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Natural photosynthesis relies on a sophisticated charge transfer pathway among multiple components with precise spatial, energetic, and temporal organizations in the aqueous environment. It continues to inspire and challenge the design and fabrication of artificial multicomponent colloidal nanostructures for solar-to-fuel conversion. Herein, we introduce a plasmonic photocatalyst synthesized with colloidal methods with five integrated components including cocatalysts installed in orthogonal locations. The precise deposition of individual inorganic components on an Au/TiO2 nanodumbell nanostructure is enabled by photoreduction and photo-oxidation, which selectively occurs at the TiO2 tip sites and Au lateral sites, respectively. Under visible-light irradiation, the photocatalyst exhibited activity of oxygen evolution from water without scavengers. We demonstrate that each component is essential for improving the photocatalytic performance. In addition, mechanistic studies suggest that the photocatalytic reaction requires combining the hot charge carriers derived from exciting both the d-sp interband transition and the localized surface plasmon resonance of Au.

Plasmonic nanostructures have a wide range of applications, including chemical and biological sensing. However, the development of techniques to fabricate submicrometer-sized plasmonic structures over large scales remains challenging. We demonstrate a high-throughput, cost-effective approach to fabricate Au nanoribbons via chemical lift-off lithography (CLL). Commercial HD-DVDs were used as large-area templates for CLL. Transparent glass slides were coated with Au/Ti films and functionalized with self-assembled alkanethiolate monolayers. Monolayers were patterned with lines via CLL. The lifted-off, exposed regions of underlying Au were selectively etched into large-area grating-like patterns (200 nm line width; 400 nm pitch; 60 nm height). After removal of the remaining monolayers, a thin In2O3 layer was deposited and the resulting gratings were used as plasmonic sensors. Distinct features in the extinction spectra varied in their responses to refractive index changes in the solution environment with a maximum bulk sensitivity of ∼510 nm/refractive index unit. Sensitivity to local refractive index changes in the near-field was also achieved, as evidenced by real-time tracking of lipid vesicle or protein adsorption. These findings show how CLL provides a simple and economical means to pattern large-area plasmonic nanostructures for applications in optoelectronics and sensing.

Optogenetics provides promising tools for the precise control of receptor-mediated cell behaviors in a spatiotemporal manner. Yet, most photoreceptors require extensive genetic manipulation and respond only to ultraviolet or visible light, which are suboptimal for in vivo applications because they do not penetrate thick tissues. Here we report a novel near-infrared light-activated DNA agonist (NIR-DA) nanodevice for nongenetic manipulation of cell signaling and phenotype in deep tissues. This nanodevice is prepared by conjugating a preinactivated DNA agonist onto the gold nanorods (AuNRs). Upon NIR light treatment, the DNA agonist is released through the localized surface plasmon resonance (LSPR)-based photothermal effect of AuNRs and becomes active. The active DNA agonist dimerizes the DNA-modified chimeric or native receptor tyrosine kinase (RTK) on cell surfaces and activates downstream signal transduction in live cells. Such NIR-DA activation of RTK signaling enables the control of cytoskeletal remodeling, cell polarization, and directional migration. Furthermore, we demonstrate that the NIR-DA system can be used in vivo to mediate RTK signaling and skeletal muscle satellite cell migration and myogenesis, which are critical cellular behaviors in the process of skeletal muscle regeneration. Thus, the NIR-DA system offers a powerful and versatile platform for exogenous modulation of deep tissues for purposes such as regenerative medicine.

Traditional deicing methods are increasingly insufficient for modern technologies like 5G infrastructure, photovoltaic systems, nearspace aerocraft, and terrestrial observatories. To address the challenge of combining anti-icing efficiency with operational performance, an innovative, spectrally selective, photo/electrothermic, ice-phobic film was prepared through a cost-effective mist deposition method. By manipulating the diameter ratio and density of nanowires, the local density of free electrons within this film is controlled to precisely dictate the position and intensity of surface plasmon resonance to achieve spectrally selective photo/electrothermal conversion. Additionally, the synthesized hydrophobic N-Boroxine-PDMS/SiO 2 layer improves thermal stability and accelerates the deicing process. It achieves rapid deicing within 86 s under photothermal conditions and 65 s with Joule heating while maintaining high optical transmittance. The film improves the operational efficiency and thermal safety of equipment while preserving aesthetics and stability, thereby underscoring its broad suitability for advanced outdoor installations in cold environments.

