Polarization‐controlled surface plasmon holography

The ability of generating arbitrary surface plasmon (SP) profiles in a controllable manner is of particular interest in designing plasmonic imaging, lithography and forcing devices. During the past decades, holography has gained enormous interest and achievements in free‐space three‐dimensional displays. Here, by applying a two‐dimensional version of holography, we experimentally demonstrate a generic method to control the SP profiles. Through controlling the orientation angles of two separated slits under circular polarization incidence, the amplitude and phase of the excited SPs can be freely manipulated, which allows direct generation of the desired SP profiles. A series of controllable SP holography schemes are theoretically and experimentally demonstrated, where the holographic SP profiles with high imaging quality can be dynamically modulated by varying the circular polarization handedness or orientation angle of linear polarization. The universality and simplicity of the proposed design strategies would offer promising opportunities for practical plasmonic applications.

     

A double‐lined metasurface for plasmonic complex‐field generation

Since the surface plasmon polariton (SPP) has received a great deal of attention because of its capability of guiding light within the subwavelength scale, finding methods for arbitrary SPP field generation has been a significant issue in the area of integrated optics. To achieve such a goal, it will be necessary to generate a plasmonic complex field. In this paper, we propose a novel method for generating a plasmonic complex field propagating with arbitrary curvatures by using double‐lined distributed nanoslits. As a unit cell, two facing nanoslits are used for tuning both the amplitude and the phase of excited SPPs as a function of their tilted angles. For verification of the proposed design rule, the authors experimentally demonstrate some plasmonic caustic curves and Airy plasmons.

     

A localized surface plasmon resonance and light confinement‐enhanced near‐infrared light photodetector

Light manipulation is paramountly important to the fabrication of high‐performance optoelectronic devices such as solar cells and photodetectors. In this study, a high‐performance near‐infrared light nanophotodetector (NIRPD) was fabricated based on a germanium nanoneedles array (GeNNs array) with strong light confining capability, and single‐layer graphene (SLG) modified with heavily doped indium tin oxide nanoparticles (ITONPs), which were capable of inducing localized surface plasmon resonance (LSPR) under NIR irradiation. An optoelectronic study shows that after modification with ITONPs the device performance including photocurrent, responsivity and detectivity was considerably improved. In addition, the ITONPs@SLG/GeNNs array NIRPD was able to monitor fast‐switching optical signals, the frequency was as high as 1 MHz, with very fast response rates. Theoretical simulations based on finite‐element method (FEM) revealed that the observed high performance was not only due to the strong light‐confining capability of the GeNNs array, but also due to the plasmonic ITONPs‐induced hot electron injection. The above results suggest that the present NIRPD will have great potential in future optoelectronic devices application.

     

A facile high‐performance SERS substrate based on broadband near‐perfect optical absorption

Plasmonic systems based on metal nanoparticles on a metal film with high optical absorption have generated great interests for surface‐enhanced Raman scattering (SERS). In this study, we prepare a broadband‐visible light absorber consisting Au nanotriangles on the surface of a continuous optically opaque gold film separated with a dielectric SiO₂ layer, which is a typical metal‐insulator‐metal (MIM) system, and demonstrate it as an efficient SERS substrate. The MIM nanostructure, prepared using nanosphere lithography with a very large area, shows a broadband with absorption exceeding 90% in the wavelength regime of 630–920 nm. We observe an average SERS enhancement factor (EF) as large as 4.9 × 10⁶ with a 22‐fold increase compared to a single layer of Au nanotriangles directly on a quartz substrate. A maximum SERS EF can be achieved by optimizing the thicknesses of the dielectric layer to control the optical absorption. Owing to the simple, productive, and inexpensive fabrication technique, our MIM nanostructure could be a potential candidate for SERS applications. Copyright © 2015 John Wiley & Sons, Ltd.     

Mapping the near fields of plasmonic nanoantennas by scattering‐type scanning near‐field optical microscopy

Near‐field optical microscopy techniques provide information on the amplitude and phase of local fields in samples of interest in nanooptics. However, the information on the near field is typically obtained by converting it into propagating far fields where the signal is detected. This is the case, for instance, in polarization‐resolved scattering‐type scanning near‐field optical microscopy (s‐SNOM), where a sharp dielectric tip scatters the local near field off the antenna to the far field. Up to now, basic models have interpreted S‐ and P‐polarized maps obtained in s‐SNOM as directly proportional to the in‐plane ( or ) and out‐of‐plane () near‐field components of the antenna, respectively, at the position of the probing tip. Here, a novel model that includes the multiple‐scattering process of the probing tip and the nanoantenna is developed, with use of the reciprocity theorem of electromagnetism. This novel theoretical framework provides new insights into the interpretation of s‐SNOM near‐field maps: the model reveals that the fields detected by polarization‐resolved interferometric s‐SNOM do not correlate with a single component of the local near field, but rather with a complex combination of the different local near‐field components at each point (, and ). Furthermore, depending on the detection scheme (S‐ or P‐polarization), a different scaling of the scattered fields as a function of the local near‐field enhancement is obtained. The theoretical findings are corroborated by s‐SNOM experiments which map the near field of linear and gap plasmonic antennas. This new interpretation of nanoantenna s‐SNOM maps as a complex‐valued combination of vectorial local near fields is crucial to correctly understand scattering‐type near‐field microscopy measurements as well as to interpret the signals obtained in field‐enhanced spectroscopy.

