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Showing papers on "Plasmon published in 2020"


Journal ArticleDOI
TL;DR: The proposed structure provides a new basis for the dual-mode on-to-off multi-function modulators in patterned graphene-based terahertz metasurface composed of graphene ribbons and graphene strips.
Abstract: The plasmon-induced transparency (PIT), which is destructive interference between the superradiation mode and the subradiation mode, is studied in patterned graphene-based terahertz metasurface composed of graphene ribbons and graphene strips. As the results of finite-difference time-domain (FDTD) simulation and coupled-mode theory (CMT) fitting, the PIT can be dynamically modulated by the dual-mode. The left (right) transmission dip is mainly tailored by the gate voltage applied to graphene ribbons (stripes), respectively, meaning a dual-mode on-to-off modulator is realized. Surprisingly, an absorbance of 50% and slow-light property of 0.7 ps are also achieved, demonstrating the proposed PIT metasurface has important applications in absorption and slow-light. In addition, coupling effects between the graphene ribbons and the graphene strips in PIT metasurface with different structural parameters also are studied in detail. Thus, the proposed structure provides a new basis for the dual-mode on-to-off multi-function modulators.

205 citations


Journal ArticleDOI
01 Mar 2020-Carbon
TL;DR: In this article, a plasmon induced tunable metasurface for multiband superabsorption and terahertz sensing is proposed, which consists of a graphene sheet that facilitates perfect absorption where the graphene pattern at the top layer creates an enhanced evanescent wave.

185 citations



Journal ArticleDOI
TL;DR: In this paper, the authors proposed a novel approach to EPs based on spatial symmetry breaking and reported their observation in plasmonics at room temperature, which can be used for biosensing with very high sensitivity.
Abstract: Singularities of open systems, known as exceptional points (EPs), have been shown to exhibit increased sensitivities, but the observation of EPs has so far been limited to wavelength-scaled systems subject to the diffraction limit. Plasmons, the collective oscillations of free electrons coupled to photons, shrink the wavelength of light to electronic and molecular length scales. We propose a novel approach to EPs based on spatial symmetry breaking and report their observation in plasmonics at room temperature. The plasmonic EPs are based on the hybridization of detuned resonances in multilayered plasmonic structures to reach a critical complex coupling rate between nanoantenna arrays, resulting in the simultaneous coalescence of the resonances and loss rates. Their utility as sensors of anti-immunoglobulin G, the most abundant immunoglobulin isotype in human serum, is evaluated. Our work opens the way to a new class of nanoscale devices, sensors and imagers based on topological polaritonic effects. The hybridized modes of an asymmetric plasmonic dimer show avoided crossing of both the real and imaginary parts. This can lead to plasmonic exceptional points, which are used for biosensing with very high sensitivity.

163 citations


Journal ArticleDOI
01 Oct 2020
TL;DR: In this paper, the authors focus on the theoretical and experimental developments in realizing new light-matter interactions with photonic quasiparticles, such as room-temperature strong coupling, ultrafast ‘forbidden’ transitions in atoms and new applications of the Cherenkov effect.
Abstract: Interactions between light and matter play an instrumental role in spectroscopy, sensing, quantum information processing and lasers. In most of these applications, light is considered in terms of electromagnetic plane waves propagating at the speed of light in vacuum. As a result, light–matter interactions can usually be treated as very weak and captured at the lowest order in quantum electrodynamics. However, progress in understanding the coupling of photons to material quasiparticles (plasmons, phonons and excitons) brings the need for a generalized view of the photon at the core of every light–matter interaction. In this new picture, the photon can have greatly different polarization and dispersion and be confined to the scale of a few nanometres. Such photonic quasiparticles enable a wealth of otherwise unobservable light–matter interaction phenomena, in interactions with both bound and free electrons. This Review focuses on the theoretical and experimental developments in realizing new light–matter interactions with photonic quasiparticles. Examples include room-temperature strong coupling, ultrafast ‘forbidden’ transitions in atoms and new applications of the Cherenkov effect, as well as breakthroughs in ultrafast electron microscopy and new concepts for compact X-ray sources. The coupling of photons to material quasiparticles such as plasmons, phonons and excitons opens new possibilities in light–matter interactions. This Review presents a generalized view of such quasiparticles and the technique that describes their interactions with matter: macroscopic quantum electrodynamics.