We report a nanoinfrared (IR) imaging study of the localized plasmon resonance modes of graphene nanoribbons (GNRs) using a scattering-type scanning near-field optical microscope (s-SNOM). By comparing the imaging data of GNRs that are aligned parallel and perpendicular to the in-plane component of the excitation laser field, we observed symmetric and asymmetric plasmonic interference fringes, respectively. Theoretical analysis indicates that the asymmetric fringes are formed due to the interplay between the localized surface plasmon resonance (SPR) mode excited by the GNRs and the propagative surface plasmon polariton (SPP) mode launched by the s-SNOM tip. With rigorous simulations, we reproduce the observed fringe patterns and address quantitatively the role of the s-SNOM tip on both the SPR and SPP modes. Furthermore, we have seen real-space signatures of both the dipole and higher-order SPR modes by varying the ribbon width.

The metal plasmonic nanostructure has the optical property of plasmon resonance, which holds great potential for development in nanophotonics, bioelectronics, and molecular detection. However, developing a general and straightforward method to prepare metal plasmonic nanostructures with a controllable size and morphology still poses a challenge. Herein, we proposed a synthesis strategy that utilized a customizable self-assembly template for shape-directed growth of metal structures. We employed gold nanoparticles (AuNPs) as connectors and DNA nanotubes as branches, customizing gold nanoparticle-DNA origami composite nanostructures with different branches by adjusting the assembly ratio between the connectors and branches. Subsequently, various morphologies of plasmonic metal nanostructures were created using this template shape guided strategy, which exhibited enhancement of surface-enhanced Raman scattering (SERS) signals. This strategy provides a new approach for synthesizing metallic nanostructures with multiple morphologies and opens up another possibility for the development of customizable metallic plasmonic structures with broader applications.

Detection and characterization of molecular interactions on membrane surfaces is important to biological and pharmacological research. Here, silver nanocubes interfaced with glass-supported model membranes form a label-free sensor that measures protein binding to the membrane. The technique utilizes plasmon resonance scattering of nanocubes, which are chemically coupled to the membrane. In contrast to other plasmonic sensing techniques, this method features simple, solution-based device fabrication and readout. Static and dynamic protein/membrane binding are monitored and quantified.

Here, we present a mapping tool based on individual light-driven nano-oscillators for label-free single-molecule monitoring of microRNA. This design uses microRNA as a single-molecule damper for nano-oscillators by forming a rigid dual-strand structure in the gap between nano-oscillators and the immobilized surface. The ultrasensitive detection is attributed to comparable dimensions of the gap and microRNA. A developed surface plasmon-coupled scattering imaging technology enables us to directly measure the real-time gap distance vibration of multiple nano-oscillators with high accuracy and fast dynamics. High-level and low-level states of the oscillation amplitude indicate melting and hybridization statuses of microRNA. Lifetimes of two states reveal that the hybridization rate of microRNA is determined by the three-dimensional diffusion. This imaging technique contributes application potentials in a single-molecule detection and nanomechanics study. [ABSTRACT FROM AUTHOR]

