Spatially Resolved Near Field Spectroscopy of Vibrational Polaritons at the Small N Limit.

Vibrational polaritons, which have been primarily studied in Fabry-Pérot cavities with a large number of molecules (N ∼ 106-1010) coupled to the resonator mode, exhibit various experimentally observed effects on chemical reactions. However, the exact mechanism is elusively understood from the theoretical side, as the large number of molecules involved in an experimental strong coupling condition cannot be represented completely in simulations. This discrepancy between theory and experiment arises from computational descriptions of polariton systems typically being limited to only a few molecules, thus failing to represent the experimental conditions adequately. To address this mismatch, we used surface phonon polariton (SPhP) resonators as an alternative platform for vibrational strong coupling. SPhPs exhibit strong electromagnetic confinement on the surface and thus allow for coupling to a small number of molecules. As a result, this platform can enhance nonlinearity and slow down relaxation to the dark modes. In this study, we fabricated a pillar-shaped quartz resonator and then coated it with a thin layer of cobalt phthalocyanine (CoPc). By employing scattering-type scanning near-field optical microscopy (s-SNOM), we spatially investigated the dependency of vibrational strong coupling on the spatially varying electromagnetic field strength and demonstrated strong coupling with 38,000 molecules only-reaching to the small N limit. Through s-SNOM analysis, we found that strong coupling was observed primarily on the edge of the quartz pillar and the apex of the s-SNOM tip, where the maximum field enhancement occurs. In contrast, a weak resonance signal and lack of coupling were observed closer to the center of the pillar. This work demonstrates the importance of spatially resolved polariton systems in nanophotonic platforms and lays a foundation to explore polariton chemistry and chemical dynamics at the small N limit-one step closer to reconcile with high-level quantum calculations.

Utilization of coupled eigenmodes in Akiyama atomic force microscopy probes for bimodal multifrequency sensing.

Akiyama atomic force microscopy probes represent a unique means of combining several of the desirable properties of tuning fork and cantilever probe designs. As a hybridized mechanical resonator, the vibrational characteristics of Akiyama probes result from a complex coupling between the intrinsic vibrational eigenmodes of its constituent tuning fork and bridging cantilever components. Through a combination of finite element analysis modeling and experimental measurements of the thermal vibrations of Akiyama probes we identify a complex series of vibrational eigenmodes and measure their frequencies, quality factors, and spring constants. We then demonstrate the viability of Akiyama probes to perform bimodal multi-frequency force sensing by performing a multimodal measurement of a surface's nanoscale photothermal response using photo-induced force microscopy imaging techniques. Further performing a parametric search over alternative Akiyama probe geometries, we propose two modified probe designs to enhance the capability of Akiyama probes to perform sensitive bimodal multifrequency force sensing measurements.

Space-Time Quantum Metasurfaces.

Metasurfaces have recently entered the realm of quantum photonics, enabling manipulation of quantum light using a compact nanophotonic platform. Realizing the full potential of metasurfaces at the deepest quantum level requires the ability to tune coherent light-matter interactions continuously in space and time. Here, we introduce the concept of space-time quantum metasurfaces for arbitrary control of the spectral, spatial, and spin properties of nonclassical light using a compact photonic platform. We show that space-time quantum metasurfaces allow on-demand tailoring of entanglement among all degrees of freedom of a single photon. We also show that spatiotemporal modulation induces asymmetry at the fundamental level of quantum fluctuations, resulting in the generation of steered and vortex photon pairs out of vacuum. Space-time quantum metasurfaces have the potential to enable novel photonic functionalities, such as encoding quantum information into high-dimensional color qudits using designer modulation protocols, sculpting multispectral and multispatial modes in spontaneous emission, and generating reconfigurable hyperentanglement for high-capacity quantum communications.

Near-Field Radiative Heat Transfer Eigenmodes.

The near-field electromagnetic interaction between nanoscale objects produces enhanced radiative heat transfer that can greatly surpass the limits established by far-field blackbody radiation. Here, we present a theoretical framework to describe the temporal dynamics of the radiative heat transfer in ensembles of nanostructures, which is based on the use of an eigenmode expansion of the equations that govern this process. Using this formalism, we identify the fundamental principles that determine the thermalization of collections of nanostructures, revealing general but often unintuitive dynamics. Our results provide an elegant and precise approach to efficiently analyze the temporal dynamics of the near-field radiative heat transfer in systems containing a large number of nanoparticles.

