Plasmonic Nanocavity Research Articles

Plasmonic Nanocavity to Boost Single Photon Emission From Defects in Thin Hexagonal Boron Nitride

AbstractEfficient and compact single photon emission platforms operating at room temperature with ultrafast speed and high brightness will be fundamental components of the emerging quantum communications and computing fields. However, so far, it is very challenging to design practical deterministic single photon emitters based on nanoscale solid‐state materials that meet the fast emission rate and strong brightness demands. Here, a solution is provided to this longstanding problem by using metallic nanocavities integrated with hexagonal boron nitride (hBN) flakes with defects acting as nanoscale single photon emitters (SPEs) at room temperature. The presented hybrid nanophotonic structure creates a rapid speedup and large enhancement in single photon emission at room temperature. Hence, the nonclassical light emission performance is substantially improved compared to plain hBN flakes and hBN on gold‐layered structures without nanocavity. Extensive theoretical calculations are also performed to accurately model the new hybrid nanophotonic system and prove that the incorporation of plasmonic nanocavity is key to efficient SPE performance. The proposed quantum nanocavity single photon source is expected to be an element of paramount importance to the envisioned room‐temperature integrated quantum photonic networks.

Quantifying the ultimate limit of plasmonic near-field enhancement

Quantitatively probing the ultimate limit of near-field enhancement around plasmonic nanostructures remains elusive, despite more than five decades since the discovery of surface-enhanced Raman scattering. Theoretical calculations have predicted an ultimate near-field enhancement exceeding 1000 using the best plasmonic material silver, but experimental estimations disperse by orders of magnitude. Here, we design a high-quality silver plasmonic nanocavity with atomic precision and precisely quantify the upper limit of near-field enhancement in ~1 nm junctions. A hot-spot averaged Raman enhancement of 4.27 × 1010 is recorded with a small fluctuation, corresponding to an averaged electric field enhancement larger than 1000 times. This result quantitatively delineates the ultimate limit of plasmonic field enhancement around plasmonic nanostructures, establishing a foundation for diverse plasmon-enhanced processes and strong light-matter interactions at the atomic scale.

Topologically Protected Plasmonic Bound States in the Continuum.

Experimental realizations of bound states in the continuum (BICs) with strong robustness and advanced maneuverability in optical loss systems remain a long-standing challenge in nanophotonics. Here, we propose and fabricate a paradigm of diatomic metagratings incorporating the Su-Schrieffer-Heeger model into the design of plasmonic nanocavities to demonstrate optical resonators with a continuous "quasi-BICs (qBICs)-BICs-qBICs" transition. These resonators feature a topological band inversion, making high-quality (Q) resonances immune to the perturbation of incident angles and geometrical parameters. Furthermore, we strive to establish theoretical models to verify the topological nature of BICs-inspired resonances and introduce nonlinear optical probes to quantify strongly enhanced local fields at high-Q resonances. Our findings may provide a simple yet feasible design strategy for facilitating the dissipationless manipulation of surface/interface-enhanced light-matter interactions at the nanoscale, substantially broadening the functional scope of metaphotonics.

2D MoS2 plasmonic nanocavity based SERS platform for bilirubin detection

Although various methods can be used to detect bilirubin at the micromolar level, achieving reliable detection in the sub-nanomolar range remains challenging. Sensitivity at these ultralow levels is vital, as new evidence strongly associates bilirubin with chronic heart, lung, and neurological disorders. This accuracy is also essential for creating diagnostic protocols that can efficiently track bilirubin levels, assisting in managing related conditions. Such advancements will lead to enhanced diagnostic tools and methods, enabling more precise bilirubin monitoring in clinical environments. Here, the aforesaid blind-spot is addressed by utilizing surface enhanced Raman spectroscopy (SERS) as fingerprint technique to detect bilirubin concentrations as low as 0.1 nM. A plasmonically active 2D MoS2 based SERS substrate is formulated and optimized for single step SERS sensing of bilirubin. Plasmonic cavity based approach is utilized to circumvent the problem related to fluorescent background overwhelming the SERS signal. The 2D MoS2 based SERS platform shows threefold enhancement of scattering in comparison to the traditional gold nanoparticle on Si/SiO2 approach. The Raman signature of bilirubin is calibrated by taking citrate as a stable reference analyte and is shown to vary linearly with logarithmic concentration across the picomolar to micromolar range.

