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Register a new userGiant Gating Tunability of Optical Refractive Index in Transition Metal Dichalcogenide Monolayers
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We report that the refractive index of transition metal dichacolgenide (TMDC) monolayers, such as MoS2, WS2, and WSe2, can be substantially tuned by > 60% in the imaginary part and > 20% in the real part around exciton resonances using CMOS-compatible electrical gating. This giant tunablility is rooted in the dominance of excitonic effects in the refractive index of the monolayers and the strong susceptibility of the excitons to the influence of injected charge carriers. The tunability mainly results from the effects of injected charge carriers to broaden the spectral width of excitonic interband transitions and to facilitate the interconversion of neutral and charged excitons. The other effects of the injected charge carriers, such as renormalizing bandgap and changing exciton binding energy, only play negligible roles. We also demonstrate that the atomically thin monolayers, when combined with photonic structures, can enable the efficiencies of optical absorption (reflection) tuned from 40% (60%) to 80% (20%) due to the giant tunability of refractive index. This work may pave the way towards the development of field-effect photonics in which the optical functionality can be controlled with CMOS circuits.
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Electrically-tunable optical properties in materials are desirable for many applications ranging from displays to lasing and optical communication. In most two-dimensional thin-films and other quantum confined materials, these constants have been measured accurately. However, the optical constants of single wall nanotubes (SWCNT) as a function of electrostatic tuning are yet to be measured due to lack of electronic purity and spatial homogeneity over large areas. Here, we measure the basic optical constants of ultrathin high-purity (>99%) semiconducting single wall carbon nanotube (s-SWCNT) films with spectroscopic ellipsometry. We extract the gate-tunable complex refractive index of s-SWCNT films and observe giant modulation of the real refractive index (~11.2% or an absolute value of >0.2) and extinction coefficient (~11.6%) in the near-infrared (IR) region (1.3-1.55 {mu}m) induced by the applied electric field significantly higher than all existing electro-optic semiconductors in this wavelength range. We further design a multilayer IR reflection phase modulator stack by combining s-SWCNT and monolayer MoS2 heterostructures that can attain >45{deg} reflection phase modulation at 1600 nm wavelength for < 200 nm total stack thickness. Our results highlight s-SWCNT as a promising material system for infrared photonics and electro-optics in telecommunication applications.
The rise of quantum science and technologies motivates photonics research to seek new platforms with strong light-matter interactions to facilitate quantum behaviors at moderate light intensities. One promising platform to reach such strong light-matter interacting regimes is offered by polaritonic metasurfaces, which represent ultrathin artificial media structured on nano-scale and designed to support polaritons - half-light half-matter quasiparticles. Topological polaritons, or topolaritons, offer an ideal platform in this context, with unique properties stemming from topological phases of light strongly coupled with matter. Here we explore polaritonic metasurfaces based on 2D transition metal dichalcogenides (TMDs) supporting in-plane polarized exciton resonances as a promising platform for topological polaritonics. We enable a spin-Hall topolaritonic phase by strongly coupling valley polarized in-plane excitons in a TMD monolayer with a suitably engineered all-dielectric topological photonic metasurface. We first show that the strong coupling between topological photonic bands supported by the metasurface and excitonic bands in MoSe2 yields an effective phase winding and transition to a topolaritonic spin-Hall state. We then experimentally realize this phenomenon and confirm the presence of one-way spin-polarized edge topolaritons. Combined with the valley polarization in a MoSe2 monolayer, the proposed system enables a new approach to engage the photonic angular momentum and valley degree of freedom in TMDs, offering a promising platform for photonic/solid-state interfaces for valleytronics and spintronics.
We examine the static non-linear optical response of monolayer transition metal dichalcogenides. Whereas the shift current is suppressed, we identify a strong, valley-dependent non-reciprocal response, which we term a textit{unidirectional valley-contrasting photo-current} (UVCP). It originates from Kramers symmetry breaking by trigonal warping, and its direction is set by the wave vector connecting the two valleys. The UVCP is proportional to the mobility and is enhanced by the excitonic Coulomb interaction and inter-valley scattering, enabling monitoring of inter-valley transitions. We discuss detection strategies in state-of-the-art experiments.
We have investigated the exciton dynamics in transition metal dichalcogenide mono-layers using time-resolved photoluminescence experiments performed with optimized time-resolution. For MoSe2 monolayers, we measure $tau_{rad}=1.8pm0.2$ ps that we interpret as the intrinsic radiative recombination time. Similar values are found for WSe2 mono-layers. Our detailed analysis suggests the following scenario: at low temperature (T $leq$ 50 K), the exciton oscillator strength is so large that the entire light can be emitted before the time required for the establishment of a thermalized exciton distribution. For higher lattice temperatures, the photoluminescence dynamics is characterized by two regimes with very different characteristic times. First the PL intensity drops drastically with a decay time in the range of the picosecond driven by the escape of excitons from the radiative window due to exciton- phonon interactions. Following this first non-thermal regime, a thermalized exciton population is established gradually yielding longer photoluminescence decay times in the nanosecond range. Both the exciton effective radiative recombination and non-radiative recombination channels including exciton-exciton annihilation control the latter. Finally the temperature dependence of the measured exciton and trion dynamics indicates that the two populations are not in thermodynamical equilibrium.
We study theoretically the Coulomb interaction between excitons in transition metal dichalcogenide (TMD) monolayers. We calculate direct and exchange interaction for both ground and excited states of excitons. The screening of the Coulomb interaction, specific to monolayer structures, leads to the unique behavior of the exciton-exciton scattering for excited states, characterized by the non-monotonic dependence of the interaction as function of the transferred momentum. We find that the nontrivial screening enables the description of TMD exciton interaction strength by approximate formula which includes exciton binding parameters. The influence of screening and dielectric environment on the exciton-exciton interaction was studied, showing qualitatively different behavior for ground state and excited states of excitons. Furthermore, we consider exciton-electron interaction, which for the excited states is governed by the dominant attractive contribution of the exchange component, which increases with the excitation number. The results provide a quantitative description of the exciton-exciton and exciton-electron scattering in transition metal dichalcogenides, and are of interest for the design of perspective nonlinear optical devices based on TMD monolayers.
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