Chiral photochemistry remains a challenge because of the very small asymmetry in the chiro-optical absorption of molecular species. However, we think that the rapidly developing fields of plasmonic chirality and plasmon-induced circular dichroism demonstrate very strong chiro-optical effects and have the potential to facilitate the development of chiral photochemistry and other related applications such as chiral separation and sensing. In this study, we propose a new type of chiral spectroscopy–photothermal circular dichroism. It is already known that the planar plasmonic superabsorbers can be designed to exhibit giant circular dichroism signals in the reflection. Therefore, upon illumination with chiral light, such planar metastructures should be able to generate a prominent asymmetry in their local temperatures. Indeed, we demonstrate this chiral photothermal effect using a chiral plasmonic absorber. Calculated temperature maps show very strong photothermal circular dichroism. One of the structures computed in this Letter could serve as a chiral bolometer sensitive to circularly polarized light. Overall, this chiro-optical effect in plasmonic metamaterials is much greater than the equivalent effect in any chiral molecular system or plasmonic bioassembly. Potential applications of this effect are in polarization-sensitive surface photochemistry and chiral bolometers. [ABSTRACT FROM AUTHOR]

In this study, we demonstrate the synthesis and application of magnetic plasmonic gyro-nanodisks (GNDs) for Fourier transform surface plasmon resonance based biodetection. Plasmonically active and magnetically responsive gyro-nanodisks were synthesized using electrochemical methods with anodized aluminum templates. Due to the unique properties of GNDs (magnetic responsiveness and surface plasmon bands), periodic extinction signals were generated under an external rotating magnetic field, which is, in turn, converted into frequency domains using Fourier transformation. After the binding of a target on GNDs, an increase in the shear force causes a shift in the frequency domain, which allows us to investigate biodetection for HA1 (the influenza virus). Most importantly, by modulating the number and the location of plasmonic nanodisks (a method for controlling the hydrodynamic forces by rationally designing the nanomaterial architecture), we achieved enhanced biodetection sensitivity. We expect that our results will contribute to improved sensing module performance, as well as a better understanding of dynamic nanoparticle systems, by harnessing the perturbed periodic fluctuation of surface plasmon bands under the modulated magnetic field. [ABSTRACT FROM AUTHOR]

Metallic nanostructures exhibit a strong plasmon resonance at a wavelength whose value is sensitive to the charge density in the nanostructure, its size, shape, interparticle coupling, and the dielectric properties of its surrounding medium. Here we use UV-visible transmission and reflectance spectroscopy to track the shifts of the plasmon resonance in an array of gold nanoparticles buried under metal-oxide layers of varying thickness produced using atomic layer deposition (ALD) and then coated with bulk layers of one of three metals: aluminum, silver, or gold. A significant shift in the plasmon resonance was observed and a precise value of ωp, the plasmon frequency of the gold comprising the nanoparticles, was determined by modeling the composite of gold nanoparticles and metal-oxide layer as an optically homogeneous film of core-shell particles bounded by two substrates: one of quartz and the other being one of the aforementioned metals, then using a Maxwell-Garnett effective medium expression to extract ωp for the gold nanoparticles before and after coating with the bulk metals. Under illumination, the change in the charge density of the gold nanoparticles per particle determined from the change in the values of ωp is found to be some 50-fold greater than what traditional electrostatic contact electrification models compute based on the work function difference of the two conductive materials. Moreover, when using bulk gold as the capping layer, which should have resulted in a negligible charge exchange between the gold nanoparticles and the bulk gold, a significant charge transfer from the bulk gold layer to the nanoparticles was observed as with the other metals. We explain these observations in terms of the "plasmoelectric effect", recently described by Atwater and co-workers, in which the gold nanoparticles modify their charge density to allow their resonant wavelength to match that of the incident light, thereby achieving, a lower value of the chemical potential due to the entropy increase resulting from the conversion of the plasmon's energy to heat. We conclude that even the act of registering the spectrum of nanoparticles is at times sufficient to alter their charge densities and hence their UV-visible spectra. [ABSTRACT FROM AUTHOR]

