Two-dimensional materials are emerging as a promising platform for ultrathin channels in field-effect transistors. To this aim, novel high-mobility semiconductors need to be found or engineered. While extrinsic mechanisms can in general be minimized by improving fabrication processes, the suppression of intrinsic scattering (driven e.g. by electron-phonon interactions) requires to modify the electronic or vibrational properties of the material. Since intervalley scattering critically affects mobilities, a powerful approach to enhance transport performance relies on engineering the valley structure. We show here the power of this strategy using uniaxial strain to lift degeneracies and suppress scattering into entire valleys, dramatically improving performance. This is shown in detail for arsenene, where a 2% strain stops scattering into 4 of the 6 valleys, and leads to a 600% increase in mobility. The mechanism is general and can be applied to many other materials, including in particular the isostructural antimonene and blue phosphorene.
Through first-principles calculations, the phonon-limited transport properties of cubic boron-V compounds (BP, BAs and BSb) are studied. We find that the high optical phonon frequency in these compounds leads to the substantial suppression of polar scattering and the reduction of inter-valley transition mediated by large-wavevector optical phonons, both of which significantly facilitate charge transport. We also discover that BAs simultaneously has a high hole mobility (2110 cm2/V-s) and electron mobility (1400 cm2/V-s) at room temperature, which is rare in semiconductors. Our findings present…
The two inequivalent valleys in graphene preclude the protection against inter-valley scattering offered by an odd-number of Dirac cones characteristic of Z2 topological insulator phases. Here we propose a way to engineer a chiral single-valley metallic phase with quadratic crossover in a honeycomb lattice through tailored \sqrt{3}N *\sqrt{3}N or 3N *3N superlattices. The possibility of tuning valley-polarization via pseudo-Zeeman field and the emergence of Dresselhaus-type valley-orbit coupling are proposed in adatom decorated graphene superlattices. Such valley manipulation mechanisms and me…
Electron-hole liquids(EHLs), a correlated state of matter and a thermodynamic liquid, have recently been found to exist at room temperature in suspended monolayers of MoS2. Appreciably higher rates of radiative recombination inside the liquid as compared to free excitons hold promise for optoelectronic applications such as broadband lasing. In this paper, we show that leveraging the valley physics in MoS2 may be a route towards achieving tunability of specific characteristics of an EHL, such as emission wavelength, linewidth, and most importantly, the liquid density. The conditions under which…
Complex electronic band structures, with multiple valleys or bands at the same or similar energies can be beneficial for thermoelectric performance, but the advantages can be offset by inter-valley and inter-band scattering. In this paper, we demonstrate how first-principles band structures coupled with recently developed techniques for rigorous simulation of electron-phonon scattering provide the capabilities to realistically assess the benefits and trade-offs associated with these materials. We illustrate the approach using n-type silicon as a model material and show that intervalley scatter…
Material defects remain as the main bottleneck to the progress of topological insulators (TIs). In particular, efforts to achieve thin TI samples with dominant surface transport have always led to increased defects and degraded mobilities, thus making it difficult to probe the quantum regime of the topological surface states. Here, by utilizing a novel buffer layer scheme composed of an In2Se3/(Bi0.5In0.5)2Se3 heterostructure, we introduce a quantum generation of Bi2Se3 films with an order of magnitude enhanced mobilities than before. This scheme has led to the first observation of the quantum…
Engineering topological flat bands in $Γ$-valley moiré systems with Ising-type SOC: twisted 1T-ZrS$_2$ and 1T-SnSe$_2$
