High Resolution Surface Plasmon Microscopy: From Nano-colloids To Single Nucleosome Imaging

Nanofocusing of Surface Plasmons at the Apex of Metallic Tips and at the Sharp Metallic Wedges. Importance of Electric Field Singularity

A high-sensitivity surface plasmon resonance (SPR) sensor based on the coupling of Au grating and Au film is investigated through simulations and experiments. The SPR sensor is designed by using a hybrid method composed of genetic algorithm (GA) and rigorous coupled wave analysis (RCWA). The numerical results indicate the sensor has an angular sensitivity of 397.3°/RIU (refractive index unit), which is approximately 2.81 times higher than the conventional Au-based sensor and it is verified by experiments. Theoretical analysis, by finite-difference time-domain (FDTD) method, demonstrates the co-coupling between surface plasmon polaritons (SPPs) propagating on the surface of Au film and localized surface plasmons (LSPs) in the Au grating nanostructure, improving the sensitivity of the SPR sensor. According to the optimized structural parameters, the proposed sensor is fabricated using e-beam lithography and magnetron sputtering. In addition, the proposed sensor is very sensitive to the detection of small molecules. The limit of detection (LOD) for okadaic acid (OA) is 0.72 ng/mL based on an indirect competitive inhibition method, which is approximately 38 times lower than the conventional Au sensor. Such a high-sensitivity SPR biosensor has potential in the applications of immunoassays and clinical diagnosis.

A surface plasmon polariton (SPP) phase imaging microscope with a subwavelength grating structure is developed for high-resolution in-plane image measurement, which can be used on biological samples. Conventionally, most of SPP image systems use prism couplers to induce surface plasmons (SPs), but this approach has some drawbacks such as non-normal incident light producing optical aberration in imaging and making the metrology instrument more complicate. It can be improved by utilizing a normal incident light to excite the SPs through subwavelength grating structure, which replaces the prism so that it can observe in-plane sample on the sensing surface and simplify the instrument. Instead of measuring the intensity of the reflectivity, the phase measurement with higher sensitivity is proposed. In this study, the proposed SPP microscope integrates a common-path phase-shift interferometry (PSI) technique to obtain the two-dimensional spatial phase variation caused by biomolecular interactions on the sensing surface without requiring additional labeling. The common-path PSI technique provides long-term stability, even when it is subjected to external disturbances, to match the requirements of biomolecular interaction analysis. The microscope is presented as a high stability, high sensitivity, and in-plane SPP phase image.

Integrating surface plasmon resonance (SPR) devices upon single-mode fiber (SMF) end facets renders label-free biosensing systems that have a dip-and-read configuration, high compatibility with fiber-optic techniques, and in vivo monitoring capability, which however meets the challenge to match the performance of free-space counterparts. We report a second-order distributed feedback (DFB) SPR cavity on an SMF end facet and its application in protein interaction analysis. In our device, a periodic array of nanoslits in a gold film is used to couple fiber guided lightwaves to surface plasmon polaritons (SPPs) with its first order spatial Fourier component, while the second order spatial Fourier component provides DFB to SPP propagation and produces an SPP bandgap. A phase shift section in the DFB structure introduces an SPR defect state within the SPP bandgap, whose mode profile is optimized to match that of the SMF to achieve a reasonable coupling efficiency. We report an experimental refractive index sensitivity of 628 nm RIU−1, a figure-of-merit of 80 RIU−1, and a limit of detection of 7 × 10−6 RIU. The measurement of the real-time interaction between human immunoglobulin G molecules and their antibodies is demonstrated.