144 citations


Journal ArticleDOI
TL;DR: In this paper, a single phthalocyanine molecule coupled to nanocavity plasmons in a tunnelling junction with a spatial resolution down to ∼8 A and locally map the molecular exciton energy and linewidth at sub-molecular resolution.
Abstract: Ambitions to reach atomic resolution with light have been a major force in shaping nano-optics, whereby a central challenge is achieving highly localized optical fields. A promising approach employs plasmonic nanoantennas, but fluorescence quenching in the vicinity of metallic structures often imposes a strict limit on the attainable spatial resolution, and previous studies have reached only 8 nm resolution in fluorescence mapping. Here, we demonstrate spatially and spectrally resolved photoluminescence imaging of a single phthalocyanine molecule coupled to nanocavity plasmons in a tunnelling junction with a spatial resolution down to ∼8 A and locally map the molecular exciton energy and linewidth at sub-molecular resolution. This remarkable resolution is achieved through an exquisite nanocavity control, including tip-apex engineering with an atomistic protrusion, quenching management through emitter–metal decoupling and sub-nanometre positioning precision. Our findings provide new routes to optical imaging, spectroscopy and engineering of light–matter interactions at sub-nanometre scales. Through the use of a plasmon-active atomically sharp tip and an ultrathin insulating film, and precise junction control in a highly confined nanocavity plasmon field at the scanning tunnelling microscope junction, sub-nanometre-resolved single-molecule near-field photoluminescence imaging with a spatial resolution down to ∼8 A is achieved.

133 citations


Journal ArticleDOI
29 Jul 2020-Nature
TL;DR: It is shown that three-dimensional crystals of plasmonic nanoparticles can realize deep strong coupling under ambient conditions, if the particles are ten times larger than the interparticle gaps, and the continuum of photons and plasmons hybridizes into polaritons that violate the rotating-wave approximation.
Abstract: In the regime of deep strong light–matter coupling, the coupling strength exceeds the transition energies of the material1–3, fundamentally changing its properties4,5; for example, the ground state of the system contains virtual photons and the internal electromagnetic field gets redistributed by photon self-interaction1,6. So far, no electronic excitation of a material has shown such strong coupling to free-space photons. Here we show that three-dimensional crystals of plasmonic nanoparticles can realize deep strong coupling under ambient conditions, if the particles are ten times larger than the interparticle gaps. The experimental Rabi frequencies (1.9 to 3.3 electronvolts) of face-centred cubic crystals of gold nanoparticles with diameters between 25 and 60 nanometres exceed their plasmon energy by up to 180 per cent. We show that the continuum of photons and plasmons hybridizes into polaritons that violate the rotating-wave approximation. The coupling leads to a breakdown of the Purcell effect—the increase of radiative damping through light–matter coupling—and increases the radiative polariton lifetime. The results indicate that metallic and semiconducting nanoparticles can be used as building blocks for an entire class of materials with extreme light–matter interaction, which will find application in nonlinear optics, the search for cooperative effects and ground states, polariton chemistry and quantum technology4,5. Photons and plasmons hybridize into polaritons in three-dimensional crystals of plasmonic nanoparticles, leading to deep strong light–matter coupling and the breakdown of the Purcell effect.

125 citations


Journal ArticleDOI
03 Jun 2020-Nature
TL;DR: In this paper, the authors couple a free-electron beam to a travelling-wave resonant cavity mode, which induces a strong phase modulation on co-propagating electrons, leading to a spectral broadening of 700 electronvolts, corresponding to the absorption and emission of hundreds of photons.
Abstract: Free-electron beams are versatile probes of microscopic structure and composition1,2, and have revolutionized atomic-scale imaging in several fields, from solid-state physics to structural biology3. Over the past decade, the manipulation and interaction of electrons with optical fields have enabled considerable progress in imaging methods4, near-field electron acceleration5,6, and four-dimensional microscopy techniques with high temporal and spatial resolution7. However, electron beams typically couple only weakly to optical excitations, and emerging applications in electron control and sensing8–11 require large enhancements using tailored fields and interactions. Here we couple a free-electron beam to a travelling-wave resonant cavity mode. The enhanced interaction with the optical whispering-gallery modes of dielectric microresonators induces a strong phase modulation on co-propagating electrons, which leads to a spectral broadening of 700 electronvolts, corresponding to the absorption and emission of hundreds of photons. By mapping the near-field interaction with ultrashort electron pulses in space and time, we trace the lifetime of the the microresonator following a femtosecond excitation and observe the spectral response of the cavity. The natural matching of free electrons to these quintessential optical modes could enable the application of integrated photonics technology in electron microscopy, with broad implications for attosecond structuring, probing quantum emitters and possible electron–light entanglement. The coupling between light and relativistic free electrons is enhanced through phase matching of electrons with optical whispering-gallery modes in dielectric microspheres and through extended modal lifetimes.