Donostia International Physics Center (DIPC)（多诺西亚国际物理中心）；Department of Physics, University of Texas at Dallas（德克萨斯大学达拉斯分校物理系）；Princeton Center for Theoretical Science, Princeton University（普林斯顿大学理论科学中心）；Department of Physics, Princeton University（普林斯顿大学物理系）；Department of Physics, University of Science and Technology of China（中国科学技术大学物理系）；Rudolf Peierls Centre for Theoretical Physics, University of Oxford（牛津大学鲁道夫·派尔斯理论物理中心）；School of Applied and Engineering Physics, Cornell University（康奈尔大学应用与工程物理学院）；Department of Physics, Cornell University（康奈尔大学物理系）；Kavli Institute at Cornell for Nanoscale Science（康奈尔纳米科学卡弗里研究所）；Max Planck Institute for the Structure and Dynamics of Matter（马克斯·普朗克物质结构与动力学研究所）
Janus two-dimensional (2D) materials have attracted much attention due to possessing unique properties caused by their out-of-plane asymmetry, which have been achieved in many 2D families. In this work, the Janus monolayers are predicted in new 2D $\mathrm{MA_2Z_4}$ family by means of first-principles calculations, $\mathrm{MoSi_2N_4}$ and $\mathrm{WSi_2N_4}$ of which have been synthesized in experiment(\textcolor[rgb]{0.00,0.00,1.00}{Science 369, 670-674 (2020)}). The predicted $\mathrm{MSiGeN_4}$ (M=Mo and W) monolayers exhibit dynamic, thermodynamical and mechanical stability, and they are …
The integration of magnetic material with semiconductors has been fertile ground for fundamental science as well as of great practical interest toward the seamless integration of information processing and storage. Here we create van der Waals heterostructures formed by an ultrathin ferromagnetic semiconductor CrI3 and a monolayer of WSe2. We observe unprecedented control of the spin and valley pseudospin in WSe2, where we detect a large magnetic exchange field of nearly 13 T and rapid switching of the WSe2 valley splitting and polarization via flipping of the CrI3 magnetization. The WSe2 phot…
Transition metal dichalcogenide (TMDC) monolayers are newly discovered semiconductors for a wide range of applications in electronics and optoelectronics. Most studies have focused on binary monolayers that share common properties: direct optical bandgap, spin-orbit (SO) splittings of hundreds of meV, light-matter interaction dominated by robust excitons and coupled spin-valley states of electrons. Studies on alloy-based monolayers are more recent, yet they may not only extend the possibilities for TMDC applications through specific engineering but also help understanding the differences betwe…
Electron valleys in transition-metal dichalcogenide monolayers drive novel physics and allow designing multifunctional architectures for applications. We propose to manipulate the electron valleys in these systems for spin/valley filter and valve devices through band engineering. Instead of the magnetic proximity effect that has been extensively used in previous studies, in our strategy, the electron valleys are directly coupled to the spin-polarized states of the two-dimensional ferromagnets. We find that this coupling results in a valley-selective gap opening due to the spin-momentum locking…
Valley-related multiple Hall effect in two-dimensional lattice is of notable interest both for its fundamental physics and for its potential applications. In this work, by means of a low energy kp model analysis, a mechanism of producing valley-related multiple Hall effect in hexagonal lattice via strain engineering is proposed, and a general picture of valley-contrasted band inversion is developed. Through first-principles calculations, this mechanism is further established in a ferromagnetic hexagonal lattice of single-layer ScI2. Single-layer ScI2 prefers in-plane magnetization and exhibits…
Our study highlights spin-polarization mechanisms in metals, by focusing on the mobilities of conducting electrons with different spins instead of their quantities. Here, we engineer electron mobility by applying chemical disorder induced by non-stoichiometric variations. As a practical example, we discuss the scheme that establishes such variations in tetragonal Mn3Ga Heusler material. We justify this approach using first-principles calculations of the spin-projected conductivity components based on the Kubo-Greenwood formalism. It follows that, in majority of the cases, even a small substitu…
Valley-Landscape Engineering in Bilayer WSe$_2$ Gate-All-Around Transistors
Research Center for Materials Nanoarchitectonics (MANA), National Institute for Materials Science (NIMS)（物质·材料纳米构筑研究中心，日本国立材料研究所）；Kwansei Gakuin University（关西学院大学）
