Thyboconley7402
The interaction between light and metal nanoparticles enables investigations of microscopic phenomena on nanometer length and ultrashort timescales, benefiting from strong confinement and enhancement of the optical field. However, the ultrafast dynamics of these nanoparticles are primarily investigated by multiphoton photoluminescence on picoseconds or photoemission on femtoseconds independently. Here, we presented two-photon photoluminescence (TPPL) measurements on individual Au nanobipyramids (AuNP) to reveal their ultrafast dynamics by double-pulse excitation on a global timescale ranging from subfemtosecond to tens of picoseconds. Two orders of magnitude photoluminescence enhancement, namely, coherent interference fringes, has been demonstrated. Power-dependent measurements uncovered the transform of the nonlinearity from 1 to 2 when the interpulse delay varied from tens of femtoseconds to tens of picoseconds. We proved that the real intermediate state plays a critical role in the observed phenomena, supported by numerical simulations with a three-state model. Our results provide insight into the role of intermediate states in the ultrafast dynamics of noble metal nanoparticles. The presence of the intermediate states in AuNP and the coherent control of state populations offer interesting perspectives for imaging, sensing, nanophotonics, and in particular, for preparing macroscopic superposition states at room temperature and low-power superresolution stimulated emission depletion microscopy.The sensitivity of current and planned gravitational wave interferometric detectors is limited, in the most critical frequency region around 100 Hz, by a combination of quantum noise and thermal noise. The latter is dominated by Brownian noise thermal motion originating from the elastic energy dissipation in the dielectric coatings used in the interferometer mirrors. The energy dissipation is a material property characterized by the mechanical loss angle. We have identified mixtures of titanium dioxide (TiO_2) and germanium dioxide (GeO_2) that show internal dissipations at a level of 1×10^-4, low enough to provide improvement of almost a factor of 2 on the level of Brownian noise with respect to the state-of-the-art materials. We show that by using a mixture of 44% TiO_2 and 56% GeO_2 in the high refractive index layers of the interferometer mirrors, it would be possible to achieve a thermal noise level in line with the design requirements. These results are a crucial step forward to produce the mirrors needed to meet the thermal noise requirements for the planned upgrades of the Advanced LIGO (Laser Interferometer Gravitational-Wave Observatory) and Virgo detectors.Magnetic oscillations of Dirac surface states of topological insulators are typically expected to be associated with the formation of Landau levels or the Aharonov-Bohm effect. We instead study the conductance of Dirac surface states subjected to an in-plane magnetic field in the presence of a barrier potential. Strikingly, we find that, in the case of large barrier potentials, the surface states exhibit pronounced oscillations in the conductance when varying the magnetic field, in the absence of Landau levels or the Aharonov-Bohm effect. These novel magnetic oscillations are attributed to the emergence of super-resonant transport by tuning the magnetic field, in which many propagating modes cross the barrier with perfect transmission. In the case of small and moderate barrier potentials, we identify a positive magnetoconductance due to the increase of the Fermi surface by tilting the surface Dirac cone. Moreover, we show that for weak magnetic fields, the conductance displays a shifted sinusoidal dependence on the field direction with period π and phase shift determined by the tilting direction with respect to the field direction. Our predictions can be applied to various topological insulators, such as HgTe and Bi_2Se_3, and provide important insights into exploring and understanding exotic magnetotransport properties of topological surface states.We present predictions for the gluon-fusion Higgs p_T spectrum at third resummed and fixed order (N^3LL^'+N^3LO) including fiducial cuts as required by experimental measurements at the Large Hadron Collider. Integrating the spectrum, we predict for the first time the total fiducial cross section to third order (N^3LO) and improved by resummation. The N^3LO correction is enhanced by cut-induced logarithmic effects and is not reproduced by the inclusive N^3LO correction times a lower-order acceptance. These are the highest-order predictions of their kind achieved so far at a hadron collider.Dissolving small amounts of polymer into a Newtonian fluid can dramatically change the dynamics of transitional and turbulent flows. We investigate the spatiotemporal dynamics of a submerged jet of dilute polymer solution entering a quiescent bath of Newtonian fluid. High-speed digital Schlieren imaging is used to quantify the evolution of Lagrangian features in the jet revealing a rich sequence of transitional and turbulent states. At high levels of viscoelasticity, we identify a new distinct transitional pathway to elastoinertial turbulence (EIT) that does not feature the conventional turbulent bursts and instead proceeds via a shear-layer instability that produces elongated filaments of polymer due to the nonlinear effects of viscoelasticity. Even though the pathways to the EIT state can be different, and within EIT the spatial details of the turbulent structures vary systematically with polymer microstructure and concentration, there is a universality in the power-law spectral decay of EIT with frequency, f^-3, independent of fluid rheology and flow parameters.The fractal velocity pattern in symmetric kink-antikink collisions in ϕ^4 theory is shown to emerge from a dynamical model with two effective moduli the kink-antikink separation and the internal shape mode amplitude. The shape mode usefully approximates Lorentz contractions of the kink and