     

Subdiffraction‐limited chemical imaging of patterned phthalocyanine films using tip‐enhanced near‐field optical microscopy

A tip‐enhanced near‐field optical microscope, based on a shear‐force atomic force microscope with plasmonic tip coupled to an inverted, confocal optical microscope, has been constructed for nanoscale chemical (Raman) imaging of surfaces. The design and validation of the instrument, along with its application to near‐field Raman mapping of patterned organic thin films (coumarin‐6 and Cu(II) phthalocyanine), are described. Lateral resolution of the instrument is estimated at 50 nm (better than λ/10), which is roughly dictated by the size of the plasmonic tip apex. Additional observations, such as the distance scaling of Raman enhancement and the inelastic scattering background generated by the plasmonic tip, are presented. Copyright © 2016 John Wiley & Sons, Ltd.     

Airy plasmons: non‐diffracting optical surface waves

Airy beams represent an important class of non‐diffracting waves which can be realized on a flat surface. Being generated in the form of surface‐plasmon polaritons, such Airy plasmons demonstrate many remarkable properties: they do not diffract while propagating along parabolic trajectories, and they recover their shape after passing through obstacles. This paper reviews the basic physics of Airy plasmons in both paraxial and non‐paraxial cases, and describes the experimental methods for generation of Airy surface waves on metal surfaces, including a control of their trajectories, as well as the interference of Airy plasmons and hot‐spot generation. Many unusual properties of Airy plasmons can be utilized for useful applications, including plasmonic circuitry and surface tweezers. Picture: Observation of two colliding Airy plasmons.     

Surface‐enhanced Raman microscopy of hemispherical shells stripped from templates of anodized aluminum

We report on the optical characterization of plasmonic metal nanostructures representing highly ordered interconnected hemispherical gold and silver shells that can be iteratively stripped from the same embossed templates (without template degradation) made from selectively etched anodized aluminum. By performing scanning high‐resolution confocal Raman microscopy of p‐aminothiophenol and Rhodamine 6G molecules homogeneously adsorbed to samples with different radii of shell curvature, we systematically investigate the applicability of the fabricated structures for surface‐enhanced Raman spectroscopy and correlate the results with linear reflection spectroscopy. We trace the origin of strong Raman signal enhancements (average relative enhancement of up to ~120) to electromagnetic hot‐spots located in sharp grooves and crevices at hemisphere shell junctions. Copyright © 2011 John Wiley & Sons, Ltd.     

Tunable nonlinear beam shaping by non‐collinear interactions

A method is proposed for nonlinear beam shaping, employing a non‐collinear quasi phase‐matched interaction in a crystal whose nonlinear coefficient is encoded by a computer generated hologram pattern. In this method the same axis is used for both satisfying the phase‐matching requirements and encoding the holographic information, the result is a single shaped beam in the generated frequency. This allows to shape beams in one‐dimension using a very simple method to fabricate patterned nonlinear crystals and to shape beams in two‐dimensions with high conversion efficiency. The one‐dimensional case is experimentally demonstrated by converting a fundamental Gaussian beam into Hermite‐Gaussian beams at the second harmonic in a KTiOPO₄ crystal. The two‐dimensional case is demonstrated by generating Hermite‐Gaussian and Laguerre‐Gaussian beams in a stoichiometric lithium tantalate crystal. The suggested scheme enables broad wavelength tuning by simply tilting the crystal.     

Ultra‐fast nano‐optics

Ultra‐fast nano‐optics is a comparatively young and rapidly growing field of research aiming at probing, manipulating and controlling ultrafast optical excitations on nanometer length scales. This ability to control light on nanometric length and femtosecond time scales opens up exciting possibilities for probing dynamic processes in nanostructures in real time and space. This article gives a brief introduction into the emerging research field of ultrafast nano‐optics and discusses recent progress made in it. A particular emphasis is laid on the recent experimental work performed in the authors' laboratories. We specifically discuss how ultrafast nano‐optical techniques can be used to probe and manipulate coherent optical excitations in individual and dipole‐coupled pairs of quantum dots, probe the dynamics of surface plasmon polariton excitations in metallic nanostructures, generate novel nanometer‐sized ultrafast light and electron sources and reveal the dipole interaction between excitons and surface plasmon polaritons in hybrid metal‐semiconductor nanostructures. Our results indicate that such hybrid nanostructures carry significant potential for realizing novel nano‐optical devices such as ultrafast nano‐optical switches as well as surface plasmon polariton amplifiers and lasers.     

