arXiv subjects

Vladimir I. Fal'ko

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

At least 55 records · Page 3Linked to original sources

arXiv2020

Broken mirror symmetry in excitonic response of reconstructed domains in twisted MoSe$_2$/MoSe$_2$ bilayers

Structural engineering of van der Waals heterostructures via stacking and twisting has recently been used to create moiré superlattices, enabling the realization of new optical and electronic properties in solid-state systems. In particular, moiré lattices in twisted bilayers of transition metal dichalcogenides (TMDs) have been shown to lead to exciton trapping, host Mott insulating and superconducting states, and act as unique Hubbard systems whose correlated electronic states can be detected and manipulated optically. Structurally, these twisted heterostructures also feature atomic reconstruction and domain formation. Unfortunately, due to the nanoscale sizes (~10 nm) of typical moiré domains, the effects of atomic reconstruction on the electronic and excitonic properties of these heterostructures could not be investigated systematically and have often been ignored. Here, we use near-0$^o$ twist angle MoSe$_2$/MoSe$_2$ bilayers with large rhombohedral AB/BA domains to directly probe excitonic properties of individual domains with far-field optics. We show that this system features broken mirror/inversion symmetry, with the AB and BA domains supporting interlayer excitons with out-of-plane (z) electric dipole moments in opposite directions. The dipole orientation of ground-state $Γ$-K interlayer excitons (X$_{I,1}$) can be flipped with electric fields, while higher-energy K-K interlayer excitons (X$_{I,2}$) undergo field-asymmetric hybridization with intralayer K-K excitons (X$_0$). Our study reveals the profound impacts of crystal symmetry on TMD excitons and points to new avenues for realizing topologically nontrivial systems, exotic metasurfaces, collective excitonic phases, and quantum emitter arrays via domain-pattern engineering.

cond-mat.mes-hall↗

arXiv2019

Composite super-moiré lattices in double aligned graphene heterostructures

When two-dimensional atomic crystals are brought into close proximity to form a van der Waals heterostructure, neighbouring crystals can start influencing each others electronic properties. Of particular interest is the situation when the periodicity of the two crystals closely match and a moiré pattern forms, which results in specific electron scattering, reconstruction of electronic and excitonic spectra, crystal reconstruction, and many other effects. Thus, formation of moiré patterns is a viable tool of controlling the electronic properties of 2D materials. At the same time, the difference in the interatomic distances for the two crystals combined, determines the range in which the electronic spectrum is reconstructed, and thus is a barrier to the low energy regime. Here we present a way which allows spectrum reconstruction at all energies. By using graphene which is aligned simultaneously to two hexagonal boron nitride layers, one can make electrons scatter in the differential moiré pattern, which can have arbitrarily small wavevector and, thus results in spectrum reconstruction at arbitrarily low energies. We demonstrate that the strength of such a potential relies crucially on the atomic reconstruction of graphene within the differential moiré super-cell. Such structures offer further opportunity in tuning the electronic spectra of two-dimensional materials.

cond-mat.mes-hall↗

arXiv2019

Films of rhombohedral graphite as two-dimensional topological semimetals

Topologically non-trivial states characterized by Berry curvature appear in a number of materials ranging from spin-orbit-coupling driven topological insulators to graphene. In multivalley conductors, such as mono- and bilayer graphene, despite a zero total Chern number for the entire Brillouin zone, Berry curvature with different signs concentrated in different valleys can affect the observable material's transport characteristics. Here we consider thin films of rhombohedral graphite, which appear to retain truly two-dimensional properties up to tens of layers of thickness and host two-dimensional electron states with a large Berry curvature, accompanied by a giant intrinsic magnetic moment carried by electrons. The size of Berry curvature and magnetization in the vicinity of each valley can be controlled by electrostatic gating leading to a tuneable anomalous Hall effect and a peculiar structure of the two-dimensional Landau level spectrum.

cond-mat.mes-hall↗

arXiv2019

Electronic phase separation in topological surface states of rhombohedral graphite

