Integration of two-dimensional (2D) van der Waals (vdWs) materials with non-2D materials to realize mixed-dimensional heterostructures has potential for creating functional devices beyond the reach of existing materials and has long been a pursuit of the material science community. Here we report the patterning of monolayer/bilayer transition metal dichalcogenide (TMD) nanostructures with nanometer-precision, tunable sizes and sites at interfaces of graphene/TMD heterostructures. Our experiments demonstrate that the TMD nanostructures can be created at selected positions of the interface using scanning tunneling microscope lithography and, more importantly, the sizes of the interfacial TMD nanostructures can be tuned with nanoscale precise by merging adjacent TMD nanostructures or by further tailoring. A structural phase transition from hexagonal phase in bulk TMD to monoclinic phase in the interfacial nanostructures is explicitly observed, which locally introduce well-defined electrostatic potentials on graphene. These results not only enable the creation of high-quality patterned p-n junctions in vdWs heterostructures, but also provide a new route to realize custom-designed mixed-dimensional heterostructures.
We present a novel approach to spin manipulation in atomic-scale nanostructures. Our ab initio calculations clearly demonstrate that it is possible to tune magnetic properties of sub-nanometer structures by adjusting the geometry of the system. By the example of two surface-based systems we demonstrate that (i) the magnetic moment of a single adatom coupled to a buried magnetic Co layer can be stabilized in either a ferromagnetic or an antiferromagnetic configuration depending on the spacer thickness. It is found that a buried Co layer has a profound effect on the exchange interaction between …
In two-dimensional van der Waals (vdWs) materials, the relative twist angle between adjacent layers not only controls their electronic properties, but also determines their stacking energy. This effect makes it much easier to realize energetically favorable configurations of the vdWs materials, for example, Bernal-stacked structure of bilayer graphene. Here we demonstrate that we can controllably tailor adhesive energy landscape of graphene nanostructures on graphene and stabilize the system with tunable twist angle by using a one-dimensional tilt grain boundary (GB). The area ratio with diffe…
We highlight the emergence of metallic states in two-dimensional transition-metal-dichalcogenide nanostructures -nanoribbons, islands, and inversion domain boundaries- as a widespread and universal phenomenon driven by the polar discontinuities occurring at their edges or boundaries. We show that such metallic states form one-dimensional wires of electrons or holes, with a free charge density that increases with the system size, up to complete screening of the polarization charge, and can also be controlled by the specific edge or boundary configurations, e.g. through chemisorption of hydrogen…
Dzyaloshinskii-Moriya interaction (DMI) is vital to form various chiral spin textures, novel behaviors of magnons and permits their potential applications in energy-efficient spintronic devices. Here, we realize a sizable bulk DMI in a transition metal dichalcogenide (TMD) 2H-TaS2 by intercalating Fe atoms, which form the chiral supercells with broken spatial inversion symmetry and also act as the source of magnetic orderings. Using a newly developed protonic gate technology, gate-controlled protons intercalation could further change the carrier density and intensely tune DMI via the Ruderman-…
Finding affordable ways of generating high-density ordered nanostructures that can be transferred to a substrate is a major challenge for industrial applications like memories or optical devices with high resolution features. In this work, we report on a novel technique to direct self-assembled structures of block copolymers by NanoImprint Lithography. Surface energy of a reusable mold and nanorheology are used to organize the copolymers in defect-free structures over tens of micrometers in size. Versatile and controlled in-plane orientations of about 25 nm half-period lamellar nanostructures …
Two-dimensional (2D) semiconducting transition metal dichalcogenides (TMDCs) and black phosphorus (BP) have beneficial electronic, optical, and physical properties at the few-layer limit. As atomically thin materials, 2D TMDCs and BP are highly sensitive to their environment and chemical modification, resulting in a strong dependence of their properties on substrate effects, intrinsic defects, and extrinsic adsorbates. Furthermore, the integration of 2D semiconductors into electronic and optoelectronic devices introduces unique challenges at metal-semiconductor and dielectric-semiconductor int…
