Meng-Hsien Lin

Layer-by-Layer Assembly of Three-Dimensional Colloidal Supercrystals with Tunable Plasmonic Properties

We present a simple and efficient method for synthesizing large-area (>1 cm(2)), three-dimensional (3D) gold and silver nanoparticle supercrystal films. In this approach, Janus nanoparticle (top face solvent-phobic and bottom face solvent-philic) films with an arbitrary number of close-packed nanoparticle monolayers can be formed using layer-by-layer (LbL) assembly from suspensions of thiolate-passivated gold or silver colloids. Furthermore, we demonstrate that these films can act as true 3D plasmonic crystals with strong transverse (intralayer) and longitudinal (interlayer) near-field coupling. In contrast to conventional polyelectrolyte-mediated LbL assembly processes, this approach allows multiple longitudinal coupling modes with a conspicuous spectral dependence on the layer number. We have found a universal scaling relation between the spectral position of the reflectance dips related to the longitudinal modes and the layer number. This relation can be understood in terms of the presence of a plasmonic Fabry-Perot nanocavity along the longitudinal direction that allows the formation of standing plasmon waves under plasmon resonance conditions. The realization of 3D plasmonic coupling enables broadband tuning of the collective plasmon response over a wide spectral range (visible and near-IR) and provides a pathway to designer plasmonic metamaterials.

Far-Field Optical Imaging of a Linear Array of Coupled Gold Nanocubes: Direct Visualization of Dark Plasmon Propagating Modes

Plasmonic nanoantenna arrays hold great promise for diffraction-unlimited light localization, confinement, and transport. Here, we report on linear plasmonic nanoantenna arrays composed of colloidal gold nanocubes precisely assembled using a nanomanipulation technique. In particular, we show the direct evidence of dark propagating modes in the plasmon coupling regime, allowing for transport of guided plasmon waves without far-field radiation losses. Additionally, we demonstrate the possibility of plasmon dispersion engineering in coupled gold nanocube chains. By assembling a nanocube chain with two sections of coupled nanocubes of different intercube separations, we are able to produce the effect of a band-pass nanofilter.

Multilength-Scale Chemical Patterning of Self-Assembled Monolayers by Spatially Controlled Plasma Exposure: Nanometer to Centimeter Range

We present a generic and efficient chemical patterning method based on local plasma-induced conversion of surface functional groups on self-assembled monolayers (SAMs). Here, spatially controlled plasma exposure is realized by elastomeric poly(dimethylsiloxane) (PDMS) contact masks or channel stamps with feature sizes ranging from nanometer, micrometer, to centimeter. This chemical conversion method has been comprehensively characterized by a set of techniques, including contact angle measurements, X-ray photoelectron spectroscopy (XPS), scanning photoelectron microscopy (SPEM), scanning electron microscopy (SEM), and scanning Kelvin probe microscopy (SKPM). In particular, XPS and SPEM can be used to distinguish regions of different surface functionalities and elucidate the mechanism of plasma-induced chemical conversion. In the case of an octadecyltrichlorosilane (OTS) monolayer, we show that exposure to low-power air plasma causes hydroxylation and oxidation of the methyl terminal group on an OTS-covered Si surface and generates polar functional groups such as hydroxyl, aldehylde, and carboxyl groups, which can allow subsequent grafting of dissimilar SAMs and adsorption of colloid nanoparticles onto the patterned areas with an achievable resolution down to the 50 nm range.

Ultrafast spectroscopy of stimulated emission in single ZnO tetrapod nanowires

Stimulated emission from single ZnO tetrapod nanowires was studied by time-resolved photoluminescence (TRPL) spectroscopy. The samples were excited by a 300 fs pulse and the emission spectra collected as a function of time. The spectra exhibit a change in the position and the shape of the emission peak with time. The time evolution of the emission spectra was studied for different pump excitation fluences. The spectra exhibited a blue shift with increasing pump fluence, while for all pump fluences a red shift of the peaks with time was obtained. Possible reasons for the observed behaviour are discussed.

