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Register a new userUnveiling the optical emission channels of monolayer semiconductors coupled to silicon nanoantennas
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Monolayers (MLs) of transition metal dichalcogenides (TMDs) such as WSe2 and MoSe2 can be placed by dry stamping directly on broadband dielectric resonators, which have the ability to enhance the spontaneous emission rate and brightness of solid-state emitters at room temperature. We show strongly enhanced emission and directivity modifications in room temperature photoluminescence mapping experiments. By varying TMD material (WSe2 versus MoSe2) transferred on silicon nanoresonators with various designs (planarized versus non-planarized), we experimentally separate the different physical mechanisms that govern the global light emission enhancement. For WSe2 and MoSe2 we address the effects of Mie Resonances and strain in the monolayer. For WSe2 an important additional contribution comes from out-of-plane exciton dipoles. This paves the way for more targeted designs of TMD-Si nanoresonator structures for room temperature applications.
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We present quantum yield measurements of single layer $textrm{WSe}_2$ (1L-$textrm{WSe}_2$) integrated with high-Q ($Q>10^6$) optical microdisk cavities, using an efficient ($eta>$90%) near-field coupling scheme based on a tapered optical fiber. Coupling of the excitonic emission is achieved by placing 1L-WSe$_2$ to the evanescent cavity field. This preserves the microresonator high intrinsic quality factor ($Q>10^6$) below the bandgap of 1L-WSe$_2$. The nonlinear excitation power dependence of the cavity quantum yield is in agreement with an exciton-exciton annihilation model. The cavity quantum yield is $textrm{QY}_textrm{c}sim10^{-3}$, consistent with operation in the textit{broad emitter} regime (i.e. the emission lifetime of 1L-WSe$_2$ is significantly shorter than the bare cavity decay time). This scheme can serve as a precise measurement tool for the excitonic emission of layered materials into cavity modes, for both in plane and out of plane excitation.
Optically generated excitons dictate the absorption and emission spectrum of doped semiconductor transition metal dichalcogenide monolayers. We show that upon increasing the electron density, the elementary optical excitations develop a roton-like dispersion, evidenced by a shift of the lowest energy state to a finite momentum on the order of the Fermi momentum. This effect emerges due to Pauli exclusion between excitons and the electron Fermi sea, but the robustness of the roton minimum in these systems is a direct consequence of the long-range nature of the Coulomb interaction and the nonlocal dielectric screening characteristic of monolayers. Finally, we show that the emergence of rotons could be related to hitherto unexplained aspects of photoluminescence spectra in doped transition metal dichalcogenide monolayers.
The optoelectronic properties of atomically thin transition-metal dichalcogenides are strongly correlated with the presence of defects in the materials, which are not necessarily detrimental for certain applications. For instance, defects can lead to an enhanced photoconduction, a complicated process involving charge generation and recombination in the time domain and carrier transport in the spatial domain. Here, we report the simultaneous spatial and temporal photoconductivity imaging in two types of WS2 monolayers by laser-illuminated microwave impedance microscopy. The diffusion length and carrier lifetime were directly extracted from the spatial profile and temporal relaxation of microwave signals respectively. Time-resolved experiments indicate that the critical process for photo-excited carriers is the escape of holes from trap states, which prolongs the apparent lifetime of mobile electrons in the conduction band. As a result, counterintuitively, the photoconductivity is stronger in CVD samples than exfoliated monolayers with a lower defect density. Our work reveals the intrinsic time and length scales of electrical response to photo-excitation in van der Waals materials, which is essential for their applications in novel optoelectronic devices.
Deterministically integrating semiconductor quantum emitters with plasmonic nano-devices paves the way towards chip-scale integrable, true nanoscale quantum photonics technologies. For this purpose, stable and bright semiconductor emitters are needed, which moreover allow for CMOS-compatibility and optical activity in the telecommunication band. Here, we demonstrate strongly enhanced light-matter coupling of single near-surface ($<10,nm$) InAs quantum dots monolithically integrated into electromagnetic hot-spots of sub-wavelength sized metal nanoantennas. The antenna strongly enhances the emission intensity of single quantum dots by up to $sim16times$, an effect accompanied by an up to $3.4times$ Purcell-enhanced spontaneous emission rate. Moreover, the emission is strongly polarised along the antenna axis with degrees of linear polarisation up to $sim85,%$. The results unambiguously demonstrate the efficient coupling of individual quantum dots to state-of-the-art nanoantennas. Our work provides new perspectives for the realisation of quantum plasmonic sensors, step-changing photovoltaic devices, bright and ultrafast quantum light sources and efficent nano-lasers.
Optical bound states in the continuum (BICs) provide a way to engineer very narrow resonances in photonic crystals. The extended interaction time in such systems is particularly promising for enhancement of nonlinear optical processes and development of the next generation of active optical devices. However, the achievable interaction strength is limited by the purely photonic character of optical BICs. Here, we mix optical BIC in a photonic crystal slab with excitons in atomically thin semiconductor MoSe$_2$ to form nonlinear exciton-polaritons with a Rabi splitting of 27~meV, exhibiting large interaction-induced spectral blueshifts. The asymptotic BIC-like suppression of polariton radiation into far-field towards the BIC wavevector, in combination with effective reduction of excitonic disorder through motional narrowing, results in small polariton linewidths below 3~meV. Together with strongly wavevector-dependent Q-factor, this provides for enhancement and control of polariton--polariton interactions and resulting nonlinear optical effects, paving the way towards tunable BIC-based polaritonic devices for sensing, lasing, and nonlinear optics.
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