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.
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…
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…
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…
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…
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 …
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…
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 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…
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 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…
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…
We demonstrate strong exciton-plasmon coupling in silver nanodisk arrays integrated with monolayer MoS2 via angle-resolved reflectance microscopy spectra of the coupled system. Strong exciton-plasmon coupling is observed with the exciton-plasmon coupling strength up to 58 meV at 77 K, which also survives at room temperature. The strong coupling involves three types of resonances: MoS2 excitons, localized surface plasmon resonances (LSPRs) of individual silver nanodisks and plasmonic lattice resonances of the nanodisk array. We show that the exciton-plasmon coupling strength, polariton composit…
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…
We report on the strong coupling between inorganic quantum well excitons and surface plasmons. For that purpose a corrugated silver film was deposited on the top of a heterostructure consisting of GaAs/GaAlAs quantum wells. The formation of plasmon/heavy-hole exciton/light-hole exciton mixed states is demonstrated with reflectometry experiments. The interaction energies amount to 21 meV for the plasmon/light-hole exciton and 22 meV for the plasmon/heavy-hole exciton. Some particularities of the plasmon-exciton coupling were also discussed and qualitatively related to the plasmon polarization.
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…
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 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-…
We have studied theoretically the exciton-plasmon coupling effects on the third-order optical nonlinearity of a coherently coupled hybrid system of a metal nanoparticle and a semiconductor quantum dot in the presence of a strong control field with a weak probe field.
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…
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…
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 thi…
We investigate second harmonic generation (SHG) from hexagonal periodic arrays of triangular nano-holes of aluminum using a self-consistent methodology based on the hydrodynamics-Maxwell-Bloch approach. It is shown that angular polarization patterns of the far-field second harmonic response abide to three-fold symmetry constraints on tensors. When a molecular layer is added to the system and its parameters are adjusted to achieve the strong coupling regime between a localized plasmon mode and molecular excitons, Rabi splitting is observed from occurrence of both single- and two-photon transiti…
The optical response of an artificial hybrid molecule system composed of two metallic nanoparticles (MNPs) and a semiconductor quantum dot (SQD) is investigated theoretically due to the plasmon-exciton-plasmon coupling effects on the absorption properties of the hybrid nanosystem, which depends on the interaction between the induced dipole moments in the SQD and the MNPs, respectively. We show that the strong coupling of exciton and localized surface plasmons in such a hybrid molecules leads to appealing, tunable optical properties by adjusting the symmetry of the hybrid molecule nanosystem wi…
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…
Polarization dependence of the exciton-plasmon-photon conversion in silver nanowire-quantum dots structure was investigated using a scanning confocal microscope system. We found that the fluorescence enhancement of the CdSe nanocrystals was correlated with the angle between the excitation light polarization and the silver nanowire direction. The polarization of the emission was also related with the nanowire direction. It was in majority in the direction parallel with nanowire.
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…
We extend the model of exciton-plasmon materials to include a ro-vibrational structure of molecules using wave-packet propagations on electronic potential energy surfaces. The new model replaces conventional two-level emitters with more complex molecules allowing to examine the influence of alignment and vibrational dynamics on strong coupling with surface plasmon-polaritons. We apply the model to a hybrid system comprising a thin layer of molecules placed on top of a periodic array of slits. Rigorous simulations are performed for two types of molecular systems described by vibrational bound-b…
Polaritons are compositional light-matter quasiparticles that arise as a result of strong coupling between a vacuum field of a resonant optical cavity and electronic excitations in quantum emitters. Reaching such a regime is often hard, as it requires materials possessing high oscillator strengths to interact with the relevant optical mode. Two dimensional transition metal dichalcogenides (TMDs) have recently emerged as promising candidates for realization of the strong coupling regime at room temperature. However, these materials typically provide coupling strengths in the range of 10-40 meV,…
Formation of dressed light-matter states in optical structures, manifested as Rabi splitting of the eigen energies of a coupled system, is one of the key effects in quantum optics. In pursuing this regime with semiconductors, light is usually made to interact with excitons $-$ electrically neutral quasiparticles of semiconductors, meanwhile interactions with charged three-particle states $-$ trions $-$ have received little attention. Here, we report on strong interaction between plasmons in silver nanoprisms and charged excitons $-$ trions $-$ in monolayer tungsten disulphide (WS$_{2}$). We sh…
We demonstrate that plasmons in graphene can be manipulated using a DC current. A source-drain current lifts the forward/backward degeneracy of the plasmons, creating two modes with different propagation properties parallel and antiparallel to the current. We show that the propagation length of the plasmon propagating parallel to the drift current is enhanced, while the propagation length for the antiparallel plasmon is suppressed. We also investigate the scattering of light off graphene due to the plasmons in a periodic dielectric environment and we find that the plasmon resonance separates i…
Plasmonic nanopatch antennas that incorporate dielectric gaps hundreds of picometers to several nanometers thick have drawn increasing attention over the past decade because they confine electromagnetic fields to grossly sub-diffraction limited volumes. Substantial control over the optical properties of excitons and color centers confined within these plasmonic cavities has already been demonstrated with far-field optical spectroscopies, but near-field optical spectroscopies are essential to an improved understanding of the plasmon-emitter interaction at the nanoscale. Here, we characterize th…
In coupled quantum systems pure dephasing mechanisms acting on one constituent of the hybrid system break symmetry and enable optical transitions which are forbidden in the non-coupled system, i.e., the pure dephasing bath opens a cascaded dissipation pathway. Here we show that this mechanism enables single-photon induced parametric down-conversion in an ultrastrongly coupled plasmon-exciton system. Fast pure dephasing of the exciton is shown to support photon pair generation as the dominant energy relaxation pathway.
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…
The evidence of strong coupling between plasmons and molecular excitons for plasmonic nanoparticle (NP) dimers exhibiting ultra-sensitive surface enhanced resonant Raman scattering is the observation of anti-crossing in the coupled resonance. However, it is not easy to experimentally tune plasmon resonance of such dimers for the observation. In this work, we theoretically investigate the anti-crossing properties of the dimers coated by the thin dye films with thicknesses greater than 0.1 nm and gap distances larger than 1.2 nm according to the principles of classical electromagnetism. The plas…