The modification and tailoring the characteristics of nanostructured materials are of great interest due to controllable and unusual inherent properties in such materials. A simple spray pyrolysis technique is used to prepare pure and La-doped ZnO films. The influence of La concentration (0, 0.33, 0.45, 0.66, 0.92 and 1.04 at. %) on the structural, optical, and magnetic properties of ZnO was investigated. The exact nominal compositions of the prepared films were determined from the field emission scanning electron microscope occupied with EDX. X-ray diffraction confirmed that the samples posse…
The low concentration of proton donors in alkaline HER, subsequently leading to the extra water adsorption and dissociation steps, identifies the value of active sites (edge and basal sites) and crystal phases in lowering the extra activation barrier and/or optimizing the H* adsorption kinetics; in addition, the outstanding morphology-based features (surface area, thickness, defects, disorders and crystallinity) of layered molybdenum dichalcogenide families pinpoint the roles of active sites and phases for more interpretable and feasible structure-activity analysis. In this context, hydrotherm…
Triple sum-frequency (TSF) spectroscopy measures multidimensional spectra by resonantly exciting multiple quantum coherences of vibrational and electronic states. In this work we demonstrate pump-TSF-probe spectroscopy in which a pump excites a sample and some time later three additional electric fields generate a probe field which is measured. We demonstrate pump-TSF-probe spectroscopy on polycrystalline, smooth, thin films and spiral nanostructures of both MoS2 and WS2. The pump-TSF-probe spectra are qualitatively similar to the more conventional transient-reflectance spectra. While transien…
In this work we focus on magnetic relaxation in Mn$_{80}$Ir$_{20}$(12 nm)/ Cu(6 nm)/ Py($d_\mathrm{F}$) antiferromagnet/Cu/ferromagnet (AFM/Cu/FM) multilayers with different thickness of the ferromagnetic permalloy layer. An effective FM-AFM interaction mediated via the conduction electrons in the nonmagnetic Cu spacer -- the spin-pumping effect -- is detected as an increase in the linewidth of the ferromagnetic resonance (FMR) spectra and a shift of the resonant magnetic field. We further find experimentally that the spin-pumping-induced contribution to the linewidth is inversely proportional…
Excitons in monolayer semiconductors have large optical transition dipole for strong coupling with light field. Interlayer excitons in heterobilayers, with layer separation of electron and hole components, feature large electric dipole that enables strong coupling with electric field and exciton-exciton interaction, at the cost that the optical dipole is substantially quenched (by several orders of magnitude). In this letter, we demonstrate the ability to create a new class of excitons in transition metal dichalcogenide (TMD) hetero- and homo-bilayers that combines the advantages of monolayer-…
We propose a theoretical approach to quantitatively determine the photothermally driven enhancement of molecular mobility of graphene-indomethacin mixtures under infrared laser irradiation. Graphene plasmons absorb incident electromagnetic energy and dissipate them into heat. The absorbed energy depends on optical properties of graphene plasmons, which are sensitive to structural parameters, and concentration of plasmonic nanostructures. By using theoretical model, we calculate temperature gradients of the bulk drug with different concentrations of graphene plasmons. From these, we determine t…
We study the electromechanical response of Janus transition metal dichalcogenide (TMD) nanotubes from first principles. In particular, considering both armchair and zigzag variants of twenty-seven select Janus TMD nanotubes, we determine the change in bandgap and charge carriers' effective mass upon axial and torsional deformations using density functional theory (DFT). We observe that metallic nanotubes remain unaffected, whereas the bandgap in semiconducting nanotubes decreases linearly and quadratically with axial and shear strains, respectively, leading to semiconductor--metal transitions.…
Patterned films of decorated nitrogenated carbon (C-N) nanotubes were catalytically synthesised by hot filament chemical vapour deposition (HF-CVD) in a nitrogen-methane-ammonia environment. The systematic study of a transition between different kinds of C-N nanostructures as a function of the local substrate temperature ranging from 700 up to 820C is presented. The morphology, the diameter as well as the properties of the generated tubular structures showed strong dependence on this parameter. By means of electron microscopy a new type of decoration covering all tubular structures was observe…