Plasmonics have been identified as an ideal platform for ultra-sensitive, label-free biosensors mainly due to the high field confinement on a metal-dielectric interface and the resulting strong light-matter interaction offered by surface plasmon resonances (SPRs) that can be entirely exposed to test analytes. Well-established SPR-based biosensors exploiting propagating SPRs yield superior specifications regarding bulk sensitivity compared to localized counterparts leading to already commercial available sensor devices. However, most of these systems require bulky prism-based configurations to couple light into the Surface Plasmon Polariton (SPP) mode impeding system miniaturization. In addition, SPR-based sensors suffer from intrinsic high propagation losses restricting the potential for multiple on-chip functionalities. In this context, co-integration of plasmonics with a low-loss photonic platform emerges as a viable solution towards highly sensitive, low-loss and small footprint optical sensors. In this work, we present an ultra-compact, interferometric plasmonic sensor co-integrated on a TiO2 photonic waveguide platform. The device consists of two access TiO2 photonic waveguides separated by a gold-based metal stripe which is located on top of an appropriately shorter TiO2 waveguide layer. Two metal/insulator interfaces are formed at the top (sensing arm) and bottom surfaces (reference arm) of the metal able to support SPP modes which upon excitation through the input photonic waveguide propagate along the two metal surfaces and interfere at the output waveguide realizing a single-arm Mach-Zehnder Interferometer. After optimization of the device in aqueous environment, we achieved sensitivity values as high as 2430 nm/RIU at near-infrared spectrum region for a 65 um long plasmonic stripe.

Herein, we experimentally demonstrate surface plasmon polariton (SPP) induced changes in the conductivity of a carbon nanotube field effect transistor (CNT FET). SPP excitation is done via Kretschmann configuration while the measured CNT FET is situated on the opposite side of the metal layer away from the laser, but within reach of the launched SPPs. We observe a shift of ∼0.4 V in effective gate voltage. SPP-intermediated desorption of physisorbed oxygen from the device is discussed as a likely explanation of the observed effect. This effect is visible even at low SPP intensities and within a near-infrared range.

Body: Surface plasmon polariton (SPP), which result from the strong coupling of bound electromagnetic (EM) waves and collective charge oscillations, enable subwavelength manipulation of light and matter interaction. Conventional noble metals-based SPP excited in the visible and near-Infrared spectra ranges suffer from large energy losses and cannot be dynamically tuned. Thanks to its 2D nature, graphene has emerged as a promising alternative plasmonic material with well- confined SPPs in the mid-infrared (MIR) and terahertz (THz) ranges and remarkable tunability. On the other hand, polar dielectric materials support low optical losses and sub-wavelength mode in the MIR and THz regions via surface phonon polariton (SPhP)mode' stimulation within the Reststrahlen band, a narrow spectral range between transverse optical (TO) and longitudinal optical (LO) frequencies. Due to the excellent polaritonic responses in both graphene and silicon carbide in the MIR and THz regions, devices combining the two materials are inferred to greatly advance photonics and THz technologies. We have recently theoretically demonstrated the strong confinement and large propagation figures of merit (FOM) for hybrid surface plasmon and surface phonon polariton in the epitaxial graphene on silicon carbide. The ability to confine such MIR light into small volume through excitation of SPP and SPhP has many implications for optoelectronic technologies such as the MIR photodetection[2], sensing[3], and solar cells[4]. Epitaxial graphene(EG) grown on silicon carbide(SiC) on silicon(Si) has been investigated as a suitable platform for graphene growth on semiconductors to meet the prospective technologies [5]. Despite this platform being very advantageous, experimental and theoretical works demonstrating the potentials properties/applications of EG on SiC on Si are still missing. Here we combine electromagnetic simulations based on finite elements method (FEM) with attenuated total reflectance Fourier transformed infrared (ATR-FTIR) spectroscopy to indicate improved MIR absorption, E field enhancement, and tunability for graphene-coated SiC nanowires (NWs). As anticipated, low absorption was confirmed from both simulations and measurements on bare SiC NWs, further supported by the calculated weak electric field due to the thin size of SiC NWs being incapable of absorbing sufficient light. On the other hand, enhanced absorption for the SiC NWs was measured by ATR-FTIR after a conformal graphitization of NWs[6]. Our previous study of this material system revealed a low-density oxide layer formed between graphene and SiC NWs[6]. This oxide layer between EG and SiC NW has been implemented in the FEM model, leading to field enhancement of incident EM field and strongly confined in the thin oxide. This substantial absorption and field enhancement originates from the coupling between the incident MIR photon and the plasmon/ phonon in graphene and SiC, respectively, with the oxide layer acting as a coupling medium. Furthermore, we demonstrate the modes' tunability whereby tuning the graphene's Fermi energy, the modes' resonance frequencies can be shifted to ~ 100 cm-1. Lastly, we realize substantial field enhancement, which is achieved by carefully tuning the graphene's Fermi energy and adjusting the spectra position of mode 1(mode on the left of LO frequency) closer to TO frequency. These results hold promise for various photonic applications such as perfect absorber to improve solar cell, MIR photodetectors, and other tunable photonics. [1]P. Rufangura, et al., J. Phys. Mater., vol. 3, no. 3, p. 032005, 2020. [2]T. Low and P. Avouris, ACS nano, vol. 8, no. 2, pp. 1086-1101, 2014. [3]A. G. Brolo, Nat. Photon., vol. 6, no. 11, p. 709, 2012. [4]H. A. Atwater and A. Polman, Nat. Mater., vol. 9, no. 3, p. 205, 2010. [5] N. Mishra et al., Phys. Status Solidi (a), vol. 213, no. 9, pp. 2277-2289, 2016. [6]N. Mishra et al., J. Appl. Phys., vol. 126, no. 6, p. 065304, 2019.

