As machine learning becomes increasingly important in engineering and science, it is inevitable that machine learning techniques will be applied to the investigation of materials, and in particular the structural phase transitions common in ferroelectric materials. Here, we build and train an artificial neural network to accurately predict the energy change associated with atom displacements and use the trained artificial neural network in Monte-Carlo simulations on ferroelectric materials to investigate their phase transitions. We apply this approach to two-dimensional monolayer SnTe and show that it can indeed be used to simulate the phase transitions and predict the transition temperature. The artificial neural network, when viewed as a universal mathematical structure, can be readily transferred to the investigation of other ferroelectric materials when training data generated with ab initio methods are available.
2H phase (trigonal prismatic D3h) of layered two-dimensional (2D) transition metal dichalcogenides (TMDs) have attracted a lot of interests due to the superior electronic and optoelectronic properties. However, flexible electronic devices and thermoelectric performances based on 2H phase have been potentially limited by the strain sensitive electronic band gap and high lattice thermal conductivity (kappa_L). Here, we predict and calculate two 1T (octahedral Oh) phase monolayer telluride materials SnTe2 and SiTe2 with soft mechanics, ultralow kappa_L and electronic properties. The calculated in…
The realization of multiferroicity in 2D nanomaterials is crucially important for designing advanced nanoelectronic devices such as non-volatile multistate data storage. In this work, the coexistence of ferromagnetism and ferroelectricity is reported in monolayer SnTe system by transition metal (TM) doping. Based on first-principles calculations, the spontaneous spin polarization could be realized by TM doping in ferroelectric SnTe monolayer. In addition to in-plane ferroelectric polarization, the out-of-plane ferroelectric polarization emerges in Mn (Fe)-doped SnTe monolayer due to the intern…
The bulk photovoltaic effect (BPVE) refers to the phenomenon of generating photocurrent or photovoltage in homogeneous noncentrosymmetric materials under illumination, and the intrinsic contribution to the BPVE is known as the shift current effect. We calculate the shift current conductivities of the ferroelectric SnTe monolayer using first-principles methods. We find that the monolayer SnTe has giant shift-current conductivity near the valley points. More remarkably, the linear optical absorption coefficient at this energy is very small, and therefore leads to an enormous Glass coefficient th…
It is desirable to realize topological phases in artificial structures by engineering electronic band structures. In this paper, we investigate $(PbTe)_m(SnTe)_{2n-m}$ superlattices along [001] direction and find a robust weak topological insulator phase for a large variety of layer numbers m and 2n-m. We confirm this topologically non-trivial phase by calculating Z2 topological invariants and topological surface states based on the first-principles calculations. We show that the folding of Brillouin zone due to the superlattice structure plays an essential role in inducing topologically non-t…
We envision that quantum spin Hall effect should be observed in $(111)$-oriented thin films of SnSe and SnTe topological crystalline insulators. Using a tight-binding approach supported by first-principles calculations of the band structures we demonstrate that in these films the energy gaps in the two-dimensional band spectrum depend in an oscillatory fashion on the layer thickness. These results as well as the calculated topological invariant indexes and edge state spin polarizations show that for films ~20-40 monolayers thick a two-dimensional topological insulator phase appears. In this ra…
Two-dimensional (2D) topological crystalline insulators (TCIs) were recently predicted in thin films of the SnTe class of IV-VI semiconductors, which can host metallic edge states protected by mirror symmetry. As thickness decreases, quantum confinement effect will increase and surpass the inverted gap below a critical thickness, turning TCIs into normal insulators. Surprisingly, based on first-principles calculations, here we demonstrate that (001) monolayers of rocksalt IV-VI semiconductors XY (X=Ge, Sn, Pb and Y= S, Se, Te) are 2D TCIs with the fundamental band gap as large as 260 meV in mo…
Twelve two-dimensional group-IV monochalcogenide monolayers (SiS, SiSe, SiTe, GeS, GeSe, GeTe, SnS, SnSe, SnTe, PbS, PbSe, and PbTe) with a buckled honeycomb atomistic structure--belonging to symmetry group P3m1--and an out-of-plane intrinsic electric polarization are shown to be metastable by three independendent methods. First, we uncover a coordination-preserving structural transformation from the low-buckled honeycomb structure onto the lower-energy Pnm2$_1$ (or Pmmn for PbS, PbSe, and PbTe) phase to estimate {\em energy barriers} $E_B$ that must be overcome during such structural transfor…