We demonstrate that coherent acoustic phonons derived from plasmonic nanoparticles can modulate electronic interactions with proximal excitonic molecular species. A series of gold bipyramids with systematically varied aspect ratios and corresponding localized surface plasmon resonance energies, functionalized with a J-aggregated thiacarbocyanine dye molecule, produces two hybridized states that exhibit clear anticrossing behavior with a Rabi splitting energy of 120 meV. In metal nanoparticles, photoexcitation generates coherent acoustic phonons that cause oscillations in the plasmon resonance energy. In the coupled system, these photogenerated oscillations alter the metal nanoparticle's energetic contribution to the hybridized system and, as a result, change the coupling between the plasmon and exciton. We demonstrate that such modulations in the hybridization are consistent across a wide range of bipyramid ensembles. We also use finite-difference time domain calculations to develop a simple model describing this behavior. Such oscillatory plasmonic-excitonic nanomaterials offer a route to manipulate and dynamically tune the interactions of plasmonic/excitonic systems and unlock a range of potential applications. [ABSTRACT FROM AUTHOR]

The existence of sub-nanometer plasmonic hot-spots and their relevance in spectroscopy and microscopy applications remain elusive despite a few recent theoretical and experimental evidence supporting this possibility. In this Letter, we present new spectroscopic evidence suggesting that Angstrom-sized hot-spots exist on the surfaces of plasmon-excited nanostructures. Surface-enhanced Raman scattering (SERS) spectra of 4,4'-biphenyl dithiols placed in metallic junctions show simultaneously blinking Stokes and anti-Stokes spectra, some of which exhibit only one prominent vibrational peak. The activated vibrational modes were found to vary widely between junction sites. Such site-specific, single-peak spectra could be successfully modeled using single-molecule SERS induced by a hot-spot with a diameter no larger than 3.5 Å, located at the specific molecular sites. Furthermore, the model, which assumes the stochastic creation of hot-spots on locally flat metallic surfaces, consistently reproduces the intensity distributions and occurrence statistics of the blinking SERS peaks, further confirming that the sources of the hot-spots are located on the metallic surfaces. This result not only provides compelling evidence for the existence of Angstrom-sized hot-spots but also opens up the new possibilities for the vibrational and electronic control of single-molecule photochemistry and real-space visualization of molecular vibration modes. [ABSTRACT FROM AUTHOR]

The optical response of ZnO nanocrystals (NCs) doped with Al (Ga) impurities is calculated using a model that incorporates the effects of quantum confinement, dielectric mismatch, surface, and ionized impurity scattering. For dopant concentrations of a few percent, the NC polarizability is dominated by a localized surface plasmon resonance (LSPR) in the infrared (IR) which follows the Drude-Lorentz law for NC diameter above ~10 nm but is strongly blue-shifted for smaller diameters due to quantum confinement effects. The intrinsic width of the LSPR peak is calculated in order to characterize plasmon losses induced by ionized impurity scattering. Widths below 80 meV are found in the best cases, in agreement with the lowest values recently measured on single NCs. These results confirm that doped ZnO NCs are very promising for the development of IR plasmonics. The width of the LSPR peak strongly increases when dopants are placed near the surface of the NCs or when additional fixed charges are present. [ABSTRACT FROM AUTHOR]

Directional antennas revolutionized modern day telecommunication by enabling precise beaming of radio and microwave signals with minimal loss of energy. Similarly, directional optical nanoantennas are expected to pave the way toward on-chip wireless communication and information processing. Currently, on-chip integration of such antennas is hampered by their multielement design or the requirement of complicated excitation schemes. Here, we experimentally demonstrate electrical driving of in-plane tunneling nanoantennas to achieve broadband unidirectional emission of light. Far-field interference, as a result of the spectral overlap between the dipolar emission of the tunnel junction and the fundamental quadrupole-like resonance of the nanoantenna, gives rise to a directional radiation pattern. By tuning this overlap using the applied voltage, we record directivities as high as 5 dB. In addition to electrical tunability, we also demonstrate passive tunability of the directivity using the antenna geometry. These fully configurable electrically driven nanoantennas provide a simple way to direct optical energy on-chip using an extremely small device footprint. [ABSTRACT FROM AUTHOR]