120 citations


Journal ArticleDOI
TL;DR: Investigation of an isolated copper naphthalocyanine molecule adsorbed on a triple-layer NaCl on Ag(111) using scanning tunnelling microscope TERS imaging reveals components of the electric field perpendicular to the tip provide sensitivity to the symmetry of the vibrational modes of the molecule.
Abstract: Tip-enhanced Raman spectroscopy (TERS) is a versatile tool for chemical analysis at the nanoscale. In earlier TERS experiments, Raman modes with components parallel to the tip were studied based on the strong electric field enhancement along the tip. Perpendicular modes were usually neglected. Here, we investigate an isolated copper naphthalocyanine molecule adsorbed on a triple-layer NaCl on Ag(111) using scanning tunnelling microscope TERS imaging. For flat-lying molecules on NaCl, the Raman images present different patterns depending on the symmetry of the vibrational mode. Our results reveal that components of the electric field perpendicular to the tip should be considered aside from the parallel components. Moreover, under resonance excitation conditions, the perpendicular components can play a substantial role in the enhancement. This single-molecule study in a well-defined environment provides insights into the Raman process at the plasmonic nanocavity, which may be useful in the nanoscale metrology of various molecular systems.

111 citations


Journal ArticleDOI
TL;DR: This article highlights the applications of plasmonic hot electrons in photodetectors, photocatalysts, photoelectrochemical cells, photovoltaics, biosensors, and chemical sensors and discusses the applications and the design principles of plAsmonic materials and devices.
Abstract: In plasmonic metals, surface plasmon resonance decays and generates hot electrons and hot holes through non-radiative Landau damping. These hot carriers are highly energetic, which can be modulated by the plasmonic material, size, shape, and surrounding dielectric medium. A plasmonic metal nanostructure, which can absorb incident light in an extended spectral range and transfer the absorbed light energy to adjacent molecules or semiconductors, functions as a "plasmonic photosensitizer." This article deals with the generation, emission, transfer, and energetics of plasmonic hot carriers. It also describes the mechanisms of hot electron transfer from the plasmonic metal to the surface adsorbates or to the adjacent semiconductors. In addition, this article highlights the applications of plasmonic hot electrons in photodetectors, photocatalysts, photoelectrochemical cells, photovoltaics, biosensors, and chemical sensors. It discusses the applications and the design principles of plasmonic materials and devices.

110 citations


Journal ArticleDOI
27 May 2020-Nature
TL;DR: These sodium-based plasmonic devices show stable performance under ambient conditions over a period of several months after packaging with epoxy, indicating that the performance of plasMonic devices can be greatly improved beyond that of devices using noble metals, with implications for applications in plAsmonics, nanophotonics and metamaterials.
Abstract: Plasmonics enables the manipulation of light beyond the optical diffraction limit1–4 and may therefore confer advantages in applications such as photonic devices5–7, optical cloaking8,9, biochemical sensing10,11 and super-resolution imaging12,13 However, the essential field-confinement capability of plasmonic devices is always accompanied by a parasitic Ohmic loss, which severely reduces their performance Therefore, plasmonic materials (those with collective oscillations of electrons) with a lower loss than noble metals have long been sought14–16 Here we present stable sodium-based plasmonic devices with state-of-the-art performance at near-infrared wavelengths We fabricated high-quality sodium films with electron relaxation times as long as 042 picoseconds using a thermo-assisted spin-coating process A direct-waveguide experiment shows that the propagation length of surface plasmon polaritons supported at the sodium–quartz interface can reach 200 micrometres at near-infrared wavelengths We further demonstrate a room-temperature sodium-based plasmonic nanolaser with a lasing threshold of 140 kilowatts per square centimetre, lower than values previously reported for plasmonic nanolasers at near-infrared wavelengths These sodium-based plasmonic devices show stable performance under ambient conditions over a period of several months after packaging with epoxy These results indicate that the performance of plasmonic devices can be greatly improved beyond that of devices using noble metals, with implications for applications in plasmonics, nanophotonics and metamaterials A thermo-assisted spin-coating process followed by packaging is used to fabricate sodium films that are stable for several months, enabling the realization of plasmonic devices with state-of-the-art performance at near-infrared wavelengths