We perform systematic investigation on the geometric, energetic and electronic properties of group IV-VI binary monolayers (XY), which are the counterparts of phosphorene, by employing density functional theory based electronic structure calculations. For this purpose, we choose the binary systems XY consisting of equal numbers of group IV (X = C, Si, Ge, Sn) and group VI elements (Y = O, S, Se, Te) in three geometrical configurations, the puckered, buckled and planar structures. The results of binding energy calculations show that all the binary systems studied are energetically stable. It is…
We derive and validate a quantitative analytical model of the near-field electrostatic effects in the vicinity (>=3Å) of two-dimensional (2D) materials. In solving the Poisson equation of a near-planar point charge ansatz for the electronic density of a 2D material, our formula quantitatively captures the out-of-plane decay and the in-plane modulation of density functional theory (DFT)-calculated potentials. We provide a method for quickly constructing the electronic density ansatz, and apply it to the case of hexagonal monolayers (BN, AlN, GaN) and monochalcogenides (GeS, GeSe, GeTe, SnS, SnS…
Since the discovery of graphene, two-dimensional materials with atomic level thickness have rapidly grown to be a prosperous field of physical science with interdisciplinary interests, for their fascinating properties and broad applications. Very recently, the experimental observation of ferromagnetism in Cr$_2$Ge$_2$Te$_6$ bilayer and CrI$_3$ monolayer opened a door to pursuit long-absent intrinsic magnetic orders in two-dimensional materials. Meanwhile, the ferroelectricity was also experimentally found in SnTe monolayer and CuInP$_2$S$_6$ few layers. The emergence of these ferroic orders in…
Doping is an effective way to modify the electronic property of two-dimensional (2D) materials and endow them with new functionalities. However, wide-range control of the substitutional doping concentration with large scale uniformity remains challenging in 2D materials. Here we report in-situ chemical vapor deposition growth of vanadium (V) doped monolayer molybdenum disulfide (MoS2) with widely tunable doping concentrations ranging from 0.3 to 13.1 at%. The key to regulate the doping concentration lies in the use of appropriate V precursors with different doping abilities, which also generat…
We theoretically investigate detuning-dependent properties of high-order harmonic generation (HHG) in monolayer transition metal dichalcogenides (TMDCs). In contrast to HHG in conventional materials, TMDCs show both parallel and perpendicular emissions with respect to the incident electric field. We find that such an anomalous emission can be artificially controlled by the frequency detuning of the incident electric fields, i.e., the parallel and perpendicular HHG can be strongly enhanced by multiphoton resonances. This peculiar phenomenon would provide a way for controlling HHG in TMDCs and s…
Displacive martensitic phase transition is potentially promising in semiconductor based data storage applications with fast switching speed. In addition to traditional phase transition materials, the recently discovered two-dimensional ferroic materials are receiving lots of attention owing to their fast ferroic switching dynamics, which could tremendously boost data storage density and enhance read/write speed. In this study, we propose that a terahertz laser with an intermediate intensity and selected frequency can trigger ferroic order switching in two-dimensional multiferroics, which is a …
Two-dimensional (2D) van der Waals ferroelectrics provide an unprecedented architectural freedom for the creation of artificial multiferroics and non-volatile electronic devices based on vertical and co-planar heterojunctions of 2D ferroic materials. Nevertheless, controlled microscopic manipulation of ferroelectric domains is still rare in monolayer-thick 2D ferroelectrics with in-plane polarization. Here we report the discovery of robust ferroelectricity with a critical temperature close to 400 K in SnSe monolayer plates grown on graphene, and the demonstration of controlled room temperature…
Strong spin-orbit coupling and inversion symmetry breaking in transition metal dichalcogenide monolayers yield the intriguing effects of valley-dependent optical selection rules. As such, it is possible to substantially polarize valley excitons with chiral light and furthermore create coherent superpositions of K and K- polarized states. Yet, at ambient conditions dephasing usually becomes too dominant, and valley coherence typically is not observable. Here, we demonstrate that valley coherence is, however, clearly observable for a single monolayer of WSe2, if it is strongly coupled to the opt…
Janus transition-metal dichalcogenide monolayers are fully artificial materials, where one plane of chalcogen atoms is replaced by chalcogen atoms of a different type. Theory predicts an in-built out-of-plane electric field, giving rise to long-lived, dipolar excitons, while preserving direct-bandgap optical transitions in a uniform potential landscape. Previous Janus studies had broad photoluminescence (>15 meV) spectra obfuscating their excitonic origin. Here, we identify the neutral, and negatively charged inter- and intravalley exciton transitions in Janus WSeS monolayer with $\sim 6$ meV …
