic graphene

We use a hybrid k dot p theory - tight binding (HkpTB) model to describe interlayer coupling simultaneously in both Bernal and twisted graphene structures. For Bernal-aligned interfaces, HkpTB is parametrized using the full Slonczewski-Weiss-McClure (SWMcC) Hamiltonian of graphite, which is then used to refine the commonly used minimal model for twisted interfaces, by deriving additional terms that reflect all details of the full SWMcC model of graphite. We find that these terms introduce some electron-hole asymmetry in the band structure of twisted bilayers, but in twistronic multilayer graphene, they produce only a subtle change of moire miniband spectra, confirming the broad applicability of the minimal model for implementing the twisted interface coupling in such systems.

cond-mat.mes-hall↗

arXiv2021

Theory of tunneling spectra for a few-electron bilayer graphene quantum dot

The tuneability and control of quantum nanostructures in two-dimensional materials offer promising perspectives for their use in future electronics. It is hence necessary to analyze quantum transport in such nanostructures. Material properties such as a complex dispersion, topology, and charge carriers with multiple degrees of freedom, are appealing for novel device functionalities but complicate their theoretical description. Here, we study quantum tunnelling transport across a few-electron bilayer graphene quantum dot. We demonstrate how to uniquely identify single- and two-electron dot states' orbital, spin, and valley composition from differential conductance in a finite magnetic field. Furthermore, we show that the transport features manifest splittings in the dot's spin and valley multiplets induced by interactions and magnetic field (the latter splittings being a consequence of bilayer graphene's Berry curvature). Our results elucidate spin- and valley-dependent tunnelling mechanisms and will help to utilize bilayer graphene quantum dots, e.g., as spin and valley qubits.

cond-mat.mes-hall↗

arXiv2021

Excited Rydberg States in TMD Heterostructures

The functional form of Coulomb interactions in the transition metal dichalcogenides and other van der Waals solids is critical to many of their unique properties, e.g. strongly-correlated electron states, superconductivity and emergent ferromagnetism. This paper presents measurements of key excitonic energy levels in MoSe2/WSe2 heterostructures. These measurements are obtained from resonance Raman experiments on specific Raman peaks only observed at excited states of the excitons. This data is used to validate a model of the Coulomb potential in these structures which predicts the exciton energies to within ~5 meV / 2.5%. This model is used to determine the effect of heterostructure formation on the single-particle band gaps of the layers and will have a wide applicability in designing the next generation of more complex transition metal dichalcogenide structures.

cond-mat.mes-hall↗

arXiv2021

Spin-valley collective modes of the electron liquid in graphene

We develop the theory of collective modes supported by a Fermi liquid of electrons in pristine graphene. Under reasonable assumptions regarding the electron-electron interaction, all the modes but the plasmon are over-damped. In addition to the $SU(2)$ symmetric spin mode, these include also the valley imbalance modes obeying a $U(1)$ symmetry, and a $U(2)$ symmetric valley spin imbalance mode. We derive the interactions and diffusion constants characterizing the over-damped modes. The corresponding relaxation rates set fundamental constraints on graphene valley- and spintronics applications.

cond-mat.mes-hall↗

arXiv2021

Ghost anti-crossings caused by interlayer umklapp hybridization of bands in 2D heterostructures

In two-dimensional heterostructures, crystalline atomic layers with differing lattice parameters can stack directly one on another. The resultant close proximity of atomic lattices with differing periodicity can lead to new phenomena. For umklapp processes, this opens the possibility for interlayer umklapp scattering, where interactions are mediated by the transfer of momenta to or from the lattice in the neighbouring layer. Using angle-resolved photoemission spectroscopy to study a graphene on InSe heterostructure, we present evidence that interlayer umklapp processes can cause hybridization between bands from neighbouring layers in regions of the Brillouin zone where bands from only one layer are expected, despite no evidence for moir/'e-induced replica bands. This phenomenon manifests itself as 'ghost' anti-crossings in the InSe electronic dispersion. Applied to a range of suitable 2DM pairs, this phenomenon of interlayer umklapp hybridization can be used to create strong mixing of their electronic states, giving a new tool for twist-controlled band structure engineering.

cond-mat.mes-hall↗

arXiv2020

Superposition of intra- and inter-layer excitons in twistronic MoSe$_2$/WSe$_2$ bilayers probed by resonant Raman scattering

Hybridisation of electronic bands of two-dimensional materials, assembled into twistronic heterostructures, enables one to tune their optoelectronic properties by selecting conditions for resonant interlayer hybridisation. Resonant interlayer hybridisation qualitatively modifies the excitons in such heterostructures, transforming these optically active modes into superposition states of interlayer and intralayer excitons. For MoSe$_2$/WSe$_2$ heterostructures, strong hybridization occurs between the holes in the spin-split valence band of WSe$_2$ and in the top valence band of MoSe$_2$, especially when both are bound to the same electron in the lowest conduction band of WSe$_2$. Here we use resonance Raman scattering to provide direct evidence for the hybridisation of excitons in twistronic MoSe$_2$/WSe$_2$ structures, by observing scattering of specific excitons by phonons in both WSe$_2$ and MoSe$_2$. We also demonstrate that resonance Raman scattering spectroscopy opens up a wide range of possibilities for quantifying the layer composition of the superposition states of the exciton and the interlayer hybridisation parameters in heterostructures of two-dimensional materials.

