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Enhanced Light-Matter Interaction in Two-Dimensional Transition Metal Dichalcogenides

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 Added by Lujun Huang
 Publication date 2021
  fields Physics
and research's language is English




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Two dimensional (2D) transition metal dichalcogenide (TMDC) materials, such as MoS2, WS2, MoSe2, and WSe2, have received extensive attention in the past decade due to their extraordinary physical properties. The unique properties make them become ideal materials for various electronic, photonic and optoelectronic devices. However, their performance is limited by the relatively weak light-matter interactions due to their atomically thin form factor. Resonant nanophotonic structures provide a viable way to address this issue and enhance light-matter interactions in 2D TMDCs. Here, we provide an overview of this research area, showcasing relevant applications, including exotic light emission, absorption and scattering features. We start by overviewing the concept of excitons in 1L-TMDC and the fundamental theory of cavity-enhanced emission, followed by a discussion on the recent progress of enhanced light emission, strong coupling and valleytronics. The atomically thin nature of 1L-TMDC enables a broad range of ways to tune its electric and optical properties. Thus, we continue by reviewing advances in TMDC-based tunable photonic devices. Next, we survey the recent progress in enhanced light absorption over narrow and broad bandwidths using 1L or few-layer TMDCs, and their applications for photovoltaics and photodetectors. We also review recent efforts of engineering light scattering, e.g., inducing Fano resonances, wavefront engineering in 1L or few-layer TMDCs by either integrating resonant structures, such as plasmonic/Mie resonant metasurfaces, or directly patterning monolayer/few layers TMDCs. We then overview the intriguing physical properties of different types of van der Waals heterostructures, and their applications in optoelectronic and photonic devices. Finally, we draw our opinion on potential opportunities and challenges in this rapidly developing field of research.



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The investigation of 2D van der Waals (vdW) materials is a vibrant, fast moving and still growing interdisciplinary area of research. 2D vdW materials are truly 2D crystals with strong covalent in-plane bonds and weak van der Waals interaction between the layers with a variety of different electronic, optical and mechanical properties. A very prominent class of 2D materials are transition metal dichalcogenides (TMDs) and amongst them particularly the semiconducting subclass. Their properties include bandgaps in the near-infrared to the visible range, decent charge carrier mobility together with high (photo-)catalytic and mechanical stability and exotic many body phenomena. These characteristics make the materials highly attractive for both fundamental research as well as innovative device applications. Furthermore, the materials exhibit a strong light matter interaction providing a high sun light absorbance of up to 15% in the monolayer limit, strong scattering cross section in Raman experiments and access to excitonic phenomena in vdW heterostructures. This review focuses on the light matter interaction in MoS2, WS2, MoSe2, and WSe2 that is dictated by the materials complex dielectric functions and on the multiplicity of studying the first order phonon modes by Raman spectroscopy to gain access to several material properties such as doping, strain, defects and temperature. 2D materials provide an interesting platform to stack them into vdW heterostructures without the limitation of lattice mismatch resulting in novel devices for application but also to study exotic many body interaction phenomena such as interlayer excitons. Future perspectives of semiconducting TMDs and their heterostructures for applications in optoelectronic devices will be examined and routes to study emergent fundamental problems and many-body quantum phenomena under excitations with photons will be discussed.
113 - Alex Krasnok , Sergey Lepeshov , 2018
Two-dimensional transition metal dichalcogenides (TMDCs) have recently become attractive semiconductor materials for several optoelectronic applications, such as photodetection, light harvesting, phototransistors, light-emitting diodes, and lasers. They are particularly appealing because their bandgap lies in the visible and near-IR range, and they possess strong excitonic resonances, high oscillator strengths, and valley-selective response. Coupling these materials to optical nanocavities enhances the quantum yield of exciton emission, enabling advanced quantum optics and nanophotonic devices. Here, we review state-of-the-art advances on hybrid exciton-polariton structures based on monolayer TMDCs coupled to plasmonic and dielectric nanocavities. We first generally discuss the optical properties of 2D WS2, WSe2, MoS2 and MoSe2 materials, paying special attention to their energy and photoluminescence/absorption spectra, excitonic fine structure, and to the dynamics of exciton formation and valley depolarization. We then discuss light-matter interactions in hybrid exciton-polariton structures. Finally, we focus on weak and strong coupling regimes in monolayer TMDCs-based exciton-polariton systems, envisioning research directions and future opportunities based on this novel material platform.
141 - J. Ribeiro-Soares 2014
Transition metal dichalcogenides (TMDCs) have emerged as a new two dimensional materials field since the monolayer and few-layer limits show different properties when compared to each other and to their respective bulk materials. For example, in some cases when the bulk material is exfoliated down to a monolayer, an indirect-to-direct band gap in the visible range is observed. The number of layers $N$ ($N$ even or odd) drives changes in space group symmetry that are reflected in the optical properties. The understanding of the space group symmetry as a function of the number of layers is therefore important for the correct interpretation of the experimental data. Here we present a thorough group theory study of the symmetry aspects relevant to optical and spectroscopic analysis, for the most common polytypes of TMDCs, i.e. $2Ha$, $2Hc$ and $1T$, as a function of the number of layers. Real space symmetries, the group of the wave vectors, the relevance of inversion symmetry, irreducible representations of the vibrational modes, optical selection rules and Raman tensors are discussed.
Recently, the celebrated Keldysh potential has been widely used to describe the Coulomb interaction of few-body complexes in monolayer transition-metal dichalcogenides. Using this potential to model charged excitons (trions), one finds a strong dependence of the binding energy on whether the monolayer is suspended in air, supported on SiO$_2$, or encapsulated in hexagonal boron-nitride. However, empirical values of the trion binding energies show weak dependence on the monolayer configuration. This deficiency indicates that the description of the Coulomb potential is still lacking in this important class of materials. We address this problem and derive a new potential form, which takes into account the three atomic sheets that compose a monolayer of transition-metal dichalcogenides. The new potential self-consistently supports (i) the non-hydrogenic Rydberg series of neutral excitons, and (ii) the weak dependence of the trion binding energy on the environment. Furthermore, we identify an important trion-lattice coupling due to the phonon cloud in the vicinity of charged complexes. Neutral excitons, on the other hand, have weaker coupling to the lattice due to the confluence of their charge neutrality and small Bohr radius.
This paper presents a theoretical description of both the valley Zeeman effect (g-factors) and Landau levels in two-dimensional H-phase transition metal dichalcogenides (TMDs) using the Luttinger-Kohn approximation with spin-orbit coupling. At the valley extrema in TMDs, energy bands split into Landau levels with a Zeeman shift in the presence of a uniform out-of-plane external magnetic field. The Landau level indices are symmetric in the $K$ and $K$ valleys. We develop a numerical approach to compute the single band g-factors from first principles without the need for a sum over unoccupied bands. Many-body effects are included perturbatively within the GW approximation. Non-local exchange and correlation self-energy effects in the GW calculations increase the magnitude of single band g-factors compared to those obtained from density functional theory. Our first principles results give spin- and valley-split Landau levels, in agreement with recent optical experiments. The exciton g-factors deduced in this work are also in good agreement with experiment for the bright and dark excitons in monolayer WSe$_2$, as well as the lowest-energy bright excitons in MoSe$_2$-WSe$_2$ heterobilayers with different twist angles.
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