On-demand pain relief systems would be very helpful additions to the armamentarium of pain management. Near-infrared triggered drug delivery systems have demonstrated the potential to provide such care. However, challenges remain in making such systems as stimulus-sensitive as possible, to enhance depth of tissue penetration, repeatability of triggering, and safety. Here we developed liposomes containing the local anesthetic tetrodotoxin and also containing a photosensitizer and gold nanorods that were excitable at the same near-infrared wavelength. The combination of triggering mechanisms enhanced the photosensitivity and repeatability of the system in vitro when compared with liposomes with a single photoresponsive component. In vivo, on-demand local anesthesia could be induced with a low irradiance and short irradiation duration, and liposomes containing both photosensitizer and gold nanorods were more effective than those containing just one photoresponsive component. Tissue reaction was benign. [ABSTRACT FROM AUTHOR]

Dynamic optical control of infrared (IR) transparency and refractive index is achieved using boron-doped silicon nanocrystals excited with mid-IR optical pulses. Unlike previous silicon-based optical switches, large changes in transmittance are achieved without a fabricated structure by exploiting strong light coupling of the localized surface plasmon resonance (LSPR) produced from free holes of p-type silicon nanocrystals. The choice of optical excitation wavelength allows for selectivity between hole heating and carrier generation through intraband or interband photoexcitation, respectively. Mid-IR optical pumping heats the free holes of p-Si nanocrystals to effective temperatures greater than 3500 K. Increases of the hole effective mass at high effective hole temperatures lead to a subpicosecond change of the dielectric function, resulting in a redshift of the LSPR, modulating mid-IR transmission by as much as 27%, and increasing the index of refraction by more than 0.1 in the mid-IR. Low hole heat capacity dictates subpicosecond hole cooling, substantially faster than carrier recombination, and negligible heating of the Si lattice, permitting mid-IR optical switching at terahertz repetition frequencies. Further, the energetic distribution of holes at high effective temperatures partially reverses the Burstein-Moss effect, permitting the modulation of transmittance at telecommunications wavelengths. The results presented here show that doped silicon, particularly in micro- or nanostructures, is a promising dynamic metamaterial for ultrafast IR photonics. [ABSTRACT FROM AUTHOR]

Comprehension and modulation of optical activity at nanoscale have attracted tremendous interest in the past decades due to its potential application in many fields including chemical/biological sensing, artificial metamaterials, asymmetric catalysis, and so forth. As for the conventional molecular materials, magnetic field is among the most effective routes in inducing and manipulating their optical activity; whereas the magnetic optical activity at nanoscale calls for deeper understanding, especially for anisotropic noble metal nanoparticles. In this work, distinctly different magnetic circular dichroism (MCD) responses are demonstrated in gold nanorods (GNRs) with a derivative-shaped MCD signal corresponding to the transverse surface plasmon resonance (TSPR) band and a Gaussian-shaped signal at the position of the longitudinal surface plasmon resonance (LSPR) band. Furthermore, changing the aspect ratio of GNRs easily regulates such magnetoplasmonic CD response. More interestingly, GNR assemblies with different geometric configuration (end-to-end and side-by-side) show structure-sensitive magnetoplasmonic CD response. Armed with theoretical calculation, we clearly elucidate the intrinsic relationship of the resultant magnetoplasmonic CD response with the optical symmetry and geometry factor inside one-dimensional GNRs. This work not only greatly benefits our understanding toward the nature of SPR mode in anisotropic plasmonic nanostructures but also opens the way to achieve tunable magnetoplasmonic response, which will significantly advance the design and application of optical nanodevices. [ABSTRACT FROM AUTHOR]

Aluminum nanostructures support tunable surface plasmon resonances and have become an alternative to gold nanoparticles. Whereas gold is the most-studied plasmonic material, aluminum has the advantage of high earth abundance and hence low cost. In addition to understanding the size and shape tunability of the plasmon resonance, the fundamental relaxation processes in aluminum nanostructures after photoexcitation must be understood to take full advantage of applications such as photocatalysis and photodetection. In this work, we investigate the relaxation following ultrafast pulsed excitation and the launching of acoustic vibrations in individual aluminum nanodisks, using single-particle transient extinction spectroscopy. We find that the transient extinction signal can be assigned to a thermal relaxation of the photoexcited electrons and phonons. The ultrafast heating-induced launching of in-plane acoustic vibrations reveals moderate binding to the glass substrate and is affected by the native aluminum oxide layer. Finally, we compare the behavior of aluminum nanodisks to that of similarly prepared and sized gold nanodisks. [ABSTRACT FROM AUTHOR]