Of the two stable forms of graphite, hexagonal (HG) and rhombohedral (RG), the former is more common and has been studied extensively. RG is less stable, which so far precluded its detailed investigation, despite many theoretical predictions about the abundance of exotic interaction-induced physics. Advances in van der Waals heterostructure technology have now allowed us to make high-quality RG films up to 50 graphene layers thick and study their transport properties. We find that the bulk electronic states in such RG are gapped and, at low temperatures, electron transport is dominated by surface states. Because of topological protection, the surface states are robust and of high quality, allowing the observation of the quantum Hall effect, where RG exhibits phase transitions between gapless semimetallic phase and gapped quantum spin Hall phase with giant Berry curvature. An energy gap can also be opened in the surface states by breaking their inversion symmetry via applying a perpendicular electric field. Moreover, in RG films thinner than 4 nm, a gap is present even without an external electric field. This spontaneous gap opening shows pronounced hysteresis and other signatures characteristic of electronic phase separation, which we attribute to emergence of strongly-correlated electronic surface states.

cond-mat.mes-hall↗

arXiv2019

Ultra-thin van der Waals crystals as semiconductor quantum wells

Control over the electronic spectrum at low energy is at the heart of the functioning of modern advanced electronics: high electron mobility transistors, semiconductor and Capasso terahertz lasers, and many others. Most of those devices rely on the meticulous engineering of the size quantization of electrons in quantum wells. This avenue, however, hasn't been explored in the case of 2D materials. Here we transfer this concept onto the van der Waals heterostructures which utilize few-layers films of InSe as quantum wells. The precise control over the energy of the subbands and their uniformity guarantees extremely high quality of the electronic transport in such systems. Using novel tunnelling and light emitting devices, for the first time we reveal the full subbands structure by studying resonance features in the tunnelling current, photoabsorption and light emission. In the future, these systems will allow development of elementary blocks for atomically thin infrared and THz light sources based on intersubband optical transitions in few-layer films of van der Waals materials.

cond-mat.mes-hall↗

arXiv2019

Tuning of impurity-bound interlayer complexes in a van der Waals heterobilayer

Due to their unique two-dimensional nature, charge carriers in semiconducting transition metal dichalcogenides (TMDs) exhibit strong unscreened Coulomb interactions and sensitivity to defects and impurities. The versatility of van der Waals layer stacking allows spatially separating electrons and holes between different TMD layers with staggered band structure, yielding interlayer few-body excitonic complexes whose nature is still debated. Here we combine quantum Monte Carlo calculations with spectrally and temporally resolved photoluminescence measurements on a top- and bottom-gated MoSe2/WSe2 heterostructure, and identify the emitters as impurity-bound interlayer excitonic complexes. Using independent electrostatic control of doping and out-of-plane electric field, we demonstrate control of the relative populations of neutral and charged complexes, their emission energies on a scale larger than their linewidth, and an increase of their lifetime into the microsecond regime. This work unveils new physics of confined carriers and is key to the development of novel optoelectronics applications.

cond-mat.mes-hall↗

arXiv2019

Resonantly hybridised excitons in moiré superlattices in van der Waals heterostructures

Atomically-thin layers of two-dimensional materials can be assembled in vertical stacks held together by relatively weak van der Waals forces, allowing for coupling between monolayer crystals with incommensurate lattices and arbitrary mutual rotation. A profound consequence of using these degrees of freedom is the emergence of an overarching periodicity in the local atomic registry of the constituent crystal structures, known as a moiré superlattice. Its presence in graphene/hexagonal boron nitride (hBN) structures led to the observation of electronic minibands, whereas its effect enhanced by interlayer resonant conditions in twisted graphene bilayers culminated in the observation of the superconductor-insulator transition at magic twist angles. Here, we demonstrate that, in semiconducting heterostructures built of incommensurate MoSe2 and WS2 monolayers, excitonic bands can hybridise, resulting in the resonant enhancement of the moiré superlattice effects. MoSe2 and WS2 are specifically chosen for the near degeneracy of their conduction band edges to promote the hybridisation of intra- and interlayer excitons, which manifests itself through a pronounced exciton energy shift as a periodic function of the interlayer rotation angle. This occurs as hybridised excitons (hX) are formed by holes residing in MoSe2 bound to a twist-dependent superposition of electron states in the adjacent monolayers. For heterostructures with almost aligned pairs of monolayer crystals, resonant mixing of the electron states leads to pronounced effects of the heterostructure's geometrical moiré pattern on the hX dispersion and optical spectrum. Our findings underpin novel strategies for band-structure engineering in semiconductor devices based on van der Waals heterostructures.

