Kin Fai Mak

Atomically Thin MoS2 : A New Direct-Gap Semiconductor

The electronic properties of ultrathin crystals of molybdenum disulfide consisting of N=1,2,…,6 S-Mo-S monolayers have been investigated by optical spectroscopy. Through characterization by absorption, photoluminescence, and photoconductivity spectroscopy, we trace the effect of quantum confinement on the materials electronic structure. With decreasing thickness, the indirect band gap, which lies below the direct gap in the bulk material, shifts upwards in energy by more than 0.6 eV. This leads to a crossover to a direct-gap material in the limit of the single monolayer. Unlike the bulk material, the MoS₂ monolayer emits light strongly. The freestanding monolayer exhibits an increase in luminescence quantum efficiency by more than a factor of 10⁴ compared with the bulk material.

Tightly bound trions in monolayer MoS2

Two-dimensional (2D) atomic crystals, such as graphene and transition-metal dichalcogenides, have emerged as a new class of materials with remarkable physical properties. In contrast to graphene, monolayer MoS(2) is a non-centrosymmetric material with a direct energy gap. Strong photoluminescence, a current on/off ratio exceeding 10(8) in field-effect transistors, and efficient valley and spin control by optical helicity have recently been demonstrated in this material. Here we report the spectroscopic identification in a monolayer MoS(2) field-effect transistor of tightly bound negative trions, a quasiparticle composed of two electrons and a hole. These quasiparticles, which can be optically created with valley and spin polarized holes, have no analogue in conventional semiconductors. They also possess a large binding energy (~ 20 meV), rendering them significant even at room temperature. Our results open up possibilities both for fundamental studies of many-body interactions and for optoelectronic and valleytronic applications in 2D atomic crystals.

The valley Hall effect in MoS2 transistors

Using the valleys in monolayer MoS2 The electronic structure of the two-dimensional material MoS2 has two distinct “valleys” of energy that may help to carry information in future electronic devices. Mak et al. observed the so-called valley Hall effect in a monolayer of MoS2. The electrons from different valleys moved in opposite directions across the sample, with one valley being overrepresented with respect to the other. The scientists achieved this by shining circularly polarized light on the material, which created an imbalance in the population of the two valleys. The findings may enable practical applications in the newly formed field of valleytronics. Science, this issue p. 1489 Circularly polarized light is used to induce valley-specific transport in a monolayer of molybdenum disulfide. Electrons in two-dimensional crystals with a honeycomb lattice structure possess a valley degree of freedom (DOF) in addition to charge and spin. These systems are predicted to exhibit an anomalous Hall effect whose sign depends on the valley index. Here, we report the observation of this so-called valley Hall effect (VHE). Monolayer MoS2 transistors are illuminated with circularly polarized light, which preferentially excites electrons into a specific valley, causing a finite anomalous Hall voltage whose sign is controlled by the helicity of the light. No anomalous Hall effect is observed in bilayer devices, which have crystal inversion symmetry. Our observation of the VHE opens up new possibilities for using the valley DOF as an information carrier in next-generation electronics and optoelectronics.

High-mobility three-atom-thick semiconducting films with wafer-scale homogeneity

The large-scale growth of semiconducting thin films forms the basis of modern electronics and optoelectronics. A decrease in film thickness to the ultimate limit of the atomic, sub-nanometre length scale, a difficult limit for traditional semiconductors (such as Si and GaAs), would bring wide benefits for applications in ultrathin and flexible electronics, photovoltaics and display technology. For this, transition-metal dichalcogenides (TMDs), which can form stable three-atom-thick monolayers, provide ideal semiconducting materials with high electrical carrier mobility, and their large-scale growth on insulating substrates would enable the batch fabrication of atomically thin high-performance transistors and photodetectors on a technologically relevant scale without film transfer. In addition, their unique electronic band structures provide novel ways of enhancing the functionalities of such devices, including the large excitonic effect, bandgap modulation, indirect-to-direct bandgap transition, piezoelectricity and valleytronics. However, the large-scale growth of monolayer TMD films with spatial homogeneity and high electrical performance remains an unsolved challenge. Here we report the preparation of high-mobility 4-inch wafer-scale films of monolayer molybdenum disulphide (MoS2) and tungsten disulphide, grown directly on insulating SiO2 substrates, with excellent spatial homogeneity over the entire films. They are grown with a newly developed, metal–organic chemical vapour deposition technique, and show high electrical performance, including an electron mobility of 30 cm2 V−1 s−1 at room temperature and 114 cm2 V−1 s−1 at 90 K for MoS2, with little dependence on position or channel length. With the use of these films we successfully demonstrate the wafer-scale batch fabrication of high-performance monolayer MoS2 field-effect transistors with a 99% device yield and the multi-level fabrication of vertically stacked transistor devices for three-dimensional circuitry. Our work is a step towards the realization of atomically thin integrated circuitry.

Experimental Demonstration of Continuous Electronic Structure Tuning via Strain in Atomically Thin MoS2

We demonstrate the continuous tuning of the electronic structure of atomically thin MoS2 on flexible substrates by applying a uniaxial tensile strain. A redshift at a rate of ~70 meV per percent applied strain for direct gap transitions, and at a rate 1.6 times larger for indirect gap transitions, has been determined by absorption and photoluminescence spectroscopy. Our result, in excellent agreement with first principles calculations, demonstrates the potential of two-dimensional crystals for applications in flexible electronics and optoelectronics.

Tightly Bound Excitons in Monolayer WSe 2

Exciton binding energy and excited states in monolayers of tungsten diselenide (WSe(2)) are investigated using the combined linear absorption and two-photon photoluminescence excitation spectroscopy. The exciton binding energy is determined to be 0.37 eV, which is about an order of magnitude larger than that in III-V semiconductor quantum wells and renders the exciton excited states observable even at room temperature. The exciton excitation spectrum with both experimentally determined one- and two-photon active states is distinct from the simple two-dimensional (2D) hydrogenic model. This result reveals significantly reduced and nonlocal dielectric screening of Coulomb interactions in 2D semiconductors. The observed large exciton binding energy will also have a significant impact on next-generation photonics and optoelectronics applications based on 2D atomic crystals.

Probing symmetry properties of few-layer MoS2 and h-BN by optical second-harmonic generation.

We have measured optical second-harmonic generation (SHG) from atomically thin samples of MoS2 and h-BN with one to five layers. We observe strong SHG from materials with odd layer thickness, for which a noncentrosymmetric structure is expected, while the centrosymmetric materials with even layer thickness do not yield appreciable SHG. SHG for materials with odd layer thickness was measured as a function of crystal orientation. This dependence reveals the rotational symmetry of the lattice and is shown to provide a purely optical method of determining the orientation of crystallographic axes. We report values for the nonlinearity of monolayers and odd-layers of MoS2 and h-BN and compare the variation as a function of layer thickness with a model that accounts for wave propagation effects.

Observation of intense second harmonic generation from MoS2atomic crystals

The nonlinear optical properties of few-layer MoS

Breaking of Valley Degeneracy by Magnetic Field in Monolayer MoSe 2

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Ising pairing in superconducting NbSe2 atomic layers

two-dimensional crystals are studied using femtosecond laser pulses. We observed highly efficient second-harmonic generation from the odd-layer crystals, which shows a polarization intensity dependence that directly reveals the underlying symmetry and orientation of the crystal. Additionally, the measured second-order susceptibility spectra provide information about the electronic structure of the material. Our results open up opportunities for studying the nonlinear optical properties in these two-dimensional crystals.