Multiferroic materials with coupled ferroelectric and ferromagnetic properties are important for multifunctional devices due to their potential ability of controlling magnetism via electric field, and vice versa. The recent discoveries of two-dimensional ferromagnetic and ferroelectric materials have ignited tremendous research interest and aroused hope to search for two-dimensional multiferroics. However, intrinsic two-dimensional multiferroic materials and, particularly, those with strong magnetoelectric couplings are still rare to date. In this paper, using first-principles simulations, we …
Hexagonal Si2Te2 monolayers (ML-Si2Te2) were predicted to show strain-dependent band-crossover between semiconducting and room-temperature quantum spin Hall phases. However, investigations on this artificial two-dimensional (2D) material have mainly been restricted to theoretical calculations because its bulk counterpart does not exist naturally. Here, we report on the successful epitaxial growth of ML-Si2Te2 films on Sb2Te3 thin film substrates. High-quality (1*1) ML-Si2Te2 films with a coverage as high as 95% were obtained as revealed by scanning tunneling microscopy. X-ray photoelectron spe…
The bilayer heterostructures composed of an ultrathin ferromagnetic metal (FM) and a material hosting strong spin-orbit (SO) coupling are principal resource for SO torque and spin-to-charge conversion nonequilibrium effects in spintronics. We demonstrate how hybridization of wavefunctions of Co layer and a monolayer of transition metal dichalcogenides (TMDs)---such as semiconducting MoSe$_2$ and WSe$_2$ or metallic TaSe$_2$---can lead to dramatic transmutation of electronic and spin structure of Co within some distance away from its interface with TMD, when compared to the bulk of Co or its su…
The rise of quantum science and technologies motivates photonics research to seek new platforms with strong light-matter interactions to facilitate quantum behaviors at moderate light intensities. One promising platform to reach such strong light-matter interacting regimes is offered by polaritonic metasurfaces, which represent ultrathin artificial media structured on nano-scale and designed to support polaritons - half-light half-matter quasiparticles. Topological polaritons, or 'topolaritons', offer an ideal platform in this context, with unique properties stemming from topological phases of…
Hyperbolic materials are of particular interest for the next generation of photonic and optoelectronic devices. Since artificial metamaterials are intrinsically limited by the size of their nanostructured components, there has been a hunt for natural hyperbolic materials in the last few years. In a first-principles work based on density-functional theory and many-body perturbation theory, we investigate the fundamental dielectric response of MoTe2 in monolayer, bilayer, and bulk form, and find that it is a natural type-II hyperbolic material with low losses between 3 and 6 eV. Going from the m…
Two-dimensional (2D) materials have been a hot research topic in the last decade, due to novel fundamental physics in the reduced dimension and appealing applications. Systematic discovery of functional 2D materials has been the focus of many studies. Here, we present a large dataset of 2D materials, with more than 6,000 monolayer structures, obtained from both top-down and bottom-up discovery procedures. First, we screened all bulk materials in the database of Materials Project for layered structures by a topology-based algorithm, and theoretically exfoliate them into monolayers. Then, we gen…
Programmable, Spontaneous Superlattice Memory in a Monolayer Topological Insulator
Boston College（波士顿学院）；Emory University（埃默里大学）；University of Tennessee, Knoxville（田纳西大学诺克斯维尔分校）；Max Planck Institute for Chemical Physics of Solids（马克斯·普朗克固体化学物理研究所）；Columbia University（哥伦比亚大学）；University of California Los Angeles（加州大学洛杉矶分校）；Harvard University（哈佛大学）
Two-dimensional materials can be crafted with structural precision approaching the atomic scale, enabling quantum defects-by-design. These defects are frequently described as artificial atoms and are emerging optically-addressable spin qubits. However, interactions and coupling of such artificial atoms with each other, in the presence of the lattice, is remarkably underexplored. Here we present the formation of artificial molecules in solids, introducing a new degree of freedom in control of quantum optoelectronic materials. Specifically, in monolayer hexagonal boron nitride as our model syste…
