Plasmon-exciton Coupling Research Articles

Kretschmann-based plasmonic excitation of 2D organic semiconductor at visible wavelengths

We studied the Kretschmann-based surface plasmon resonance (K-SPR) of two-dimensional organic semiconductor materials, namely manganese (III) phthalocyanine chloride (MnPcCl) and vanadyl-2,9,16,23-tetraphenoxy-29H,31H-phthalocyanine (VOPcPhO). The K-SPR measurements indicate that VOPcPhO exhibits superior performance compared to MnPcCl, as evidenced by the stronger absorption and narrower SPR peaks. Oxygen-vanadium coupling in the central metal atom facilitates high absorption, potentially enabling strong plasmon-exciton coupling, which can be harnessed for efficient photovoltaic and optical memory devices.

Photoresponse mediated by exciton-plasmon coupling in two-dimensional hybrid phototransistors

Photoresponse mediated by exciton-plasmon coupling in two-dimensional hybrid phototransistors

Tuning the Plexcitonic Optical Chirality Using Discrete Structurally Chiral Plasmonic Nanoparticles.

Constructing chiral plexcitonic systems with tunable plasmon-exciton coupling may advance the scientific exploitation of strong light-matter interactions. Because of their intriguing chiroptical properties, chiral plasmonic materials have shown promising applications in photonics, sensing, and biomedicine. However, the strong coupling of chiral plasmonic nanoparticles with excitons remains largely unexplored. Here we demonstrate the construction of a chiral plasmon-exciton system using chiral AuAg nanorods and J aggregates for tuning the plexcitonic optical chirality. Circular dichroism spectroscopy was employed to characterize chiral plasmon-exciton coupling, in which Rabi splitting and anticrossing behaviors were observed, whereas the extinction spectra exhibited less prominent phenomena. By controlling the number of molecular excitons and the energy detuning between plasmons and excitons, we have been able to fine-tune the plexcitonic optical chirality. The ability to fine-tune the plexcitonic optical chirality opens up unique opportunities for exploring chiral light-matter interactions and boosting the development of emerging chiroptical devices.

Plasmon-induced hot electron injection and local surface potential modification in WS2/Au-nanogratings

The integration of metal nanostructures and transition metal dichalcogenides (TMDs) can lead to exciton-plasmon coupling, which can provide a platform to investigate intriguing physics and cutting-edge applications. In this work, we fabricated hybrid systems, consisting of WS2 multilayer flakes and Au nanogratings (AuNGs), and investigated their optical and electrical characteristics. WS2 flakes were directly exfoliated on large-area AuNGs, prepared by evaporation of Au thin films on Blu-ray disc templates. The polarization- and angle-dependence of the reflectance spectra of WS2/AuNGs indicated surface plasmon polariton (SPP) excitation and SPP-exciton coupling in the visible wavelength range. The surface potential maps in WS2/AuNGs, acquired by Kelvin probe force microscopy, could visualize how the SPP-exciton coupling affected the creation and redistribution of charge carriers. The SPP-induced hot electron injection from AuNG to WS2 as well as band-to-band excitation in WS2 contributed to the local modification of the potential distribution under light illumination.

Quantum Plexcitonic Sensing.

While fundamental to quantum sensing, quantum state control has been traditionally limited to extreme conditions. This restricts the impact of the practical implementation of quantum sensing on a broad range of physical measurements. Plexcitons, however, provide a promising path under ambient conditions toward quantum state control and thus quantum sensing, owing to their origin from strong plasmon-exciton coupling. Herein, we harness plexcitons to demonstrate quantum plexcitonic sensing by strongly coupling excitonic particles to a plasmonic hyperbolic metasurface. As compared to classical sensing in the weak-coupling regime, our model of quantum plexcitonic sensing performs at a level that is ∼40 times more sensitive. Noise-modulated sensitivity studies reinforce the quantum advantage over classical sensing, featuring better sensitivity, smaller sensitivity uncertainty, and higher resilience against optical noise. The successful demonstration of quantum plexcitonic sensing opens the door for a variety of physical, chemical, and biological measurements by leveraging strongly coupled plasmon-exciton systems.

Optical bistability in a heterodimer composed of a quantum dot and a metallic nanoshell.

