arXiv subjects

Lede Xian

Publications and source records attributed to Lede Xian.

At least 37 records · Page 2Linked to original sources

arXiv2021

Ultra-Strong Spin-Orbit Coupling and Topological Moiré Engineering in Twisted ZrS2 Bilayers

We predict that twisted bilayers of 1T-ZrS$_2$ realize a novel and tunable platform to engineer two-dimensional topological quantum phases dominated by strong spin-orbit interactions. At small twist angles, ZrS$_2$ heterostructures give rise to an emergent and twist-controlled moiré Kagomé lattice, combining geometric frustration and strong spin-orbit coupling to give rise to a moiré quantum spin Hall insulator with highly controllable and nearly-dispersionless bands. We devise a generic pseudo-spin theory for group-IV transition metal dichalcogenides that relies on the two-component character of the valence band maximum of the 1T structure at $Γ$, and study the emergence of a robust quantum anomalous Hall phase as well as possible fractional Chern insulating states from strong Coulomb repulsion at fractional fillings of the topological moiré Kagomé bands. Our results establish group-IV transition metal dichalcogenide bilayers as a novel moiré platform to realize strongly-correlated topological phases in a twist-tunable setting.

cond-mat.str-el↗

arXiv2021

Moire flat bands in twisted 2D hexagonal vdW material

Moire superlattices in twisted bilayer graphene (TBG) and its derived structures can host exotic correlated quantum phenomena because the narrow moire flat minibands in those systems effectively enhance the electron-electron interaction. Correlated phenomena are also observed in 2H-transitional metal dichalcogenides moire superlattices. However, the number of moire systems that have been explored in experiments are still very limited. Here we theoretically investigate a series of two-dimensional (2D) twisted bilayer hexagonal materials (TBHMs) beyond TBG at fixed angles of 7.34 and 67.34 degree with 22 2D van der Waals (vdW) layered materials that are commonly studied in experiments. First-principles calculations are employed to systemically study the moire minibands in these systems. We find that flat bands with narrow bandwidth generally exist in these systems. Some of the systems such as twisted bilayer In2Se3, InSe, GaSe, GaS and PtS2 even host ultra-flat bands with bandwidth less than 20 meV even for such large angles, which make them especially appealing for further experimental investigations. We further analysis the characters of moire flat bands and provides guidance for further exploration of 2D moire superlattices that could host strong electron correlations.

cond-mat.mtrl-sci↗

arXiv2021

Engineering Three Dimensional Moiré Flat Bands

We demonstrate that the concept of moiré flat bands can be generalized to achieve electronic band engineering in all three spatial dimensions. For many two dimensional van der Waals materials, twisting two adjacent layers with respect to each other leads to flat electronic bands in the two corresponding spatial directions -- a notion sometimes referred to as twistronics as it enables a wealth of physical phenomena. Within this two dimensional plane, large moiré patterns of nanometer size form. The basic concept we propose here is to stack multiple twisted layers on top of each other in a predefined pattern. If the pattern is chosen such that with respect to the stacking direction of layers, the large spatial moiré features are spatially shifted from one twisted layer to the next, the system exhibits twist angle controlled flat bands in all of the three spatial directions. With this, our proposal extends the use of twistronic to three dimensions. We exemplify the general concept by considering graphitic systems, boron nitride and WSe$_2$ as candidate materials, but the approach is applicable to any two-dimensional van der Waals material. For hexagonal boron nitride we develope an ab initio fitted tight binding model that captures the corresponding three dimensional low-energy electronic structure. We outline that interesting three dimensional correlated phases of matter can be induced and controlled following this route, including quantum magnets and unconventional superconducting states.