Surface-enhanced Raman spectroscopy (SERS) enables sensitive chemical studies and materials identification, relying on electromagnetic (EM) and chemical-enhancement mechanisms. Here we introduce a tool for the correlative nanoimaging of EM and SERS hotspots, areas of strongly enhanced EM fields and Raman scattering, respectively. To that end, we implemented a grating spectrometer into a scattering-type scanning near-field optical microscope (s-SNOM) for mapping of both the elastically and inelastically (Raman) scattered light from the near-field probe, that is, a sharp silicon tip. With plasmon-resonant gold dimers (canonical SERS substrates) we demonstrate with nanoscale spatial resolution that the enhanced Raman scattering from the tip is strongly correlated with its enhanced elastic scattering, the latter providing access to the EM-field enhancement at the illumination frequency. Our technique has wide application potential in the correlative nanoimaging of local-field enhancement and SERS efficiency as well as in the investigation and quality control of novel SERS substrates. [ABSTRACT FROM AUTHOR]

Quantum emitters in two-dimensional materials are promising candidates for studies of light-matter interaction and next generation, integrated on-chip quantum nanophotonics. However, the realization of integrated nanophotonic systems requires the coupling of emitters to optical cavities and resonators. In this work, we demonstrate hybrid systems in which quantum emitters in 2D hexagonal boron nitride (hBN) are deterministically coupled to high-quality plasmonic nanocavity arrays. The plasmonic nanoparticle arrays offer a high-quality, low-loss cavity in the same spectral range as the quantum emitters in hBN. The coupled emitters exhibit enhanced emission rates and reduced fluorescence lifetimes, consistent with Purcell enhancement in the weak coupling regime. Our results provide the foundation for a versatile approach for achieving scalable, integrated hybrid systems based on low-loss plasmonic nanoparticle arrays and 2D materials. [ABSTRACT FROM AUTHOR]

Doped metal oxides are plasmonic materials that boast both synthetic and postsynthetic spectral tunability. They have already enabled promising smart window and optoelectronic technologies and have been proposed for use in surface enhanced infrared absorption spectroscopy (SEIRA) and sensing applications. Herein, we report the first step toward realization of the former utilizing cubic F and Sn codoped In2O3 nanocrystals (NCs) to couple to the C-H vibration of surface-bound oleate ligands. Electron energy loss spectroscopy is used to map the strong near-field enhancement around these NCs that enables localized surface plasmon resonance (LSPR) coupling between adjacent nanocrystals and LSPR-molecular vibration coupling. Fourier transform infrared spectroscopy measurements and finite element simulations are applied to observe and explain the nature of the coupling phenomena, specifically addressing coupling in mesoscale assembled films. The Fano line shape signatures of LSPR-coupled molecular vibrations are rationalized with two-port temporal coupled mode theory. With this combined theoretical and experimental approach, we describe the influence of coupling strength and relative detuning between the molecular vibration and LSPR on the enhancement factor and further explain the basis of the observed Fano line shape by deconvoluting the combined response of the LSPR and molecular vibration in transmission, absorption and reflection. This study therefore illustrates various factors involved in determining the LSPR-LSPR and LSPR-molecular vibration coupling for metal oxide materials and provides a fundamental basis for the design of sensing or SEIRA substrates. [ABSTRACT FROM AUTHOR]

Tunnel resistance can be modulated with bias via the Coulomb blockade effect, which gives a highly nonlinear response current. Here we investigate the optical response of a metal-insulator-nanoparticle-insulator-metal structure and show switching of a plasmonic gap from insulator to conductor via Coulomb blockade. By introducing a sufficiently large charging energy in the tunnelling gap, the Coulomb blockade allows for a conductor (tunneling) to insulator (capacitor) transition. The tunnelling electrons can be delocalized over the nanocapacitor again when a high energy penalty is added with bias. We demonstrate that this has a huge impact on the plasmonic resonance of a 0.51 nm tunneling gap with ~70% change in normalized optical loss. Because this structure has a tiny capacitance, there is potential to harness the effect for high-speed switching. [ABSTRACT FROM AUTHOR]