Journal ArticleDOI
TL;DR: A single, nanometer-scale acoustic graphene plasmon cavity device that can confine mid-infrared and terahertz radiation with mode volume confinement factors of 5 × 1010, and provides a platform for studying ultrastrong-coupling phenomena, such as chemical manipulation via vibrational strong coupling, as well as a path to efficient detectors and sensors operating in this long-wavelength spectral range.
Abstract: Acoustic-graphene-plasmons (AGPs) are highly confined electromagnetic modes, carrying large momentum and low loss in the mid-infrared/Terahertz spectra. Owing to their ability to confine light to extremely small dimensions, they bear great potential for ultra-strong light-matter interactions in this long wavelength regime, where molecular fingerprints reside. However, until now AGPs have been restricted to micron-scale areas, reducing their confinement potential by several orders-of-magnitude. Here, by utilizing a new type of graphene-based magnetic-resonance, we realize single, nanometric-scale AGP cavities, reaching record-breaking mode-volume confinement factors of $\thicksim5\cdot10^{-10}$. This AGP cavity acts as a mid-infrared nanoantenna, which is efficiently excited from the far-field, and electrically tuneble over an ultra-broadband spectrum. Our approach provides a new platform for studying ultra-strong-coupling phenomena, such as chemical manipulation via vibrational-strong-coupling, and a path to efficient detectors and sensors, in this challenging spectral range.

Journal ArticleDOI
24 Apr 2020-Science
TL;DR: A new technique, time-resolved vector microscopy, is introduced that enables us to compose entire movies on a subfemtosecond time scale and a 10-nm spatial scale of the electric field vectors of surface plasmon polaritons (SPPs).
Abstract: Plasmonic skyrmions are an optical manifestation of topological defects in a continuous vector field. Identifying them requires characterization of the vector structure of the electromagnetic near field on thin metal films. Here we introduce time-resolved vector microscopy that creates movies of the electric field vectors of surface plasmons with subfemtosecond time steps and a 10-nanometer spatial scale. We image complete time sequences of propagating surface plasmons as well as plasmonic skyrmions, resolving all vector components of the electric field and their time dynamics, thus demonstrating dynamic spin-momentum coupling as well as the time-varying skyrmion number. The ability to image linear optical effects in the spin and phase structures of light in the single-nanometer range will allow for entirely novel microscopy and metrology applications.

Journal ArticleDOI
02 Jun 2020-Analyst
TL;DR: A roadmap to deploy plasmonic sensors is provided by reviewing the current successes and by laying out the directions the field is currently taking to increase the use of field-deployed plasMonic sensors at the point-of-care, in the environment and in industries.
Abstract: Plasmonic sensors are ideally suited for the design of small, integrated, and portable devices that can be employed in situ for the detection of analytes relevant to environmental sciences, clinical diagnostics, infectious diseases, food, and industrial applications. To successfully deploy plasmonic sensors, scaled-down analytical devices based on surface plasmon resonance (SPR) and localized surface plasmon resonance (LSPR) must integrate optics, plasmonic materials, surface chemistry, fluidics, detectors and data processing in a functional instrument with a small footprint. The field has significantly progressed from the implementation of the various components in specifically designed prism-based instruments to the use of nanomaterials, optical fibers and smartphones to yield increasingly portable devices, which have been shown for a number of applications in the laboratory and deployed on site for environmental, biomedical/clinical, and food applications. A roadmap to deploy plasmonic sensors is provided by reviewing the current successes and by laying out the directions the field is currently taking to increase the use of field-deployed plasmonic sensors at the point-of-care, in the environment and in industries.

