Dynamic Ultrastrong Coupling in a 2 nm Gap Plasmonic Cavity at the Sub-Picosecond Scale.

Localized surface plasmon resonances (LSPRs) can enhance the electromagnetic fields on metallic nanostructures upon light illumination, providing an approach for manipulating light-matter interactions at the sub-wavelength scale. However, currently, there is no thorough investigation of the physical mechanism in the dynamic formation of the strongly coupled LSPRs on sub-5 nm plasmonic cavities at the sub-picosecond scale. In this work, through femtosecond broadband transient absorption spectroscopy, we reveal the dynamic ultrastrong coupling processes in a nanoparticle-in-trench (NPiT) structure containing 2 nm gap cavities, and demonstrate a coherent motional coupling between vibrating AuNPs and the nanogaps. We achieve a maximum Rabi splitting energy of ∼660 meV in the sub-picosecond hot-electron relaxation time scale under the resonant excitation of the nanogap cavity's LSPR, reaching the ultrastrong coupling regime. This leads to a change of global vibration modes for the 2 nm gap cavity, potentially related to the dynamical Casimir effect with nanogap resonators.

Mode-Specific Coupling of Nanoparticle-on-Mirror Cavities with Cylindrical Vector Beams.

Nanocavities formed by ultrathin metallic gaps permit the reproducible engineering and enhancement of light-matter interaction, with mode volumes reaching the smallest values allowed by quantum mechanics. While the enhanced vacuum field in metallic nanogaps has been firmly evidenced, fewer experimental reports have examined the far-field to near-field input coupling under strongly focused laser beam. Here, we experimentally demonstrate selective excitation of nanocavity modes controlled by the polarization and frequency of the laser beam. We reveal mode selectivity by recording confocal maps of Raman scattering excited by cylindrical vector beams, which are compared to the known excitation near-field patterns. Our measurements reveal the transverse vs longitudinal polarization of the excited antenna mode and how the input coupling rate depends on laser wavelength. The method introduced here is easily applicable to other experimental scenarios, and our results help connect far-field with near-field parameters in quantitative models of nanocavity-enhanced phenomena.

Molecular Polaritonics: Chemical Dynamics Under Strong Light-Matter Coupling.

Chemical manifestations of strong light-matter coupling have recently been a subject of intense experimental and theoretical studies. Here we review the present status of this field. Section 1 is an introduction to molecular polaritonics and to collective response aspects of light-matter interactions. Section 2 provides an overview of the key experimental observations of these effects, while Section 3 describes our current theoretical understanding of the effect of strong light-matter coupling on chemical dynamics. A brief outline of applications to energy conversion processes is given in Section 4. Pending technical issues in the construction of theoretical approaches are briefly described in Section 5. Finally, the summary in Section 6 outlines the paths ahead in this exciting endeavor.

Plasmonic Nanocavity Induced Coupling and Boost of Dark Excitons in Monolayer WSe2 at Room Temperature.

Spin-forbidden excitons in monolayer transition metal dichalcogenides are optically inactive at room temperature. Probing and manipulating these dark excitons are essential for understanding exciton spin relaxation and valley coherence of these 2D materials. Here, we show that the coupling of dark excitons to a metal nanoparticle-on-mirror cavity leads to plasmon-induced resonant emission with the intensity comparable to that of the spin-allowed bright excitons. A three-state quantum model combined with full-wave electrodynamic calculations reveals that the radiative decay rate of the dark excitons can be enhanced by nearly 6 orders of magnitude through the Purcell effect, therefore compensating its intrinsic nature of weak radiation. Our nanocavity approach provides a useful paradigm for understanding the room-temperature dynamics of dark excitons, potentially paving the road for employing dark exciton in quantum computing and nanoscale optoelectronics.

Hyperbolic Cooper-Pair Polaritons in Planar Graphene/Cuprate Plasmonic Cavities.

Hyperbolic Cooper-pair polaritons (HCP) in cuprate superconductors are of fundamental interest due to their potential for providing insights into the nature of unconventional superconductivity. Here, we critically assess an experimental approach using near-field imaging to probe HCP in Bi2Sr2CaCu2O8+x (Bi-2212) in the presence of graphene surface plasmon polaritons (SPP). Our simulations show that inherently weak HCP features in the near-field can be strongly enhanced when coupled to graphene SPP in layered graphene/hexagonal boron nitride (hBN)/Bi-2212 heterostructures. This enhancement arises from our multilayered structures effectively acting as plasmonic cavities capable of altering collective modes of a layered superconductor by modifying its electromagnetic environment. The degree of enhancement can be selectively controlled by tuning the insulating spacer thickness with atomic precision. Finally, we verify the expected renormalization of room-temperature graphene SPP using near-field infrared imaging. Our modeling, augmented with data, attests to the validity of our approach for probing HCP modes in cuprate superconductors.