We theoretically explore the conditions for generating optical bistability (OB) in a heterodimer comprised of a semiconductor quantum dot (SQD) and a metallic nanoshell (MNS). The MNS is made of a metallic nanosphere as a core and a dielectric material as a shell. For the specific hybrid system considered, the bistable effect appears only if the frequency of the pump field is equal to (or slightly less than) the exciton frequency for a proper shell thickness. Bistability phase diagrams, when plotted, show that the dipole-induced bistable region can be greatly broadened by changing the shell thickness of the MNS in a strong exciton-plasmon coupling regime. In particular, we demonstrate that the multipole polarization not only narrows the bistable zone but also enlarges the corresponding thresholds for a given intermediate scaled pumping intensity. On the other hand, when the SQD couples strongly with the MNS, the multipole polarization can also significantly broaden the bistable region and induce a great suppression of the FWM (four-wave mixing) signal for a fixed shell thickness. These interesting findings offer a fresh understanding of the bistability conditions in an SQD/MNS heterodimer, and may be useful in the fabrication of high-performance and low-threshold optical bistable nanodevices.

Solvent effects on the drop cast films of few layers of MoS2 primed by facile exfoliation to realize optical and structural properties

MoS2, a two-dimensional (2D) layered material with variable bandgap and high stability, can be employed in optical and electronic applications due to its outstanding structural, electrical, and optical properties. The fabrication of MoS2 devices in a facile way is highly inevitable to minimize the time consumption and the cost due to its far-reaching and ceaseless applications. On behalf of their various applications, we have employed sonication-assisted liquid phase exfoliation of MoS2 followed by drop casting the sample in a glass plate for further characterization. MoS2 nanosheets were fabricated by exfoliating bulk MoS2 powder in different solvents with varying surface tension such as Ethanol, Ethylene Glycol (EG), Polyvinyl Pyrrolidone (PVP), Dimethylformamide (DMF), and Dimethyl Sulfoxide (DMSO). The structural and optical properties of the sample were analyzed using XRD, AFM, UV spectroscopy, photoluminescence (Pl) and Raman spectroscopy. The formation of 2D MoS2 film with (0 0 2) planes were identified and the thickness of the exfoliated nanosheets was confirmed to be in the nano regime. The optical properties of MoS2 revealed the existence of the spin–orbit coupling and the exciton-plasmon (plexitonic) coupling induced Rabi splitting in the Pl spectra, which increased with a reduction in layer number, and a negative correlation between Pl intensity and Rabi splitting is established. The variation in layer number of MoS2 on different solvents has been studied using the difference in Raman shift between E12g and A1g modes.

Tunable strong plasmon–exciton coupling based modulator employing borophene and deep subwavelength perovskite grating

Two-dimensional materials support deeply confined and tunable plasmonic modes, which have great potential for achieving device miniaturization and flexible manipulation. In this paper, we propose a diffraction-unlimited system (period ≈ λ/20) composed of borophene layer and perovskite grating to investigate the strong coupling between the borophene guiding plasmon (BGP) and perovskite exciton (PE) modes. The resonant energy of the BGP mode could be electrically tuned to match the energy of the PE mode, and a remarkable Rabi splitting is attained under zero-detuning conditions. The splitting energy could reach 230 meV due to the strong field enhancement provided by the BGP mode. Taking advantage of the proposed electrically tunable hybrid system, not only is the reflective amplitude modulation depth up to 99.9%, but the 1.76π phase range modulation is achieved. Furthermore, by increasing the distance between the borophene layer and perovskite grating, a passive parity-time symmetry breaking could be observed with the vanished energy splitting. Our results deepen our understanding of light–matter interactions at the sub-wavelength scale and provide a guideline for designing active plasmonic devices.

Plasmon-exciton coupling in Au nanosphere/carbocyanine J-aggregate hybrids assessed by magnetic circular dichroism (MCD) spectroscopy

In this study, we evaluate plasmon-exciton coupling in Au nanosphere/carbocyanine J-aggregate hybrids by magnetic circular dichroism (MCD) spectroscopy. The carbocyanine dye we used is JC-1, which adsorbs onto Au nanospheres to form J-aggregates. The hybrids exhibit a double-peaked extinction spectrum, and a shallow dip appears at the resonance position of the native J-aggregates, indicating the presence of plasmon-exciton interactions. MCD spectra of the hybrids show a derivative-like profile originated from the surface plasmon resonance of Au nanospheres accompanied by an additional distinct dip (or bump) caused by the exciton resonance of the adsorbed J-aggregates. Importantly, the MCD dip (or bump) position does not correspond to that of the observed new extinction peak, but agrees well with the extinction dip. Moreover, we find that the linewidths of the MCD dip (or bump) are narrow and comparable to that of the J-band of the dye aggregates. All the results suggest that the present hybrid systems are categorized in a weak-coupling regime. Hence we believe that MCD will be a useful spectroscopic method to effectively assess the plasmon-exciton interactions in various kinds of plasmonic-excitonic nanohybrid systems.