Semiconductor heterostructures have played a critical role as the enabler for new science and technology. The emergence of transition metal dichalcogenides (TMDs) as atomically thin semiconductors has opened new frontiers in semiconductor heterostructures either by stacking different TMDs to form vertical heterojunctions or by stitching them laterally to form lateral heterojunctions via direct growth. In conventional semiconductor heterostructures, the design of multi-junctions is critical to achieve carrier confinement. Analogously, we report successful synthesis of monolayer WS2/WS2(1-x)Se2x…
Magnetic transition metal dichalcogenide (TMD) films have recently emerged as promising candidates to host novel magnetic phases relevant to next-generation spintronic devices. However, systematic control of the magnetization orientation, or anisotropy, and its thermal stability, characterized by Curie temperature (Tc) remains to be achieved in such films. Here we present self-intercalated epitaxial Cr1+δTe2 films as a platform for achieving systematic/smooth magnetic tailoring in TMD films. Using a molecular beam epitaxy (MBE) based technique, we have realized epitaxial Cr1+δTe2 films with sm…
Monolayer transition metal dichalcogenides (TMDs) bare large Berry curvature hotspots readily exploitable for geometric band effects. Tailoring and enhancement of these features via strain is an active research direction. Here, we consider spinless two- and three-band, and spinful four-band models capable to quantify Berry curvature and orbital magnetic moment of strained TMDs. First, we provide a $k\cdot p$ parameter set for MoS$_2$, MoSe$_2$, WS$_2$, and WSe$_2$ in the light of the recently released ab initio and experimental band properties. Its validity range extends from $K$ valley edge t…
Ti$_{1-x-y}$Al$_{x}$Zr$_{y}$N cubic alloys within the 25-70\% Al composition range have high age-hardening capabilities due to metastable phase transition pathways at high temperatures. They are thus ideal candidates for ultra-hard nano-coating materials. There is growing evidence that this effect is associated with the elasto-chemical field-induced phase separation into compositionally-segregated nanocrystaline nitride phases. Here, we studied the microstructural evolution in this pseudo-ternary system within spinodal regions at 1200 $^\circ$C by using an elasto-chemical phase field model. Ou…
Controlling magnetism of transition metal atoms by pairing with $π$ electronic states of graphene is intriguing. Herein, through first - principle computation we explore the possibility of switching magnetization by forming the tetrahedral $sp^3$ - metallic $d$ hybrid bonds. Graphene multilayers capped by single - layer cobalt atoms can transform into the $sp^3$ - bonded diamond films upon the hydrogenation of the bottom surface. While the conversion is favored by hybridization between the $sp^3$ dangling bonds and metallic $d_{z^2}$ states, such a strong hybridization can lead to the reorient…
Van der Waals epitaxy on the surface of two-dimensional (2D) layered crystals has gained significant research interest for the assembly of well-ordered nanostructures and fabrication of vertical heterostructures based on 2D crystals. Although van der Waals epitaxial assembly on the hexagonal phase of transition metal dichalcogenides (TMDCs) has been relatively well characterized, a comparable study on the distorted octahedral phase (1T' or Td) of TMDCs is largely lacking. Here we investigate the assembly behavior of one-dimensional (1D) AgCN microwires on various distorted TMDC crystals, namel…
The manipulation of two-dimensional materials via their dielectric environment offers novel opportunities to control electronic as well as optical properties and allows to imprint nanostructures in a non-invasive way. Here we asses the potential of monolayer semiconducting transition metal dichalcogenides (TMDCs) for Coulomb engineering in a material realistic and quantitative manner. We compare the response of different TMDC materials to modifications of their dielectric surrounding, analyze effects of dynamic substrate screening, i.e. frequency dependencies in the dielectric functions, and d…
The ability to extract materials just a few atoms thick has led to discovery of graphene, monolayer transition metal dichalcogenides (TMDs), and other important two-dimensional materials. The next step in promoting understanding and utility of the flatland physics beyond the state-of-the-art is to study one-dimensional edges of such two-dimensional materials as well as to control the edge-plane ratio. Edges typically exhibit properties that are unique and distinctly different from those of planes and bulk. Thus, controlling them allows to design principally new materials with synthetic edge-pl…
