No Arabic abstract
Recently, two-dimensional (2D) materials with strong in-plane anisotropic properties such as black phosphorus have demonstrated great potential for developing new devices that can take advantage of its reduced lattice symmetry with potential applications in electronics, optoelectronics and thermoelectrics. However, the selection of 2D material with strong in-plane anisotropy has so far been very limited and only sporadic studies have been devoted to transition metal dichalcogenides (TMDC) materials with reduced lattice symmetry, which is yet to convey the full picture of their optical and phonon properties, and the anisotropy in their interlayer interactions. Here, we study the anisotropic interlayer interactions in an important TMDC 2D material with reduced in-plane symmetry - atomically thin rhenium diselenide (ReSe2) - by investigating its ultralow frequency interlayer phonon vibration modes, the layer dependent optical bandgap, and the anisotropic photoluminescence (PL) spectra for the first time. The ultralow frequency interlayer Raman spectra combined with the first study of polarization-resolved high frequency Raman spectra in mono- and bi-layer ReSe2 allows deterministic identification of its layer number and crystal orientation. PL measurements show anisotropic optical emission intensity with bandgap increasing from 1.26 eV in the bulk to 1.32 eV in monolayer, consistent with the theoretical results based on first-principle calculations. The study of the layer-number dependence of the Raman modes and the PL spectra reveals the relatively weak van der Waals interaction and 2D quantum confinement in atomically-thin ReSe2.
Stacking order can significantly influence the physical properties of two-dimensional (2D) van der Waals materials. The recent isolation of atomically thin magnetic materials opens the door for control and design of magnetism via stacking order. Here we apply hydrostatic pressure up to 2 GPa to modify the stacking order in a prototype van der Waals magnetic insulator CrI3. We observe an irreversible interlayer antiferromagnetic (AF) to ferromagnetic (FM) transition in atomically thin CrI3 by magnetic circular dichroism and electron tunneling measurements. The effect is accompanied by a monoclinic to a rhombohedral stacking order change characterized by polarized Raman spectroscopy. Before the structural change, the interlayer AF coupling energy can be tuned up by nearly 100% by pressure. Our experiment reveals interlayer FM coupling, which is the established ground state in bulk CrI3, but never observed in native exfoliated thin films. The observed correlation between the magnetic ground state and the stacking order is in good agreement with first principles calculations and suggests a route towards nanoscale magnetic textures by moire engineering.
Excitons in semiconductors, bound pairs of excited electrons and holes, can form the basis for new classes of quantum optoelectronic devices. A van der Waals heterostructure built from atomically thin semiconducting transition metal dichalcogenides (TMDs) enables the formation of excitons from electrons and holes in distinct layers, producing interlayer excitons with large binding energy and a long lifetime. Employing heterostructures of monolayer TMDs, we realize optical and electrical generation of long-lived neutral and charged interlayer excitons. We demonstrate the transport of neutral interlayer excitons across the whole sample that can be controlled by excitation power and gate electrodes. We also realize the drift motion of charged interlayer excitons using Ohmic-contacted devices. The electrical generation and control of excitons provides a new route for realizing quantum manipulation of bosonic composite particles with complete electrical tunability.
We investigate the interactions between exciton-polaritons in N two-dimensional semiconductor layers embedded in a planar microcavity. In the limit of low-energy scattering, where we can ignore the composite nature of the excitons, we obtain exact analytical expressions for the spin-triplet and spin-singlet interaction strengths, which go beyond the Born approximation employed in previous calculations. Crucially, we find that the strong light-matter coupling enhances the strength of polariton-polariton interactions compared to that of the exciton-exciton interactions, due to the Rabi coupling and the small photon-exciton mass ratio. We furthermore obtain the dependence of the polariton interactions on the number of layers N, and we highlight the important role played by the optically dark states that exist in multiple layers. In particular, we predict that the singlet interaction strength is stronger than the triplet one for a wide range of parameters in most of the currently used transition metal dichalcogenides. This has consequences for the pursuit of polariton condensation and other interaction-driven phenomena in these materials.
Atomically thin boron nitride (BN) nanosheets are important two-dimensional nanomaterials with many unique properties distinct from those of graphene, but the investigation of their mechanical properties still greatly lacks. Here we report that high-quality single-crystalline mono- and few-layer BN nanosheets are one of the strongest electrically insulating materials. More intriguingly, few-layer BN shows mechanical behaviors quite different from those of few-layer graphene under indentation. In striking contrast to graphene, whose strength decreases by more than 30% when the number of layers increases from 1 to 8, the mechanical strength of BN nanosheets is not sensitive to increasing thickness. We attribute this difference to the distinct interlayer interactions and hence sliding tendencies in these two materials under indentation. The significantly better mechanical integrity of BN nanosheets makes them a more attractive candidate than graphene for several applications, e.g. as mechanical reinforcements.
The observation and electrical manipulation of infrared surface plasmons in graphene have triggered a search for similar photonic capabilities in other atomically thin materials that enable electrical modulation of light at visible and near-infrared frequencies, as well as strong interaction with optical quantum emitters. Here, we present a simple analytical description of the optical response of such kinds of structures, which we exploit to investigate their application to light modulation and quantum optics. Specifically, we show that plasmons in one-atom-thick noble-metal layers can be used both to produce complete tunable optical absorption and to reach the strong-coupling regime in the interaction with neighboring quantum emitters. Our methods are applicable to any plasmon-supporting thin materials, and in particular, we provide parameters that allow us to readily calculate the response of silver, gold, and graphene islands. Besides their interest for nanoscale electro-optics, the present study emphasizes the great potential of these structures for the design of quantum nanophotonics devices.