Tunable Hybridization Between Electronic States of Graphene and Physisorbed Hexacene

Non-covalent functionalization via physisorption of organic molecules provides a scalable approach for modifying the electronic structure of graphene while preserving its excellent carrier mobilities. Here we investigated the physisorption of long-chain acenes, namely, hexacene and its fluorinated derivative perfluorohexacene, on bilayer graphene for tunable graphene devices using first principles methods. We find that the adsorption of these molecules leads to the formation of localized states in the electronic structure of graphene close to its Fermi level, which could be readily tuned by an external electric field. The electric field not only creates a variable band gap as large as 250 meV in bilayer graphene, but also strongly influences the charge redistribution within the molecule-graphene system. This charge redistribution is found to be weak enough not to induce strong surface doping, but strong enough to help preserve the electronic states near the Dirac point of graphene.Comment: 17 pages, 7 figures, supporting informatio

Selective Control of Surface Spin Current in Topological Materials based on Pyrite-type OsX2 (X = Se, Te) Crystals

Topological materials host robust surface states, which could form the basis for future electronic devices. As such states have spins that are locked to the momentum, they are of particular interest for spintronic applications. Understanding spin textures of the surface states of topologically nontrivial materials, and being able to manipulate their polarization, is therefore essential if they are to be utilized in future technologies. Here we use first-principles calculations to show that pyrite-type crystals OsX2 (X= Se, Te) are a class of topological material that can host surface states with spin polarization that can be either in-plane or out-of-plane. We show that the formation of low-energy states with symmetry-protected energy- and direction-dependent spin textures on the (001) surface of these materials is a consequence of a transformation from a topologically trivial to nontrivial state, induced by spin orbit interactions. The unconventional spin textures of these surface states feature an in-plane to out-of-plane spin polarization transition in the momentum space protected by local symmetries. Moreover, the surface spin direction and magnitude can be selectively filtered in specific energy ranges. Our demonstration of a new class of topological material with controllable spin textures provide a platform for experimentalists to detect and exploit unconventional surface spin textures in future spin-based nanoelectronic devices

Extracting unconventional spin texture in two dimensional topological crystalline insulators via tuning bulk-edge interactions

Tuning the interaction between the bulk and edge states of topological materials is a powerful tool for manipulating edge transport behavior, opening up exciting opportunities for novel electronic and spintronic applications. This approach is particularly suited to topological crystalline insulators (TCI), a class of topologically nontrivial compounds that are endowed with multiple degrees of topological protection. In this study, we investigate how bulk-edge interactions can influence the edge transport in planar bismuthene, a TCI with metallic edge states protected by in-plane mirror symmetry, using first principles calculations and symmetrized Wannier tight-binding models. By exploring the impact of various perturbation effects, such as device size, substrate potentials, and applied transverse electric field, we examine the evolution of the electronic structure and edge transport in planar bismuthene. Our findings demonstrate that the TCI states of planar bismuthene can be engineered to exhibit either a gapped or conducting unconventional helical spin texture via a combination of substrate and electric field effects. Furthermore, under strong electric fields, the edge states can be stabilized through a delicate control of the bulk-edge interactions. These results open up new directions for discovering novel spin transport patterns in topological materials and provide critical insights for the fabrication of topological spintronic devices.Comment: 23 pages, 8 figure

Near-direct bandgap WSe2WSe_2/ReS2ReS_2 type-II pn heterojunction for enhanced ultrafast photodetection and high-performance photovoltaics

PN heterojunctions comprising layered van der Waals (vdW) semiconductors have been used to demonstrate current rectifiers, photodetectors, and photovoltaic devices. However, a direct or near-direct bandgap at the heterointerface that can significantly enhance optical generation, for high light absorbing few/multi-layer vdW materials, has not yet been shown. In this work, for the first time, few-layer group-6 transition metal dichalcogenide (TMD) $WSe_2$ is shown to form a sizeable (0.7 eV) near-direct bandgap with type-II band alignment at its interface with the group-7 TMD $ReS_2$ through density functional theory calculations. Further, the type-II alignment and photogeneration across the interlayer bandgap have been experimentally confirmed through micro-photoluminescence and IR photodetection measurements, respectively. High optical absorption in few-layer flakes, large conduction and valence band offsets for efficient electron-hole separation and stacking of light facing, direct bandgap $ReS_2$ on top of gate tunable $WSe_2$ are shown to result in excellent and tunable photodetection as well as photovoltaic performance through flake thickness dependent optoelectronic measurements. Few-layer flakes demonstrate ultrafast response time (5 $\mu$s) at high responsivity (3 A/W) and large photocurrent generation and responsivity enhancement at the heterostructure overlap region (10-100X) for 532 nm laser illumination. Large open-circuit voltage of 0.64 V and short-circuit current of 2.6 $\mu$A enables high output electrical power. Finally, long term air-stability and a facile single contact metal fabrication process makes the multi-functional few-layer $WSe_2$/$ReS_2$ heterostructure diode technologically promising for next-generation optoelectronic applications.Comment: Manuscript- 27 pages, 8 figures. Supporting Information- 17 pages, 17 figure

Gate control of Mott metal-insulator transition in a 2D metal-organic framework

Strong electron-electron Coulomb interactions in materials can lead to a vast range of exotic many-body quantum phenomena, including Mott metal-insulator transitions, magnetic order, quantum spin liquids, and unconventional superconductivity. These many-body phases are strongly dependent on band occupation and can hence be controlled via the chemical potential. Flat electronic bands in two-dimensional (2D) and layered materials such as the kagome lattice, enhance strong electronic correlations. Although theoretically predicted, correlated-electron phases in monolayer 2D metal-organic frameworks (MOFs) - which benefit from efficient synthesis protocols and tunable properties - with a kagome structure have not yet been realised experimentally. Here, we synthesise a 2D kagome MOF comprised of 9,10-dicyanoanthracene molecules and copper atoms on an atomically thin insulator, monolayer hexagonal boron nitride (hBN) on Cu(111). Scanning tunnelling microscopy (STM) and spectroscopy reveal an electronic energy gap of ~200 meV in this MOF, consistent with dynamical mean-field theory predictions of a Mott insulating phase. By tuning the electron population of kagome bands, via either template-induced (via local work function variations of the hBN/Cu(111) substrate) or tip-induced (via the STM probe) gating, we are able to induce Mott metal-insulator transitions in the MOF. These findings pave the way for devices and technologies based on 2D MOFs and on electrostatic control of many-body quantum phases therein.Comment: 19 pages, 4 figure

Gigantic Anisotropy of Self-Induced Spin-Orbit Torque in Weyl Ferromagnet Co2MnGa

Spin-orbit torque (SOT) is receiving tremendous attention from both fundamental and application-oriented aspects. Co2MnGa, a Weyl ferromagnet that is in a class of topological quantum materials, possesses cubic-based high structural symmetry, the L21 crystal ordering, which should be incapable of hosting anisotropic SOT in conventional understanding. Here we show the discovery of a gigantic anisotropy of self-induced SOT in Co2MnGa. The magnitude of the SOT is comparable to that of heavy metal/ferromagnet bilayer systems despite the high inversion symmetry of the Co2MnGa structure. More surprisingly, a sign inversion of the self-induced SOT is observed for different crystal axes. This finding stems from the interplay of the topological nature of the electronic states and their strong modulation by external strain. Our research enriches the understanding of the physics of self-induced SOT and demonstrates a versatile method for tuning SOT efficiencies in a wide range of materials for topological and spintronic devices.Comment: 15pages, 4figures (To appear Nano Lett.