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Register a new userFrequency-dependent substrate screening of excitons in atomically thin transition metal dichalcogenide semiconductors
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Alexander Steinhoff-List
Publication date
2018
fields
Physics
and research's language is
English
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Atomically thin layers of transition metal dichalcogenides (TMDCs) exhibit exceptionally strong Coulomb interaction between charge carriers due to the two-dimensional carrier confinement in connection with weak dielectric screening. The van der Waals nature of interlayer coupling makes it easy to integrate TMDC layers into heterostructures with different dielectric or metallic substrates. This allows to tailor electronic and optical properties of these materials, as Coulomb interaction inside atomically thin layers is very susceptible to screening by the environment. Here we theoretically investigate dynamical screening effects in TMDCs due to bulk substrates doped with carriers over a large density range, thereby offering three-dimensional plasmons as tunable degree of freedom. We report a wide compensation of renormalization effects leading to a spectrally more stable exciton than predicted for static substrate screening, even if plasmons and excitons are in resonance. We also find a nontrivial dependence of the single-particle band gap on substrate doping density due to dynamical screening. Our investigation provides microscopic insight into the mechanisms that allow for manipulations of TMDC excitons by means of arbitrary plasmonic environments on the nanoscale.
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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.
The formation of interfacial moire patterns from angular and/or lattice mismatch has become a powerful approach to engineer a range of quantum phenomena in van der Waals heterostructures. For long-lived and valley-polarized interlayer excitons in transition-metal dichalcogenide (TMDC) heterobilayers, signatures of quantum confinement by the moire landscape have been reported in recent experimental studies. Such moire confinement has offered the exciting possibility to tailor new excitonic systems, such as ordered arrays of zero-dimensional (0D) quantum emitters and their coupling into topological superlattices. A remarkable nature of the moire potential is its dramatic response to strain, where a small uniaxial strain can tune the array of quantum-dot-like 0D traps into parallel stripes of one-dimensional (1D) quantum wires. Here, we present direct evidence for the 1D moire potentials from real space imaging and the corresponding 1D moire excitons from photoluminescence (PL) emission in MoSe2/WSe2 heterobilayers. Whereas the 0D moire excitons display quantum emitter-like sharp PL peaks with circular polarization, the PL emission from 1D moire excitons has linear polarization and two orders of magnitude higher intensity. The results presented here establish strain engineering as a powerful new method to tailor moire potentials as well as their optical and electronic responses on demand.
When electron-hole pairs are excited in a semiconductor, it is a priori not clear if they form a fermionic plasma of unbound particles or a bosonic exciton gas. Usually, the exciton phase is associated with low temperatures. In atomically thin transition metal dichalcogenide semiconductors, excitons are particularly important even at room temperature due to strong Coulomb interaction and a large exciton density of states. Using state-of-the-art many-body theory including dynamical screening, we show that the exciton-to-plasma ratio can be efficiently tuned by dielectric substrate screening as well as charge carrier doping. Moreover, we predict a Mott transition from the exciton-dominated regime to a fully ionized electron-hole plasma at excitation densities between $3times10^{12}$ cm$^{-2}$ and $1times10^{13}$ cm$^{-2}$ depending on temperature, carrier doping and dielectric environment. We propose the observation of these effects by studying excitonic satellites in photoemission spectroscopy and scanning tunneling microscopy.
Long-range and fast transport of coherent excitons is important for development of high-speed excitonic circuits and quantum computing applications. However, most of these coherent excitons have only been observed in some low-dimensional semiconductors when coupled with cavities, as there are large inhomogeneous broadening and dephasing effects on the exciton transport in their native states of the materials. Here, by confining coherent excitons at the 2D quantum limit, we firstly observed molecular aggregation enabled super-transport of excitons in atomically thin two-dimensional (2D) organic semiconductors between coherent states, with a measured a high effective exciton diffusion coefficient of 346.9 cm2/sec at room temperature. This value is one to several orders of magnitude higher than the reported values from other organic molecular aggregates and low-dimensional inorganic materials. Without coupling to any optical cavities, the monolayer pentacene sample, a very clean 2D quantum system (1.2 nm thick) with high crystallinity (J type aggregation) and minimal interfacial states, showed superradiant emissions from the Frenkel excitons, which was experimentally confirmed by the temperature-dependent photoluminescence (PL) emission, highly enhanced radiative decay rate, significantly narrowed PL peak width and strongly directional in-plane emission. The coherence in monolayer pentacene samples was observed to be delocalized over 135 molecules, which is significantly larger than the values (a few molecules) observed from other organic thin films. In addition, the super-transport of excitons in monolayer pentacene samples showed highly anisotropic behaviour. Our results pave the way for the development of future high-speed excitonic circuits, fast OLEDs, and other opto-electronic devices.
The intricate interplay between optically dark and bright excitons governs the light-matter interaction in transition metal dichalcogenide monolayers. We have performed a detailed investigation of the spin-forbidden dark excitons in WSe2 monolayers by optical spectroscopy in an out-of-plane magnetic field Bz. In agreement with the theoretical predictions deduced from group theory analysis, magneto-photoluminescence experiments reveal a zero field splitting $delta=0.6 pm 0.1$ meV between two dark exciton states. The low energy state being strictly dipole forbidden (perfectly dark) at Bz=0 while the upper state is partially coupled to light with z polarization (grey exciton). The first determination of the dark neutral exciton lifetime $tau_D$ in a transition metal dichalcogenide monolayer is obtained by time-resolved photoluminescence. We measure $tau_D sim 110 pm 10$ ps for the grey exciton state, i.e. two orders of magnitude longer than the radiative lifetime of the bright neutral exciton at T=12 K.
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