Effect of nanoshell geometries, sizes, and quantum emitter parameters on the sensitivity of plasmon-exciton hybrid nanoshells for sensing application

A proposed nanosensor based on hybrid nanoshells consisting of a core of metal nanoparticles and a coating of molecules is simulated by plasmon-exciton coupling in semi classical approach. We study the interaction of electromagnetic radiation with multilevel atoms in a way that takes into account both the spatial and the temporal dependence of the local fields. Our approach has a wide range of applications, from the description of pulse propagation in two-level media to the elaborate simulation of optoelectronic devices, including sensors. We have numerically solved the corresponding system of coupled Maxwell-Liouville equations using finite difference time domain (FDTD) method for different geometries. Plasmon-exciton hybrid nanoshells with different geometries are designed and simulated, which shows more sensitive to environment refractive index (RI) than nanosensor based on localized surface plasmon. The effects of nanoshell geometries, sizes, and quantum emitter parameters on the sensitivity of nanosensors to changes in the RI of the environment were investigated. It was found that the cone-like nanoshell with a silver core and quantum emitter shell had the highest sensitivity. The tapered shape of the cone like nanoshell leads to a higher density of plasmonic excitations at the tapered end of the nanoshell. Under specific conditions, two sharp, deep LSPR peaks were evident in the scattering data. These distinguishing features are valuable as signatures in nanosensors requiring fast, noninvasive response.

Observation of ultra-large Rabi splitting in the plasmon-exciton polaritons at room temperature

Abstract Modifying the light–matter interactions in the plasmonic structures and the two-dimensional (2D) materials not only advances the deeper understanding of the fundamental studies of many-body physics but also provides the opportunities for exploration of novel 2D plasmonic polaritonic devices. Here, we report the plasmon-exciton coupling in the hybrid system with a plasmonic metasurface which can confine the electric field in an extremely compact mode volume. Because of the 2D feature of the designed and fabricated Al plasmonic metasurface, the confined electronic field is distributed in the plane with the same orientation as that of the exciton dipole moment in the transition metal dichalcogenides monolayers. By finely tuning the geometric size of the plasmonic nanostructures, we can significantly modify the dispersion relation of the coupled plasmon and the exciton. Our system shows a strong coupling behavior with an achieved Rabi splitting up to ∼200 meV at room temperature, in ambient conditions. The effective tailoring of the plasmon-exciton coupling with the plasmonic metasurfaces provides the testing platform for studying the quantum electromagnetics at the subwavelength scale as well as exploring plasmonic polariton Bose–Einstein condensation at room temperature.

Fano-resonant propagating plexcitons and Rabi-splitting local plexcitons of bilayer borophene in TERS

Optical nanocavity provides an opportunity to deeply study the light–matter interaction with notable findings such as Rabi splitting in strong coupling and Fano resonance in weak coupling. Here, we theocratically explore the plexcitons of a bilayer (BL) borophene synthesized on an Ag (1 1 1) film in a tip-enhanced Raman scattering (TERS) system, where the BL borophene is located in the nanocavity between the tip and substrate, stimulated by recent experimental synthesis [Liu et al., Nat. Mater. 21, 35 (2022)]. In the strong-coupling region, the negative real part of the dielectric function of the BL borophene manifests; the BL borophene is of plasmonic properties resulting in Rabi splitting of plexcitons with 310 meV. In the weak-coupling region, the spectra show typical asymmetry with a sharp change between a dip and a peak (Fano resonance). A balanced gain and loss facilitates single-mode lasing in the parity-time symmetry-broken regime, where single-mode lasing with a very narrow half-width is of ultrahigh enhancement factor up to 108. Fano-resonant propagating plexcitons are observed in the dip of Fano resonance, which is extremely sensitive to the excitation wavelength. Our results not only deepen the physical understanding of the plasmon–exciton coupling interaction in the TERS system but also provide a way to manipulate the light–matter interaction in the TERS system.