cond-mat.mes-hall↗

arXiv2019

Interlayer hybridization and moiré superlattice minibands for electrons and excitons in heterobilayers of transition-metal dichalcogenides

Geometrical moiré patterns, generic for almost aligned bilayers of two-dimensional (2D) crystals with similar lattice structure but slightly different lattice constants, lead to zone folding and miniband formation for electronic states. Here, we show that moiré superlattice (mSL) effects in $\mathrm{MoSe}_2/\mathrm{WS}_2$ and $\mathrm{MoTe}_2/\mathrm{MoSe}_2$ heterobilayers that feature alignment of the band edges are enhanced by resonant interlayer hybridization, and anticipate similar features in twisted homobilayers of TMDs, including examples of narrow minibands close to the actual band edges. Such hybridization determines the optical activity of interlayer excitons in transition-metal dichalcogenide (TMD) heterostructures, as well as energy shifts in the exciton spectrum. We show that the resonantly hybridized exciton (hX) energy should display a sharp modulation as a function of the interlayer twist angle, accompanied by additional spectral features caused by umklapp electron-photon interactions with the mSL. We analyze the appearance of resonantly enhanced mSL features in absorption and emission of light by the interlayer exciton hybridization with both intralayer A and B excitons in $\mathrm{MoSe}_2/\mathrm{WS}_2$, $\mathrm{MoTe}_2/\mathrm{MoSe}_2$, $\mathrm{MoSe}_2/\mathrm{MoS}_2$, $\mathrm{WS}_2/\mathrm{MoS}_2$, and $\mathrm{WSe}_2/\mathrm{MoSe}_2$.

cond-mat.mes-hall↗

arXiv2019

Indirect to direct gap crossover in two-dimensional InSe revealed by ARPES

Atomically thin films of III-VI post-transition metal chalcogenides (InSe and GaSe) form an interesting class of two-dimensional semiconductor that feature strong variations of their band gap as a function of the number of layers in the crystal [1-4] and, specifically for InSe, an earlier predicted crossover from a direct gap in the bulk [5,6] to a weakly indirect band gap in monolayers and bilayers [7-11]. Here, we apply angle resolved photoemission spectroscopy with submicrometer spatial resolution ($μ$ARPES) to visualise the layer-dependent valence band structure of mechanically exfoliated crystals of InSe. We show that for 1 layer and 2 layer InSe the valence band maxima are away from the $\mathbfΓ$-point, forming an indirect gap, with the conduction band edge known to be at the $\mathbfΓ$-point. In contrast, for six or more layers the bandgap becomes direct, in good agreement with theoretical predictions. The high-quality monolayer and bilayer samples enables us to resolve, in the photoluminescence spectra, the band-edge exciton (A) from the exciton (B) involving holes in a pair of deeper valence bands, degenerate at $\mathbfΓ$, with the splitting that agrees with both $μ$ARPES data and the results of DFT modelling. Due to the difference in symmetry between these two valence bands, light emitted by the A-exciton should be predominantly polarised perpendicular to the plane of the two-dimensional crystal, which we have verified for few-layer InSe crystals.

cond-mat.mtrl-sci↗

arXiv2018

Infrared-to-violet tunable optical activity in atomic films of GaSe, InSe, and their heterostructures