Journal ArticleDOI
TL;DR: Both the localized surface plasmons resonances of the individual dimer-on-film structures as well as their collective surface lattice resonances (SLR) show a highly sensitive refractive index sensing response.
Abstract: Dimers, two closely spaced metallic nanostructures, are one of the primary nanoscale geometries in plasmonics, supporting high local field enhancements in their interparticle junction under excitation of their hybridized "bonding" plasmon. However, when a dimer is fabricated on a metallic substrate, its characteristics are changed profoundly. Here we examine the properties of a Au dimer on a Au substrate. This structure supports a bright "bonding" dimer plasmon, screened by the metal, and a lower energy magnetic charge transfer plasmon. Changing the dielectric environment of the dimer-on-film structure reveals a broad family of higher-order hybrid plasmons in the visible region of the spectrum. Both of the localized surface plasmons resonances (LSPR) of the individual dimer-on-film structures as well as their collective surface lattice resonances (SLR) show a highly sensitive refractive index sensing response. Implementation of such all-metal magnetic-resonant nanostructures offers a promising route to achieve higher-performance LSPR- and SLR-based plasmonic sensors.

Journal ArticleDOI
12 Jun 2020-Science
TL;DR: In this article, the authors used a graphene-based magnetic resonator to realize single, nanometer-scale acoustic graphene plasmon cavities, reaching mode volume confinement factors of 5 × 1010.
Abstract: Acoustic graphene plasmons are highly confined electromagnetic modes carrying large momentum and low loss in the mid-infrared and terahertz spectra. However, until now they have been restricted to micrometer-scale areas, reducing their confinement potential by several orders of magnitude. Using a graphene-based magnetic resonator, we realized single, nanometer-scale acoustic graphene plasmon cavities, reaching mode volume confinement factors of ~5 × 1010 Such a cavity acts as a mid-infrared nanoantenna, which is efficiently excited from the far field and is electrically tunable over an extremely large broadband spectrum. Our approach provides a platform for studying ultrastrong-coupling phenomena, such as chemical manipulation via vibrational strong coupling, as well as a path to efficient detectors and sensors operating in this long-wavelength spectral range.

Journal ArticleDOI
TL;DR: A team of Chinese researchers has used ultrafast femtosecond laser plasmonic lithography (FPL) to create subwavelength grates on GO films 140 nanometres thick, which has, for the first, demonstrated the practical use of FPL for producing structures on two-dimensional films of GO for use in novel devices for applications in optoelectronics.
Abstract: Micro/nanoprocessing of graphene surfaces has attracted significant interest for both science and applications due to its effective modulation of material properties, which, however, is usually restricted by the disadvantages of the current fabrication methods. Here, by exploiting cylindrical focusing of a femtosecond laser on graphene oxide (GO) films, we successfully produce uniform subwavelength grating structures at high speed along with a simultaneous in situ photoreduction process. Strikingly, the well-defined structures feature orientations parallel to the laser polarization and significant robustness against distinct perturbations. The proposed model and simulations reveal that the structure formation is based on the transverse electric (TE) surface plasmons triggered by the gradient reduction of the GO film from its surface to the interior, which eventually results in interference intensity fringes and spatially periodic interactions. Further experiments prove that such a regular structured surface can cause enhanced optical absorption (>20%) and an anisotropic photoresponse (~0.46 ratio) for the reduced GO film. Our work not only provides new insights into understanding the laser-GO interaction but also lays a solid foundation for practical usage of femtosecond laser plasmonic lithography, with the prospect of expansion to other two-dimensional materials for novel device applications.

Journal ArticleDOI
TL;DR: In this paper, a ternary heterojunction photocatalytic degradation ratio of 2,4-dichlorophenol reaches 99.2% under visible light irradiation.
Abstract: Plasmon Ag nanoparticle/Bi2S3 ultrathin nanobelt/oxygen-doped flower-like MoS2 nanosphere ternary heterojunction photocatalysts are fabricated via hydrothermal and photoreduction strategies. The introduction of Ag nanoparticles and defective MoS2 and the formation of heterojunctions can induce localized surface plasmon resonance and promote charge separation, respectively, which can extend the photoresponse to the visible light and near-infrared regions and obviously enhance the photothermal and photocatalytic performances. The ternary heterojunction photocatalysts show that the photocatalytic degradation ratio of 2,4-dichlorophenol reaches 99.2% under visible light irradiation. In addition, the photocatalytic hydrogen evolution rate reaches 526.3 μmol h−1 g−1, which is several times higher than that of pristine MoS2 and Bi2S3. This study offers a new strategy for designing other highly efficient heterojunction photocatalysts. In addition, these ternary heterojunctions show high stability, which is favorable for practical applications in the environmental and energy fields.

