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Alexei Barinov

Publications and source records attributed to Alexei Barinov.

At least 19 recordsLinked to original sources

Van der Waals devices for surface-sensitive experiments

In-operando characterization of van der Waals (vdW) devices using surface-sensitive methods provides critical insights into phase transitions and correlated electronic states. Yet, integrating vdW materials in functional devices while maintaining pristine surfaces is a key challenge for combined transport and surface-sensitive experiments. Conventional lithographic techniques introduce surface contamination, limiting the applicability of state-of-the-art spectroscopic probes. We present a stencil lithography-based approach for fabricating vdW devices, producing micron-scale electrical contacts, and exfoliation in ultra-high vacuum. The resist-free patterning method utilizes a shadow mask to define electrical contacts and yields thin flakes down to the single-layer regime via gold-assisted exfoliation. As a demonstration, we fabricate devices from 1$T-$TaS$_2$ flakes, achieving reliable contacts for application of electrical pulses and resistance measurements, as well as clean surfaces allowing for angle-resolved photoemission spectroscopy. The approach provides a platform for studying the electronic properties of vdW systems with surface-sensitive probes in well-defined device geometries.

cond-mat.mes-hall

Revealing the conduction band and pseudovector potential in 2D moiré semiconductors

Stacking monolayer semiconductors results in moiré patterns that host many correlated and topological electronic phenomena, but measurements of the basic electronic structure underpinning these phenomena are scarce. Here, we investigate the properties of the conduction band in moiré heterobilayers using submicron angle-resolved photoemission spectroscopy with electrostatic gating, focusing on the example of WS2/WSe2. We find that at all twist angles the conduction band edge is the K-point valley of the WS2, with a band gap of 1.58 +- 0.03 eV. By resolving the conduction band dispersion, we observe an unexpectedly small effective mass of 0.15 +- 0.02 m_e. In addition, we observe replicas of the conduction band displaced by reciprocal lattice vectors of the moiré superlattice. We present arguments and evidence that the replicas are due to modification of the conduction band states by the moiré potential rather than to final-state diffraction. Interestingly, the replicas display an intensity pattern with reduced, 3-fold symmetry, which we show implicates the pseudo vector potential associated with in-plane strain in moiré band formation.

cond-mat.mes-hall

Tunable Electron Transport in Defect-Engineered PdSe$_\mathrm{2}$

Tuning the ambipolar behavior in charge carrier transport via defect-engineering is crucial for achieving high mobility transistors for nonlinear logic circuits. Here, we present the electric-field tunable electron and hole transport in a microchannel device consisting of highly air-stable van der Waals (vdW) noble metal dichalcogenide (NMDC), PdSe$_\mathrm{2}$, as an active layer. Pristine bulk PdSe$_\mathrm{2}$ constitutes Se surface vacancy defects created during the growth or exfoliation process and offers an ambipolar transfer characteristics with a slight electron dominance recorded in field-effect transistor (FET) characteristics showing an ON/OFF ratio < 10 and electron mobility ~ 21 cm$^2$/V.s. However, transfer characteristics of PdSe$_\mathrm{2}$ can be tuned to a hole-dominated transport while using hydrochloric acid (HCl) as a $p$-type dopant. On the other hand, the chelating agent EDTA, being a strong electron donor, enhances the electron-dominance in PdSe$_\mathrm{2}$ channel. In addition, $p$-type behavior with a 100 times higher ON/OFF ratio is obtained while cooling the sample down to 10 K. Low-temperature angle-resolved photoemission spectroscopy resembles the $p$-type band structure of PdSe$_\mathrm{2}$ single crystal. Also, first principle density functional theory calculations justify the tunability observed in PdSe$_\mathrm{2}$ as a result of defect-engineering. Such a defect-sensitive ambipolar vdW architecture may open up new possibilities towards future CMOS (Complementary Metal-Oxide-Semiconductor) device fabrications and high performance integrated circuits.

cond-mat.mes-hall

Robustness of momentum-indirect interlayer excitons in MoS2/WSe2 heterostructure against charge carrier doping

