We theoretically demonstrate the coupling between excitons in 2D semiconductors and surface plasmons in a thin metal film by means of a surface acoustic wave (SAW), proving that the generated exciton-plasmon polaritons (or plexcitons) are in the strong coupling regime. The strain field of the SAW creates a dynamic diffraction grating providing the momentum match for the surface plasmons, whereas the piezoelectric field, that could dissociate the excitons, is cancelled out by the metal. This is exemplified for monolayer MoS$\mathrm{_{2}}$ and mono- and few-layer black phosphorus on top of a thin silver layer on a LiNbO$\mathrm{_{3}}$ piezoelectric substrate, providing Rabi splittings of 100-150 meV. Thus, we demonstrate that SAWs are powerful tools to modulate the optical properties of supported 2D semiconductors by means of the high-frequency localized deformations tailored by the acoustic transducers, that can serve as electrically switchable launchers of propagating plexcitons suitable for active high-speed nanophotonic applications.
Chirality is a fundamental asymmetry phenomenon, with chiral optical elements exhibiting asymmetric response in reflection or absorption of circularly polarized light. Recent realizations of such elements include nanoplasmonic systems with broken mirror symmetry and polarization-contrasting optical absorption known as circular dichroism. An alternative route to circular dichroism is provided by spin-valley polarized excitons in atomically thin semiconductors. In the presence of magnetic fields, they exhibit an imbalanced coupling to circularly polarized photons and thus circular dichroism. Her…
Strong light-matter interactions between resonantly coupled metal plasmons and spin decoupled bright excitons from two dimensional (2D) transition metal dichalcogenides (TMDs) can produce discrete spin-resolved exciton-plasmon polariton (plexciton). A few efforts have been made to perceive the spin induced exciton-polaritons in nanocavities at cryogenic conditions, however, successful realization of spin-resolved plexciton in time-domain is still lacking. Here, we are able to identify both the spin-resolved plexcitons discretely at room temperature and investigate their ultrafast temporal dyna…
We investigate the propagation of surface plasmons (SPPs) in a thin layer of copper surrounded by copper oxide Cu$_2$O. It is shown that particularly strong excitons in Cu$_2$O can have considerable impact on plasmon propagation, providing many opportunities for plasmon-exciton and plasmon-plasmon interactions. It is demonstrated that by the use of sufficiently thin metal layer, one can excite the so-called long range plasmons (LRSPPs) which can overcome the inherently high ohmic losses of Cu as compared to usual plasmonic metals such as silver. Analytical results are confirmed by numerical ca…
In cavity quantum electrodynamics, optical emitters that are strongly coupled to cavities give rise to polaritons with characteristics of both the emitters and the cavity excitations. We show that carbon nanotubes can be crystallized into chip-scale, two-dimensionally ordered films and that this new material enables intrinsically ultrastrong emitter-cavity interactions: rather than interacting with external cavities, nanotube excitons couple to the near-infrared plasmon resonances of the nanotubes themselves. Our polycrystalline nanotube films have a hexagonal crystal structure, ~25 nm domains…
The multi-scale computational method of combining first-principles calculation and finite element electromagnetic simulations is used to study plasmon-enhanced interlayer charge transfer (ICT) exciton of 2D lateral and van der Waals MoS2/WS2 heterostructure with 2H phase. The weak ICT excitons are observed in the 2H lateral and van der Waals MoS$_2$/WS$_2$ heterostructures. Theoretical results reveal the physical principle of plexciton resulting from strong coupling between plasmonic and ICT exciton. The weak CT exciton can be strongly enhanced by metal plasmon, can provide a new way to observ…
Plasmonic structures are known to support the modes with subwavelength volumes in which the field matter interactions are greatly enhanced. Coupling between the molecular excitations and plasmons leading to formation of plexcitons has been investigated for a number of organic molecules. However, plasmon-exciton coupling in metal semiconductor structures have not experienced the same degree of attention. In this work we show that the very strong coupling regime in which the Rabi energy exceeds the exciton binding energy is attainable in semiconductor cladded plasmonic nanoparticles and leads to…