The advances in recent nanofabrication techniques have facilitated explorations of metal structures into nanometer scales, where the traditional local-response Drude model with hard-wall boundary conditions fails to accurately describe their optical responses. The emerging nonlocal effects in single ultrasmall silver nanoparticles have been experimentally observed in single-particle spectroscopy enabled by the unprecedented high spatial resolution of electron energy loss spectroscopy (EELS). However, the unambiguous optical observation of such new effects in gold nanoparticles has yet not been reported, due to the extremely weak scattering and the obscuring fingerprint of strong interband transitions. Here we present a nanosystem, a superlattice monolayer formed by sub-10 nm gold nanoparticles. Plasmon resonances are spectrally well-separated from interband transitions, while exhibiting clearly distinguishable blueshifts compared to predictions by the classical local-response model. Our far-field spectroscopy was performed by a standard optical transmission and reflection setup, and the results agreed excellently with the hydrodynamic nonlocal model, opening a simple and widely accessible way for addressing quantum effects in nanoplasmonic systems. [ABSTRACT FROM AUTHOR]

In this work, the impact of metallic and dielectric conducting substrates, gold and indium tin oxide (ITO)-coated glass, on the whispering gallery modes (WGMs) of semiconductor π-conjugated polymer microspheres is investigated. Hyperspectral mapping was performed to obtain the excitation-position-dependent emission spectra of the microspheres. Substrate-dependent quenching of WGMs sensitive to mode polarization was observed and explained. On a glass substrate, both transverse-electric (TE) and transverse-magnetic (TM) WGMs are quenched due to frustrated total internal reflection. On a gold substrate, however, only the TM WGMs are allowed in symmetry to leak into surface plasmons. An atomically flat gold substrate with subwavelength slits was used to experimentally verify the leakage of WGMs into the surface plasmon polaritons (SPPs). This work provides insight into the damping mechanisms of WGMs in microspheres on metallic and dielectric substrates.

Plasmonic polymeric nanoassemblies offer valuable opportunities in photoconversion applications. Localized surface plasmon mechanisms behind such nanoassemblies govern their functionalities under light illumination. However, an in-depth investigation at the single nanoparticle (NP) level is still challenging, especially when the buried interface is involved, due to the availability of suitable techniques. Here, we synthesized an anisotropic heterodimer composed of a self-assembled polymer vesicle (THPG) capped with a single gold NP, enabling an 8-fold enhancement in hydrogen generation compared to the nonplasmonic THPG vesicle. We explored the anisotropic heterodimer at the single particle level by employing advanced transmission electron microscopes, including one equipped with a femtosecond pulsed laser, which allows us to visualize the polarization- and frequency-dependent distribution of the enhanced electric near fields at the vicinity of Au cap and Au-polymer interface. These elaborated fundamental findings may guide designing new hybrid nanostructures tailored for plasmon-related applications.

Understanding of DNA-mediated charge transport (CT) is significant for exploring circuits at the molecular scale. However, the fabrication of robust DNA wires remains challenging due to the persistence length and natural flexibility of DNA molecules. Moreover, CT regulation in DNA wires often relies on predesigned sequences, which limit their application and scalability. Here, we addressed these issues by preparing self-assembled DNA nanowires with lengths of 30-120 nm using structural DNA nanotechnology. We employed these nanowires to plug individual gold nanoparticles into a circuit and measured the transport current in nanowires with an optical imaging technique. Contrary to the reported cases with shallow or no length dependence, a fair current attenuation was observed with increasing nanowire length, which experimentally confirmed the prediction of the incoherent hopping model. We also reported a mechanism for the reversible CT regulation in DNA nanowires, which involves dynamic transitions in the steric conformation.