Monolayer transition-metal dichalcogenide (TMD) semiconductors exhibit strong excitonic effects and hold promise for optical and optoelectronic applications. Yet, electron doping of TMDs leads to the conversion of neutral excitons into negative trions, which recombine predominantly non-radiatively at room temperature. As a result, the photoluminescence (PL) intensity is quenched. Here we study the optical and electronic properties of a MoS2/WSe2 heterostructure as a function of chemical doping by Cs atoms performed under ultra-high vacuum conditions. By PL measurements we identify two interlayer excitons and assign them to the momentum-indirect Q-Gamma and K-Gamma transitions. The energies of these excitons are in a very good agreement with ab initio calculations. We find that the Q-Gamma interlayer exciton is robust to the electron doping and is present at room temperature even at a high charge carrier concentration. Submicrometer angle-resolved photoemission spectroscopy (micro-ARPES) reveals charge transfer from deposited Cs adatoms to both the upper MoS2 and the lower WSe2 monolayer without changing the band alignment. This leads to a small (10 meV) energy shift of interlayer excitons. Robustness of the momentum-indirect interlayer exciton to charge doping opens up an opportunity of using TMD heterostructures in light-emitting devices that can work at room temperature at high densities of charge carriers.

cond-mat.mes-hall

A robust weak topological insulator in a bismuth halide Bi4Br2I2

We apply a topological material design concept for selecting a bulk topology of 3D crystals by different van-der-Waals stacking of 2D topological insulator layers, and find a bismuth halide Bi4Br2I2 to be an ideal weak topological insulator (WTI) with the largest band gap (~230 meV) among all the WTI candidates, by means of angle-resolved photoemission spectroscopy (ARPES), density functional theory (DFT) calculations, and resistivity measurements. Our results vastly expand future opportunities for fundamental research and device applications with a robust WTI.

cond-mat.mtrl-sci

Observation of Γ-valley moiré bands and emergent hexagonal lattice in twisted transition metal dichalcogenides

Twisted van der Waals heterostructures have recently been proposed as a condensed-matter platform for realizing controllable quantum models due to the low-energy moiré bands with specific charge distributions in moiré superlattices. Here, combining angle-resolved photoemission spectroscopy with sub-micron spatial resolution (μ-ARPES) and scanning tunneling microscopy (STM), we performed a systematic investigation on the electronic structure of 5.1° twisted bilayer WSe2 that hosts correlated insulating and zero-resistance states. Interestingly, contrary to one's expectation, moiré bands were observed only at Γ-valley but not K-valley in μ-ARPES measurements; and correspondingly, our STM measurements clearly identified the real-space honeycomb- and Kagome-shaped charge distributions at the moiré length scale associated with the Γ-valley moiré bands. These results not only reveal the unsual valley dependent moiré-modified electronic structure in twisted transition metal dichalcogenides, but also highlight the Γ-valley moiré bands as a promising platform for exploring strongly correlated physics in emergent honeycomb and Kagome lattices at different energy scales.

cond-mat.str-el

Large anomalous Hall effect induced by weak ferromagnetism in the noncentrosymmetric antiferromagnet $\mathrm{Co}\mathrm{Nb}_3\mathrm{S}_6$

We study the mechanism of the exceptionally large anomalous Hall effect (AHE) in the noncentrosymmetric antiferromagnet $\mathrm{Co}\mathrm{Nb}_3\mathrm{S}_6$ by angle-resolved photoemission spectroscopy (ARPES) and magnetotransport measurements. From ARPES measurements of $\mathrm{Co}\mathrm{Nb}_3\mathrm{S}_6$ and its family compounds ($\mathrm{Fe}\mathrm{Nb}_3\mathrm{S}_6$ and $\mathrm{Ni}\mathrm{Nb}_3\mathrm{S}_6$), we find a band dispersion unique to the Co intercalation existing near the Fermi level. We further demonstrate that a slight deficiency of sulfur in $\mathrm{Co}\mathrm{Nb}_3\mathrm{S}_6$ eliminates the ferromagnetism and the AHE simultaneously while hardly changing the band structure, indicating that the weak ferromagnetism is responsible for the emergence of the large AHE. Based on our results, we propose Weyl points near the Fermi level to cause the large AHE.