cond-mat.mtrl-sci↗

arXiv2021

Spatially indirect intervalley excitons in bilayer WSe2

Spatially indirect excitons with displaced wavefunctions of electrons and holes play a pivotal role in a large portfolio of fascinating physical phenomena and emerging optoelectronic applications, such as valleytronics, exciton spin Hall effect, excitonic integrated circuit and high-temperature superfluidity. Here, we uncover three types of spatially indirect excitons (including their phonon replicas) and their quantum-confined Stark effects in hexagonal boron nitride encapsulated bilayer WSe2, by performing electric field-tunable photoluminescence measurements. Because of different out-of-plane electric dipole moments, the energy order between the three types of spatially indirect excitons can be switched by a vertical electric field. Remarkably, we demonstrate, assisted by first-principles calculations, that the observed spatially indirect excitons in bilayer WSe2 are also momentum-indirect, involving electrons and holes from Q and K/Γ valleys in the Brillouin zone, respectively. This is in contrast to the previously reported spatially indirect excitons with electrons and holes localized in the same valley. Furthermore, we find that the spatially indirect intervalley excitons in bilayer WSe2 can exhibit considerable, doping-sensitive circular polarization. The spatially indirect excitons with momentum-dark nature and highly tunable circular polarization open new avenues for exotic valley physics and technological innovations in photonics and optoelectronics.

cond-mat.mes-hall↗

arXiv2021

Moiré heterostructures as a condensed matter quantum simulator

Twisted van der Waals heterostructures have latterly received prominent attention for their many remarkable experimental properties, and the promise that they hold for realising elusive states of matter in the laboratory. We propose that these systems can, in fact, be used as a robust quantum simulation platform that enables the study of strongly correlated physics and topology in quantum materials. Among the features that make these materials a versatile toolbox are the tunability of their properties through readily accessible external parameters such as gating, straining, packing and twist angle; the feasibility to realize and control a large number of fundamental many-body quantum models relevant in the field of condensed-matter physics; and finally, the availability of experimental readout protocols that directly map their rich phase diagrams in and out of equilibrium. This general framework makes it possible to robustly realize and functionalize new phases of matter in a modular fashion, thus broadening the landscape of accessible physics and holding promise for future technological applications.

quant-ph↗

arXiv2020

Moiré metrology of energy landscapes in van der Waals heterostructures

The emerging field of twistronics, which harnesses the twist angle between two-dimensional materials, represents a promising route for the design of quantum materials, as the twist-angle-induced superlattices offer means to control topology and strong correlations. At the small twist limit, and particularly under strain, as atomic relaxation prevails, the emergent moiré superlattice encodes elusive insights into the local interlayer interaction. Here we introduce moiré metrology as a combined experiment-theory framework to probe the stacking energy landscape of bilayer structures at the 0.1 meV/atom scale, outperforming the gold-standard of quantum chemistry. Through studying the shapes of moiré domains with numerous nano-imaging techniques, and correlating with multi-scale modelling, we assess and refine first-principle models for the interlayer interaction. We document the prowess of moiré metrology for three representative twisted systems: bilayer graphene, double bilayer graphene and H-stacked $MoSe_2/WSe_2$. Moiré metrology establishes sought after experimental benchmarks for interlayer interaction, thus enabling accurate modelling of twisted multilayers.

cond-mat.mes-hall↗

arXiv2020

Universal moiré nematic phase in twisted graphitic systems

Graphene moiré superlattices display electronic flat bands. At integer fillings of these flat bands, energy gaps due to strong electron-electron interactions are generally observed. However, the presence of other correlation-driven phases in twisted graphitic systems at non-integer fillings is unclear. Here, we report scanning tunneling microscopy (STM) measurements that reveal the existence of threefold rotational (C3) symmetry breaking in twisted double bilayer graphene (tDBG). Using spectroscopic imaging over large and uniform areas to characterize the direction and degree of C3 symmetry breaking, we find it to be prominent only at energies corresponding to the flat bands and nearly absent in the remote bands. We demonstrate that the C3 symmetry breaking cannot be explained by heterostrain or the displacement field, and is instead a manifestation of an interaction-driven electronic nematic phase, which emerges even away from integer fillings. Comparing our experimental data with a combination of microscopic and phenomenological modeling, we show that the nematic instability is not associated with the local scale of the graphene lattice, but is an emergent phenomenon at the scale of the moiré lattice, pointing to the universal character of this ordered state in flat band moiré materials.