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 a…
Active control of light-matter interactions in semiconductors is critical for realizing next generation optoelectronic devices, with tunable control of the systems optical properties via external fields. The ability to manipulate optical interactions in active materials coupled to cavities via geometrical parameters, which are fixed along with dynamic control with applied fields opens up possibilities of controlling exciton lifetimes, oscillator strengths and their relaxation properties. Here, we demonstrate electrical control of exciton-plasmon polariton coupling strength of a two-dimensional…
We investigate the dynamics of photon echo exhibited by exciton-plasmon systems under strong coupling conditions. Using a self-consistent model based on coupled Maxwell-Bloch equations we investigate femtosecond time dynamics of ensembles of interacting molecules optically coupled to surface plasmon supporting materials. It is shown that observed photon echoes under two pulse pump-probe sequence are highly dependent on various material parameters such as molecular concentration and periodicity. Simulations of photon echoes in exciton-plasmon materials reveal a unique signature of the strong ex…
Strong exciton-plasmon interaction between the layered two-dimensional (2D) semiconductors and gap plasmons shows a great potential to implement cavity quantum-electrodynamics in ambient condition. However, achieving a robust plasmon-exciton coupling with nanocavity is still very challenging, because the layer area is usually small with conventional approaches. Here, we report on a robust strong exciton-plasmon coupling between the gap mode of bowtie and the excitons in MoS$_2$ layers with gold-assisted mechanical exfoliation and the nondestructive wet transfer techniques for large-area layer.…
The plasmon-mediated manipulation of light-matter interaction in two-dimensional atomically transition-metal dichalcogenides (TMDs) critically depends on the design of plasmonic nanostructures to achieve the maximum optical field in TMDs. Here, a metal-isolator-metal Salisbury-type perfect absorber was fabricated to serve as a generator of the localized surface plasmons. The significant photoluminescence (PL) enhancement up to 60-fold was observed experimentally in the monolayer (ML) MoS2 on the top of this gold plasmonic hybrid nanostructures. Furthermore, the PL linear polarization can appro…
We present a model for exciton-plasmon coupling based on an energy exchange mechanism between quantum emitters (QE) and localized surface plasmons in metal-dielectric structures. Plasmonic correlations between QEs give rise to a collective state exchanging its energy cooperatively with a resonant plasmon mode. By defining carefully the plasmon mode volume for a QE ensemble, we obtain a relation between QE-plasmon coupling and a cooperative energy transfer rate that is expressed in terms of local fields. For a single QE near a sharp metal tip, we find analytically the enhancement factor for QE-…
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-exc…
Hybrid systems of excitons strongly coupled to localized surface plasmons supported by metallic nanoparticles define a new approach to control light-matter interactions. Here, we report exciton-plasmon coupling in two-dimensional (2D) semiconductors, such as MoS2 and WS2, hybridized with silver nanoparticles. Prominent photoluminescence enhancement in monolayer MoS2 was observed with localized surface plasmon resonance (LSPR) tuned to the exciton resonance. By tuning the excitation energy, the contributions from near field enhancement and radiative emission rate enhancement via Purcell effect …
We study theoretically optical response of WS2 monolayer located near periodic metal nanostructured arrays in two and three dimensions. The emphasis of simulations is on the strong coupling regime of excitons supported by WS2 and surface plasmon-polaritons supported by various periodic plasmonic interfaces. It is demonstrated that a monolayer of WS2 placed in a close proximity of periodic arrays of either slits or holes results in a Rabi splitting of the corresponding surface plasmon-polariton resonance as revealed in calculated transmission and reflection spectra. The nonlinear regime, at whi…