Exploring the Magnetic and Electric Side of Light through Plasmonic Nanocavities.

Light-matter interactions are often considered to be mediated by the electric component of light only, neglecting the magnetic contribution. However, the electromagnetic energy density is equally distributed between both parts of the optical fields. Within this scope, we experimentally demonstrate here, in excellent agreement with numerical simulations, that plasmonic nanostructures can selectively manipulate and tune the magnetic versus electric emission of luminescent nanocrystals. In particular, we show selective enhancement or decay of magnetic and electric emission from trivalent europium-doped nanoparticles in the vicinity of plasmonic nanocavities, designed to efficiently couple to either the electric or magnetic emission of the quantum emitter. Specifically, by precisely controlling the spatial position of the emitter with respect to our plasmonic nanostructures, by means of a near-field optical microscope, we record local distributions of both magnetic and electric radiative local densities of states (LDOS) with nanoscale precision. The distribution of the radiative LDOS reveals the modification of both the magnetic and electric optical quantum environments induced by the presence of the metallic nanocavities. This manipulation and enhancement of magnetic light-matter interaction by means of plasmonic nanostructures opens up new possibilities for the research fields of optoelectronics, chiral optics, nonlinear and nano-optics, spintronics, and metamaterials, among others.

Single quantum dot controls a plasmonic cavity's scattering and anisotropy.

Plasmonic cavities represent a promising platform for controlling light-matter interaction due to their exceptionally small mode volume and high density of photonic states. Using plasmonic cavities for enhancing light's coupling to individual two-level systems, such as single semiconductor quantum dots (QD), is particularly desirable for exploring cavity quantum electrodynamic (QED) effects and using them in quantum information applications. The lack of experimental progress in this area is in part due to the difficulty of precisely placing a QD within nanometers of the plasmonic cavity. Here, we study the simplest plasmonic cavity in the form of a spherical metallic nanoparticle (MNP). By controllably positioning a semiconductor QD in the close proximity of the MNP cavity via atomic force microscope (AFM) manipulation, the scattering spectrum of the MNP is dramatically modified due to Fano interference between the classical plasmonic resonance of the MNP and the quantized exciton resonance in the QD. Moreover, our experiment demonstrates that a single two-level system can render a spherical MNP strongly anisotropic. These findings represent an important step toward realizing quantum plasmonic devices.

Accurate Transfer of Individual Nanoparticles onto Single Photonic Nanostructures.

Controlled integration of metallic nanoparticles (NPs) onto photonic nanostructures enables the realization of complex devices for extreme light confinement and enhanced light-matter interaction. For instance, such NPs could be massively integrated on metal plates to build nanoparticle-on-mirror (NPoM) nanocavities or photonic integrated waveguides (WGs) to build WG-driven nanoantennas. However, metallic NPs are usually deposited via drop-casting, which prevents their accurate positioning. Here, we present a methodology for precise transfer and positioning of individual NPs onto different photonic nanostructures. Our method is based on soft lithography printing that employs elastomeric stamp-assisted transfer of individual NPs onto a single nanostructure. It can also parallel imprint many individual NPs with high throughput and accuracy in a single step. Raman spectroscopy confirms enhanced light-matter interactions in the resulting NPoM-based nanophotonic devices. Our method mixes top-down and bottom-up nanofabrication techniques and shows the potential of building complex photonic nanodevices for multiple applications ranging from enhanced sensing and spectroscopy to signal processing.

Revealing Nanostructures through Plasmon Polarimetry.

Polarized optical dark-field spectroscopy is shown to be a versatile noninvasive probe of plasmonic structures that trap light to the nanoscale. Clear spectral polarization splittings are found to be directly related to the asymmetric morphology of nanocavities formed between faceted gold nanoparticles and an underlying gold substrate. Both experiment and simulation show the influence of geometry on the coupled system, with spectral shifts Δλ = 3 nm from single atoms. Analytical models allow us to identify the split resonances as transverse cavity modes, tightly confined to the nanogap. The direct correlation of resonance splitting with atomistic morphology allows mapping of subnanometre structures, which is crucial for progress in extreme nano-optics involving chemistry, nanophotonics, and quantum devices.