antikink, and the previously problematic null vector in the shape mode amplitude at zero separation is regularized.A simple and efficient mechanochemical-induced approach for the synthesis of 1,2-diketoindolizine derivatives has been developed. BaTiO3 was used as the piezoelectric material in this transformation. This method features no usage of solvent, simple experimental operation, scalable potential, and high conversion efficiency, which make it attractive and practical.Smart wearable electronic accessories (e.g., watches) have found wide adoption; conversely, progress in electronic textiles has been slow due to the difficulty of embedding rigid electronic materials into flexible fabrics. Electronic clothing requires fibers that are conductive, robust, biocompatible, and can be produced on a large scale. Here, we create sewable electrodes and signal transmission wires from neat carbon nanotube threads (CNTT). These threads are soft like standard sewing thread, but they have metal-level conductivity and low interfacial impedance with skin. Electrocardiograms (EKGs) obtained by CNTT electrodes were comparable (P > 0.05) to signals obtained with commercial electrodes. CNTT can also be used as transmission wires to carry signals to other parts of a garment. Finally, the textiles can be machine-washed and stretched repeatedly without signal degradation. These results demonstrate promise for textile sensors and electronic fabric with the feel of standard clothing that can be incorporated with traditional clothing manufacturing techniques.It remains unclear how the precise length of one-dimensional nanovehicles influences the characters of vaccination. Here, a unimolecular nanovehicle with tailored size and aspect ratio (AR) is applied to deliver CpG oligodeoxynucleotide, a Toll-like receptor (TLR) 9 agonist, as an adjuvant of recombinant hepatitis B virus surface antigen (rHBsAg), for treating chronic hepatitis B (CHB). Cationic nanovehicles with fixed width (ca. 45 nm) but varied length (46 nm-180 nm), AR from 1 to 4, are prepared through controlled polymerization and are loaded with CpG by electrostatic interaction. We reveal that the nanoadjuvant with AR = 2 shows the highest retention in proximal lymph nodes. Ertugliflozin ic50 Importantly, it is more easily internalized into antigen-presenting cells and accumulates in the late endosome, where TLR9 is located. Such a nanoadjuvant exhibits the strongest immune response with rHBsAg to clear the hepatitis B virus in the CHB mouse model, showing that the AR of nanovehicles governs the efficiency of vaccination.We describe a synergistic utilization of copper catalysis and proton-transfer catalysis that enables an atom- and step-economical aza-[4 + 2] cycloaddition reaction of readily available N-arylamino carbonyl compounds with simple 1,3-dienes. The reaction proceeds smoothly under an air atmosphere and produces water as the sole side product. Whereas the amines can directly serve as the C- and N-atom donors, this operationally simple protocol provides green, rapid, and efficient access to 1,2,3,6-tetrahydropyridines with a broad scope.The concise synthesis of dysifragilones A and B and dysidavarones has been accomplished for the first time in a divergent way from a common intermediate. The synthetic route features an intramolecular reductive Heck reaction to construct the 6/5/6/6/-tetracycle of dysifragilones A and B and an intramolecular palladium-catalyzed α-arylation of a sterically hindered ketone to forge the tetracyclo[7.7.1.02,7.010,15]heptadecane core structure of dysidavarone C. The late-stage introduction of amino and ethoxy groups is effective.The absolute configuration of rakicidin C was predicted by comparison of optical rotation data and absolute configuration of APD-cyclic depsipeptides and further determined by total synthesis. The absolute configuration of five chiral centers was determined as 2R, 15R, 16R, 17S, and 19S. Our efficient route involves 19 longest linear steps with an overall yield of 1.49%.A photochemical protocol that couples diarylamines and α-ketoesters to afford the chiral 3-hydroxyoxindoles through tandem photoredox and chiral phosphoric acid catalysis is developed. The reaction involves an enantioselective photochemical radical-radical cross-coupling process. The chiral phosphoric acid is discovered to play crucial roles by decreasing the reductive potentials of α-ketoesters and stereocontrolling the downstream asymmetric radical-radical cross-coupling via the formation of pentacoordinate complex.Herein, we report the total synthesis of the phosphorylated zwitterionic trisaccharide repeating unit of Photorhabdus temperata subsp. cinerea 3240. The efficient route involves regio- and stereoselective assembly of trisaccharide with rare deoxyamino sugar AAT at the nonreducing end, late stage oxidation, and installation of a phosphate linker on the trisaccharide. The total synthesis was completed via a longest linear sequence of 24 steps in 6.5% overall yield.Plasmonic metasurfaces supporting collective lattice resonances have attracted increasing interest due to their exciting properties of strong spatial coherence and enhanced light-matter interaction. Although the focusing of light by high-numerical-aperture (NA) objectives provides an essential way to boost the field intensities, it remains challenging to excite high-quality resonances by using high-NA objectives due to strong angular dispersion. Here, we address this challenge by employing the physics of bound states in the continuum (BICs). We design a novel anisotropic plasmonic metasurface combining a two-dimensional lattice of high-aspect-ratio pillars with a one-dimensional plasmonic grating, fabricated by a two-photon polymerization technique and gold sputtering. We demonstrate experimentally multiple resonances with absorption amplitudes exceeding 80% at mid-IR using an NA = 0.4 reflective objective. This is enabled by the weak angular dispersion of quasi-BIC resonances in such hybrid plasmonic metasurfaces.