Thin Semiconducting Transition Metal Dichalcogenides Research Articles

Giant Faraday rotation in atomically thin semiconductors

Faraday rotation is a fundamental effect in the magneto-optical response of solids, liquids and gases. Materials with a large Verdet constant find applications in optical modulators, sensors and non-reciprocal devices, such as optical isolators. Here, we demonstrate that the plane of polarization of light exhibits a giant Faraday rotation of several degrees around the A exciton transition in hBN-encapsulated monolayers of WSe2 and MoSe2 under moderate magnetic fields. This results in the highest known Verdet constant of -1.9 × 107 deg T−1 cm−1 for any material in the visible regime. Additionally, interlayer excitons in hBN-encapsulated bilayer MoS2 exhibit a large Verdet constant (VIL ≈ +2 × 105 deg T−1 cm−2) of opposite sign compared to A excitons in monolayers. The giant Faraday rotation is due to the giant oscillator strength and high g-factor of the excitons in atomically thin semiconducting transition metal dichalcogenides. We deduce the complete in-plane complex dielectric tensor of hBN-encapsulated WSe2 and MoSe2 monolayers, which is vital for the prediction of Kerr, Faraday and magneto-circular dichroism spectra of 2D heterostructures. Our results pose a crucial advance in the potential usage of two-dimensional materials in ultrathin optical polarization devices.

Creating a Nanoscale Lateral Junction in a Semiconductor Monolayer with a Large Built-in Potential

The ability to engineer atomically thin nanoscale lateral junctions is critical to lay the foundation for future two-dimensional (2D) device technology. However, the traditional approach to creating a heterojunction by direct growth of a heterostructure of two different materials constrains the available band offsets, and it is still unclear if large built-in potentials are attainable for 2D materials. The electronic properties of atomically thin semiconducting transition metal dichalcogenides (TMDs) are not static, and their exciton binding energy and quasiparticle band gap depend strongly on the proximal environment. Recent studies have shown that this effect can be harnessed to engineer the lateral band profile of a monolayer TMD to create a lateral electronic junction. Here we demonstrate the synthesis of a nanoscale lateral junction in monolayer MoSe2 by intercalating Se at the interface of an hBN/Ru(0001) substrate. The Se intercalation creates a spatially abrupt modulation of the local hBN/Ru work function, which is imprinted directly onto an overlying MoSe2 monolayer to create a lateral junction with a large built-in potential of 0.83 ± 0.06 eV. We spatially resolve the MoSe2 band profile and work function using scanning tunneling spectroscopy to map out the nanoscale depletion region. The Se intercalation also modifies the dielectric environment, influencing the local band gap renormalization and increasing the MoSe2 band gap by ∼0.26 ± 0.1 eV. This work illustrates that environmental proximity engineering provides a robust method to indirectly manipulate the band profile of 2D materials outside the limits of their intrinsic properties.

Spectroscopic view of ultrafast charge carrier dynamics in single- and bilayer transition metal dichalcogenide semiconductors

The quasiparticle spectra of atomically thin semiconducting transition metal dichalcogenides (TMDCs) and their response to an ultrafast optical excitation critically depend on interactions with the underlying substrate. Here, we present a comparative time- and angle-resolved photoemission spectroscopy (TR-ARPES) study of the transient electronic structure and ultrafast carrier dynamics in the single- and bilayer TMDCs MoS2 and WS2 on three different substrates: Au(111), Ag(111) and graphene/SiC. The photoexcited quasiparticle bandgaps are observed to vary over the range of 1.9–2.5 eV between our systems. The transient conduction band signals decay on a sub-50 fs timescale on the metals, signifying an efficient removal of photoinduced carriers into the bulk metallic states. On graphene, we instead observe a fast timescale on the order of 170 fs, followed by a slow dynamics for the conduction band decay in MoS2. These timescales are explained by Auger recombination involving MoS2 and in-gap defect states. In bilayer TMDCs on metals we observe a complex redistribution of excited holes along the valence band that is substantially affected by interactions with the continuum of bulk metallic states.

Excitons in 2D heterostructures

Stacks of atomically thin semiconducting transition metal dichalcogenides offer exciting opportunities for the study of new optical phenomena. In 2019, a number of studies uncovered many aspects of the underlying physics that can be understood in terms of well-known, but also new, exotic, types of exciton. In 2019, new optical phenomena have been revealed in stacks of atomically thin semiconducting transition metal dichalcogenides. These effects can be understood in terms of well-known, but also new, exotic, types of exciton.

