Restructuring of plasmonic nanoparticle aggregates with arbitrary particle size distribution in pulsed laser fields

We have studied processes of interaction of pulsed laser radiation with resonant groups of plasmonic nanoparticles(resonant domains) in large colloidal nanoparticle aggregates having different interparticle gaps and particle size distributions.These processes are responsible for the origin of nonlinear optical effects and photochromic reactions in multiparticle aggregates.To describe photo-induced transformations in resonant domains and alterations in their absorption spectra remaining after the pulse action,we introduce the factor of spectral photomodification.Based on calculation of changes in thermodynamic,mechanical,and optical characteristics of the domains,the histograms of the spectrum photomodification factor have been obtained for various interparticle gaps,an average particle size,and the degree of polydispersity.Variations in spectra have been analyzed depending on the intensity of laser radiation and various combinations of size characteristics of domains.The obtained results can be used to predict manifestation of photochromic effects in composite materials containing different plasmonic nanoparticle aggregates in pulsed laser fields.     

Controllable femtosecond laser‐induced dewetting for plasmonic applications

Dewetting of thin metal films is one of the most widespread method for functional plasmonic nanostructures fabrication. However, simple thermal‐induced dewetting does not allow to control degree of nanostructures order without additional lithographic process steps. Here we propose a novel method for lithography‐free and large‐scale fabrication of plasmonic nanostructures via controllable femtosecond laser‐induced dewetting. The method is based on femtosecond laser surface pattering of a thin film followed by a nanoscale hydrodynamical instability, which is found to be very controllable under specific irradiation conditions. We achieve control over degree of nanostructures order by changing laser irradiation parametrs and film thickness. This allowed us to exploit the method for the broad range of applications: resonant light absorbtion and scattering, sensing, and potential improving of thin‐film solar cells.

     

Dynamic and Reversible Accumulation of Plasmonic Core‐Satellite Nanostructures in a Light‐Induced Temperature Gradient for In Situ SERS Detection

A surface‐enhanced Raman spectroscopy (SERS) detection method that allows dynamic on‐demand generation of SERS substrates at locations of interest for in situ molecular sensing is demonstrated. Thermal convection and thermophoresis, which are both generated in a laser‐induced temperature gradient, are used to accumulate suspended plasmonic nanostructures to form 3D SERS substrate. Raman signals of melamine, which is used as a model analyte, increase to ≈117‐fold within 2 min of laser irradiation because of the accumulation. In addition, it is demonstrated that the accumulation of the nanostructures is reversible, and that reproducible SERS effects can be obtained during a repeated heating and cooling process. Because of the capability of on‐demand generation of a high density of SERS hot spots at different locations in solution, this particle manipulation and SERS detection method is applicable to monitor temporal and spatial variations of the concentrations of molecules. The complexity of the detection system remains the same when using this method since all the measurements are performed with a conventional Raman system and simple fluid channels. The required temperature gradient is generated by the laser used to excite Raman signals, and no nanofabricated substrates and complicated microfluidic or optical components are needed.     

Two‐Dimensionally Ordered Plasmonic and Magnetic Nanostructures on Transferable Electron‐Transparent Substrates

Discovery of new plasmonic behaviors from nanostructured materials can be greatly accelerated by the ability to prepare and characterize their near‐field behaviors with high resolution in a rapid manner. Here, an efficient and cost‐effective way is reported to make 2D periodic nanostructures on electron‐transparent substrates for rapid characterization by transmission electron microscopy. By combining nanosphere lithography with a substrate float‐off technique, large areas of electron‐transparent periodic nanostructures can be achieved. For this study, the synthesis of plasmonic nanostructures of Ag, magnetic nanostructures of Co, and bimetallic nanostructures of Ag–Co are investigated. Characterization of the materials by a combination of transmission electron microscopy, far‐field optical spectroscopy, and magnetization measurements reveals that this new approach can yield useful nanostructures on transparent, flexible, and transferable substrates with desirable plasmonic and/or magnetic properties.     