Nonlinear dynamics of topological Dirac fermions in 2D spin-orbit coupled materials.

The graphene family materials are two-dimensional staggered monolayers with a gapped energy band structure due to intrinsic spin-orbit coupling. The mass gaps in these materials can be manipulated on-demand via biasing with a static electric field, an off-resonance circularly polarized laser, or an exchange interaction field, allowing the monolayer to be driven through a multitude of topological phase transitions. We investigate the dynamics of spin-orbit coupled graphene family materials to unveil topological phase transition fingerprints embedded in the nonlinear regime and show how these signatures manifest in the nonlinear Kerr effect and in third-harmonic generation processes. We show that the resonant nonlinear spectral response of topological fermions can be traced to specific Dirac cones in these materials, enabling characterization of topological invariants in any phase by detecting the cross-polarized component of the electromagnetic field. By shedding light on the unique processes involved in harmonic generation via topological phenomena our findings open an encouraging path towards the development of novel nonlinear systems based on two-dimensional semiconductors of the graphene family.

Surface-wave-assisted nonreciprocity in spatio-temporally modulated metasurfaces.

Emerging photonic functionalities are mostly governed by the fundamental principle of Lorentz reciprocity. Lifting the constraints imposed by this principle could circumvent deleterious effects that limit the performance of photonic systems. Most efforts to date have been limited to waveguide platforms. Here, we propose and experimentally demonstrate a spatio-temporally modulated metasurface capable of complete violation of Lorentz reciprocity by reflecting an incident beam into far-field radiation in forward scattering, but into near-field surface waves in reverse scattering. These observations are shown both in nonreciprocal beam steering and nonreciprocal focusing. We also demonstrate nonreciprocal behavior of propagative-only waves in the frequency- and momentum-domains, and simultaneously in both. We develop a generalized Bloch-Floquet theory which offers physical insights into Lorentz nonreciprocity for arbitrary spatial phase gradients, and its predictions are in excellent agreement with experiments. Our work opens exciting opportunities in applications where free-space nonreciprocal wave propagation is desired.

Highly Plasmonic Titanium Nitride by Room-Temperature Sputtering.

Titanium nitride (TiN) has recently emerged as an attractive alternative material for plasmonics. However, the typical high-temperature deposition of plasmonic TiN using either sputtering or atomic layer deposition has greatly limited its potential applications and prevented its integration into existing CMOS device architectures. Here, we demonstrate highly plasmonic TiN thin films and nanostructures by a room-temperature, low-power, and bias-free reactive sputtering process. We investigate the optical properties of the TiN films and their dependence on the sputtering conditions and substrate materials. We find that our TiN possesses one of the largest negative values of the real part of the dielectric function as compared to all other plasmonic TiN films reported to date. Two-dimensional periodic arrays of TiN nanodisks are then fabricated, from which we validate that strong plasmonic resonances are supported. Our room-temperature deposition process can allow for fabricating complex plasmonic TiN nanostructures and be integrated into the fabrication of existing CMOS-based photonic devices to enhance their performance and functionalities.

High-Temperature Refractory Metasurfaces for Solar Thermophotovoltaic Energy Harvesting.

Solar energy promises a viable solution to meet the ever-increasing power demand by providing a clean, renewable energy alternative to fossil fuels. For solar thermophotovoltaics (STPV), high-temperature absorbers and emitters with strong spectral selectivity are imperative to efficiently couple solar radiation into photovoltaic cells. Here, we demonstrate refractory metasurfaces for STPV with tailored absorptance and emittance characterized by in situ high-temperature measurements, featuring thermal stability up to at least 1200 °C. Our tungsten-based metasurface absorbers have close-to-unity absorption from visible to near-infrared and strongly suppressed emission at longer wavelengths, while our metasurface emitters provide wavelength-selective emission spectrally matched to the band-edge of InGaAsSb photovoltaic cells. The projected overall STPV efficiency is as high as 18% when a fully integrated absorber/emitter metasurface structure is employed, which is comparable to the efficiencies of the best currently available commercial single-junction PV cells and can be further improved to potentially exceed those in mainstream photovoltaic technologies. Our work opens a path forward for high-performance STPV systems based on refractory metasurface structures.

