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Register a new userRevealing Strong Plasmon-Exciton Coupling Between Nano-gap Resonators and Two-Dimensional Semiconductors at Ambient Conditions
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Strong coupling of two-dimensional semiconductor excitons with plasmonic resonators enables control of light-matter interaction at the subwavelength scale. Here we develop strong coupling in plasmonic nano-gap resonators that allow modification of exciton number contributing to the coupling. Using this system, we not only demonstrate a large vacuum Rabi splitting up to 163 meV and splitting features in photoluminescence spectra, but also reveal that the exciton number can be reduced down to single-digit level (N<10), which is an order lower than that of traditional systems, close to single-exciton based strong coupling. In addition, we prove that the strong coupling process is not affected by the large exciton coherence size that was previously believed to be detrimental to the formation of plasmon-exciton interaction. Our work provides a deeper understanding of storng coupling in two-dimensional semiconductors, paving the way for room temperature quantum optics applications.
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Plasmon decay via the surface or interface is a critical process for practical energy conversion and plasmonic catalysis. However, the relationship between plasmon damping and the coupling between the plasmon and 2D materials is still unclear. The spectral splitting due to plasmon-exciton interaction impedes the conventional single-particle method to evaluate the plasmon damping rate by the spectral linewidth directly. Here, we investigated the interaction between a single gold nanorod (GNR) and 2D materials using the single-particle spectroscopy method assisted with in situ nanomanipulation technique by comparing scattering intensity and linewidth together. Our approach allows us to indisputably identify that the plasmon-exciton coupling in the GNR-WSe2 hybrid would induce plasmon damping. We can also isolate the contribution between the charge transfer channel and resonant energy transfer channel for the plasmon decay in the GNR-graphene hybrid by comparing that with thin hBN layers as an intermediate medium to block the charge transfer. We find out that the contact layer between the GNR and 2D materials contributes most of the interfacial plasmon damping. These findings contribute to a deep understanding of interfacial excitonic effects on the plasmon and 2D materials hybrid.
Time-resolved Raman spectroscopy techniques offer various ways to study the dynamics of molecular vibrations in liquids or gases and optical phonons in crystals. While these techniques give access to the coherence time of the vibrational modes, they are not able to reveal the fragile quantum correlations that are spontaneously created between light and vibration during the Raman interaction. Here, we present a scheme leveraging universal properties of spontaneous Raman scattering to demonstrate Bell correlations between light and a collective molecular vibration. We measure the decay of these hybrid photon-phonon Bell correlations with sub-picosecond time resolution and find that they survive over several hundred oscillations at ambient conditions. Our method offers a universal approach to generate entanglement between light and molecular vibrations. Moreover, our results pave the way for the study of quantum correlations in more complex solid-state and molecular systems in their natural state.
The phase delay of a local electric field, being well-known in plasmonic nanostructures, has seldom been investigated to modulate the plasmon-exciton interaction. Here, with the single-particle spectroscopy method, we experimentally investigate the phase effect in plasmon-exciton coupling systems consisting of monolayer WSe2 and an individual gold nanorod. The local plasmon phase delay is tuned by adopting various nanorods with different resonant energies respective to the exciton. We find that the local plasmon phase delay between the excitons and the plasmonic modes is as equally essential as the amplitude. The phase delay modulates the plasmon-exciton coupling considerably, resulting in an asymmetric spectral line-shape due to the interference behavior. There is an excellent agreement for the phase delay between the numerically calculated near-field phase distribution and the experimental results. The local phase delay can act as an effective way to modulate the properties of plexcitonic coupling at the nanoscale, which may have potential applications in nanoscale sensing, solar energy devices, and enhancing nonlinear processes.
Polaritonic devices exploit the coherent coupling between excitonic and photonic degrees of freedom to perform highly nonlinear operations with low input powers. Most of the current results exploit excitons in epitaxially grown quantum wells and require low temperature operation, while viable alternatives have yet to be found at room temperature. Here we show that large single-crystal flakes of two-dimensional layered perovskite are able to sustain strong polariton nonlinearities at room temperature with no need to be embedded in an optical cavity. In particular, exciton-exciton interaction energies are measured to be remarkably similar to the ones known for inorganic quantum wells at cryogenic temperatures, and more than one order of magnitude larger than alternative room temperature polariton devices reported so far. Thanks to their easy fabrication, large dipolar oscillator strengths and strong nonlinearities, these materials hold great promises to realize actual polariton devices at room temperature.
Peculiar ring gap modes on the surface of disk close to the metallic thin film are excited in the visible light regime. We apply plasmon hybridization method to illustrate the ring gap modes arising from the interaction between localized disk plasmons and continuum surface plasmons, which cannot be easily excited by the plane wave with polarization parallel to the film interface. In the coupled system, the hybrid modes energy and the surface charge distribution of nanoparticle are investigated both in simulation and hybridization method, showing consistence with each other. The excitation of ring gap modes provides further insight into strong coupling of the plasmon and the design of novel nanostructures.
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