High-Throughput On-Demand Design Platform for Plasmonic Nanocavities: A Wavefunction Theory Approach.

Surface plasmon polaritons from plasmonic nanocavity have aroused great interest due to their applications in various fields, in which on-demand design is hindered by the lack of theoretical frameworks. Herein, based on its wave nature, we developed a wavefunction theory to explicitly describe individual surface plasmon polaritons and the resultant near-field and far-field behaviors, which serves as an efficient platform for high-throughput on-demand design of nanocavities. We found an applicative wavefunction form and proposed a two-body interaction function and a "shell" model for many-body interactions in surface plasmon polaritons' coupling. The wavefunction of individual surface plasmon polaritons and resultant near-field and far-field behaviors can be given explicitly and precisely. The theory provides a fundamental and quantitative understanding of surface plasmon polaritons and enables highly efficient on-demand design of plasmonic metamaterials and devices, leading to further methodological applications in numerous aspects.

Integration of highly ordered plasmonic nanocavity array structure with the electrostatic driving force for dynamic control of SERS signals and label-free detection of λ-DNA

Integration of highly ordered plasmonic nanocavity array structure with the electrostatic driving force for dynamic control of SERS signals and label-free detection of λ-DNA

Purcell Enhancement and Spin Spectroscopy of Silicon Vacancy Centers in Silicon Carbide Using an Ultrasmall Mode-Volume Plasmonic Cavity.

Silicon vacancy (VSi) centers in 4H-silicon carbide have emerged as a strong candidate for quantum networking applications due to their robust electronic and optical properties, including a long spin coherence lifetime and bright, stable emission. Here, we report the integration of VSi centers with a plasmonic nanocavity to Purcell enhance the emission, which is critical for scalable quantum networking. Employing a simple fabrication process, we demonstrate plasmonic cavities that support a nanoscale mode volume and exhibit an increase in the spontaneous emission rate with a measured Purcell factor of up to 48. In addition to investigating the optical resonance modes, we demonstrate an improvement in the optical stability of the spin-preserving resonant optical transitions relative to the radiation-limited value. The results highlight the potential of nanophotonic structures for advancing quantum networking technologies and emphasize the importance of optimizing emitter-cavity interactions for efficient quantum photonic applications.

Plasmon-driven chemical transformation of a secondary amide probed by surface enhanced Raman scattering

Plasmon-driven chemical conversion is gaining burgeoning interest in the field of heterogeneous catalysis. Herein, we study the reactivity of N-methyl-4-sulfanylbenzamide (NMSB) at nanocavities of gold and silver nanoparticle aggregates under plasmonic excitation to gain understanding of the respective reaction mechanism. NMSB is a secondary amide, which is a frequent binding motive found in peptides and a common coupling product of organic molecules and biomolecules. Surface-enhanced Raman scattering (SERS) is used as a two-in-one in-situ spectroscopic tool to initiate the molecular transformation process and simultaneously monitor and analyze the reaction products. Supported by dissociative electron attachment (DEA) studies with the gas phase molecule, a hot electron-mediated conversion of NMSB to p-mercaptobenzamide and p-mercaptobenzonitrile is proposed at the plasmonic nanocavities. The reaction rate showed negligible dependence on the external temperature, ruling out the dominant role of heat in the chemical transformation at the plasmonic interface. This is reflected in the absence of a superlinear relationship between the reaction rate constant and the laser power density, and DEA and SERS studies indicate a hot-electron mediated pathway. We conclude that the overall reaction rate is limited by the availability of energetic hot electrons to the NMSB molecule.