Casimir force phase transitions in the graphene family.

The Casimir force is a universal interaction induced by electromagnetic quantum fluctuations between any types of objects. The expansion of the graphene family by adding silicene, germanene and stanene (2D allotropes of Si, Ge, and Sn), lends itself as a platform to probe Dirac-like physics in honeycomb staggered systems in such a ubiquitous interaction. We discover Casimir force phase transitions between these staggered 2D materials induced by the complex interplay between Dirac physics, spin-orbit coupling and externally applied fields. In particular, we find that the interaction energy experiences different power law distance decays, magnitudes and dependences on characteristic physical constants. Furthermore, due to the topological properties of these materials, repulsive and quantized Casimir interactions become possible.

Metasurface Broadband Solar Absorber.

We demonstrate a broadband, polarization independent, wide-angle absorber based on a metallic metasurface architecture, which accomplishes greater than 90% absorptance in the visible and near-infrared range of the solar spectrum, and exhibits low absorptivity (emissivity) at mid- and far-infrared wavelengths. The complex unit cell of the metasurface solar absorber consists of eight pairs of gold nano-resonators that are separated from a gold ground plane by a thin silicon dioxide spacer. Our experimental measurements reveal high-performance absorption over a wide range of incidence angles for both s- and p-polarizations. We also investigate numerically the frequency-dependent field and current distributions to elucidate how the absorption occurs within the metasurface structure.

Lipopolysaccharide from the periodontal pathogen Porphyromonas gingivalis prevents apoptosis of HL60-derived neutrophils in vitro.

Lipopolysaccharide (LPS) from Porphyromonas gingivalis prevented apoptosis of HL60-derived neutrophils, which could not be restored upon the addition of interleukin-10. Signaling of P. gingivalis LPS through Toll-like receptor 2 (TLR2), not TLR4, may account for the inhibiting effect of P. gingivalis LPS on apoptosis and provide a mechanism for the development of destructive periodontal inflammation.

Neutrophils die in the gingival crevice, periodontal pocket, and oral cavity by necrosis and not apoptosis.

BACKGROUND: Neutrophils play important roles in the homeostasis of periodontal tissues. However, remarkably little is known about how these cells live and die in the gingival crevice and periodontal pocket. We have examined whether subgingival neutrophils die by necrosis or apoptosis and have begun to study the mechanisms controlling the functional lifespan of these cells. METHODS: Neutrophils collected from clinically healthy gingival crevices, periodontal pockets, and the oral cavity (saliva) were examined with Hoechst dye 33342, propidium iodide/eithidium bromide, and FITC-annexin V to identify live, dead, and apoptotic cells. Blood neutrophils were cultured for 17 to 20 hours in the presence or absence of gingival crevice washings (GC-w) to study the effect of GC-w on neutrophil apoptosis. In addition, endotoxin was removed from GC-w by affinity resin to investigate the contribution of LPS to the inhibitory effect of GC-w on blood neutrophils. RESULTS: The percentage of dead neutrophils in all subgingival sites and in all oral samples far exceeded the percentage of apoptotic neutrophils. In all 3 locations, approximately 30% of neutrophils were dead, whereas less than 1% of neutrophils were apoptotic. We conclude that the majority of neutrophils which lose their viability within gingival crevices, periodontal pockets and the oral cavity die by necrosis and not by apoptosis. Washings obtained from clinically healthy gingival crevices (GC-w) variably, but significantly, delayed apoptosis of peripheral blood neutrophils (mean suppression 45.7% +/- SD 22.3). Removal of endotoxin from GC-w significantly reduced this inhibitory effect. CONCLUSIONS: Our findings provide insights into the mechanisms of neutrophil death and the control of the functional lifespan of neutrophils in gingival crevices and periodontal pockets and therefore into the pathogenesis of periodontal diseases.

Permeability of the gingival tissues to IgM during an experimental gingivitis study in man.