Exciton harvesting is demonstrated in an ensemble of quantum emitters coupled to localized surface plasmons. When the interaction between emitters and the dipole mode of a metallic nanosphere reaches the strong coupling regime, the exciton conductance is greatly increased. The spatial map of the conductance matches the plasmon field intensity profile, which indicates that transport properties can be tuned by adequately tailoring the field of the plasmonic resonance. Under strong coupling, we find that pure dephasing can have detrimental or beneficial effects on the conductance, depending on th…
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 conve…
Manipulating strong light-matter interaction in semiconductor microcavities is crucial for developing high-performance exciton polariton devices with great potentials in next-generation all-solid state quantum technologies. In this work, we report surface plasmon enhanced strong exciton-photon interaction in CH3NH3PbBr3 perovskite nanowires. Characteristic anti-crossing behaviors, indicating Rabi splitting energy up to ~ 560 meV, are observed near exciton resonance in hybrid semiconductor-insulator-metallic waveguide cavity at room temperature. An exciton-photon coupling strength enhancement f…
Transport properties of a single plasmon interacting with a hybrid system composed of a semiconductor quantum dot (SQD) and a metal nanoparticle (MNP) coupled to one-dimensional surface plasmonic waveguide are investigated theoretically via the real-space approach. We considered that the MNP-SQD interaction leads to the formation of a hybrid exciton and the transmission and reflection of a single incident plasmon could be controlled by adjusting the frequency of the classical control field applied to the MNP-SQD hybrid nanosystem, the kinds of metallic nanoparticles and the background media, r…
The concept of quantum plasmonic excitations in plasmonic lattices, which similarly to Frenkel excitons in molecular crystals propagate by hopping from one nanoparticle to another, is introduced. A consistent quantum theory of such plasmonic excitons, beginning with the quantization of localized surface plasmons in a metal nanoparticle and including the radiative relaxation in both 1D and 2D lattices near a reflective substrate surface, is developed. A possible room-temperature Bose-Einstein condensation in the quantum gas of plasmonic excitons is also discussed.
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 t…
We develop a non-local dielectric response theory to describe the temperature dependence of exciton lifetime in metal-semiconductor heterostructures. Coupling between excitons and surface plasmons results in a strongly nonmonotonous behaviour of exciton radiative decay rate versus temperature. Tuning the plasmon frequency one can control the efficiency of exciton emission of light.
Just as photons are the quanta of light, plasmons are the quanta of orchestrated charge-density oscillations in conducting media. Plasmon phenomena in normal metals, superconductors and doped semiconductors are often driven by long-wavelength Coulomb interactions. However, in crystals whose Fermi surface is comprised of disconnected pockets in the Brillouin zone, collective electron excitations can also attain a shortwave component when electrons transition between these pockets. Here, we show that the band structure of monolayer transition-metal dichalcogenides gives rise to an intriguing mec…
We present a microscopic model for exciton-induced transparency (ExIT) in a hybrid system comprised of an emitter resonantly coupled to a surface plasmon in a metal-dielectric structure. We obtain an effective optical polarizability of such a system with coupling between the system components expressed in terms of energy transfer rates. We demonstrate that, in the weak coupling regime, the underlying mechanism of ExIT is the energy exchange imbalance between the plasmon and the emitter in a narrow frequency region. We derive in analytic form a frequency-dependent function that accurately descr…
Polaritons are compositional light-matter quasiparticles that have recently enabled remarkable breakthroughs in quantum and nonlinear optics, as well as in material science. Despite the enormous progress, however, a direct nanometer-scale visualization of polaritons has remained an open challenge. Here, we demonstrate that plasmon-exciton polaritons, or plexcitons, generated by a hybrid system composed of an individual silver nanoparticle and a few-layer transition metal dichalcogenide can be spectroscopically mapped with nanometer spatial resolution using electron energy loss spectroscopy in …