The two-dimensional (2D) semiconductor indium selenide (InSe) has attracted significant interest due its unique electronic band structure, high electron mobility and wide tunability of its band gap energy achieved by varying the layer thickness. All these features make 2D InSe a potential candidate for advanced electronic and optoelectronic applications. Here, we report on the discovery of new polymorphs of InSe with enhanced electronic properties. Using a global structure search that combines artificial swarm intelligence with first-principles energetic calculations, we identify polymorphs th…
Van der Waals (vdW) solids, as a new type of artificial materials that consist of alternating layers bonded by weak interactions, have shed light on fascinating optoelectronic device concepts. As a result, a large variety of vdW devices have been engineered via layer-by-layer stacking of two-dimensional materials, although shadowed by the difficulties of fabrication. Alternatively, direct growth of vdW solids has proven as a scalable and swift way, highlighted by the successful synthesis of graphene/h-BN and transition metal dichalcogenides (TMDs) vertical heterostructures from controlled vapo…
Heterostructures of atomically thin van der Waals bonded monolayers have opened a unique platform to engineer Coulomb correlations, shaping excitonic, Mott insulating, or superconducting phases. In transition metal dichalcogenide heterostructures, electrons and holes residing in different monolayers can bind into spatially indirect excitons with a strong potential for optoelectronics, valleytronics, Bose condensation, superfluidity, and moiré-induced nanodot lattices. Yet these ideas require a microscopic understanding of the formation, dissociation, and thermalization dynamics of correlations…
Two-dimensional van der Waals crystals arise limitless scope for designing novel combinations of physical properties via controlling the stacking order or twist angle of individual layers. Lattice orientation between stacked monolayers is significant not only for the engineering symmetry breaking but also for the study of many-body quantum phases and band topology. So far the state-of-art exfoliation approaches focusing on achievements of quality, size, yield, and scalability while lacking sufficient information on lattice orientation. Consequently, interlayer alignment is usually determined b…
Recently, a new class of second-order topological insulators (SOTIs) characterized by an electronic dipole has been theoretically introduced and proposed to host topological corner states. As a novel topological state, it has been attracting great interest and experimentally realized in artificial systems of various fields of physics based on multi-sublattice models, e.g., breathing kagome lattice. In order to realize such kind of SOTI in natural materials, we proposed a symmetry-faithful multi-orbital model. Then, we reveal several familiar transition metal dichalcogenide (TMD) monolayers as …
Twisted 2D bilayer materials are created by artificial stacking of two monolayer crystal networks of 2D materials with a desired twisting angle $θ$. The material forms a moiré superlattice due to the periodicity of both top and bottom layer crystal structure. The optical properties are modified by lattice reconstruction and phonon renormalization, which makes optical spectroscopy an ideal characterization tool to study novel physics phenomena. Here, we report a Raman investigation on a full period of the twisted bilayer (tB) WSe$_2$ moiré superlattice (\textit i.e. 0° $\leq θ\leq$ 60°). We obs…
Materials with reduced dimensions have been shown to host a wide variety of exotic properties and novel quantum states that often defy textbook wisdom1-5. Ferroelectric polarization and metallicity are well-known examples of mutually exclusive properties that cannot coexist in bulk solids because the net electric field in a metal can be fully screened by free electrons6. An atomically thin metallic layer capped by insulating layers has shown decent conductivity at room temperature7. Moreover, a penetrating polarization field can be employed to induce an ion displacement and create an intrinsic…
Two-dimensional (2D) heterostructures (HS) formed by transition-metal dichalcogenide (TMDC) monolayers offer a unique platform for the study of intralayer and interlayer excitons as well as moiré-pattern-induced features. Particularly, the dipolar charge-transfer exciton comprising an electron and a hole, which are confined to separate layers of 2D semiconductors and Coulomb-bound across the heterojunction interface, has drawn considerable attention in the research community. On the one hand, it bears significance for optoelectronic devices, e.g. in terms of charge carrier extraction from phot…
\textit{Ab initio} calculations of electron-phonon interactions including the polar Fröhlich coupling have advanced considerably in recent years. The Fröhlich electron-phonon matrix element is by now well understood in the case of bulk three-dimensional (3D) materials. In the case of two-dimensional (2D) materials, the standard procedure to include Fröhlich coupling is to employ Coulomb truncation, so as to eliminate artificial interactions between periodic images of the 2D layer. While these techniques are well established, the transition of the Fröhlich coupling from three to two dimensions …