The valley degree of freedom of electrons in materials promises routes toward energy-efficient information storage with enticing prospects towards quantum information processing. Current challenges in utilizing valley polarization are symmetry conditions that require monolayer structures or specific material engineering, non-resonant optical control to avoid energy dissipation, and the ability to switch valley polarization at optical speed. We demonstrate all-optical and non-resonant control over valley polarization using bulk MoS$_2$, a centrosymmetric material with zero Berry curvature at th…
We report on a study of magnetotransport in LaAlO3/SrTiO3 interfaces characterized by mobilities of the order of several thousands cm$^{2}$/Vs. We observe Shubnikov-de Haas oscillations that indicate a two-dimensional character of the Fermi surface. The frequency of the oscillations signals a multiple sub-bands occupation in the quantum well or a multiple valley configuration. From the temperature dependence of the oscillation amplitude we extract an effective carrier mass $m^{*}\simeq1.45$\,$m_{e}$. An electric field applied in the back-gate geometry increases the mobility, the carrier densit…
Alloyed transition metal dichalcogenides provide an opportunity for coupling band engineering with valleytronic phenomena in an atomically-thin platform. However, valley properties in alloys remain largely unexplored. We investigate the valley degree of freedom in monolayer alloys of the phase change candidate material WSe$_{2(1-x)}$Te$_{2x}$. Low temperature Raman measurements track the alloy-induced transition from the semiconducting 1H phase of WSe$_2$ to the semimetallic 1T$_d$ phase of WTe$_2$. We correlate these observations with density functional theory calculations and identify new Ra…
Motivated by the recently synthesized layered material MoSi2N4, we investigated excitonic response of quasiparticle of monolayer MoSi2N4 by using G0W0 and Bethe-Salpeter equation (BSE) calculations. With a dually sandwiched structure consisting of a central MoN2 layer analogue of 2H-MoS2 capped with silicon-nitrogen (SiN) honeycomb outer layers, MoSi2N4 possesses frontier orbitals confined at the central MoN2 layer with similar sub-valley at K-point as 2H-MoS2. The valley splitting (~130 meV) due to the spin-orbital coupling (SOC) gives rise to a doublet in the spectrum. Excitons in MoSi2N4 sh…
In this paper, spin properties of monolayer MX (M=Ga, In and X=S, Se, Te) in the presence of strain are studied. Density functional theory is used to investigate spin properties. The strain changes modification of bandgap due to spin-orbit coupling, the results indicate the spin-orbit coupling has a higher effect in the compressive regime. Also, spin splitting in the conduction and valence bands respect to strain are compared for six materials. The location of conduction band minimum (CBM) imposed a type of spin properties. These materials with mirror symmetry can display the Rashba effect whi…
We propose a general and tunable platform to realize high-density arrays of quantum spin-valley Hall kink (QSVHK) states with spin-valley-momentum locking based on a two-dimensional hexagonal topological insulator. Through the analysis of Berry curvature and topological charge, the QSVHK states are found to be topologically protected by the valley-inversion and time-reversal symmetries. Remarkably, the conductance of QSVHK states remains quantized against either nonmagnetic or long-range magnetic disorder, verified by the Green function calculations. Based on first-principles results, we show …
Breaking space-time symmetries in two-dimensional crystals (2D) can dramatically influence their macroscopic electronic properties. Monolayer transition-metal dichalcogenides (TMDs) are prime examples where the intrinsically broken crystal inversion symmetry permits the generation of valley-selective electron populations, even though the two valleys are energetically degenerate, locked by time-reversal symmetry. Lifting the valley degeneracy in these materials is of great interest because it would allow for valley-specific band engineering and offer additional control in valleytronic applicati…
Topological materials with both insulating and semimetal phases can be protected by crystalline (e.g. mirror) symmetry. The insulating phase, called topological crystalline insulator (TCI), has been intensively investigated and observed in three-dimensional materials. However, the predicted two-dimensional (2D) materials with TCI phase are explored much less than 3D TCIs and 2D topological insulator, while so far considered 2D TCIs almost exclusively possess a square lattice structure with the mirror Chern number $\mathcal C_{M} =-2$. Here, we predict theoretically that hexagonal monolayer of …
