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Register a new userEnhancement of the Monolayer WS2 Exciton Photoluminescence with a 2D-Material/Air/GaP In-Plane Microcavity
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Light-matter interaction with two-dimensional materials gained significant attention in recent years leading to the reporting of weak and strong coupling regimes, and effective nano-laser operation with various structures. Particularly, future applications involving monolayer materials in waveguide-coupled on-chip integrated circuitry and valleytronic nanophotonics require controlling, directing and optimizing photoluminescence. In this context, photoluminescence enhancement from monolayer transition-metal dichalcogenides on patterned semiconducting substrates becomes attractive. It is demonstrated in our work using focussed-ion-beam-etched GaP and monolayer WS2 suspended on hexagonal-BN buffer sheets. We present a unique optical microcavity approach capable of both efficient in-plane and out-of-plane confinement of light, which results in a WS2 photoluminescence enhancement by a factor of 10 compared to the unstructured substrate at room temperature. The key concept is the combination of interference effects in both the horizontal direction using a bulls-eye-shaped circular Bragg grating and in vertical direction by means of a multiple reflection model with optimized etch depth of circular air-GaP structures for maximum constructive interference effects of the applied pump and expected emission light.
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Monolayer WSe$_2$ hosts a series of exciton Rydberg states denoted by the principal quantum number n = 1, 2, 3, etc. While most research focuses on their absorption properties, their optical emission is also important but much less studied. Here we measure the photoluminescence from the 1s - 5s exciton Rydberg states in ultraclean monolayer WSe$_2$ encapsulated by boron nitride under magnetic fields from -31 T to 31 T. The exciton Rydberg states exhibit similar Zeeman shifts but distinct diamagnetic shifts from each other. From their luminescence spectra, Zeeman and diamagnetic shifts, we deduce the binding energies, g-factors and radii of the 1s - 4s exciton states. Our results are consistent with theoretical predictions and results from prior magneto-reflection experiments.
Hyperbolic materials exhibit unique properties that enable a variety of intriguing applications in nanophotonics. The topological insulator Bi2Se3 represents a natural hyperbolic optical medium, both in the THz and visible range. Here, using cathodoluminescence spectroscopy and electron energy-loss spectroscopy, we demonstrate that Bi2Se3, in addition to being a hyperbolic material, supports room-temperature exciton polaritons. Moreover, we explore the behavior of hyperbolic edge exciton polaritons in Bi2Se3. Edge polaritons are hybrid modes that result from the coupling of the polaritons bound to the upper and lower edges of Bi2Se3 nanoplatelets. In particular, we use electron energy-loss spectroscopy to compare Fabry-Perot-like resonances emerging in edge polariton propagation along pristine and artificially structured edges of the nanoplatelets. The experimentally observed scattering of edge polaritons by defect structures was found to be in good agreement with finite-difference time-domain simulations. Moreover, we experimentally proved coupling of localized polaritons in identical open and closed circular nanocavities to the propagating edge polaritons. Our findings are testimony to the extraordinary capability of the hyperbolic polariton propagation to cope with the presence of defects. This provides an excellent basis for applications such as nanooptical circuitry, cloaking at the nanometer scale, as well as nanoscopic quantum technology on the nanoscale.
Two-dimensional (2D) materials and heterostructures have recently gained wide attention due to potential applications in optoelectronic devices. However, the optical properties of the heterojunction have not been properly characterized due to the limited spatial resolution, requiring nano-optical characterization beyond the diffraction limit. Here, we investigate the lateral monolayer MoS2-WS2 heterostructure using tip-enhanced photoluminescence (TEPL) spectroscopy on a non-metallic substrate with picoscale tip-sample distance control. By placing a plasmonic Au-coated Ag tip at the heterojunction, we observed more than three orders of magnitude photoluminescence (PL) enhancement due to the classical near-field mechanism and charge transfer across the junction. The picoscale precision of the distance-dependent TEPL measurements allowed for investigating the classical and quantum tunneling regimes above and below the ~320 pm tip-sample distance, respectively. Quantum plasmonic effects usually limit the maximum signal enhancement due to the near-field depletion at the tip. We demonstrate a more complex behavior at the 2D lateral heterojunction, where hot electron tunneling leads to the quenching of the PL of MoS2, while simultaneously increasing the PL of WS2. Our simulations show agreement with the experiments, revealing the range of parameters and enhancement factors corresponding to various regimes. The controllable photoresponse of the lateral junction can be used in novel nanodevices.
Atomically thin layer transition metal dichalcogenides have been intensively investigated for their rich optical properties and potential applications in nano-electronics. In this work, we study the incoherent optical phonon and exciton population dynamics in monolayer WS2 by time-resolved spontaneous Raman scattering spectroscopy. Upon excitation of the exciton transition, both the Stokes and anti-Stokes optical phonon scattering strength exhibit a large reduction. Based on the detailed balance, the optical phonon population is retrieved, which shows an instant build-up and a relaxation lifetime of around 4 ps at an exciton density E12 cm-2. The corresponding optical phonon temperature rises by 25 K, eventually, after some 10s of picoseconds, leading to a lattice heating by only around 3 K. The exciton relaxation dynamics extracted from the transient vibrational Raman response shows a strong excitation density dependence, signaling an important bi-molecular contribution to the decay. The exciton relaxation rate is found to be (70 ps)-1 and exciton-exciton annihilation rate 0.1 cm2s-1. These results provide valuable insight into the thermal dynamics after optical excitation and enhance the understanding of the fundamental exciton dynamics in two-dimensional transition metal materials.
We report on scattering induced valley polarization enhancement in monolayer molybdenum disulfide. With thermally activated and charge doping introduced scattering, our sample exhibits seven? and twelve-folds of improvements respectively. This counter-intuitive effect is attributed to disruptions to valley pseudospin precession caused by rapid modulation of exciton momentum and concomitant local exchange interaction field, at time scales much shorter than the precession period. In contrast, the valley coherence is improved by thermally activated scattering, but not by charge doping induced scattering. We propose that this is due to anisotropic pseudospin scattering and generalize the Maialle-Silva-Sham model to quantitatively explain our experimental results. Our work illustrates that cleaner samples with minimal scattering, such as those carefully suspended or protected by hexagonal boron nitride, do not necessarily lead to good valley polarization. Well-controlled scattering can in fact provide an interesting approach for improving valleytronic devices.
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