No Arabic abstract
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.
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.
Light-matter momentum transfer in plasmonic materials is theoretically discussed in the framework of plasmonic pressure mechanism taking into account non-equilibrium electron dynamics and thermalization process. We show that our approach explains the experimentally observed relationship between the plasmon-related electromotive force and absorption and allows one to correctly predict the magnitude of the plasmon drag emf in flat metal films. We extend our theory to metal films with modulated profiles and show that the simple relationship between plasmonic energy and momentum transfer holds at relatively small amplitudes of height modulation and an approximation of laminar electron drift. Theoretical groundwork is laid for further investigations of shape-controlled plasmon drag in nanostructured metal.
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.
Scattering processes have played a crucial role in the development of quantum theory. In the field of optics, scattering phase shifts have been utilized to unveil interesting forms of light-matter interactions. Here, we investigate the mode-coupling phase of single photons to surface plasmon polaritons in a quantum plasmonic tritter. We observe that the coupling process induces a phase jump that occurs when photons scatter into surface plasmons and vice versa. This interesting coupling phase dynamics is of particular relevance for quantum plasmonic experiments. Furthermore, it is demonstrated that this photon-plasmon interaction can be modeled through a quantum-mechanical tritter. We show that the visibility of a double-slit and a triple-slit interference patterns are convenient observables to characterize the interaction at a slit and determine the coupling phase. Our accurate and simple model of the interaction, validated by simulations and experiments, has important implications not only for quantum plasmonic interference effects, but is also advantageous to classical applications.
We consider a hybrid plasmon-exciton system comprised of a resonant molecular subsystem and three Au wires supporting a dipole mode which can be coupled to a dark mode in controllable fashion by variation of a symmetry parameter. The physics of such a system under strong coupling conditions is examined in detail. It is shown that if two wires supporting the dark mode are covered with molecular layers the system exhibits four resonant modes for a strong coupling regime due to asymmetry and lifted degeneracy of the molecular state in this case, while upon having molecular aggregates covering the top wire with dipolar mode, three resonant modes appear. Pump-probe simulations are performed to scrutinize the quantum dynamics and find possible ways to control plasmon-exciton materials. It is demonstrated that one can design hybrid nanomaterials with highly pronounced Fano-type resonances when excited by femtosecond lasers.