Layered hexagonal Gamma--GeSe, a new polymorph of GeSe synthesized recently, shows strikingly high electronic conductivity in its bulk form (even higher than graphite) while semiconducting in the case of monolayer (1L). In this work, by using first-principles calculations, we demonstrate that, different from its orthorhombic phases of GeSe, the Gamma--GeSe shows a small spatial anisotropic dependence and a strikingly thickness-dependent behavior with transition from semimetal (bulk, 0.04 eV) to semiconductor (1L, 0.99 eV), and this dual conducting characteristic realized simply with thickness …
The discovery of double perovskites A2B(I)B(III)X6 (A=monovalent cation; B(I)/B(III) = metal cation; X = halogen) as Pb(II)-free alternatives has attracted widespread attention, making it possible to introduce d-block metal cations (e.g., d0 and d10) into halide perovskites. However, at present, there are quite limited insights into the underlying bonding orbitals for d-block metal cation-based halide perovskites. Here, we present an orbital engineering strategy to construct two-dimensional (2D) electronic structures in three-dimensional (3D) halide perovskites by rationally controlling the d …
Spatially varying strained graphene can acquire interesting electronic properties because of the strain-induced valley-dependent gauge (pseudomagnetic) fields1,2. Here we report the realization of strained graphene regions located close to the step edges of Cu(111), obtained by using thermal strain engineering3,4. We study these strained structures with sub-nanometre-resolved scanning tunnelling microscopy and spectroscopy and identify their spatially modulated Dirac points, demonstrating the effect of overlap of Cu and graphene wave functions on the charge transfer between them5. By applying …
We investigate the electronic and vibrational spectra of SrTiO$_3$, as well as the coupling between them, using first-principles calculations. We compute electron-phonon scattering rates for the three lowest-energy conduction bands and use Boltzmann transport theory to calculate the room-temperature mobility of SrTiO$_3$. The results agree with experiment and highlight the strong impact of longitudinal optical phonon scattering. Our analysis provides important insights into the key factors that determine room temperature mobility, such as the number of conduction bands and the nature and frequ…
Thermal engineering of quantum devices has attracted much attention since the discovery of quantized thermal conductance of phonons. Although easily submerged in numerous excitations in macro-systems, quantum behaviors of phonons manifest in nanoscale low-dimensional systems even at room temperature. Especially in nano transport devices, phonons move quasi-ballistically when the transport length is smaller than their bulk mean free paths. It has been shown that phonon nonequilibrium Green's function method (NEGF) is effective for the investigation of nanoscale quantum transport of phonons. In …
Topological properties of electronic states in multivalley two-dimensional materials, such as mono- and bilayer graphene, or thin films of rhombohedral graphite, give rise to various unusual magneto-transport regimes. Here, we investigate the tunability of the topological magnetic moment (related to the Berry curvature) of electronic states in bilayer graphene using strain and vertical bias. We show how one can controllably vary the valley $g$-factor of the band-edge electrons, $g_v^*$, across the range $10 < |g_v^*| < 200$, and we discuss the manifestations of the topological magnetic moment …
Beijing Institute of Technology（北京理工大学）；Beijing Key Laboratory of Quantum Matter State Control and Ultra-Precision Measurement Technology（北京量子物质态控制与超精密测量技术重点实验室）
Few-layer GaSe is one of the latest additions to the family of 2D semiconducting crystals whose properties under strain are still relatively unexplored. Here, we study rippled nanosheets that exhibit a periodic compressive and tensile strain of up to 5%. The strain profile modifies the local optoelectronic properties of the alternating compressive and tensile regions, which translates into a remarkable shift of the optical absorption band-edge of up to 1.2 eV between crests and valleys. Our experimental observations are supported by theoretical results from density functional theory calculatio…