Enhancing Optical Nonlinearity from Monolayer WS2 in Magnetic Plasmonic Nanocavities at 1 nm Spatial Resolution

Enhancing Optical Nonlinearity from Monolayer WS₂ in Magnetic Plasmonic Nanocavities at 1 nm Spatial Resolution

Theoretical study of tip-enhanced photoluminescence of single molecule in nanocavity formed by apex protrusion and substrate

Tip-enhanced photoluminescence techniques, characterized by ultra-high detection sensitivity and spatial resolution, have exhibited unprecedented capabilities in exploring optoelectronic phenomena and unraveling intrinsic physical mechanism at the single-molecule level. To suppress the quenching of molecular luminescence and achieve high-resolution optical imaging, a rational design of the tip-substrate configuration is required. In this paper, we systematically investigate the tip-enhanced photoluminescence characteristics of single molecules located within the plasmonic nanocavity formed by the tip protrusion and the substrate from a theoretical perspective. The impacts of electron tunneling and electron-hole pair creation on localized electric field and quantum yield are discussed using the quantum correction model and nonlocal dielectric theory, respectively. The crucial roles of atomic-scale protrusion at the tip apex and the decoupling layer on the substrate in enhancing vertical and horizontal electric fields as well as quantum yields have been emphasized. The results indicate that in smaller sub-nanometer cavities, electron tunneling and nonlocal dielectric effects greatly weaken the electric field intensity and fluorescence quantum yield. Meanwhile, due to the sharp lightning rod effect, the presence of atomic-level protrusion at the tip apex can provide a strong and highly localized plasmonic field. We find that the added NaCl layer not only blocks charge transfer between molecules and the substrate but also effectively prevents fluorescence quenching. The maximum fluorescence and Raman enhancement factors near the tip apex approach up to 5 and 12 orders of magnitude, respectively, achieving sub-nanometer spatial resolution. Finally, compared to vertical electric field and dipole, sharp protrusion can excite a stronger horizontal electric field and couple with horizontal dipoles to yield a higher quantum yield, resulting in a three orders of magnitude higher in the fluorescence enhancement of horizontal dipole compared to the tip without protrusion. Our theoretical research not only confirms the experimental results of spectral enhancement with the proximity of the tip to the molecule in tip-enhanced photoluminescence, but also provides effective guidance for a deeper understanding of the mechanism of tip-enhanced fluorescence and Raman spectroscopy, as well as optimizing the experimental system.

Graphene oxide based plasmonic nano-cavity sensor for high-performance refractive index sensing

Abstract In this work, a nano-cavity based metal-insulator-metal structure is proposed which can be used as a high-performance refractive index sensor. The analysis of its sensing capabilities is done by determining the transmission characteristics of light through the insulating air channel between the metal layer. The loss in transmission in this channel is indicative of light leaking out of it and portion of it getting coupled to nano-cavities considered in the metal layers on both sides of the air channel. The analyte, whose refractive index is to be sensed, is kept in these nano-cavities. The basic structure is modified by introducing graphene oxide (GO) on the inner wall of the nano-cavity, which further improves the confinement of light in the nano-cavities. It is also shown that increasing the number of nano-cavity duos enhances the transmission loss through the waveguide and as a result the light energy confinement in the cavity increases. Calculated values of sensitivities and Figure of Merit of the proposed sensor structure are much higher than similar works done previously. The uniqueness of the work is two-fold; namely use of graphene oxide as an inner layer of the nano-cavity improves the sensitivity of the sensor and secondly calculating the waveguide transmission to indirectly determine the confinement of light energy in nano-cavity simplifies the analysis of the performance of the proposed sensor. The structure is simple and can be easily fabricated using a standard fabrication process.

Robust consistent single quantum dot strong coupling in plasmonic nanocavities

Strong coupling between a single quantum emitter and an optical cavity (at rate Ω) accesses fundamental quantum optics and provides an essential building block for photonic quantum technologies. However, the minimum mode volume of conventional dielectric cavities restricts their operation to cryogenic temperature for strong coupling. Here we harness surface self-assembly to make deterministic strong coupling at room temperature using CdSe/CdS quantum dots (QDs) in nanoparticle-on-mirror (NPoM) plasmonic nanocavities. We achieve a fabrication yield of ~70% for single QD strong coupling by optimizing their size and nano-assembly. A clear and reliable Rabi splitting is observed both in the scattering of each nanocavity and their photoluminescence, which are however not equal. Integrating these quantum elements with electrical pumping allows demonstration of strong coupling in their electroluminescence. This advance provides a straightforward way to achieve practical quantum devices at room temperature, and opens up exploration of their nonlinear, electrical, and quantum correlation properties.