cond-mat.mtrl-sci

Moiré superlattice effects and band structure evolution in near-30-degree twisted bilayer graphene

In stacks of two-dimensional crystals, mismatch of their lattice constants and misalignment of crystallographic axes lead to formation of moiré patterns. We show that moiré superlattice effects persist in twisted bilayer graphene (tBLG) with large twists and short moiré periods. Using angle-resolved photoemission, we observe dramatic changes in valence band topology across large regions of the Brillouin zone, including the vicinity of the saddle point at $M$ and across 3 eV from the Dirac points. In this energy range, we resolve several moiré minibands and detect signatures of secondary Dirac points in the reconstructed dispersions. For twists $θ>21.8^{\circ}$, the low-energy minigaps are not due to cone anti-crossing as is the case at smaller twist angles but rather due to moiré scattering of electrons in one graphene layer on the potential of the other which generates intervalley coupling. Our work demonstrates robustness of mechanisms which enable engineering of electronic dispersions of stacks of two-dimensional crystals by tuning the interface twist angles. It also shows that large-angle tBLG hosts electronic minigaps and van Hove singularities of different origin which, given recent progress in extreme doping of graphene, could be explored experimentally.

cond-mat.mes-hall

Material design with the van der Waals stacking of bismuth-halide chains realizing a higher-order topological insulator

The van der Waals (vdW) materials with low dimensions have been extensively studied as a platform to generate exotic quantum properties. Advancing this view, a great deal of attention is currently paid to topological quantum materials with vdW structures. Here, we provide a new concept of designing topological materials by the vdW stacking of quantum spin Hall insulators (QSHIs). Most interestingly, a slight shift of inversion center in the unit cell caused by a modification of stacking is found to induce the topological variation from a trivial insulator to a higher-order topological insulator (HOTI). Based on that, we present the first experimental realization of a HOTI by investigating a bismuth bromide Bi4Br4 with angle-resolved photoemission spectroscopy (ARPES). The unique feature in bismuth halides capable of selecting various topology only by differently stacking chains, combined with the great advantage of the vdW structure, offers a fascinating playground for engineering topologically non-trivial edge-states toward future spintronics applications.

cond-mat.mtrl-sci

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

Atomic and electronic structure of two-dimensional Mo(1-x)WxS2 alloys

Alloying enables engineering of the electronic structure of semiconductors for optoelectronic applications. Due to their similar lattice parameters, the two-dimensional semiconducting transition metal dichalcogenides of the MoWSeS group (MX2 where M= Mo or W and X=S or Se) can be grown as high-quality materials with low defect concentrations. Here we investigate the atomic and electronic structure of Mo(1-x)WxS2 alloys using a combination of high-resolution experimental techniques and simulations. Analysis of the Mo and W atomic positions in these alloys, grown by chemical vapour transport, shows that they are randomly distributed, consistent with Monte Carlo simulations that use interaction energies determined from first-principles calculations. Electronic structure parameters are directly determined from angle resolved photoemission spectroscopy measurements. These show that the spin-orbit splitting at the valence band edge increases linearly with W content from MoS2 to WS2, in agreement with linear-scaling density functional theory (LS-DFT) predictions. The spin-orbit splitting at the conduction band edge is predicted to reduce to zero at intermediate compositions. Despite this, polarisation-resolved photoluminescence spectra on monolayer Mo0.5W0.5S2 show significant circular dichroism, indicating that spin-valley locking is retained. These results demonstrate that alloying is an important tool for controlling the electronic structure of MX2 for spintronic and valleytronic applications.

