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Register a new userOptical nonlinearities in the excited carrier density of atomically thin transition metal dichalcogenides
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Daniel Erben
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In atomically thin semiconductors based on transition metal dichalcogenides, photoexcitation can be used to generate high densities of electron-hole pairs. Due to optical nonlinearities, which originate from Pauli blocking and many-body effects of the excited carriers, the generated carrier density will deviate from a linear increase in pump fluence. In this paper, we use a theoretical approach that combines results from ab-initio electronic-state calculations with a many-body treatment of optical excitation to describe nonlinear absorption properties and the resulting excited carrier dynamics. We determine the validity range of a linear approximation for the excited carrier density vs. pump power and identify the role and magnitude of optical nonlinearities at elevated excitation carrier densities for MoS2, MoSe2, WS2, and WSe2 considering various excitation conditions. We find that for above-band-gap photoexcitation, the use of a linear absorption coefficient of the unexcited system can strongly underestimate the achievable carrier density for a wide range of pump fluences due to many-body renormalizations of the two-particle density-of-states.
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Atomically thin materials such as graphene and monolayer transition metal dichalcogenides (TMDs) exhibit remarkable physical properties resulting from their reduced dimensionality and crystal symmetry. The family of semiconducting transition metal dichalcogenides is an especially promising platform for fundamental studies of two-dimensional (2D) systems, with potential applications in optoelectronics and valleytronics due to their direct band gap in the monolayer limit and highly efficient light-matter coupling. A crystal lattice with broken inversion symmetry combined with strong spin-orbit interactions leads to a unique combination of the spin and valley degrees of freedom. In addition, the 2D character of the monolayers and weak dielectric screening from the environment yield a significant enhancement of the Coulomb interaction. The resulting formation of bound electron-hole pairs, or excitons, dominates the optical and spin properties of the material. Here we review recent progress in our understanding of the excitonic properties in monolayer TMDs and lay out future challenges. We focus on the consequences of the strong direct and exchange Coulomb interaction, discuss exciton-light interaction and effects of other carriers and excitons on electron-hole pairs in TMDs. Finally, the impact on valley polarization is described and the tuning of the energies and polarization observed in applied electric and magnetic fields is summarized.
Strain engineering in single-layer semiconducting transition metal dichalcogenides aims to tune their bandgap energy and to modify their optoelectronic properties by the application of external strain. In this paper we study transition metal dichalcogenides monolayers deposited on polymeric substrates under the application of biaxial strain, both tensile and compressive. We can control the amount of biaxial strain applied by letting the substrate thermally expand or compress by changing the substrate temperature. After modelling the substrate-dependent strain transfer process with a finite elements simulation, we performed micro-differential spectroscopy of four transition metal dichalcogenides monolayers (MoS2, MoSe2, WS2, WSe2) under the application of biaxial strain and measured their optical properties. For tensile strain we observe a redshift of the bandgap that reaches a value as large as 94 meV/% in the case of single-layer WS2 deposited on polypropylene. The observed bandgap shifts as a function of substrate extension/compression follow the order WS2 > WSe2 > MoS2 > MoSe2.
Based on first-principles calculations and symmetry analysis, we predict atomically thin ($1-N$ layers) 2H group-VIB TMDs $MX_2$ ($M$ = Mo, W; $X$ = S, Se, Te) are large-gap higher-order topological crystalline insulators protected by $C_3$ rotation symmetry. We explicitly demonstrate the nontrivial topological indices and existence of the hallmark corner states with quantized fractional charge for these familiar TMDs with large bulk optical band gaps ($1.64-1.95$ eV for the monolayers), which would facilitate the experimental detection by STM. We find that the well-defined corner states exist in the triangular finite-size flakes with armchair edges of the atomically thin ($1-N$ layers) 2H group-VIB TMDs, and the corresponding quantized fractional charge is the number of layers $N$ divided by 3 modulo integers, which will simply double including spin degree of freedom.
Atomically thin transition metal dichalcogenides (TMDs) have distinct opto-electronic properties including enhanced luminescence and high on-off current ratios, which can be further modulated by making more complex TMD heterostructures. However, resolution limits of conventional optical methods do not allow for direct optical-structural correlation measurements in these materials, particularly of buried interfaces in TMD heterostructures. Here we use, for the first time, electron beam induced cathodoluminescence in a scanning transmission electron microscope (CL-STEM) to measure optical properties of monolayer TMDs (WS2, MoS2 and WSSe alloy) encapsulated between layers of hBN. We observe dark areas resulting from localized (~ 100 nm) imperfect interfaces and monolayer folding, which shows that the intimate contact between layers in this application-relevant heterostructure is required for proper inter layer coupling. We also realize a suitable imaging method that minimizes electron-beam induced changes and provides measurement of intrinsic properties. To overcome the limitation of small electron interaction volume in TMD monolayer (and hence low photon yield), we find that encapsulation of TMD monolayers with hBN and subsequent annealing is important. CL-STEM offers to be a powerful method to directly measure structure-optical correspondence in lateral or vertical heterostructures and alloys.
Motivated by the triumph and limitation of graphene for electronic applications, atomically thin layers of group VI transition metal dichalcogenides are attracting extensive interest as a class of graphene-like semiconductors with a desired band-gap in the visible frequency range. The monolayers feature a valence band spin splitting with opposite sign in the two valleys located at corners of 1st Brillouin zone. This spin-valley coupling, particularly pronounced in tungsten dichalcogenides, can benefit potential spintronics and valleytronics with the important consequences of spin-valley interplay and the suppression of spin and valley relaxations. Here we report the first optical studies of WS2 and WSe2 monolayers and multilayers. The efficiency of second harmonic generation shows a dramatic even-odd oscillation with the number of layers, consistent with the presence (absence) of inversion symmetry in even-layer (odd-layer). Photoluminescence (PL) measurements show the crossover from an indirect band gap semiconductor at mutilayers to a direct-gap one at monolayers. The PL spectra and first-principle calculations consistently reveal a spin-valley coupling of 0.4 eV which suppresses interlayer hopping and manifests as a thickness independent splitting pattern at valence band edge near K points. This giant spin-valley coupling, together with the valley dependent physical properties, may lead to rich possibilities for manipulating spin and valley degrees of freedom in these atomically thin 2D materials.
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