Near‐field optical enhancement by lead‐sulfide quantum dots and metallic nanoparticles for SERS

There is a growing interest in using quantum dots (QDs) and metallic nanoparticles (NPs), both for luminescence enhancement and surface‐enhanced Raman scattering (SERS). Here, we study the electromagnetic‐field enhancement that can be generated by lead‐sulfide (PbS) QDs using three‐dimensional finite‐element simulations. We investigate the field enhancement associated with combinations of PbS QDs with metallic NPs and substrates. The results show that high field enhancement can be achieved by combining PbS QDs with metallic NPs of larger sizes. The ideal size for Ag NPs is 25 nm, providing a SERS enhancement factor of ~5*10⁸ for light polarization parallel to the NP dimer axis and a gap of 0.6 nm. For Au NPs, the bigger the size, the higher is the field for the studied diameters, up to 50 nm. The near‐field values for PbS QDs above metallic substrates were found to be lower compared to the case of PbS QD‐metal NP dimers. This study provides the understanding for the design and application of QDs for the enhancement of near‐field phenomena. Copyright © 2013 John Wiley & Sons, Ltd.     

Deep‐UV tip‐enhanced Raman scattering

We report for the first time the tip‐enhancement of resonance Raman scattering using deep ultraviolet (DUV) excitation wavelength. The tip‐enhancement was successfully demonstrated with an aluminum‐coated silicon tip that acts as a plasmonic material in DUV wavelengths. Both the crystal violet and adenine molecules, which were used as test samples, show electronic resonance at the 266‐nm excitation used in the experiments. With results demonstrated here, molecular analysis and imaging with nanoscale spatial resolution in DUV resonance Raman spectroscopy can be realized using the tip‐enhancement effect. Copyright © 2009 John Wiley & Sons, Ltd.     

Enhanced photon emission by field emission resonances and local surface plasmon in tunneling junction

We investigated the photon emission spectra on Ag (111) surface excited by tunneling electrons using a low temperature scanning tunneling microscope in ultrahigh vacuum. Characteristic plasmon modes were illustrated as a function of the bias voltage. The one electron excitation process was revealed by the linear relationship between the luminescence intensity and the tunneling current. Luminescence enhancement is observed in the tunneling regime for the relatively high bias voltages, as well as at the field emission resonance with bias voltage increased up to 9 V. Presence of a silver (Ag) nanoparticle in the tunneling junction results in an abnormally strong photon emission at the high field emission resonances, which is explained by the further enhancement due to coupling between the localized surface plasmon and the vacuum. The results are of potential value for applications where ultimate enhancement of photon emission is desired.     

A study on the spectral characteristics of surface enhanced Raman scattering based on far‐field extinction and near‐field electromagnetic field intensity of 2D nanostructures

A new solid‐state electrochemical patterning technique was applied to fabrication of high‐resolution silver bowtie antennas and hexagonal arrays. These silver nanofeatures were used to investigate the relation among surface enhanced Raman scattering (SERS) enhancement factor (EF), extinction, local electromagnetic (EM) field maxima of the features. It is found that spectral extinction property or the plasmonic resonance of a given SERS substrate alone is not sufficient for determining optimal EF; the number of points of high local EM field, or ‘hot spots’, and the distribution of those high‐field spots, too, play a role. Copyright © 2014 John Wiley & Sons, Ltd.     

Surface‐enhanced Raman scattering and fluorescence emission of gold nanoparticle–multiwalled carbon nanotube hybrids

Multiwalled carbon nanotubes (MWCNTs) are grafted with gold (Au) nanoparticles of different sizes (1–12 and 1–20 nm) to form Au–MWCNT hybrids. The Au nanoparticles pile up at defect sites on the edges of MWCNTs in the form of chains. The micro‐Raman scattering studies of these hybrids were carried using visible to infrared wavelengths (514.5 and 1064 nm). Enhanced Raman scattering and fluorescence is observed at an excitation wavelength of 514.5 nm. It is found that the graphitic (G) mode intensity enhances by 10 times and down shifts by approximately 3 cm⁻¹ for Au–MWCNT hybrids in comparison with pristine carbon nanotubes. This enhancement in G mode due to surface‐enhanced Raman scattering effect is related to the interaction of MWCNTs with Au nanoparticles. The enhancement in Raman scattering and fluorescence for large size nanoparticles for Au–MWCNTs hybrids is corroborated with localized surface plasmon polaritons. The peak position of localized surface plasmons of Au nanoparticles shifts with the change in environment. Further, no enhancement in G mode was observed at an excitation wavelength of 1064 nm. However, the defect mode (D) mode intensity enhances, and peak position is shifted by approximately 40 cm⁻¹ to lower side at the same wavelength. The enhanced intensity of D mode at 1064 nm excitation wavelength is related to the double resonance phenomenon and shift in the particular mode occurs due to more electron phonon interactions near Fermi level. Copyright © 2012 John Wiley & Sons, Ltd.     