The ability to distinguish between specific and nonspecific binding is important for assessing the interactions between protein receptors and ligands. Surface plasmon resonance (SPR) spectroscopy is an advanced tool to measure binding events, yet the ability to distinguish between specific and nonspecific binding remains a limitation. To address this problem, we use SPR spectroscopy correlated with surface enhanced Raman scattering (SERS). The chemical information present in SERS spectra provides insight into the molecular interactions between functionalized nanoparticles and proteins, which are not detectable by SPR alone. Using a custom instrument with the Kretschmann configuration, we successfully demonstrate simultaneous affinity and the chemical characterization of streptavidin-functionalized gold nanoparticles (STV-NPs) binding to biotin immobilized on a gold film in both air and flowing phosphate buffered saline (PBS). The SPR performance is consistent with that of previous reports. The association constant (KA) for streptavidin/biotin and STV-NPs/biotin interactions observed (2 ± 1 × 107 M-1 and 2.4 ± 0.3 × 1010 M-1, respectively) agree with literature values and show a strong avidity effect associated with the STV-NPs. The SERS scattering from STV-NPs is excited by the surface plasmon polariton and collected from an objective lens mounted over the fluidic channel. The SERS spectra are recorded simultaneously with the SPR sensorgram, and the detected Raman bands provide chemical insight into the binding event. Multivariate curve resolution analysis of the spectra can differentiate specific from nonspecific binding. This label-free, real time, and surface sensitive detection method provides chemical information to protein/ligand binding affinity measurements.

Surface plasmon resonance (SPR) reflectance imaging: Far-field recognition of near-field phenomena

Surface plasmon polariton (SPP) is a kind of electromagnetic oscillation coupling due to the undulation of charge intensity, which is excited at the interface between metal and dielectric. With the help of near-field enhancement, surface plasmon polariton plays an important role in nano-photonics. When the effect of SPP is used to fabricate the single photon resource, not only the volume can be miniaturized, but also the single photon radiation and collection efficiency can be effectively improved. According to the relationship between the factor of Purcell effect and the density of states, we calculate the local density of electromagnetic states(LDOS) and Purcell factor. By analyzing the local densities of electromagnetic states of different metallic materials, we find that silver is the most suitable metal. For a certain metal, the detection distance and the dielectric material also have influences on local density of electromagnetic states and Purcell factor, and they provide important parameters for the designing of single photon resource based on surface plasmon resonances.

Surface plasmon (SP) coupling behaviors of an InGaN/GaN quantum well (QW) with surface plasmon polariton (SPP) induced on a smooth Ag-film/GaN interface and localized surface plasmon (LSP) induced on randomly distributed surface Ag nanoparticles (NPs) are compared based on temperature-dependent, excitation power-dependent, and time-resolved photoluminescence (PL) measurements. By comparing the variations of PL excitation power-dependent emission at 10 and 300 K, the contribution of SP coupling to the increase of PL intensity can be differentiated from that of PL excitation-intensity increase at the QW due to the enhanced reflection at the Ag/GaN interface. The observed stronger SP coupling effect through SPP, when compared with that through LSP, is attributed to its larger available SP state number per unit area for coupling with the QW. Although the SP coupling strength through LSP on the surface Ag NPs is weakly dependent on PL excitation power, that through SPP at the smooth Ag-film/GaN interface increases significantly with PL excitation power. Such different behavior is due to the abundant SPP states available for coupling with the QW of a higher carrier density. It can also be attributed to the spectral blueshift of QW emission through the screening of the quantum-confined Stark effect and the band filling effect for QW coupling with SPP of a higher density of state.