Nanolasers Enabled by Metallic Nanoparticles: From Spasers to Random Lasers

Owing to exotic optical responses, metallic nanoparticles and nanostructures are finding broad applications in laser science, leading to numerous design variations of plasmonic nanolasers. Nowadays, two of the most intriguing plasmonic nanolasing devices are spasers and random lasers. While a spaser is based on a single metallic nanoparticle resonator with the optical feedback provided by the localized surface plasmon resonance, the operation of a random laser relies on multiple light scattering within randomly distributed metallic nanoparticles. In this paper, an up‐to‐date review on the applications of metallic nanoparticles in spasers and random lasers is provided. Principles of a random spaser, a device combining the features of a spaser and a random laser, are briefly discussed as well. The paper is focused on major theoretical and experimental approaches to control the core metrics of lasing performance, including threshold, resonant wavelength, and emission directionality. The applications of spasers and random lasers in the fields of sensing and imaging are also mentioned. Finally, the challenges and future perspectives in this area of research are discussed.     

Nano‐opto‐mechanical effects in plasmonic waveguides

In order to achieve interaction between light beams, a mediating material object is required. Nonlinear materials are commonly used for this purpose. Here a new approach to control light with light, based on a nano‐opto‐mechanical system integrated in a plasmonic waveguide is proposed. Optomechanics of a free‐floating resonant nanoparticle in a subwavelength plasmonic V‐groove waveguide is studied. It is shown that nanoparticle auto‐oscillations in the waveguide induced by a control light result in the periodic modulation of a transmitted plasmonic signal. The modulation depth of 10% per single nanoparticle of 25 nm diameter with the clock frequencies of tens of MHz and the record low energy‐per‐bit energies of 10⁻¹⁸ J is observed. The frequency of auto‐oscillations depends on the intensity of the continuous control light. The efficient modulation and deep‐subwavelength dimensions make this nano‐optomechanical system of significant interest for opto‐electronic and opto‐fluidic technologies.     

Lasing action assisted by long‐range surface plasmons

It is shown that lasing action at subwavelength scales can be achieved in realistic plasmonic systems supporting long‐range surface plasmons (LRSPPs). To this end, a general numerical framework has been developed that is able to accurately account for the full spatio‐temporal lasing dynamics and the vastly different length‐ and time‐scales featured by this class of systems. Starting from a loss compensation regime for propagating LRSPPs, it is shown how the introduction of an optical feedback mechanism induces the formation of a self‐sustained laser oscillation at moderate pump intensities. The simplicity of the proposed subwavelength scale laser offers significant potential as a novel class of planar light sources in complex plasmonic circuits.     

Optical properties of femtosecond laser-treated diamond

Coupling effect in spiral-shaped metamaterials composed of four half rings at different sizes is investigated to achieve tunability in THz range. This novel spiral-shaped structure was fabricated on flexible substrate with laser micro-lens array (MLA) lithography and measured by THz time domain spectroscopy (THz-TDS). The experimental results suggest that mutual capacitance and inductance coupling in the spiral-shaped structure would result in frequency shifts of the four resonances. The observed shifting trends of the four resonant frequencies are in good agreement with simulation and are further explained by the electric field distribution. By varying the gap sizes among the half rings, four resonant frequencies can be tuned flexibly. Such a spiral-shaped design has potential applications in multi-band tunable THz MEMS devices.     

Manipulating electromagnetic resonances in meta-molecules with double split ring resonators

We proposed meta-molecules structure composed of stacked double split ring resonators (DSRRs) and studied its electromagnetic resonances in the optical frequency range. We demonstrated that, for the first order plasmonic modes, the coupling between the outer and the inner SRRs in plane strongly influences on the resonant frequency splitting of the stacked DSRRs. And their resonant dips change with the arrangement of SRRs. However, the resonant frequencies for the high order plasmonic modes always remain immobile as the configuration varies. Our investigation offers an effective way to manipulate the resonant behavior in metamaterials.     