cond-mat.mes-hall↗

arXiv2020

Atomic reconstruction in twisted bilayers of transition metal dichalcogenides

Van der Waals heterostructures form a massive interdisciplinary research field, fueled by the rich material science opportunities presented by layer assembly of artificial solids with controlled composition, order and relative rotation of adjacent atomic planes. Here we use atomic resolution transmission electron microscopy and multiscale modeling to show that the lattice of MoS$_2$ and WS$_2$ bilayers twisted to a small angle, $θ<3^{\circ}$, reconstructs into energetically favorable stacking domains separated by a network of stacking faults. For crystal alignments close to 3R stacking, a tessellated pattern of mirror reflected triangular 3R domains emerges, separated by a network of partial dislocations which persist to the smallest twist angles. Scanning tunneling measurements show that the electronic properties of those 3R domains appear qualitatively different from 2H TMDs, featuring layer-polarized conduction band states caused by lack of both inversion and mirror symmetry. In contrast, for alignments close to 2H stacking, stable 2H domains dominate, with nuclei of an earlier unnoticed metastable phase limited to $\sim$ 5nm in size. This appears as a kagome-like pattern at $θ\sim 1^{\circ}$, transitioning at $θ\rightarrow 0$ to a hexagonal array of screw dislocations separating large-area 2H domains.

cond-mat.mes-hall↗

arXiv2020

Crossover from weakly indirect to direct excitons in atomically thin films of InSe

We perform a $\mathbf{k \cdot p}$ theory analysis of the spectra of the lowest energy and excited states of the excitons in few-layer atomically thin films of InSe taking into account in-plane electric polarizability of the film and the influence of the encapsulation environment. For the thinner films, the lowest-energy state of the exciton is weakly indirect in momentum space, with its dispersion showing minima at a layer-number-dependent wave number, due to an inverted edge of a relatively flat topmost valence band branch of the InSe film spectrum and we compute the activation energy from the momentum dark exciton ground state into the bright state. For the films with more than seven In$_2$Se$_2$ layers, the exciton dispersion minimum shifts to $Γ$-point.

cond-mat.mes-hall↗

arXiv2020

Tunable van Hove Singularities and Correlated States in Twisted Trilayer Graphene

Understanding and tuning correlated states is of great interest and significance to modern condensed matter physics. The recent discovery of unconventional superconductivity and Mott-like insulating states in magic-angle twisted bilayer graphene (tBLG) presents a unique platform to study correlation phenomena, in which the Coulomb energy dominates over the quenched kinetic energy as a result of hybridized flat bands. Extending this approach to the case of twisted multilayer graphene would allow even higher control over the band structure because of the reduced symmetry of the system. Here, we study electronic transport properties in twisted trilayer graphene (tTLG, bilayer on top of monolayer graphene heterostructure). We observed the formation of van Hove singularities which are highly tunable by twist angle and displacement field and can cause strong correlation effects under optimum conditions, including superconducting states. We provide basic theoretical interpretation of the observed electronic structure.

cond-mat.mes-hall↗

arXiv2020

Raman spectroscopy of GaSe and InSe post-transition metal chalcogenides layers

III-VI post-transition metal chalcogenides (InSe and GaSe) are a new class of layered semiconductors, which feature a strong variation of size and type of their band gaps as a function of number of layers (N). Here, we investigate exfoliated layers of InSe and GaSe ranging from bulk crystals down to monolayer, encapsulated in hexagonal boron nitride, using Raman spectroscopy. We present the N-dependence of both intralayer vibrations within each atomic layer, as well as of the interlayer shear and layer breathing modes. A linear chain model can be used to describe the evolution of the peak positions as a function of N, consistent with first principles calculations.

cond-mat.mtrl-sci↗

arXiv2020

Design of van der Waals Interfaces for Broad-Spectrum Optoelectronics

Van der Waals (vdW) materials offer new ways to assemble artificial electronic media with properties controlled at the design stage, by combining atomically defined layers into interfaces and heterostructures. Their potential for optoelectronics stems from the possibility to tailor the spectral response over a broad range by exploiting interlayer transitions between different compounds with an appropriate band-edge alignment. For the interlayer transitions to be radiative, however, a serious challenge comes from details of the materials --such as lattice mismatch or even a small misalignment of the constituent layers-- that can drastically suppress the electron-photon coupling. The problem was evidenced in recent studies of heterostructures of monolayer transition metal dichalcogenides, whose band edges are located at the K-point of reciprocal space. Here we demonstrate experimentally that the solution to the interlayer coupling problem is to engineer type-II interfaces by assembling atomically thin crystals that have the bottom of the conduction band and the top of the valence band at the $Γ$-point, thus avoiding any momentum mismatch. We find that this type of vdW interfaces exhibits radiative optical transition irrespective of lattice constant, rotational/translational alignment of the two layers, or whether the constituent materials are direct or indirect gap semiconductors. The result, which is robust and of general validity, drastically broadens the scope of future optoelectronics device applications based on 2D materials.

cond-mat.mes-hall↗