Journal ArticleDOI
TL;DR: In this article, the authors demonstrate that by crossly stacking even-layered anisotropic 2D material nanostructures, surface plasmons resonant in the two lattice directions are complementary excited, leading to polarization-independent absorption at any layer distance.
Abstract: Here we study the possibility to achieve polarization-independent optical absorption in stacked anisotropic 2D material nanostructures (NSs). Focusing on black phosphorus, we demonstrate that by crossly stacking even-layered NSs, surface plasmons resonant in the two lattice directions are complementary excited, leading to polarization-independent absorption at any layer distance. This property is numerically validated using full electromagnetic simulations and theoretically predicted by a two-particle model. Our proposal can open up the possibility of anisotropic 2D materials to develop polarization-independent plasmon devices such as sensors and absorbers.


Journal ArticleDOI
TL;DR: In this article, the authors demonstrate how excitonic resonances in atomically thin semiconductors can be harnessed as a different, third type of resonance to create mutable, flat optics.
Abstract: The highly engineerable scattering properties of resonant optical antennas underpin the operation of metasurface-based flat optics. Thus far, the choice of antenna has been limited to shaped metallic and high-index semiconductor nanostructures that support geometrical plasmonic or Mie resonances. Whereas these resonant elements offer strong light–matter interaction and excellent control over the scattering phase and amplitude, their electrical tunability has proven to be quite limited. Here, we demonstrate how excitonic resonances in atomically thin semiconductors can be harnessed as a different, third type of resonance to create mutable, flat optics. These strong materials-based resonances are unmatched in their tunability with various external stimuli. To illustrate the concept, we first demonstrate how excitons can enhance the focusing efficiency of a millimetre-scale, patterned WS2 zone plate lens. We also show how electrical gating can completely turn on and off the exciton resonance and thereby modulate the focusing efficiency by 33%. By harnessing the excitonic resonances of a monolayer of WS2 in the visible spectral range, large-area, actively tunable and atomically thin optical lenses can be realized.

Journal ArticleDOI
24 Jul 2020-Science
TL;DR: Transport measurements from single-molecule junctions, created by trapping suitably chosen single molecules between an ultrathin gold film supporting surface plasmon polaritons and a scanning probe tip, that can provide quantification of plAsmonic hot-carrier distributions are presented.
Abstract: Hot carriers in plasmonic nanostructures, generated via plasmon decay, play key roles in applications such as photocatalysis and in photodetectors that circumvent bandgap limitations. However, direct experimental quantification of steady-state energy distributions of hot carriers in nanostructures has so far been lacking. We present transport measurements from single-molecule junctions, created by trapping suitably chosen single molecules between an ultrathin gold film supporting surface plasmon polaritons and a scanning probe tip, that can provide quantification of plasmonic hot-carrier distributions. Our results show that Landau damping is the dominant physical mechanism of hot-carrier generation in nanoscale systems with strong confinement. The technique developed in this work will enable quantification of plasmonic hot-carrier distributions in nanophotonic and plasmonic devices.

Journal ArticleDOI
TL;DR: In this article, a systematic study of CO2 photoreduction performance on as-prepared samples was conducted using different wavelengths and illumination sequences, and the results point to optical control of the selectivity of high-rate CO2-photoreduction through selection of one of two different mechanistic pathways.
Abstract: Photonic crystals consisting of TiO2 nanotube arrays (PMTiNTs) with periodically modulated diameters were fabricated using a precise charge-controlled pulsed anodization technique. The PMTiNTs were decorated with gold nanoparticles (Au NPs) to form plasmonic photonic crystal photocatalysts (Au-PMTiNTs). A systematic study of CO2 photoreduction performance on as-prepared samples was conducted using different wavelengths and illumination sequences. A remarkable selectivity of the mechanism of CO2 photoreduction could be engineered by merely varying the spectral composition of the illumination sequence. Under AM1.5 G simulated sunlight (pathway#1), the Au-PMTiNTs produced methane (302 μmol g c a t . - 1 h−1) from CO2 with high selectivity (89.3 %). When also illuminated by a UV-poor white lamp (pathway#2), the Au-PMTiNTs produced formaldehyde (420 μmol g c a t . - 1 h−1) and carbon monoxide (323 μmol g c a t . - 1 h−1) with almost no methane evolved. We confirmed the photoreduction results by 13C isotope labeling experiments using GC MS. These results point to optical control of the selectivity of high-rate CO2 photoreduction through selection of one of two different mechanistic pathways. Pathway#1 implicates electron-hole pairs generated through interband transitions in TiO2 and Au as the primary active species responsible for reducing CO2 to methane. Pathway#2 involves excitation of both TiO2 and surface plasmons in Au. Hot electrons produced by plasmon damping and photogenerated holes in TiO2 proceed to reduce CO2 to HCHO and CO through a plasmonic Z-scheme.

