Achieving strong coupling between plasmonic oscillators can significantly modulate their intrinsic optical properties. Here, we report the direct observation of ultrafast plasmonic hot electron transfer from an Au grating array to an MoS2 monolayer in the strong coupling regime between localized surface plasmons (LSPs) and surface plasmon polaritons (SPPs). By means of femtosecond pump-probe spectroscopy, the measured hot electron transfer time is approximately 40 fs with a maximum external quantum yield of 1.65%. Our results suggest that strong coupling between LSPs and SPPs has synergetic effects on the generation of plasmonic hot carriers, where SPPs with a unique nonradiative feature can act as an ‘energy recycle bin’ to reuse the radiative energy of LSPs and contribute to hot carrier generation. Coherent energy exchange between plasmonic modes in the strong coupling regime can further enhance the vertical electric field and promote the transfer of hot electrons between the Au grating and the MoS2 monolayer. Our proposed plasmonic strong coupling configuration overcomes the challenge associated with utilizing hot carriers and is instructive in terms of improving the performance of plasmonic opto-electronic devices.
Molybdenum disulfide (MoS) monolayer as one of the atomic thickness two-dimensional materials has remarkable electronic and optical properties, which is an ideal candidate for a wide range of optoelectronic applications. However, the atomic monolayer thickness poses a significant challenge in MoS photoluminescence emission due to weak light-matter interaction. Here, we investigate the MoS exciton-plasmon interaction with spin-orbit coupling of light. The plasmonic spiral rings with subwavelength dimensions are designed and fabricated on hybrid substrates. MoS photoluminescence enhancement can be actively controlled by changing the incident optical spin states, laser powers, and the nanospiral geometries, which is arising from the change of field enhancement at near-field region. Planar light-emitting devices based on spin-orbit coupling (SOC) effect were further realized and flexibly controlled by changing the polarization of light. The SOC effect is discussed by the accumulation of geometric and dynamic phases, which can be demonstrated and elaborated by the Majorana sphere model. Our results provide a way to manipulate MoS light-matter interaction actively and can be further applied in the spin-dependent light-emitting devices at the nanoscale.
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