Two-dimensional semiconductors - atomic layers of materials with covalent intra-layer bonding and weak (van der Waals or quadrupole) coupling between the layers - are a new class of materials with great potential for optoelectronic applications. Among those, a special position is now being taken by post-transition metal chalcogenides (PTMC), InSe and GaSe. It has recently been found that the band gap in 2D crystals of InSe more than doubles in the monolayer compared to thick multilayer crystals, while the high mobility of conduction band electrons is promoted by their light in-plane mass. Here, we use Raman and PL measurements of encapsulated few layer samples, coupled with accurate atomic force and transmission electron microscope structural characterisation to reveal new optical properties of atomically thin GaSe preserved by hBN encapsulation. The band gaps we observe complement the spectral range provided by InSe films, so that optical activity of these two almost lattice-matched PTMC films and their heterostructures densely cover the spectrum of photons from violet to infrared. We demonstrate the realisation of the latter by the first observation of interlayer excitonic photoluminescence in few-layer InSe-GaSe heterostructures. The spatially indirect transition is direct in k-space and therefore is bright, while its energy can be tuned in a broad range by the number of layers.

cond-mat.mes-hall↗

arXiv2018

Topologically non-trivial valley states in bilayer graphene quantum point contacts

We present measurements of quantized conductance in electrostatically induced quantum point contacts in bilayer graphene. The application of a perpendicular magnetic field leads to an intricate pattern of lifted and restored degeneracies with increasing field: at zero magnetic field the degeneracy of quantized one-dimensional subbands is four, because of a twofold spin and a twofold valley degeneracy. By switching on the magnetic field, the valley degeneracy is lifted. Due to the Berry curvature states from different valleys split linearly in magnetic field. In the quantum Hall regime fourfold degenerate conductance plateaus reemerge. During the adiabatic transition to the quantum Hall regime, levels from one valley shift by two in quantum number with respect to the other valley, forming an interweaving pattern that can be reproduced by numerical calculations.

cond-mat.mes-hall↗

arXiv2018

Hybrid k$\cdot$p tight-binding model for subbands and infrared intersubband optics in few-layer films of transition-metal dichalcogenides: MoS$_2$, MoSe$_2$, WS$_2$ and WSe${}_2$

We present a density functional theory parametrized hybrid k$\cdot$p tight binding model for electronic properties of atomically thin films of transition-metal dichalcogenides, 2H-$MX_2$ ($M$=Mo, W; $X$=S, Se). We use this model to analyze intersubband transitions in $p$- and $n$-doped $2{\rm H}-MX_2$ films and predict the line shapes of the intersubband excitations, determined by the subband-dependent two-dimensional electron and hole masses, as well as excitation lifetimes due to emission and absorption of optical phonons. We find that the intersubband spectra of atomically thin films of the 2H-${MX_2}$ family with thicknesses of $N=2$ to $7$ layers densely cover the infrared spectral range of wavelengths between $2$ and $30\ {\rm μm}$. The detailed analysis presented in this paper shows that for thin $n$-doped films, the electronic dispersion and spin-valley degeneracy of the lowest-energy subbands oscillate between odd and even number of layers, which may also offer interesting opportunities for quantum Hall effect studies in these systems.

cond-mat.mes-hall↗

arXiv2018

Tunable Berry curvature, valley and spin Hall effect in Bilayer MoS$_2$

The chirality of electronic Bloch bands is responsible for many intriguing properties of layered two-dimensional materials. We show that in bilayers of transition metal dichalcogenides (TMDCs), unlike in few-layer graphene and monolayer TMDCs, both intra-layer and inter-layer couplings give important contributions to the Berry-curvature in the $K$ and $-K$ valleys of the Brillouin zone. The inter-layer contribution leads to the stacking dependence of the Berry curvature and we point out the differences between the commonly available 3R type and 2H type bilayers. Due to the inter-layer contribution the Berry curvature becomes highly tunable in double gated devices. We study the dependence of the valley Hall and spin Hall effects on the stacking type and external electric field. Although the valley and spin Hall conductivities are not quantized, in MoS$_2$ 2H bilayers they may change sign as a function of the external electric field which is reminiscent of the behaviour of lattice Chern insulators.