Tuning of near‐ and far‐field properties of all‐dielectric dimer nanoantennas via ultrafast electron‐hole plasma photoexcitation

All‐optical ultrafast signal modulation and routing by low‐loss nanodevices is a crucial step towards an ultracompact optical chip with high performance. Here, we propose a specifically designed silicon dimer nanoantenna, which is tunable via photoexcitation of dense electron‐hole plasma with ultrafast relaxation rate. On the basis of this concept, we demonstrate the effect of beam steering by up to 20 degrees through simple variation of the intensity of incident light. The effect, which is suitable for ultrafast light routing in an optical chip, is demonstrated both in the visible and near‐IR spectral regions for silicon‐ and germanium‐based nanoantennas. We also reveal the effect of electron‐hole plasma photoexcitation on the local density of states (LDOS) in the dimer gap and find that the orientation averaged LDOS can be altered by 50%, whereas modification of the projected LDOS can be even more dramatic, almost five‐fold for transverse dipole orientation. Moreover, our analytical model sheds light on the transient dynamics of the studied nonlinear nanoantennas, yielding all temporal characteristics of the suggested ultrafast nanodevice. The proposed concept paves the way to the creation of low‐loss, ultrafast, and compact devices for optical signal modulation and routing.

     

Single‐beam coherent anti‐Stokes Raman scattering (CARS) spectroscopy of gas‐phase CO2 via phase and polarization shaping of a broadband continuum

Coherent anti‐Stokes Raman scattering (CARS) spectroscopy of gas‐phase CO₂ is demonstrated using a single femtosecond (fs) laser beam. A shaped ultrashort laser pulse with a transform‐limited temporal width of ∼7 fs and spectral bandwidth of ∼225 nm (∼3500 cm⁻¹) is employed for simultaneous excitation of the CO₂ Fermi dyads at ∼1285 and ∼1388 cm⁻¹. CARS signal intensities for the two Raman transitions and their ratio as a function of pressure are presented. The signal‐to‐noise ratio of the single beam–generated CO₂ CARS signal is sufficient to perform concentration measurements at a rate of 1 kHz. The implications of these experiments for measuring CO₂ concentrations and rapid pressure fluctuations in hypersonic and detonation‐based chemically reacting flows are also discussed. Copyright © 2010 John Wiley & Sons, Ltd.     

Broadband and high‐efficiency conversion from guided waves to spoof surface plasmon polaritons

The conversion from spatial propagating waves to surface plasmon polaritons (SPPs) has been well studied, and shown to be very efficient by using gradient‐index metasurfaces. However, feeding energies into and extracting signals from functional plasmonic devices or circuits through transmission lines require the efficient conversion between SPPs and guided waves, which has not been reported, to the best of our knowledge. In this paper, a smooth bridge between the conventional coplanar waveguide (CPW) with 50 Ω impedance and plasmonic waveguide (e.g., an ultrathin corrugated metallic strip) has been proposed in the microwave frequency, which converts the guided waves to spoof SPPs with high efficiency in broadband. A matching transition has been proposed and designed, which is constructed by gradient corrugations and flaring ground, to match both the momentum and impedance of CPW and the plasmonic waveguide. Simulated and measured results on the transmission coefficients and near‐filed distributions show excellent transmission efficiency from CPW to a plasmonic waveguide to CPW in a wide frequency band. The high‐efficiency and broadband conversion between SPPs and guided waves opens up a new avenue for advanced conventional plasmonic integrated functional devices and circuits.     

Design of plasmonic bowtie nanoring array with high sensitivity and reproducibility for surface‐enhanced Raman scattering spectroscopy

A metallic bowtie nanoring array is designed to gain high sensitive and reproducible substrate for surface‐enhanced Raman scattering (SERS) spectroscopy. The localized surface plasmon resonance (LSPR), the electric field enhancement factors (EFs) and the electric field distribution of the bowtie and bowtie nanoring array are numerically investigated by means of the finite‐difference time domain (FDTD) method. After the optimization of the particle size and the array period, the maximum electromagnetic field EF approaches 153, and the corresponding SERS electromagnetic enhancement factor (EMEF) reaches 5.4 × 10⁸. This highly sensitive and reproducible substrate can be a good candidate for SERS applications. Copyright © 2011 John Wiley & Sons, Ltd.