Novel biomimetic hybrid plasmonic nanocavity-based ECL strategy for the detection of extracellular vesicles

Tumor-derived extracellular vesicles detection has emerged as an important clinical liquid biopsy approach for cancer diagnosis. In this work, we developed a novel hybrid plasmonic nanocavity consisting of hexagonal Au nanoplates nanoarray, SnS2/Au nanosheet layer and biomimetic lipid bilayer. Firstly, the hybrid plasmonic nanocavity combined the optical confinement for the ECL regulation and the biological recognition for the detection of extracellular vesicles. Secondly, MXene-derived Ti2N QDs have been prepared as ECL nanoprobe to label extracellular vesicles. Moreover, biomimetic lipid bilayer with specific aptamer was used to identify extracellular vesicles and integrate Ti2N QDs into the nanocavity with membrane fusion strategy. Due to the significant electromagnetic field enhancement at the cavity region, the hybrid plasmonic nanocavity provided strong field confinement to concentrate and redistribute the ECL emission of QDs with a 9.3-fold enhancement. The hybrid plasmonic nanocavity-based ECL sensing system improved the spatial controllability of EVs analysis and the accurate resolution of specific protein. It achieved the sensitive detection of extracellular vesicles in ascites and successfully distinguished the peritoneal metastasis of gastric cancer.

Electrically driven cavity plasmons in Au nanowire over Au film

Light emission via inelastic tunneling electrons is appealing for integrated optoelectronic devices due to its femtosecond time scale that can in principle allow terahertz modulation bandwidth. It has gained renewed interest since 2015 due to the improved quantum efficiency, highly tunable emission wavelength, linewidth, or directionality once the electrodes are designed as a plasmonic nanocavity. However, efficient construction of stable tunnel junctions with desired plasmonic resonances is still technically challenging because of the subnanometer precision required in the electrical and optical design. Here, we demonstrate an easily accessible electrically driven cavity plasmon in metal-insulator-metal (MIM) tunnel junctions, comprised by a Au nanowire (NW) across two separate ultrasmooth Au electrodes. Two layers of self-assembled thiol molecule defines a reliable tunneling barrier. The contribution from the localized cavity plasmons to the total light emission is found to be dominant over that from the propagating surface plasmon polariton in the MIM waveguide, different from the traditional explanations. This work introduces a simplified method for constructing electrically driven cavity plasmons using crystalline metals, which holds promise for applications in in situ chemical or biosensing and the development of flexible light-emitting metasurfaces.

Uncovering low-frequency vibrations in surface-enhanced Raman of organic molecules

Accessing the terahertz (THz) spectral domain through surface-enhanced Raman spectroscopy (SERS) is challenging and opens up the study of low-frequency molecular and electronic excitations. Compared to direct THz probing of heterogenous ensembles, the extreme plasmonic confinement of visible light to deep sub-wavelength scales allows the study of hundreds or even single molecules. We show that self-assembled molecular monolayers of a set of simple aromatic thiols confined inside single-particle plasmonic nanocavities can be distinguished by their low-wavenumber spectral peaks below 200 cm−1, after removal of a bosonic inelastic contribution and an exponential background from the spectrum. Developing environment-dependent density-functional-theory simulations of the metal-molecule configuration enables the assignment and classification of their THz vibrations as well as the identification of intermolecular coupling effects and of the influence of the gold surface configuration. Furthermore, we show dramatically narrower THz SERS spectra from individual molecules at picocavities, which indicates the possibility to study intrinsic vibrational properties beyond inhomogeneous broadening, further supporting the key role of local environment.

Room-temperature quantum nanoplasmonic coherent perfect absorption

Light-matter superposition states obtained via strong coupling play a decisive role in quantum information processing, but the deleterious effects of material dissipation and environment-induced decoherence inevitably destroy coherent light-matter polaritons over time. Here, we propose the use of coherent perfect absorption under near-field driving to prepare and protect the polaritonic states of a single quantum emitter interacting with a plasmonic nanocavity at room temperature. Our scheme of quantum nanoplasmonic coherent perfect absorption leverages an inherent frequency specificity to selectively initialize the coupled system in a chosen plasmon-emitter dressed state, while the coherent, unidirectional and non-perturbing near-field energy transfer from a proximal plasmonic waveguide can in principle render the dressed state robust against dynamic dissipation under ambient conditions. Our study establishes a previously unexplored paradigm for quantum state preparation and coherence preservation in plasmonic cavity quantum electrodynamics, offering compelling prospects for elevating quantum nanophotonic technologies to ambient temperatures.