Structuring of Surfaces with Gold Nanoparticles by Using Bessel‐Like Beams

Here, the structuring of surfaces with gold nanoparticles by using Bessel‐like beam array is demonstrated. The experimental results show that the fabricated microring structures containing gold nanoparticles have a surface plasmon resonance in the spectral range of 520–540 nm, which can be tuned by selecting the laser treatment parameters. Fabricated microring structures exhibit a lower light transmittance comparing with the randomly distributed gold nanoparticles for wavelengths 500–570 nm due to the growth in the size of nanoparticles. In the spectral range of 600–700 nm, the light transmittance through microring structures is higher compared with the randomly distributed gold nanoparticles because of the removal of gold nanoparticles as gold has high reflectivity for wavelengths longer than 600 nm. The demonstrated method enables an easy fabrication of microring structures having tunable plasmonic properties.     

Efficient Integrated Graphene Photonics in the Visible and Near‐IR

Graphene photonics has emerged as a promising platform for providing desirable optical functionality. However, graphene's monolayer‐scale thickness fundamentally restricts the available light matter interaction, posing a critical design challenge for integrated devices, particularly in wavelength regimes where graphene plasmonics is untenable. While several plasmonic designs have been proposed to enhance graphene light interaction in these regimes, they suffer from substantial insertion loss due to metal absorption. Here we report a non‐resonant metamaterial‐based waveguide platform to overcome the design bottleneck associated with graphene device. Such metamaterial structure enables low insertion loss even though metal is being utilized. By examining waveguide dispersion characteristics via closed‐form analysis, it is demonstrated that the metamaterial approach can provide optimized optical field that overlaps with the graphene monolayer. This enables graphene‐based integrated components with superior optical performance. Specifically, the metamaterial‐assisted graphene modulator can provide 5‐fold improvement in extinction ratio compared to Si nanowire, while reducing insertion loss by one order magnitude compared to plasmonic structures. Such a waveguide configuration thus allows one to maximize the optical potential that graphene holds in the telecom and visible regimes.     

Photoetching of spherical microlenses on glasses using a femtosecond laser

We fabricated spherical microlenses on optical glasses by femtosecond laser direct writing (FLDW) in ambient air. To achieve good appearances of the microlenses, a meridian-arcs scanning method was used after a selective multilayer removal process with spiral scanning paths. A positive spherical microlens with diameter of 48 μm and height of 13.2 μm was fabricated on the surface of the glass substrate. The optical performances of the microlens were also tested. Compared to the conventional laser direct writing (LDW) technique, this work could provide an effective method for precise shape-controlled fabrication of three-dimensional (3D) microstructures with curved surfaces on difficult-to-cut materials for practical applications.     

All‐Optical Transmission Modulation Due to Inelastic Interactions of Ultrashort Pulses in a Disordered Resonant Medium

Random resonant media being one of the possible realizations of disordered metamaterials open a room of opportunities for achieving new fundamental effects and designing advanced nanophotonic devices. Strongly nonlinear optical properties of such media attract ever increasing attention nowadays from both theoretical and experimental points of view. Hereinafter, the case of the photonic‐crystal‐like structure with a randomly varying light–matter coupling provided by the random density of quantum particles is considered. Using numerical solution of the Maxwell–Bloch equations, the effects of the pulse collisions in the medium are studied. It is shown that disorder enables the qualitative changes of the system's response for co‐propagating pulses, whereas this is not the case for the counter‐propagating ones. The scheme for an all‐optical transmission modulation due to the disorder‐induced inelasticity of collisions of co‐propagating pulses is proposed. The ability of precise tuning the modulation via the inter‐pulse distance and background refractive index adjustment is revealed. This novel approach for light control can be utilized for some high demand applications, such as modulation and switching of a pulsed radiation.     