Changes in the permeability of the underlying vasculature of the gingival crevice region may occur either as part of an inflammatory response during gingivitis or as a response to trauma during collection of gingival crevicular fluid IgM was selected as a marker of permeability and the concentration in gingival crevicular fluid was determined immunochemically by dot blotting, using rabbit antihuman IgM specific for mu chain. Gingival crevicular fluid samples were derived from experimental (non-cleaning) and control (cleaning) sites in six individuals participating in a 28-day experimental gingivitis study using a split-mouth protocol. The fluid was collected by a filter-paper method. At each site, four gingival crevicular fluid samples were collected for 5 s each over a 3-min period and a fifth sample was collected after a further 6 min. IgM was detected in 7/30 experimental strips at baseline (after intensive professional prophylaxis) and this increased to 21/30 by 24 days: control values were 13/30 and 12/30, respectively. The data indicate that IgM was detected with greater frequency as gingivitis becomes evident, suggesting increased permeability in response to plaque accumulation. IgM was detected in 17/120 of the first strip samples, collected over the 66-day study period, whereas in the fifth strip samples IgM was detected in 68/120, and the concentration of IgM in gingival crevicular fluid also increased, indicating that sequential collection induced permeability. It is concluded that the permeability of the gingiva changes in response to both an inflammatory stimulus and trauma due to collection.

Elevated opsonic activity for Porphyromonas (Bacteroides) gingivalis in serum from patients with a history of destructive periodontal disease. A case: control study.

We have measured the opsonic capacity of serum for the phagocytosis of Porphyromonas (Bacteroides) gingivalis by polymorphonuclear leucocytes (PMN) in 35 patients with a history of destructive periodontitis and 35 matched control subjects. The serum from cases, tested at concentrations of 8% and 0.8% opsonised P. gingivalis for phagocytosis by PMN to a level significantly greater than controls (p < 0.0001 and < 0.01 respectively). IgG antibody levels to P. gingivalis whole cells estimated by ELISA were also significantly higher in the cases (p < 0.0001). The IgG antibody levels correlated significantly with the opsonic capacity of the serum tested at 8% concentration in controls (r = 0.371, p = 0.03) but not in cases (r = 0.235, p = 0.17); in 0.8% serum, the opsonic capacity of the cases and controls were not significantly correlated. Elevated opsonisation by serum was a significant predictor that a subject was a case rather than a control, even after allowing for the effect of elevated IgG antibody in the cases. The data suggest that an elevated capacity of serum to opsonise P. gingivalis is a distinctive feature in patients with past destructive periodontal disease.

Serum immunoglobulin G antibodies to Porphyromonas gingivalis, Prevotella intermedia, Fusobacterium nucleatum and Streptococcus sanguis during experimental gingivitis in young adults.

Twenty-eight young, healthy adults completed an experimental gingivitis study in which blood and clinical recordings were obtained at baseline; after a 4-week period of thorough oral hygiene; after a subsequent 3-week period of plaque accumulation; and after another 2 weeks of thorough oral hygiene. Serum immunoglobulin G antibodies against whole cells of Porphyromonas gingivalis, Prevotella intermedia, Fusobacterium nucleatum and Streptococcus sanguis were determined using enzyme-linked immunosorbent assay. Mean serum immunoglobulin G antibody levels to P. intermedia, F. nucleatum and S. sanguis remained essentially constant during the experiment, whereas the immunoglobulin G antibodies to P. gingivalis declined during the initial period of oral hygiene and the subsequent period of plaque accumulation to an average of 84.5% of the baseline value. This reduction could be attributed to the people who developed marked gingival inflammation during the period of plaque accumulation, indicating that the systemic host response may be associated with local tissue responses to variations in oral hygiene. These people were, however, also characterized by higher initial serum immunoglobulin G responses to P. gingivalis than people who developed less pronounced gingival inflammation during the experiment. The variability and individuality noted in the host response to potential pathogens have important implications for attempts to use such measures for establishing a diagnosis or prognosis for the individual patient.

Inhibition of polymorphonuclear leucocyte phagocytosis by Porphyromonas gingivalis culture products in patients with adult periodontitis.

Porphyromonas gingivalis culture products and a purified trypsin-like protease (TLPase) from the organism were tested for their effects on the phagocytosis of P. gingivalis by polymorphonuclear leucocytes (PMN) from 16 patients with adult periodontitis and 16 healthy subjects in a case-control study. Both the culture products (p < 0.0001) and the TLPase (p < 0.0001) significantly inhibited PMN phagocytosis by both case and control samples. Culture products were significantly more inhibitory in both cases (p < 0.0019) and controls (p < 0.0198) than that TLPase. The case PMNs were significantly more susceptible to inhibition by culture products than the control PMNs (p < 0.0238). The data suggest that patients with adult periodontitis have PMNs that are more susceptible than normal to the inhibitory effects of P. gingivalis and might be at greater risk than healthy subjects to infection by this pathogen.