The optical properties of transition metal dichalcogenide monolayers are widely dominated by excitons, Coulomb-bound electron-hole pairs. These quasi-particles exhibit giant oscillator strength and give rise to narrow-band, well-pronounced optical transitions, which can be brought into resonance with electromagnetic fields in microcavities and plasmonic nanostructures. Due to the atomic thinness and robustness of the monolayers, their integration in van der Waals heterostructures provides unique opportunities for engineering strong light-matter coupling. We review first results in this emergin…
Recent developments in the area of resonant dielectric nanostructures has created attractive opportunities for the concentrating and manipulating light at the nanoscale and the establishment of new exciting field of all-dielectric nanophotonics. Transition metal dichalcogenides (TMDCs) with nanopatterned surfaces are especially promising for these tasks. Still, the fabrication of these structures requires sophisticated lithographic processes, drastically complicating application prospects. To bridge this gap and broaden the application scope of TMDC nanomaterials, we report here femtosecond la…
Two dimensional (2D) materials, e.g. graphene, transition metal dichalcogenides (TMDs), black phosphorus (BP), have demonstrated fascinating electrical and optical characteristics and exhibited great potential in optoelectronic applications. High performance and multifunctional devices were achieved by employing diverse designs of architectures, such as hybrid systems with nanostructured materials, bulk semiconductors and organics, forming 2D heterostructures. In this review, we mainly discuss the recent progresses of 2D materials in high responsive photodetectors, light-emitting devices and s…
Transition metal dichalcogenides (TMDs) are a class of widely studied 2D layered materials which exist in various polymorphs. The 1T' phase of MoTe2 is of prime importance as it has been reported to show quantum spin hall (QSH) behavior with a fairly large band-gap of ~ 60 meV, in contrast to most QSH materials known. It is noteworthy that though the monolayer 1T'-MoTe2 was initially predicted to show the QSH behavior, recent theoretical studies claim that the few-layered counterparts also exhibit higher order topological behavior. Besides, 1T'-MoTe2 also undergoes a hysteretic phase transitio…
Two-dimensional (2D) transition metal dichalcogenides (TMDs) are prospective materials for quantum devices owing to their inherent 2D confinements. They also provide a platform to realize even lower-dimensional in-plane electron confinement, e.g., 0D quantum dots, for exotic physical properties. However, fabrication of such laterally confined monolayer (1L) nanostructure in 1L crystals remains challenging. Here we report the realization of 1L ReS2 quantum dots epitaxially inlaid in 1L MoS2 by a two-step chemical vapor deposition method combining with plasma treatment. The lateral lattice misma…
Plasmon coupling and hybridization in complex nanostructures constitutes a fertile playground for controlling light at the nanoscale. Here, we present a semi-analytical model to describe the emergence of hybrid plasmon modes guided along 2D nano-slits. In particular, we find two new coupled plasmonic resonances arising from symmetric and antisymmetric hybridizations of the edge plasmons of the constituent half-sheets. These give rise to an antibonding and a bonding mode, lying above and below the energy of the bare edge plasmon. Our treatment is notably generic, being able to account for slits…
Nanostructuring allows altering of the electronic and photonic properties of two-dimensional (2D) materials. The efficiency, flexibility, and convenience of top-down lithography processes are however compromised by nm-scale edge roughness and resolution variability issues, which especially affects the performance of 2D materials. Here we study how dry anisotropic etching of multilayer 2D materials with sulfur hexafluoride (SF6) may overcome some of these issues, showing results for hexagonal boron nitride (hBN), tungsten disulfide (WS2), tungsten diselenide (WSe2), molybdenum disulfide (MoS2),…
We have established a rigorous theoretical formalism for Floquet engineering, or investigating and eventually tailoring most crucial electronic properties of tetragonal molybdenum disulfide (1T$^\prime$-MoS$_2$), by applying an external high-frequency dressing field in the off-resonant regime. It was recently demonstrated that monolayer semiconducting1T$^\prime$-MoS$_2$ may assume a distorted tetragonal structure which exhibits tunable and gapped spin- and valley-polarized tilted Dirac bandstructure. From the viewpoint of electronics, 1T$^\prime$-MoS$_2$ is one of the most technologically prom…