Van der Waals materials and heterostructures manifesting strongly bound room temperature exciton states exhibit emergent physical phenomena and are of a great promise for optoelectronic applications. Here, we demonstrate that nanostructured multilayer transition metal dichalcogenides by themselves provide an ideal platform for excitation and control of excitonic modes, paving the way to exciton-photonics. Hence, we show that by patterning the TMDCs into nanoresonators, strong dispersion and avoided crossing of excitons and hybrid polaritons with interaction potentials exceeding 410 meV may be …
We present a microscopic model describing the transition to strong coupling regime for an emitter resonantly coupled to a surface plasmon in a metal-dielectric structure. We demonstrate that the shape of scattering spectra is determined by an interplay of two distinct mechanisms. First is the near-field coupling between the emitter and the plasmon mode which underpins energy exchange between the system components and gives rise to exciton-induced transparency minimum in scattering spectra prior the transition to strong coupling regime. The second mechanism is Fano interference between the plas…
The realization and control of polaritons is of paramount importance in the prospect of novel photonic devices. Here, we investigate the emergence of plasmon-exciton polaritons in hybrid structures consisting of a two-dimensional (2D) transition metal dichalcogenide (TMDC) deposited onto a metal substrate or coating a metallic thin-film. We determine the polaritonic spectrum and show that, in the former case, the addition of a top dielectric layer, and, in the latter, the thickness of the metal film,can be used to tune and promote plasmon-exciton interactions well within the strong coupling re…
Metallic nanostructures provide a toolkit for the generation of coherent light below the diffraction limit. Plasmonic based lasing relies on the population inversion of emitters (such as organic fluorophores) along with feedback provided by plasmonic resonances. In this regime, known as weak light matter coupling, the radiative characteristics of the system can be described by the Purcell effect. Strong light matter coupling between the molecular excitons and electromagnetic field generated by the plasmonic structures leads to the formation of hybrid quasi-particles known as plasmon exciton po…
We study theoretically the interactions of excitonic states with surface electromagnetic modes of small-diameter (~1 nm) semiconducting single-walled carbon nanotubes. We show that these interactions can result in strong exciton-surface-plasmon coupling. The exciton absorption lineshapes exhibit the line (Rabi) splitting $~0.1-0.3$ eV as the exciton energy is tuned to the nearest interband surface plasmon resonance of the nanotube. We expect this effect to open a path to new optoelectronic device applications of semiconducting carbon nanotubes.
We simulate the near-field effects of strong coupling between molecular excitons and localized surface plasmons, supported by aluminum nanodisks. The simulations are done using a simple model of a two-level system, implemented in a commercial electromagnetic finite-difference time-domain solver. While the Rabi splitting is present in the near-field, its spectral gap is seen to be smaller than the one obtained in the far-field, although it follows a clear square root dependence on the molecular density as expected. Moreover, the energy exchange between the plasmonic mode and the excitonic mater…
We study theoretically the interactions of excitonic states with surface electromagnetic modes of small-diameter (~1 nm) semiconducting single-walled carbon nanotubes. We show that these interactions can result in strong exciton-surface-plasmon coupling. The exciton absorption line shape exhibits Rabi splitting ~0.1 eV as the exciton energy is tuned to the nearest interband surface plasmon resonance of the nanotube. We also show that the quantum confined Stark effect may be used as a tool to control the exciton binding energy and the nanotube band gap in carbon nanotubes in order, e.g., to bri…
In this article, we explore the anisotropic electron energy loss spectrum (EELS) in monolayer phosphorene based on ab-initio time dependent density functional theory calculations. Similar to black phosphorous, the EELS of undoped monolayer phosphorene is characterized by anisotropic excitonic peaks for energies in vicinity of the bandgap, and by interband plasmon peaks for higher energies. On doping, an additional intraband plasmon peak also appears for energies within the bandgap. Similar to other two dimensional systems, the intraband plasmon peak disperses as $ω_{\rm pl} \propto \sqrt{q}$ i…