Journal ArticleDOI
TL;DR: In this article, a multi-scale computational method combining the first-principles calculation and finite element electromagnetic simulations is used to study the plasmon-enhanced interlayer charge transfer (CT) exciton of 2D lateral and van der Waals MoS2/WS2 heterostructures with the 2H phase.
Abstract: The multi-scale computational method of combining the first-principles calculation and finite element electromagnetic simulations is used to study the plasmon-enhanced interlayer charge transfer (CT) exciton of 2D lateral and van der Waals MoS2/WS2 heterostructures with the 2H phase. The weak interlayer CT excitons are observed in the 2H lateral and van der Waals MoS2/WS2 heterostructures. Theoretical results reveal the physical principle of plexcitons resulting from the strong coupling between plasmons and interlayer CT excitons. The weak CT excitons can be strongly enhanced by a metal plasmon, which provides a way to observe the weak CT excitons. Our results can promote a deeper understanding of the plexciton resulting from strong coupling interaction between the plasmon and the exciton of lateral and van der Waals heterostructures.

Journal ArticleDOI
TL;DR: In this article, the authors measured interferometric autocorrelations of the ultrafast currents induced by optical field emission at the nanogap of a single plasmonic nanocircuit.
Abstract: The strong fields associated with few-cycle pulses can drive highly nonlinear phenomena, allowing the direct control of electrons in condensed matter systems. In this context, by employing near-infrared single-cycle pulse pairs, we measure interferometric autocorrelations of the ultrafast currents induced by optical field emission at the nanogap of a single plasmonic nanocircuit. The dynamics of this ultrafast electron nanotransport depends on the precise temporal field profile of the optical driving pulse. Current autocorrelations are acquired with sub-femtosecond temporal resolution as a function of both pulse delay and absolute carrier-envelope phase. Quantitative modelling of the experiments enables us to monitor the spatiotemporal evolution of the electron density and currents induced in the system and to elucidate the physics underlying the electron transfer driven by strong optical fields in plasmonic gaps. Specifically, we clarify the interplay between the carrier-envelope phase of the driving pulse, plasmonic resonance and quiver motion. Single-cycle interferometric autocorrelation measurements of electrons tunnelling across the gap of a plasmonic bowtie antenna and quantitative models provide insight into the physical interactions that drive the electron transfer.

Journal ArticleDOI
TL;DR: In this review, the present sensors are compared and analyzed from the aspects of the geometry, material and dimensions of plasmonic nano-arrays and the main research directions and progress are summarized.
Abstract: For sensors based on the electromagnetic resonance whether the surface plasmon resonance (SPR) or localized surface plasmon resonance (LSPR), enhancing the light-matter interactions is the most critical and important way to improve their performance. Plasmonic nano-arrays are a kind of periodic metal or dielectric nanostructure formed by nanofabrication technology and can effectively enhance the light-matter interactions by tuning structural parameters to cause different optical effects due to their ultra-high degree of freedom. At the same time, a plug-and-play, remote microsensor suitable for limited environments (such as in vivo systems) may be realized due to the rise of lab-on-fiber technology and the progress of nanofabrication technology for unconventional substrates (such as an optical fiber tip). In this paper, the advantages and disadvantages of different nanofabrication technologies are briefly introduced and compared firstly, and then the applications of optical fiber sensors (OFS) based on different plasmonic nano-arrays are reviewed. Plasmonic nano-array OFS are divided into two categories: refractive index sensors based on the sensitivity of the array to the surrounding environment and surface enhanced Raman scattering (SERS) sensors based on the enhancement ability of the local electric field around the array. In this review, the present sensors are compared and analyzed from the aspects of the geometry, material and dimensions of plasmonic nano-arrays and the main research directions and progress are summarized. Finally, the future development trend is proposed.