cond-mat.str-el↗

arXiv2020

Nonlinear twistoptics at symmetry-broken interfaces

Broken symmetries induce strong nonlinear optical responses in materials and at interfaces. Twist angle can give complete control over the presence or lack of inversion symmetry at a crystal interface, and is thus an appealing knob for tuning nonlinear optical systems. In contrast to conventional nonlinear crystals with rigid lattices, the weak interlayer coupling in van der Waals (vdW) heterostructures allows for arbitrary selection of twist angle, making nanomechanical manipulation of fundamental interfacial symmetry possible within a single device. Here we report highly tunable second harmonic generation (SHG) from nanomechanically rotatable stacks of bulk hexagonal boron nitride (BN) crystals, and introduce the term twistoptics to describe studies of optical properties in dynamically twistable vdW systems. We observe SHG intensity modulated by a factor of more than 50, polarization patterns determined by moiré interface symmetry, and enhanced conversion efficiency for bulk crystals by stacking multiple pieces of BN joined by symmetry-broken interfaces. Our study provides a foundation for compact twistoptics architectures aimed at efficient, scalable, and tunable frequency-conversion, and demonstrates SHG as a robust probe of buried vdW interfaces.

cond-mat.mes-hall↗

arXiv2020

Graphene/$α$-RuCl$_3$: An Emergent 2D Plasmonic Interface

Work function-mediated charge transfer in graphene/$α$-RuCl$_3$ heterostructures has been proposed as a strategy for generating highly-doped 2D interfaces. In this geometry, graphene should become sufficiently doped to host surface and edge plasmon-polaritons (SPPs and EPPs, respectively). Characterization of the SPP and EPP behavior as a function of frequency and temperature can be used to simultaneously probe the magnitude of interlayer charge transfer while extracting the optical response of the interfacial doped $α$-RuCl$_3$. We accomplish this using scanning near-field optical microscopy (SNOM) in conjunction with first-principles DFT calculations. This reveals massive interlayer charge transfer (2.7 $\times$ 10$^{13}$ cm$^{-2}$) and enhanced optical conductivity in $α$-RuCl$_3$ as a result of significant electron doping. Our results provide a general strategy for generating highly-doped plasmonic interfaces in the 2D limit in a scanning probe-accessible geometry without need of an electrostatic gate.

cond-mat.mtrl-sci↗

arXiv2020

Realization of Nearly Dispersionless Bands with Strong Orbital Anisotropy from Destructive Interference in Twisted Bilayer MoS2

Recently, the twist angle between adjacent sheets of stacked van der Waals materials emerged as a new knob to engineer correlated states of matter in two-dimensional heterostructures in a controlled manner, giving rise to emergent phenomena such as superconductivity or correlated insulating states. Here,we use an ab initio based approach to characterize the electronic properties of twisted bilayer MoS2. We report that, in marked contrast to twisted bilayer graphene, slightly hole-doped MoS2 realizes a strongly asymmetric px-py Hubbard model on the honeycomb lattice, with two almost entirely dispersionless bands emerging due to destructive interference. We study the collective behavior of twisted bilayer MoS2 in the presence of interactions, and characterize an array of different magnetic and orbitally-ordered correlated phases,which may be susceptible to quantum fluctuations giving rise to exotic, purely quantum, states of matter.

cond-mat.mes-hall↗

arXiv2019

Moiré-less Correlations in ABCA Graphene

Atomically thin van der Waals materials stacked with an interlayer twist have proven to be an excellent platform towards achieving gate-tunable correlated phenomena linked to the formation of flat electronic bands. In this work we demonstrate the formation of emergent correlated phases in multilayer rhombohedral graphene - a simple material that also exhibits a flat electronic band but without the need of having a moiré superlattice induced by twisted van der Waals layers. We show that two layers of bilayer graphene that are twisted by an arbitrary tiny angle host large (micron-scale) regions of uniform rhombohedral four-layer (ABCA) graphene that can be independently studied. Scanning tunneling spectroscopy reveals that ABCA graphene hosts an unprecedentedly sharp flat band of 3-5 meV half-width. We demonstrate that when this flat band straddles the Fermi level, a correlated many-body gap emerges with peak-to-peak value of 9.5 meV at charge neutrality. Mean field theoretical calculations indicate that the two primary candidates for the appearance of this broken symmetry state are a charge transfer excitonic insulator and a ferrimagnet. Finally, we show that ABCA graphene hosts surface topological helical edge states at natural interfaces with ABAB graphene which can be turned on and off with gate voltage, implying that small angle twisted double bilayer graphene is an ideal programmable topological quantum material.