Photonic integrated circuits are an enabling technology in modern communications systems. The continually increasing demands for higher-speed and lower operating power devices have resulted in the continued impetus to shrink photonic components. In this work, we demonstrate a primitive nanophotonic integrated circuit element composed of a single silver nanowire and single-layer molybdenum disulfide (MoS2) flake. We show that nanowire plasmons can excite MoS2 photoluminescence via direct plasmon-to-exciton conversion along the wire and plasmon-to-photon-to-exciton conversion at the MoS2-covered…
Plasmon exciton coupling enhances second order nonlinear response in borophene ZnO hybrid structures
Institute of Experimental and Applied Physics, Kiel University（基尔大学实验与应用物理研究所）；Department of Physics, University of Tehran（德黑兰大学物理系）；Kiel Nano, Surface, and Interface Science KiNSIS, Kiel University（基尔大学基尔纳米、表面与界面科学(KiNSIS)）
Two dimensional (2D) semiconductor materials of transition-metal dichalcogenides (TMDCs) manifest many peculiar physical phenomena in the light-matter interaction. Due to their ultrathin property, strong interaction with light and the robust excitons at room temperature, they provide a perfect platform for studying the physics of strong coupling in low dimension and at room temperature. Here we report the strong coupling between 2D semiconductor excitons and Tamm plasmon polaritons (TPPs). We observe a Rabi splitting of about 54 meV at room temperature by measuring the angle resolved different…
Polaritons are quasiparticles arising from the strong coupling of electromagnetic waves in cavities and dipolar oscillations in a material medium. In this framework, localized surface plasmon in metallic nanoparticles defining optical nanocavities have attracted increasing interests in the last decade. This interest results from their sub-diffraction mode volume, which offers access to extremely high photonic densities by exploiting strong scattering cross-sections. However, high absorption losses in metals have hindered the observation of collective coherent phenomena, such as condensation. I…
We study the transfer of electromagnetic energy across a subwavelength gap separating two co-axial metal nanorodes. The absence of spacer in the gap separating the rods the system exhibits the strong coupling between longitudinal plasmons in the two rods. The nature and magnitude of this coupling is studied by varying various geometrical parameters. When the length of one rod is varied this mode spectrum exhibits the familiar anti-crossing behavior that depends on the coupling strength determined by the gap width. As a function of frequency the transmission is dominated by a splitted longitudi…
Coherent energy exchange between plasmons and excitons is a phenomenon that arises in the strong coupling regime resulting in distinct hybrid states. The DNA-origami technique provides an ideal framework to custom-tune plasmon-exciton nanostructures. By employing this well controlled self-assembly process, we realized hybrid states by precisely positioning metallic nanoparticles in a defined spatial arrangement with fixed nanometer-sized interparticle spacing. Varying the nanoparticle diameter between 30 nm and 60 nm while keeping their separation distance constant allowed us to precisely adju…
We demonstrate the strong coupling of direct transition excitons in tungsten disulfide (WS2) with collective plasmonic resonances at room temperature. We use open plasmonic cavities formed by periodic arrays of metallic nanoparticles. We show clear anti-crossings with monolayer, bilayer and thicker multilayer WS2 on top of the nanoparticle array. The Rabi energy of such hybrid system varies from 50 to 110 meV from monolayer to sixteen layers, while it does not scale with the square root of the number of layers as expected for collective strong coupling. We prove that out-of-plane coupling comp…
The design of novel functional materials in silico is severely hampered by the lack of robust and computationally efficient methods for describing both molecular absorbance and screening on substrates. Here we employ our hybrid $G_0[W_0+ΔW]$-BSE implementation, which incorporates the substrate via its screening $ΔW$ at both the quasiparticle $G_0W_0$ level and when solving the Bethe-Salpeter equation (BSE). We show this method can be used to both efficiently and accurately describe the absorption spectra of physisorbed molecules on metal substrates and thereby tailor the molecule's absorbance …