Selectively probing vibrations in a plasmonic supracrystal

The coupling of plasmonic resonances with the multiple phonon modes of a plasmonic supracrystal is studied. Ultrafast optical pump-probe spectroscopy with variable wavelength allows the selective detection of the breathing mode, the interparticle vibrations, and the vibration of the whole structure. Thanks to this selectivity, the characterization of the bonding strength between nanoparticles in different directions of the supracrystal is possible. The observation of these vibrations could be useful for the realization of future phonon modulated photonic and plasmonic devices.

Optical Observation of Plasmonic Nonlocal Effects in a 2D Superlattice of Ultrasmall Gold Nanoparticles

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.

Cascaded exciton energy transfer in a monolayer semiconductor lateral heterostructure assisted by surface plasmon polariton

Atomically thin lateral heterostructures based on transition metal dichalcogenides have recently been demonstrated. In monolayer transition metal dichalcogenides, exciton energy transfer is typically limited to a short range (~1 μm), and additional losses may be incurred at the interfacial regions of a lateral heterostructure. To overcome these challenges, here we experimentally implement a planar metal-oxide-semiconductor structure by placing a WS2/MoS2 monolayer heterostructure on top of an Al2O3-capped Ag single-crystalline plate. We find that the exciton energy transfer range can be extended to tens of microns in the hybrid structure mediated by an exciton-surface plasmon polariton–exciton conversion mechanism, allowing cascaded exciton energy transfer from one transition metal dichalcogenides region supporting high-energy exciton resonance to a different transition metal dichalcogenides region in the lateral heterostructure with low-energy exciton resonance. The realized planar hybrid structure combines two-dimensional light-emitting materials with planar plasmonic waveguides and offers great potential for developing integrated photonic and plasmonic devices.Exciton energy transfer in monolayer transition metal dichalcogenides is limited to short distances. Here, Shi et al. fabricate a planar metal-oxide-semiconductor structure and show that exciton energy transfer can be extended to tens of microns, mediated by an exciton-surface-plasmon-polariton–exciton conversion mechanism.

Ultracompact Pseudowedge Plasmonic Lasers and Laser Arrays

Concentrating light at the deep subwavelength scale by utilizing plasmonic effects has been reported in various optoelectronic devices with intriguing phenomena and functionality. Plasmonic waveguides with a planar structure exhibit a two-dimensional degree of freedom for the surface plasmon; the degree of freedom can be further reduced by utilizing metallic nanostructures or nanoparticles for surface plasmon resonance. Reduction leads to different lightwave confinement capabilities, which can be utilized to construct plasmonic nanolaser cavities. However, most theoretical and experimental research efforts have focused on planar surface plasmon polariton (SPP) nanolasers. In this study, we combined nanometallic structures intersecting with ZnO nanowires and realized the first laser emission based on pseudowedge SPP waveguides. Relative to current plasmonic nanolasers, the pseudowedge plasmonic lasers reported in our study exhibit extremely small mode volumes, high group indices, high spontaneous emission factors, and high Purell factors beneficial for the strong interaction between light and matter. Furthermore, we demonstrated that compact plasmonic laser arrays can be constructed, which could benefit integrated plasmonic circuits.

Substantially Enhancing Quantum Coherence of Electrons in Graphene via Electron-Plasmon Coupling

The interplays between different quasiparticles in solids lay the foundation for a wide spectrum of intriguing quantum effects, yet how the collective plasmon excitations affect the quantum transport of electrons remains largely unexplored. Here we provide the first demonstration that when the electron-plasmon coupling is introduced, the quantum coherence of electrons in graphene is substantially enhanced with the quantum coherence length almost tripled. We further develop a microscopic model to interpret the striking observations, emphasizing the vital role of the graphene plasmons in suppressing electron-electron dephasing. The novel and transformative concept of plasmon-enhanced quantum coherence sheds new insight into interquasiparticle interactions, and further extends a new dimension to exploit nontrivial quantum phenomena and devices in solid systems.