cond-mat.mes-hall↗

arXiv2019

Magic continuum in twisted bilayer WSe2

Emergent quantum phases driven by electronic interactions can manifest in materials with narrowly dispersing, i.e. "flat", energy bands. Recently, flat bands have been realized in a variety of graphene-based heterostructures using the tuning parameters of twist angle, layer stacking and pressure, and resulting in correlated insulator and superconducting states. Here we report the experimental observation of similar correlated phenomena in twisted bilayer tungsten diselenide (tWSe2), a semiconducting transition metal dichalcogenide (TMD). Unlike twisted bilayer graphene where the flat band appears only within a narrow range around a "magic angle", we observe correlated states over a continuum of angles, spanning 4 degree to 5.1 degree. A Mott-like insulator appears at half band filling that can be sensitively tuned with displacement field. Hall measurements supported by ab initio calculations suggest that the strength of the insulator is driven by the density of states at half filling, consistent with a 2D Hubbard model in a regime of moderate interactions. At 5.1 degree twist, we observe evidence of superconductivity upon doping away from half filling, reaching zero resistivity around 3 K. Our results establish twisted bilayer TMDs as a model system to study interaction-driven phenomena in flat bands with dynamically tunable interactions.

cond-mat.mes-hall↗

arXiv2019

Topological Floquet Engineering of Twisted Bilayer Graphene

We investigate the topological properties of Floquet-engineered twisted bilayer graphene above the magic angle driven by circularly polarized laser pulses. Employing a full Moiré-unit-cell tight-binding Hamiltonian based on first-principles electronic structure we show that the band topology in the bilayer, at twisting angles above 1.05$^\circ$, essentially corresponds to the one of single-layer graphene. However, the ability to open topologically trivial gaps in this system by a bias voltage between the layers enables the full topological phase diagram to be explored, which is not possible in single-layer graphene. Circularly polarized light induces a transition to a topologically nontrivial Floquet band structure with the Berry curvature of a Chern insulator. Importantly, the twisting allows for tuning electronic energy scales, which implies that the electronic bandwidth can be tailored to match realistic driving frequencies in the ultraviolet or mid-infrared photon-energy regimes. This implies that Moiré superlattices are an ideal playground for combining twistronics, Floquet engineering, and strongly interacting regimes out of thermal equilibrium.

cond-mat.mtrl-sci↗

arXiv2018

Magic Angle Spectroscopy

The electronic properties of heterostructures of atomically-thin van der Waals (vdW) crystals can be modified substantially by Moiré superlattice potentials arising from an interlayer twist between crystals. Moiré-tuning of the band structure has led to the recent discovery of superconductivity and correlated insulating phases in twisted bilayer graphene (TBLG) near the so-called "magic angle" of $\sim$1.1°, with a phase diagram reminiscent of high T$_c$ superconductors. However, lack of detailed understanding of the electronic spectrum and the atomic-scale influence of the Moiré pattern has so far precluded a coherent theoretical understanding of the correlated states. Here, we directly map the atomic-scale structural and electronic properties of TBLG near the magic angle using scanning tunneling microscopy and spectroscopy (STM/STS). We observe two distinct van Hove singularities (vHs) in the LDOS which decrease in separation monotonically through 1.1° with the bandwidth (t) of each vHs minimized near the magic angle. When doped near half Moiré band filling, the conduction vHs shifts to the Fermi level and an additional correlation-induced gap splits the vHs with a maximum size of 7.5 meV. We also find that three-fold (C$_3$) rotational symmetry of the LDOS is broken in doped TBLG with a maximum symmetry breaking observed for states near the Fermi level, suggestive of nematic electronic interactions. The main features of our doping and angle dependent spectroscopy are captured by a tight-binding model with on-site (U) and nearest neighbor Coulomb interactions. We find that the ratio U/t is of order unity, indicating that electron correlations are significant in magic angle TBLG. Rather than a simple maximization of the DOS, superconductivity arises in TBLG at angles where the ratio U/t is largest, suggesting a pairing mechanism based on electron-electron interactions.