Electrical control of interlayer exciton dynamics in atomically thin heterostructures.

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. By employing heterostructures of monolayer TMDs, we realize optical and electrical generation of long-lived neutral and charged interlayer excitons. We demonstrate that neutral interlayer excitons can propagate across the entire sample and that their propagation can be controlled by excitation power and gate electrodes. We also use devices with ohmic contacts to facilitate the drift motion of charged interlayer excitons. The electrical generation and control of excitons provide a route for achieving quantum manipulation of bosonic composite particles with complete electrical tunability.

Efficient Photocarrier Transfer and Effective Photoluminescence Enhancement in Type I Monolayer MoTe2/WSe2 Heterostructure

AbstractArtificial van der Waals heterostructures of 2D layered materials are attractive from the viewpoint of the possible discovery of new physics together with improved functionalities. Stacking various combinations of atomically thin semiconducting transition metal dichalcogenides, MX2 (M = Mo, W; X = S, Se, Te) with a hexagonal crystal structure, typically leads to the formation of a staggered Type II band alignment in the heterostructure, where electrons and holes are confined in different layers. Here, the comprehensive studies are performed on heterostructures prepared from monolayers of WSe2 and MoTe2 using differential reflectance, photoluminescence (PL), and PL excitation spectroscopy. The MoTe2/WSe2 heterostructure shows strong PL from the MoTe2 layer at ≈1.1 eV, which is different from the quenched PL from the WSe2 layer. Moreover, enhancement of PL intensity from the MoTe2 layer is observed because of the near‐unity highly efficient photocarrier transfer from WSe2 to MoTe2. These experimental results suggest that the MoTe2/WSe2 heterostructure has a Type I band alignment where electrons and holes are confined in the MoTe2 layer. The findings extend the diversity and usefulness of ultrathin layered heterostructures based on transition metal dichalcogenides, leading to possibilities toward future optoelectronic applications.

Dual Functionalization of Liquid‐Exfoliated Semiconducting 2H‐MoS2 with Lanthanide Complexes Bearing Magnetic and Luminescence Properties

AbstractLiquid exfoliated, atomically thin semiconducting transition metal dichalcogenides (TMDs), as inorganic equivalents of graphene, have attracted great interest due to their distinctive physical, optoelectronic, and chemical properties. Functionalization of 2D TMDs brings new prospects for applications in optoelectronics, quantum technologies, catalysis, and medicine. In this report, dual functionalization of 2D semiconducting 2H‐MoS2 nanosheets through simultaneous incorporation of magnetic and luminescent properties is demonstrated. A facile method is proposed for tuning the properties of the TDM semiconductors and accessing multimodal platforms, consisting in covalent grafting of lanthanide complexes onto the surface of 2D TMDs. Dual functionalization of liquid‐exfoliated MoS2 nanosheets is demonstrated simultaneously with both europium (III) and gadolinium (III) complexes to form a colloidally stable luminescent (with millisecond lifetimes) and paramagnetic MoS2‐based nanohybrid material. This work is the first example of transition metal dichalcogenide nanosheets functionalized with preformed lanthanide complexes. These findings open new prospects for covalent functionalization of TMDs with molecular species bearing specific functionalities as a means to tune the optoelectronic properties of the semiconductors, in order to create advanced materials and devices with a wide range of functionalities.

Strong Coulomb scattering effects on low frequency noise in monolayer WS2 field-effect transistors

When atomically thin semiconducting transition metal dichalcogenides are used as a channel material, they are inevitably exposed to supporting substrates. This situation can lead to masking of intrinsic properties by undesired extrinsic doping and/or additional conductance fluctuations from the largely distributed Coulomb impurities at the interface between the channel and the substrate. Here, we report low-frequency noise characteristics in monolayer WS2 field-effect transistors on silicon/silicon-oxide substrate. To mitigate the effect of extrinsic low-frequency noise sources, a nitrogen annealing was carried out to provide better interface quality and to suppress the channel access resistance. The carrier number fluctuation and the correlated mobility fluctuation (CNF-CMF) model was better than the sole CNF one to explain our low-frequency noise data, because of the strong Coulomb scattering effect on the effective mobility caused by carrier trapping/detrapping at oxide traps. The temperature-dependent field-effect mobility in the four-probe configuration and the Coulomb scattering parameters are presented to support this strong Coulomb scattering effect on carrier transport in monolayer WS2 field-effect transistor.