cond-mat.mes-hall

Observation of topological electronic structure in quasi-1D superconductor TaSe3

Topological superconductors (TSCs), with the capability to host Majorana bound states that can lead to non-Abelian statistics and application in quantum computation, have been one of the most intensively studied topics in condensed matter physics recently. Up to date, only a few compounds have been proposed as candidates of intrinsic TSCs, such as doped topological insulator CuxBi2Se3 and iron-based superconductor FeTe0.55Se0.45. Here, by carrying out synchrotron and laser based angle-resolved photoemission spectroscopy (ARPES), we systematically investigated the electronic structure of a quasi-1D superconductor TaSe3, and identified the nontrivial topological surface states. In addition, our scanning tunneling microscopy (STM) study revealed a clean cleaved surface with a persistent superconducting gap, proving it suitable for further investigation of potential Majorana modes. These results prove TaSe3 as a stoichiometric TSC candidate that is stable and exfoliable, therefore a great platform for the study of rich novel phenomena and application potentials.

cond-mat.mtrl-sci

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

Direct evidence for flat bands in twisted bilayer graphene from nano-ARPES

Transport experiments in twisted bilayer graphene revealed multiple superconducting domes separated by correlated insulating states. These properties are generally associated with strongly correlated states in a flat mini-band of the hexagonal moiré superlattice as it was predicted by band structure calculations. Evidence for such a flat band comes from local tunneling spectroscopy and electronic compressibility measurements, reporting two or more sharp peaks in the density of states that may be associated with closely spaced van Hove singularities. Direct momentum resolved measurements proved difficult though. Here, we combine different imaging techniques and angle resolved photoemission with simultaneous real and momentum space resolution (nano-ARPES) to directly map the band dispersion in twisted bilayer graphene devices near charge neutrality. Our experiments reveal large areas with homogeneous twist angle that support a flat band with spectral weight that is highly localized in momentum space. The flat band is separated from the dispersive Dirac bands which show multiple moiré hybridization gaps. These data establish the salient features of the twisted bilayer graphene band structure.

cond-mat.str-el

Visualizing electrostatic gating effects in two-dimensional heterostructures

The ability to directly observe electronic band structure in modern nanoscale field-effect devices could transform understanding of their physics and function. One could, for example, visualize local changes in the electrical and chemical potentials as a gate voltage is applied. One could also study intriguing physical phenomena such as electrically induced topological transitions and many-body spectral reconstructions. Here we show that submicron angle-resolved photoemission (micro-ARPES) applied to two-dimensional (2D) van der Waals heterostructures affords this ability. In graphene devices, we observe a shift of the chemical potential by 0.6 eV across the Dirac point as a gate voltage is applied. In several 2D semiconductors we see the conduction band edge appear as electrons accumulate, establishing its energy and momentum, and observe significant band-gap renormalization at low densities. We also show that micro-ARPES and optical spectroscopy can be applied to a single device, allowing rigorous study of the relationship between gate-controlled electronic and excitonic properties.

cond-mat.mes-hall

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

VUV Pump and probe of phase separation and oxygen interstitials in La2NiO4+y using spectromicroscopy

While it is known that strongly correlated transition metal oxides described by multi-band Hubbard model show microscopic multiscale phase separation little is known on the possibility to manipulate them with vacuum ultraviolet (VUV) 27 eV lighting. We have investigated the photo-induced effects of VUV illumination of a super-oxygenated La2NiO4+y single crystal by means of scanning photoelectron microscopy. VUV light exposure induces the increase of the density of states (DOS) in the binding energy range around Eb =1.4 eV below EF. The photo-induced states in this energy region have been predicted as due to clustering of oxygen interstitials by band structure calculations for large supercell of La2CuO4.125. We finally show that it possible to generate and manipulate oxygen rich domains by VUV illumination as it was reported for X-ray illumination of La2CuO4+y. This phenomenology is assigned to oxygen-interstitials ordering and clustering by photo-illumination forming segregated domains in the La2NiO4+y surface

cond-mat.str-el

Spin Texture in Type-II Weyl Semimetal WTe2

We determine the band structure and spin texture of WTe2 by spin- and angle-resolved photoemission spectroscopy (SARPES). With the support of first-principles calculations, we reveal the existence of spin polarization of both the Fermi arc surface states and bulk Fermi pockets. Our results support WTe2 to be a type-II Weyl semimetal candidate and provide important information to understand its extremely large and nonsaturating magnetoresistance.

cond-mat.mtrl-sci