cond-mat.mes-hall↗

arXiv2018

Multi-flat bands and strong correlations in Twisted Bilayer Boron Nitride

In a groundbreaking experimental advance it was recently shown that by stacking two sheets of graphene atop of each other at a twist angle close to one of the so called "magic angles", an effective two-dimensional correlated system emerges. In this system the kinetic energy of the low-energy electrons is much reduced and consequently interactions become very relevant, providing a new platform into the physics of two-dimensional correlated materials. Evidence of a proposed Mott insulating as well as superconducting state in these highly tunable systems has spurred much attention as they could pave the way to understanding long-standing questions of high-$T_c$ superconductivity or provide candidate systems for topological chiral superconductors; key to highly relevant quantum technologies. Here, we demonstrate that twisted bilayer boron nitride (TBBN) is an exciting and even richer alternative to twisted bilayer graphene (TBG). Crucially, we show that in TBBN multiple flat bands emerge without having to fine tuning close to a "magic angle" that upon doping lead to correlated phases of matter (insulating and superconducting). TBBN could thus be much less sensitive to small deviations in the twist angle and therefore provide a particularly suited experimental platform to study correlation physics in two dimensions. Furthermore, we find that in marked contrast to TBG at small twist angle families of 2,4 and 6-fold degenerate, well separated, bands emerge within the gap, considerably broadening the addressable physics.

cond-mat.mes-hall↗

arXiv2016

Square selenene and tellurene: novel group VI elemental 2D semi-Dirac materials and topological insulators

With first principles calculations, we predict a novel stable 2D layered structure for group VI elements Se and Te that we call square selenene and square tellurene, respectively. They have chair-like buckled structures similar to other layered materials such as silicene and germanene but with a square unit cell rather than hexagonal. This special structure gives rise to anisotropic band dispersions near the Fermi level that can be described by a generalized semi-Dirac Hamiltonian. We show that the considerably large band gap ($\sim$0.1 eV) opened by spin-orbit coupling makes square selenene and tellurene topological insulators, hosting non-trivial edge states. Therefore, square selenene and tellurene are promising materials for novel electronic and spintronic applications. Finally, we show that this new type of 2D elemental material can potentially be grown on proper substrates, such as a Au(100) surface.

cond-mat.mes-hall↗

arXiv2014

Instantaneous band gap collapse in photoexcited monoclinic VO$_2$ due to photocarrier doping

Using femtosecond time-resolved photoelectron spectroscopy we demonstrate that photoexcitation transforms monoclinic VO$_2$ quasi-instantaneously into a metal. Thereby, we exclude an 80 femtosecond structural bottleneck for the photoinduced electronic phase transition of VO$_2$. First-principles many-body perturbation theory calculations reveal a high sensitivity of the VO$_2$ bandgap to variations of the dynamically screened Coulomb interaction, supporting a fully electronically driven isostructral insulator-to-metal transition. We thus conclude that the ultrafast band structure renormalization is caused by photoexcitation of carriers from localized V 3d valence states, strongly changing the screening \emph{before} significant hot-carrier relaxation or ionic motion has occurred.

cond-mat.str-el↗

arXiv2014

The atomic structure of the $\sqrt{3} \times \sqrt{3}$ phase of silicene on Ag(111)

The growth of the $\sqrt{3} \times \sqrt{3}$ reconstructed silicene on Ag substrate has been frequently observed in experiments while its atomic structure and formation mechanism is poorly understood. Here by first-principles calculations we show that $\sqrt{3} \times \sqrt{3}$ reconstructed silicene is constituted by dumbbell units of Si atoms arranged in a honeycomb pattern. Our model shows excellent agreement with the experimentally reported lattice constant and STM image. We propose a new mechanism for explaining the spontaneous and consequential formation of $\sqrt{3} \times \sqrt{3}$ structures from $3 \times 3$ structures on Ag substrate. We show that the $\sqrt{3} \times \sqrt{3}$ reconstruction is mainly determined by the interaction between Si atoms and have weak influence from Ag substrate. The proposed mechanism opens the path to understanding of multilayer silicon.

cond-mat.mes-hall↗