The refractive index sensing characteristics of the side-polished photonic crystal fiber (PCF) surface plasmon resonance (SPR) sensor are detailed investigated in this paper. We used the finite element method (FEM) to study the influences of the side-polished depth, air hole size, lattice constant, and the refractive index (RI) of the PCF material on sensing performance. The simulation results show that the side-polished depth, air hole size, lattice pitch have significant influence on the coupling strength between core mode and surface plasmon polaritons (SPPs), but have little influence on sensitivity; the coupling strength and sensitivity will significant increase with the decrease of RI of the PCF material. The sensitivity of the D-shaped PCF sensor is obtained to be as high as 21700 nm/RIU in the refractive index environment of 1.33-1.34, when the RI of the PCF material is controlled at 1.36. It revealed a new method of making ultra-high sensitivity SPR fiber sensor. Then we experimental demonstrated a SPR refractive sensor based on the side-polished single mode PCF and investigated the sensing performance. The experimental results of the plasmon resonance wavelength sensitivity agree well with the theoretical results. The presented gold-coated D-shaped PCF SPR sensor could be used as a simple, cost-effective, high sensitivity device in bio-chemical detection.

We study the coupling interactions between a progressively elongated silver nanoparticle and a silver film on a glass substrate. Specifically, we investigate how the coupling between localized surface plasmons (LSPs) and propagating surface plasmon polaritons (SPPs) is influenced by nanoparticle length. Although the multiple resonances supported by the nanoparticle are effectively standing wave surface plasmons, their interaction with the SPP continuum of the underlying Ag film indicates that their spectral response is still localized in nature. It is found that these LSP-SPP interactions are not limited to small particles, but that they are present as well for extremely long particles, with a transition to the SPP coupling interactions of a bilayer metallic film system beginning at a particle length of approximately 5 μm.

In recent years, light management based on localized surface plasmon resonance (LSPR) effects in perovskite solar cells (PSCs) has received significant attention. However, the use of surface plasmon polariton (SPP) excitations in PSCs has been less studied. Meanwhile, hole transport layer-free perovskite solar cells (HTL-free PSCs) have garnered interest due to their lower cost. In this study, we improve light absorption in HTL-free PSCs by simultaneously utilizing LSPR and SPP effects. Au nanotriangles are employed on the surface of the back electrode to excite SPPs. The thickness of the perovskite layer is varied from 100 nm to 400 nm. The optimal periodicity and dimensions of the triangular nanoparticles are determined for each perovskite layer thickness. In the optimal structures with perovskite layer thicknesses of 100 nm, 200 nm, 300 nm, and 400 nm, absorption enhancements of 25%, 12.4%, 13%, and 4.3% are achieved, respectively. The interaction of light with SPP and LSP modes leads to improved solar cell performance. Furthermore, the short circuit current density (JSC) in structures with layer thicknesses of 100 nm and 200 nm increased from 16.7 mA cm−2 to 20.71 mA cm−2 and from 19.8 mA cm−2 to 21.86 mA cm−2, respectively. Other photovoltaic characteristics of the solar cell were obtained through optical-electrical numerical analysis. For the improved solar cell with a perovskite thickness of 100 nm, the values of open circuit voltage, efficiency, and fill factor were 0.847 V, 0.81, and 14.24%, respectively, representing increases of 1.1%, 2.4%, and 28.7% compared to the bare device. Additionally, in the solar cell with a thickness of 200 nm, an efficiency of 17.03% was achieved, showing a 12.5% improvement compared to the bare structure. Our research results facilitate the design of high-performance, ultra-thin, semi-transparent solar cells.

Surface plasmon resonance biosensor based on a D-shaped photonic crystal fiber using Ti3C2Tx MXene material