Multipole polarization assisted optical bistability in a semiconductor quantum dot/metal nanoparticle hybrid molecule

We theoretically study the optical bistability assisted by multipole polarizations in a semiconductor quantum dot (SQD)/metal nanoparticle (MNP) hybrid molecule. We map out bistability phase diagrams within the parameter subspace spanned by (the pumping intensity Ipu, interparticle distance, d) under dipole and multipole approximations. It is shown that the Ipu-correlated bistable region will be broadened greatly in the strong exciton–plasmon coupling regime, and the corresponding lower (upper) bistable threshold is enlarged significantly due to multipole polarization (N = 10) in comparison to that in the dipole approximation (N = 1). However, under the same conditions, the d-correlated bistable region is shrunk at high pump intensities. Our contribution not only offers a better understanding of exciton–plasmon coupling systems but also expands the application of SQD/MNP hybrid molecules in the field of optical bistable nanodevices.

Coherent Second Harmonic Generation Enhanced by Coherent Plasmon–Exciton Coupling in Plasmonic Nanocavities

Coherent Second Harmonic Generation Enhanced by Coherent Plasmon–Exciton Coupling in Plasmonic Nanocavities

Gap plasmon modes and plasmon-exciton coupling in a hybrid Au/MoSe2/Au tunneling junction.

The light-matter interaction between plasmonic nanocavity modes and excitons at the nanometer scale is here addressed in the scanning tunneling microscope configuration where an MoSe2 monolayer is located between the tip and the substrate. We investigate by optical excitation the electromagnetic modes of this hybrid Au/MoSe2/Au tunneling junction using numerical simulations where electron tunneling and the anisotropic character of the MoSe2 layer are taken into account. In particular, we pointed out gap plasmon modes and Fano-type plasmon-exciton coupling taking place at the MoSe2/Au substrate interface. The spectral properties and spatial localization of these modes are studied as a function of the tunneling parameters and incident polarization.

Promising Photoluminescence Enhancement of Tris(8-hydroxyquinoline)aluminum by Simultaneous Localized and Propagating Surface Plasmons of Ag Nanostructures

The continuous performance optimization of tris(8-hydroxyquinoline)aluminum (Alq3) materials is of great significance during the commercialization process of organic light-emitting diodes (OLEDs). In incorporating Ag nanostructures into Alq3, the photophysical properties are greatly improved by the plasmon–exciton coupling effect. Localized surface plasmons (LSPs) in Ag nanoparticles (NPs) efficiently increased the absorption ability. The coexistence of LSPs and propagating surface plasmons (PSPs) in Ag nanowires (NWs) leads to a PL enhancement of 5.3-fold and a full-width at half maximum (FWHM) narrowed by 10 nm. Temperature-dependent PL measurements exhibit that the plasmonic density of states (DOS) increases with decreasing temperature below 40 °C, and the thermal exchange can be accelerated by the introduction of Ag nanostructures. Effective suppression of the thermal accumulation effect is further proved by excitation intensity (EI)-dependent PL measurements. We also found that Ag nanostructures could mainly change the y coordinates in International Commission on Illumination (CIE), leading to a higher brightness. The 5372 K color temperature of an Ag NWs-embedded composite is suitable for daylight-type fluorescent OLEDs. The results would pave an effective way for further optimizing the optical performance of light-emitting materials in OLEDs.

Perspective on functional metal-oxide plasmonic metastructures

Plasmonic nanostructures and metasurfaces are appealing hosts for investigation of novel optical devices and exploration of new frontiers in physical/optical processes and materials research. Recent studies have shown that these structures hold the promise of greater control over the optical and electronic properties of quantum emitters, offering a unique horizon for ultra-fast spin-controlled optical devices, quantum computation, laser systems, and sensitive photodetectors. In this Perspective, we discuss how heterostructures consisting of metal oxides, metallic nanoantennas, and dielectrics can offer a material platform wherein one can use the decay of plasmons and their near fields to passivate the defect sites of semiconductor quantum dots while enhancing their radiative decay rates. Such a platform, called functional metal-oxide plasmonic metasubstrates (FMOPs), relies on formation of two junctions at very close vicinity of each other. These include an Au/Si Schottky junction and an Si/Al oxide charge barrier. Such a double junction allows one to use hot electrons to generate a field-passivation effect, preventing migration of photo-excited electrons from quantum dots to the defect sites. Prospects of FMOP, including impact of enhancement exciton–plasmon coupling, collective transport of excitation energy, and suppression of quantum dot fluorescence blinking, are discussed.

