No Arabic abstract
Chemically stable quantum-confined 2D metals are of interest in next-generation nanoscale quantum devices. Bottom-up design and synthesis of such metals could enable the creation of materials with tailored, on-demand, electronic and optical properties for applications that utilize tunable plasmonic coupling, optical non-linearity, epsilon-near-zero behavior, or wavelength-specific light trapping. In this work, we demonstrate that the electronic, superconducting and optical properties of air-stable two-dimensional metals can be controllably tuned by the formation of alloys. Environmentally robust large-area two-dimensional InxGa1-x alloys are synthesized by Confinement Heteroepitaxy (CHet). Near-complete solid solubility is achieved with no evidence of phase segregation, and the composition is tunable over the full range of x by changing the relative elemental composition of the precursor. The optical and electronic properties directly correlate with alloy composition, wherein the dielectric function, band structure, superconductivity, and charge transfer from the metal to graphene are all controlled by the indium/gallium ratio in the 2D metal layer.
Quasi-two-dimensional (2D) films of layered metal-chalcogenides have attractive optoelectronic properties. However, photonic applications of thin films may be limited owing to weak light absorption and surface effects leading to reduced quantum yield. Integration of 2D films in optical microcavities will permit these limitations to be overcome owing to modified light coupling with the films. Here we present tunable microcavities with embedded monolayer MoS2 or few monolayer GaSe films. We observe significant modification of spectral and temporal properties of photoluminescence (PL): PL is emitted in spectrally narrow and wavelength-tunable cavity modes with quality factors up to 7400; PL life-time shortening by a factor of 10 is achieved, a consequence of Purcell enhancement of the spontaneous emission rate. This work has potential to pave the way to microcavity-enhanced light-emitting devices based on layered 2D materials and their heterostructures, and also opens possibilities for cavity QED in a new material system of van der Waals crystals.
We design a multiferroic metal that combines seemingly incompatible ferromagnetism, ferroelectricity, and metallicity by hole doping a two-dimensional (2D) ferroelectric with high density of states near the Fermi level. The strong magnetoelectric effect is demonstrated in hole-doped and arsenic-doped monolayer {alpha}-In2Se3 using first-principles calculations. Taking advantage of the oppositely charged surfaces created by an out-of-plane polarization, the 2D magnetization and metallicity can be electrically switched on and off in an asymmetrically doped monolayer. The substitutional arsenic defect pair exhibits an intriguing electric field-tunable charge disproportionation process accompanied with an on-off switch of local magnetic moments. The charge ordering process can be controlled by tuning the relative strength of on-site Coulomb repulsion and defect dipole-polarization coupling via strain engineering. Our design principle relying on no transition metal broadens the materials design space for 2D multiferroic metals.
Transition metal dichalcogenides (TMDCs) have emerged as a new two dimensional materials field since the monolayer and few-layer limits show different properties when compared to each other and to their respective bulk materials. For example, in some cases when the bulk material is exfoliated down to a monolayer, an indirect-to-direct band gap in the visible range is observed. The number of layers $N$ ($N$ even or odd) drives changes in space group symmetry that are reflected in the optical properties. The understanding of the space group symmetry as a function of the number of layers is therefore important for the correct interpretation of the experimental data. Here we present a thorough group theory study of the symmetry aspects relevant to optical and spectroscopic analysis, for the most common polytypes of TMDCs, i.e. $2Ha$, $2Hc$ and $1T$, as a function of the number of layers. Real space symmetries, the group of the wave vectors, the relevance of inversion symmetry, irreducible representations of the vibrational modes, optical selection rules and Raman tensors are discussed.
Two-dimensional (2D) transition metal dichalcogenides (TMDCs) with unique electrical properties are fascinating materials used for future electronics. However, the strong Fermi level pinning effect at the interface of TMDCs and metal electrodes always leads to high contact resistance, which seriously hinders their application in 2D electronics. One effective way to overcome this is to use metallic TMDCs or transferred metal electrodes as van der Waals (vdW) contacts. Alternatively, using highly conductive doped TMDCs will have a profound impact on the contact engineering of 2D electronics. Here, a novel chemical vapor deposition using mixed molten salts is established for vapor-liquid-solid growth of high-quality rhenium (Re) and vanadium (V)-doped TMDC monolayers with high controllability and reproducibility. A tunable semiconductor to metal transition is observed in the Re and V-doped TMDCs. Electrical conductivity increases up to a factor of 108 in the degenerate V-doped WS2 and WSe2. Using V-doped WSe2 as vdW contact, the on-state current and on/off ratio of WSe2-based field-effect transistors have been substantially improved (from ~10-8 to 10-5 A; ~104 to 108), compared to metal contacts. Future studies on lateral contacts and interconnects using doped TMDCs will pave the way for 2D integrated circuits and flexible electronics.
Growth of two-dimensional metals has eluded materials scientists since the discovery of the atomically thin graphene and other covalently bound 2D materials. Here, we report a two-atom-thick hexagonal copper-gold alloy, grown through thermal evaporation on freestanding graphene and hexagonal boron nitride. The structures are imaged at atomic resolution with scanning transmission electron microscopy and further characterized with spectroscopic techniques. Electron irradiation in the microscope provides sufficient energy for a phase transformation of the 2D structure--atoms are released from their lattice sites with the gold atoms eventually forming face-centered cubic nanoclusters on top of 2D regions during observation. The presence of copper in the alloy enhances sticking of gold to the substrate, which has clear implications for creating atomically thin electrodes for applications utilizing 2D materials. Its practically infinite surface-to-bulk ratio also makes the 2D CuAu particularly interesting for catalysis applications.