Journal ArticleDOI
TL;DR: The polarization dependence of plasmonic charge separation and spatial distribution in Au/TiO2 nanoparticles under 45° incident light illumination at the single-particle level is revealed using a combination of photon-irradiated Kelvin probe force microscopy (KPFM), electromagnetic field simulation and polarization-dependent surface photovoltage (SPV).
Abstract: Controlling the interaction of polarization light with an asymmetric nanostructure such as a metal/semiconductor heterostructure provides opportunities for tuning surface plasmon excitation and near-field spatial distribution. However, light polarization effects on interfacial charge transport and the photocatalysis of plasmonic metal/semiconductor photocatalysts are unclear. Herein, we reveal the polarization dependence of plasmonic charge separation and spatial distribution in Au/TiO2 nanoparticles under 45° incident light illumination at the single-particle level using a combination of photon-irradiated Kelvin probe force microscopy (KPFM) and electromagnetic field simulation. We quantitatively uncover the relationship between the local charge density and polarization angle by investigating the polarization-dependent surface photovoltage (SPV). The plasmon-induced photocatalytic activity is enhanced when the polarization direction is perpendicular to the Au/TiO2 interface.

Journal ArticleDOI
TL;DR: In this article, a hyperbolic plasmonic surface based on thin films of WTe2 in the light wavelength range of 16 to 23 microns by far infrared absorption spectroscopy is presented.
Abstract: A hyperbolic plasmonic surface supports highly directional propagating polaritons with extremely large density of states. Such plasmon polaritons have been realized in artificially structured metasurfaces. However, the upper bound of the achievable plasmon wave vector is limited by the structure size, which calls for a natural hyperbolic surface without any structuring. Here, we experimentally demonstrate a natural hyperbolic plasmonic surface based on thin films of WTe2 in the light wavelength range of 16 to 23 microns by far infrared absorption spectroscopy. The topological transition from the elliptic to the hyperbolic regime is further manifested by mapping the isofrequency contours of the plasmon. Moreover, the anisotropy character and plasmon frequency exhibit prominent temperature dependence. Our study demonstrates the first natural platform to host 2D hyperbolic plasmons, which opens exotic avenues for the manipulation of plasmon propagation, light-matter interaction and light emission in planar photonics.

Journal ArticleDOI
TL;DR: In this paper, the anisotropic optical properties and plasmons of black phosphorus (BP) are discussed and other possible 2D material candidates for hyperbolic plasmon are examined.
Abstract: In the fast growing two-dimensional (2D) materials family, anisotropic 2D materials, with their intrinsic in-plane anisotropy, exhibit a great potential in optoelectronics. One such typical material is black phosphorus (BP), with a layer-dependent and highly tunable band gap. Such intrinsic anisotropy adds a new degree of freedom to the excitation, detection and control of light. Particularly, hyperbolic plasmons with hyperbolic q-space dispersion are predicted to exist in BP films, where highly directional propagating polaritons with divergent densities of states are hosted. Combined with a tunable electronic structure, such natural hyperbolic surfaces may enable a series of exotic applications in nanophotonics. In this review, the anisotropic optical properties and plasmons (especially hyperbolic plasmons) of BP are discussed. In addition, other possible 2D material candidates (especially anisotropic layered semimetals) for hyperbolic plasmons are examined. This review may stimulate further research interest in anisotropic 2D materials and fully unleash their potential in flatland photonics.

Journal ArticleDOI
TL;DR: It is proved that the strong coupling process is not affected by the large exciton coherence size that was previously believed to be detrimental to the formation of plasmon-exciton interaction, paving the way for room-temperature quantum optics applications.
Abstract: Strong coupling of two-dimensional semiconductor excitons with plasmonic resonators enables control of light-matter interaction at the subwavelength scale. Here we develop such strong coupling in plasmonic nanogap resonators, which allows modification of exciton strength by altering electromagnetic environments in nearby semiconductor monolayers. Using this system, we not only demonstrate a large vacuum Rabi splitting up to 163 meV and splitting features in photoluminescence spectra but also reveal that the effective exciton number contributing to the coupling can be reduced down to the single-digit level ($Nl10$), which is 2 orders lower than that of previous systems, close to single-exciton based strong coupling. In addition, we prove that the strong coupling process is not affected by the large exciton coherence size that was previously believed to be detrimental to the formation of plasmon-exciton interaction. We provide a deeper understanding of strong coupling in two-dimensional semiconductors, paving the way for room-temperature quantum optics applications.