cond-mat.mes-hall↗

arXiv2018

Localized interlayer complexes in heterobilayer transition metal dichalcogenides

We present theoretical results for the radiative rates and doping-dependent photoluminescence spectrum of interlayer excitonic complexes localized by donor impurities in MoSe$_2$/WSe$_2$ twisted heterobilayers, supported by quantum Monte Carlo calculations of binding energies and wave-function overlap integrals. For closely aligned layers, radiative decay is made possible by the momentum spread of the localized complexes' wave functions, resulting in few $μ$s$^{-1}$ radiative rates. For strongly misaligned layers, the short-range interaction between the carriers and impurity provides a finite radiative rate with a strong asymptotic twist angle dependence $\propto θ^{-8}$. Finally, phonon-assisted recombination is considered, with emission of optical phonons in both layers resulting in additional weaker emission lines, redshifted by the phonon energy.

cond-mat.mes-hall↗

arXiv2018

Hybrid $\mathbf{k\cdot p}$-tight-binding model for intersubband optics in atomically thin InSe films

We propose atomic films of n-doped $γ$-InSe as a platform for intersubband optics in the infrared (IR) and far infrared (FIR) range, coupled to out-of-plane polarized light. Depending on the film thickness (number of layers) of the InSe film these transitions span from $\sim 0.7$ eV for bilayer to $\sim 0.05$ eV for 15-layer InSe. We use a hybrid $\mathbf{k} \cdot \mathbf{p}$ theory and tight-binding model, fully parametrized using density functional theory, to predict their oscillator strengths and thermal linewidths at room temperature.

cond-mat.mes-hall↗

arXiv2018

Cyclotron resonance of the magnetic ratchet effect and second harmonic generation in bilayer graphene

We model the magnetic ratchet effect in bilayer graphene in which a dc electric current is produced by an ac electric field of frequency $ω$ in the presence of a steady in-plane magnetic field and inversion-symmetry breaking. In bilayer graphene, the ratchet effect is tunable by an external metallic gate which breaks inversion symmetry. For zero in-plane magnetic field, we show that trigonal warping and inversion-symmetry breaking are able to produce a large dc valley current, but not a non-zero total dc charge current. For the magnetic ratchet in a tilted magnetic field, the perpendicular field component induces cyclotron motion with frequency $ω_c$ and we find that the dc current displays cyclotron resonance at $ω_c = ω$, although this peak in the current is actually smaller than its value at $ω_c = 0$. Second harmonic generation, however, is greatly enhanced by resonances at $ω_c = ω$ and $ω_c = 2ω$ for which the current is generally much larger than at $ω_c = 0$.

cond-mat.mes-hall↗

arXiv2018

Suppressed compressibility of quantum Hall effect edge states in epitaxial graphene on SiC

We determine conditions for the formation of compressible stripes near the quantum Hall effect (QHE) edges of top-gated epitaxial graphene on Si-terminated SiC (G/SiC) and compare those to graphene exfoliated onto insulating substrate in the field-effect-transistor (GraFET) geometry. For G/SiC, a large density of localised surface states on SiC just underneath graphene layer and charge transfer between them lead both to doping of graphene and to screening of potential profile near its edge. This suppresses formation of compressible stripes near QHE edges in graphene, making them much narrower than the corresponding compressible stripes in GraFETs.

cond-mat.mes-hall↗

arXiv2017

Graphene hot-electron light bulb: incandescence from hBN-encapsulated graphene in air

The excellent electronic and mechanical properties of graphene allow it to sustain very large currents, enabling its incandescence through Joule heating in suspended devices. Although interesting scientifically and promising technologically, this process is unattainable in ambient environment, because graphene quickly oxidises at high temperatures. Here, we take the performance of graphene-based incandescent devices to the next level by encapsulating graphene with hexagonal boron nitride (hBN). Remarkably, we found that the hBN encapsulation provides an excellent protection for hot graphene filaments even at temperatures well above 2000 K. Unrivalled oxidation resistance of hBN combined with atomically clean graphene/hBN interface allows for a stable light emission from our devices in atmosphere for many hours of continuous operation. Furthermore, when confined in a simple photonic cavity, the thermal emission spectrum is modified by a cavity mode, shifting the emission to the visible range spectrum. We believe our results demonstrate that hBN/graphene heterostructures can be used to conveniently explore the technologically important high-temperature regime and to pave the way for future optoelectronic applications of graphene-based systems.

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