Tunable plasmonic tweezers based on nanocavity array structure for multi-site nanoscale particles trapping

The ability of plasmonic optical tweezers based on metal nanostructure to stably trap and dynamically manipulate nanoscale objects at low laser power has been widely used in the fields of nanotechnology and life sciences. In particular, their plasmonic nanocavity structure can improve the local field intensity and trap depth by confining electromagnetic fields to subwavelength volumes. In this paper, the R6G dye molecules with 10−6 M were successfully trapped by using the Ag@Polydimethylsiloxane nanocavity array structure, and a R6G micro-ring was formed under the combined action of plasmonic optical force and thermophoresis. Subsequently, the theoretical investigation revealed that the trapping performance can be flexibly adjusted by changing the structural parameters of the conical nanocavity unit, and it can provide a stable potential well for polystyrene particles of RNP = 14 nm when the cavity depth is 140 nm. In addition, it is found that multiple trapping sites can be activated simultaneously in the laser irradiation area by investigating the trapping properties of the hexagonal conical nanocavity array structure. This multi-site stable trapping platform makes it possible to analyze multiple target particles contemporaneously.

Coupling polyatomic molecules to lossy nanocavities: Lindblad vs Schrödinger description.

The use of cavities to impact molecular structure and dynamics has become popular. As cavities, in particular plasmonic nanocavities, are lossy and the lifetime of their modes can be very short, their lossy nature must be incorporated into the calculations. The Lindblad master equation is commonly considered an appropriate tool to describe this lossy nature. This approach requires the dynamics of the density operator and is thus substantially more costly than approaches employing the Schrödinger equation for the quantum wave function when several or many nuclear degrees of freedom are involved. In this work, we compare numerically the Lindblad and Schrödinger descriptions discussed in the literature for a molecular example where the cavity is pumped by a laser. The laser and cavity properties are varied over a range of parameters. It is found that the Schrödinger description adequately describes the dynamics of the polaritons and emission signal as long as the laser intensity is moderate and the pump time is not much longer than the lifetime of the cavity mode. Otherwise, it is demonstrated that the Schrödinger description gradually fails. We also show that the failure of the Schrödinger description can often be remedied by renormalizing the wave function at every step of time propagation. The results are discussed and analyzed.

Influence of Quadrupolar Molecular Transitions within Plasmonic Cavities.

Optical nanocavities have revolutionized the manipulation of radiative properties of molecular and semiconductor emitters. Here, we investigate the amplified photoluminescence arising from exciting a dark transition of β-carotene molecules embedded within plasmonic nanocavities. Integrating a molecular monolayer into nanoparticle-on-mirror nanostructures unveils enhancements surpassing 4 orders of magnitude in the initially light-forbidden excitation. Such pronounced enhancements transcend conventional dipolar mechanisms, underscoring the presence of alternative enhancement pathways. Notably, Fourier-plane scattering spectroscopy shows that the photoluminescence excitation resonance aligns with a higher-order plasmonic cavity mode, which supports strong field gradients. Combining quantum chemistry calculations with electromagnetic simulations reveals an important interplay between the Franck-Condon quadrupole and Herzberg-Teller dipole contributions in governing the absorption characteristics of this dark transition. In contrast to free space, the quadrupole moment plays a significant role in photoluminescence enhancement within nanoparticle-on-mirror cavities. These findings provide an approach to access optically inactive transitions, promising advancements in spectroscopy and sensing applications.

Strong coupling between plasmonic nanocavity gold nanorods and quantum dots emitter

The discovery of hybrid states in strong coupling interaction has gained growing attention in cavity-quantum electrodynamics research owing to its fundamental directives and potential in advanced optical applications. The ultra-confined mode volume of plasmonic cavity gold nanorods (AuNRs), particularly at the nanorod tip “hotspot” provides a large coupling strength, a prerequisite for a coherent energy exchange in the strong coupling regime. Here, we reported a remarkable Rabi splitting of ∼231 meV between gold nanorods longitudinal localized surface plasmon resonance (LLSPR) mode and quantum dots (QDs) at ambient conditions, monitored by dielectric medium tuning. Numerical simulations confirmed the result, displaying absorption spectral splitting.