Realizing strong light-matter interactions between individual 2-level systems and resonating cavities in atomic and solid state systems opens up possibilities to study optical nonlinearities on a single photon level, which can be useful for future quantum information processing networks. However, these efforts have been hampered by the unfavorable experimental conditions, such as cryogenic temperatures and ultrahigh vacuum, required to study such systems and phenomena. Although several attempts to realize strong light-matter interactions at room-temperature using so-called plasmon resonances h…
Strong interactions between surface plasmons in ultra-compact nanocavities and excitons in two dimensional materials have attracted wide interests for its prospective realization of polariton devices at room temperature. Here, we propose a continuous transition from weak coupling to strong coupling between excitons in MoS2 monolayer and highly localized plasmons in ultra-compact nanoantenna. The nanoantenna is assembled by a silver nanocube positioned over a gold film and separated by a dielectric spacer layer. We observed a 1570-fold enhancement in the photoluminescence at weak coupling regim…
The radiative decay of quantum dot (QD) excitons into surface plasmons in a cylindrical nanowire is investigated theoretically. Maxwell's equations with appropriate boundary conditions are solved numerically to obtain the dispersion relations of surface plasmons. The radiative decay rate of QD excitons is found to be greatly enhanced at certain values of the exciton bandgap. Analogous to the decay of a two-level atom in the photonic crystal, we first point out that such an enhanced phenomenon allows one to examine the non-Markovian dynamics of the QD exciton. Besides, due to the one dimensiona…
Resonant optical excitation was used to create a macroscopic non-equilibrium ensemble of dark excitons with unprecedentedly long lifetime in a two-dimensional (2D) electron system placed in a quantizing magnetic field. Exotic three-particle and four-particle states, plasmarons and plasmon-exciton molecules, coupled with the surrounding electrons through the collective plasma oscillations are engineered. Plasmarons and plasmon-exciton molecules are manifested as new features in the recombination spectra of non-equilibrium systems. Magnetoplasmarons and magnetotrions in a two-dimensional Hall in…
Solid state cavity quantum electrodynamics is a rapidly advancing field which explores the frontiers of light-matter coupling. Plasmonic approaches are of particular interest in this field, since they carry the potential to squeeze optical modes to spaces significantly below the diffraction limit1,2, enhancing light-matter coupling. They further serve as an architecture to design ultra-fast, non-linear integrated circuits with smallest footprints3. Transition metal dichalcogenides are ideally suited as the active material in such circuits as they interact strongly with light at the ultimate mo…
We consider the effect of electromagnetic coupling between localized surface plasmons in a metallic nanoparticle (NP) and excitons or weakly interacting electron-hole pairs in a semiconductor matrix where the NP is embedded. An expression is derived for the NP polarizability renormalized by this coupling and two possible situations are analyzed, both compatable with the conditions for Fano-type resonances: (i) a narrow bound exciton transition overlapping with the NP surface plasmon resonance (SPR), and (ii) SPR overlapping with a parabolic absorption band due to electron-hole transitions in t…
Strong spatial confinement and highly reduced dielectric screening provide monolayer transition metal dichalcogenides (TMDCs) with strong many-body effects, thereby possessing optically forbidden excitonic states (i.e., dark excitons) at room temperature. Herein, we explore the interaction of surface plasmons with dark excitons in hybrid systems consisting of stacked gold nanotriangles (AuNTs) and monolayer WS2. We observe a narrow Fano resonance when the hybrid system is surrounded by water, and we attribute the narrowing of the spectral Fano linewidth to the plasmon-enhanced decay of dark K-…
Using the ultrafast pump-probe transient absorption spectroscopy, the femtosecond-resolved plasmon-exciton interaction of graphene-Ag nanowire hybrids is experimentally investigated, in the VIS-NIR region. The plasmonic lifetime of Ag nanowire is about 150 femtosecond (fs). For a single layer of graphene, the fast dynamic process at 275 fs is due to the excitation of graphene excitons, and the slow process at 1.4 picosecond (ps) is due to the plasmonic hot electron interaction with phonons of graphene. For the graphene-Ag nanowire hybrids, the time scale of the plasmon-induced hot electron tra…