Interleukin-1 beta and IgG subclass concentrations in gingival crevicular fluid from patients with adult periodontitis.

Interleukin-1 beta (IL-1 beta) and the four IgG subclasses were measured in gingival crevicular fluid (GCF) at 35 sites in 19 patients with adult periodontitis. Serum concentrations of the IgG subclasses were assayed in 16 patients. IL-1 beta was detected in GCF at 88.6% of sites at concentrations ranging from 12.38-420.90 pg/microliters (mean 138.35 +/- 112.61 pg/microliters). IgG1 was detected at 81.2% sites, IgG2 at 93.6%, IgG3 at 71% and IgG4 at 71%. Absolute concentrations in GCF were: IgG1--2.419 g/l +/- (SD) 3.389; IgG2--2.945 +/- 6.434; IgG3--0.118 +/- 0.144; IgG4 0.864 +/- 1.336. There were no significant correlations between IL-1 beta concentrations, GCF volume or the clinical status of the sample site. IL-1 beta was not correlated with any of the IgG subclasses. The absolute concentrations of all subclasses in GCF were significantly negatively correlated with GCF volume and positively correlated with the Bleeding Index. Only IgG4 was significantly negatively correlated with the probeable crevice depth index. The concentration of each IgG subclass was positively correlated with the other three IgG subclasses. Subclass concentrations in GCF, relative to serum concentrations, were not correlated with GCF volume or clinical status. Relative concentrations of IgG1, IgG2 and IgG3 showed significant positive correlation with each absolute concentration of the other subclasses but IgG4 did not show this relation. It was concluded that IL-1 beta is not related to clinical measurements of inflammation or previous attachment loss. The data suggest that IgG in GCF is largely derived from plasma but that some IgG4 may be locally synthesized.

Leukocyte activation and function-associated antigens in inflammatory disease.

Expression of adhesion molecules, CD11a, CD11b and CD18, and of the function-associated molecules CD3, CD4, CD8, CD16, CD19, CD56 and CD57 was assayed on peripheral blood leukocytes from normal control subjects (n = 10), and from patients with adult periodontitis PD (n = 9), ankylosing spondylitis AS (n = 11) and rheumatoid arthritis RA (n = 14). A novel rapid fixation leukocyte preparation technique was used which prevents artefactual up-regulation of surface antigens. In RA patients, the percentage of CD18+ lymphocytes was decreased and that of CD11b+ neutrophils was increased. On lymphocytes the mean fluorescence intensity (MFI) of both CD11b and CD18 was decreased whereas that of CD57 was increased. In AS patients the percentages of CD11b+ lymphocytes and neutrophils were increased and CD18+ lymphocytes and neutrophils were decreased. On lymphocytes the MFIs of CD11b and CD18 were decreased, whilst that of CD16 was increased. On neutrophils the MFI for CD18 was increased. No significant differences (p < 0.01) were seen for the periodontitis patients. It is suggested that the antigen expression on peripheral blood cells from RA and AS patients is consistent with leukocyte activation.

IgG subclass antibodies to Porphyromonas gingivalis in patients with destructive periodontal disease. A case: control study.

We have estimated by ELISA the levels of IgG subclass antibodies against P. gingivalis strain W83 whole cells in 35 cases of adult periodontitis and 35 age, sex, ethnic origin and plaque index-matched healthy controls. The mean levels of IgG1 (p < 0.0003) and IgG2 (p < 0.0416) were significantly elevated in the cases. Many sera had no detectable IgG4 antibodies but by categorising IgG4 responses into high, low and absent, this subclass was more often present (p < 0.002) in the cases. Analysis of the paired differences between cases and controls showed that only IgG1 (p < 0.0005) and IgG4 (p < 0.003) levels were significantly greater in the cases. The data support the role of P. gingivalis as a key pathogen in adult periodontitis and high levels of IgG4 antibodies might possibly provide a marker of patients with active disease.