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Register a new userLinear and nonlinear optics of hybrid plasmon-exciton nanomaterials in the presence of overlapping resonances
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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.
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The detailed understanding of the physical parameters that determine Localized Surface Plasmon Resonances (LSPRs) is essential to develop new applications for plasmonics. A relatively new area of research has been opened by the identification of LSPRs in low carrier density systems obtained by doping semiconductor quantum dots. We investigate theoretically how diffuse surface scattering of electrons in combination with the effect of quantization due to size (QSE) impact the evolution of the LSPRs with the size of these nanosystems. Two key parameters are the length $R_0$ giving the strength of the QSE and the velocity $beta_T$ of the electronic excitations entering in the length scale for diffuse surface scattering. While the QSE itself only produces a blueshift in energy of the LSPRs, the diffuse surface scattering mechanism gives to both energy and linewidth an oscillatory-damped behavior as a function of size, with characteristic lengths that depend on material parameters. Thus, the evolution of the LSPRs with size at the nanometer scale is very dependent on the relation of size to these lengths, which we illustrate with several examples. The variety of behaviors we find could be useful for designing plasmonic devices based on doped semiconductor nano structures having desired properties.
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.
Carbon nanotubes provide a rare access point into the plasmon physics of one-dimensional electronic systems. By assembling purified nanotubes into uniformly sized arrays, we show that they support coherent plasmon resonances, that these plasmons enhance and hybridize with phonons, and that the phonon-plasmon resonances have quality factors as high as 10. Because coherent nanotube plasmonics can strengthen light-matter interactions, it provides a compelling platform for surface-enhanced infrared spectroscopy and tunable, high-performance optical devices at the nanometer scale.
Optical control of electronic spins is the basis for ultrafast spintronics: circularly polarized light in combination with spin-orbit coupling of the electronic states allows for spin manipulation in condensed matter. However, the conventional approach is limited to spin orientation along one particular orientation that is dictated by the direction of photon propagation. Plasmonics opens new capabilities, allowing one to tailor the light polarization at the nanoscale. Here, we demonstrate ultrafast optical excitation of electron spin on femtosecond time scales via plasmon to exciton spin conversion. By time-resolving the THz spin dynamics in a hybrid (Cd,Mn)Te quantum well structure covered with a metallic grating, we unambiguously determine the orientation of the photoexcited electron spins which is locked to the propagation direction of surface plasmon-polaritons. Using the spin of the incident photons as additional degree of freedom, one can orient the photoexcited electron spin at will in a two-dimensional plane.
We predict the simultaneous occurrence of two fundamental phenomena for metal nanoparticles possessing sharp corners: First, the main plasmonic dipolar mode experiences strong red shift with decreasing corner curvature radius; its resonant frequency is controlled by the apex angle of the corner and the normalized (to the particle size) corner curvature. Second, the split-off plasmonic mode experiences strong localization at the corners. Altogether, this paves the way for tailoring of metal nano-structures providing wavelength-selective excitation of localized plasmons and a strong near-field enhancement of linear and nonlinear optical phenomena.
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