Strong coupling of multiple plasmon modes and excitons with excitation light controlled active tuning

Abstract While the strong coupling between cavity modes and quantum emitters has been investigated in various systems, multiple surface plasmon modes in single nanostructures strongly coupling with excitons are rarely explored. Here, we investigate the strong coupling between three surface plasmon modes in silver nanowires and excitons in monolayer WSe2 at room temperature. Four plasmon-exciton polariton (plexciton) states are observed in the scattering spectra. The photoluminescence (PL) spectra of the hybrid system show clear splitting due to strong coupling, and the energies of the emission corresponding to the two lower plexciton states agree with that of the scattering very well. In addition, we show that the plasmon-exciton interaction in this system can be efficiently tuned by controlling the excitation power. These results reveal the fundamental properties of strong coupling between multiple plasmon modes and excitons, deepen the understanding of the correlation between scattering and PL spectra of plasmon-exciton strong coupling systems, and open up a new way to actively control the coupling between plasmonic nanostructures and two-dimensional semiconductors.

Plasmon-Exciton Coupling Effect in Nanostructured Arrays for Optical Signal Amplification and SARS-CoV-2 DNA Sensing.

A surface plasmon resonance (SPR)-enhanced optical signal using a nanoslit array and acridine orange (AO) dye system at a flexible poly(dimethylsiloxane) (PDMS) substrate was achieved in this work and demonstrated a simple sensing scheme to directly detect SARS-CoV-2 nucleic acid via DNA hybridization. A simple nanoimprinting pattern transfer technique was introduced to form uniform reproducible nanoslit arrays where the dimensions of the slit array were controlled by the thickness of the gold film. The plasmon-exciton coupling effect on the optical enhancement of different dye molecules, i.e., AO, propidium iodide (PI), or dihydroethidium (DHE) attached to the nanoslit surfaces, was examined thoroughly by measuring the surface reflection and fluorescence imaging. The results indicate that the best overlap of the plasmon resonance wavelength to the excitation spectrum of AO presented the largest optical enhancement (∼57×) compared to the signal at flat gold surfaces. Based on this finding, a sensitive assay for detecting DNA hybridization was generated using the interaction of the selected SARS-CoV-2 ssDNA and dsDNA with AO to trigger the metachromatic behavior of the dye at the nanoarray surfaces. We found strong optical signal amplification on the formation of acridine-ssDNA complexes and a quenched signal upon hybridization to the complementary target DNA (ct-DNA) along with a blue shift in the fluorescence of AO-dsDNAs. A quantitative evaluation of the ct-DNA concentration in a range of 100-0.08 nM using both the reflection and emission imaging signals demonstrated two linear regimes with a lowest detection limit of 0.21 nM. The sensing method showed high sensitivity and distinguished signals from 1-, 2-, and 3-base mismatched DNA targets, as well as high stability and reusability. This approach toward enhancing optical signal for DNA sensing offers promise in a general, rapid, and direct vision detection method for nucleic acid analytes.

The Effect of the Core on the Absorption in a Hybrid Semiconductor Quantum Dot—Metal Nanoshell System

We examine the optical absorption in a hybrid structure composed of a metal nanoshell and a semiconductor quantum dot, while interacting with a linearly polarized probe electromagnetic field. First, we derive the equations of motion, in the rotating wave approximation. Then we procced to the derivation of analytical expressions for the linear susceptibility of the metal nanoshell and the semiconductor quantum dot. The imaginary part of the susceptibility expresses the absorption coefficient. We find that by properly engineering the thickness of the metal nanoshell, the material of the dielectric core and the interparticle distance, we may achieve an optimum response. We identify the emergence of two distinct types of hybrid exciton states. One of them emerges in the strong exciton–plasmon coupling regime for low values of the dielectric constant and the radius of the dielectric core. This type of hybrid exciton exhibits an amplified gain without population inversion and a quenched absorption resonance accompanied by a suppressed exciton lifetime. The second type of hybrid exciton emerges in the weak exciton–plasmon coupling regime and presents the opposite spectral characteristics. Here, the exciton lifetime presents a substantial increase, especially for small interparticle distances, in which case the semiconductor quantum dot and the metal nanoshell are strongly coupled with one another.