Nano‐imaging through tip‐enhanced Raman spectroscopy: Stepping beyond the classical limits

The spatial resolution in optical imaging is restricted by so‐called diffraction limit, which prevents it to be better than about half of the wavelength of the probing light. Tip‐enhanced Raman spectroscopy (TERS), which is based on the SPP‐induced plasmonic enhancement and confinement of light near a metallic nanostructure, can however, overcome this barrier and produce optical images far beyond the diffraction limit. Here in this article, the basic phenomenon involved in TERS is reviewed, and the high spatial resolution achieved in optical imaging through this technique is discussed. Further, it is shown that when TERS is combined with some other physical phenomena, the spatial resolution can be dramatically improved. Particularly, by including tip‐applied extremely localized pressure in TERS process, it has been demonstrated that a spatial resolution as high as 4 nm could be achieved.     

Rapid,Reversible Release from Thermosensitive Liposomes Triggered by Near‐Infra‐Red Light

A novel drug carrier is presented consisting of plasmonic hollow gold nanoshells (HGN) chemically tethered to liposomes made temperature sensitive with lysolipids (TSL). Continuous‐wave irradiation by physiologically friendly near‐infra‐red light at 800 nm for 2.5 min at laser intensities an order of magnitude below that known to damage skin generates heating localized to the liposome membrane. The heating increases the liposome permeability in an irradiation dose dependent, but reversible manner, resulting in rapid release of small molecules such as the self‐quenching dye carboxyfluorescein or the chemotherapeutic doxorubicin, without raising the bulk temperature. The local rise in nanoshell temperature under laser irradiation is inferred by comparing dye release rates from the TSL via bulk heating to that induced by irradiation. Laser‐irradiation of TSL enables precise control of contents release with low temperature gradients confined to areas irradiated by the laser focus. The combined effects of rapid local release and localized hyperthermia provide a synergistic effect as shown by a near doubling of androgen resistant PPC‐1 prostate cancer cell toxicity compared to the same concentration of free doxorubicin.     

The distributions of enhancement factors in close‐packed and nonclose‐packed surface‐enhanced Raman substrates

A method employing photochemical hole burning, previously developed to measure the distribution of Raman enhancement factors on a nanostructured substrate for surface‐enhanced Raman scattering, is used to compare the enhancement distributions of benzenethiol adsorbed on substrates optimized for 532 nm laser excitation consisting of close‐packed (CP) or nonclose‐packed (NCP) nanospheres. The ensemble‐averaged Raman enhancement factor was 2.8 times smaller for the NCP substrate. The measured distributions revealed additional information. For instance, 92% of the molecules on the CP substrate and 93.6% of the molecules on the NCP substrate had Raman enhancements below average. The minimum enhancements on both substrates were ~10⁴, but on the NCP substrate the maximum enhancement was 1.2 × 10⁸, whereas on the CP substrate the maximum was 2 × 10¹⁰. The Ag‐coated nanospheres form hemisphere‐on‐cylinder mushroom‐like structures on both lattices, but on the NCP lattice, one third of the molecules are on the flat regions between the mushrooms. The flats on the NCP lattice have enhancements of ~10⁴, showing they are part of a resonant plasmonic structure. The highest NCP enhancements of ~10⁸ are tentatively associated with regions at the bases of the mushrooms, whereas the highest CP enhancements of 2 × 10¹⁰ are tentatively associated with gaps between nanospheres where 0.0025% of the molecules reside. Copyright © 2011 John Wiley & Sons, Ltd.     

Enhanced Photoelectric and Photothermal Responses on Silicon Platform by Plasmonic Absorber and Omni‐Schottky Junction

Recent progresses in plasmon‐induced hot electrons open up the possibility to achieve photon harvesting beyond the fundamental limit imposed by band‐to‐band transitions in semiconductors. To obtain high efficiency, both the optical absorption and electron emission/collection are crucial factors that need to be addressed in the design of hot electron devices. Here, we demonstrate a photoresponse as high as 3.3mA/W at 1500nm on a silicon platform by plasmonic absorber (PA) and omni‐Schottky junction integrated photodetector, reverse biased at 5V and illuminated with 10mW. The PA fabricated on silicon consists of a monolayer of random Au nanoparticles (NPs), a wide‐band gap semiconductor (TiO₂) and an optically thick Au electrode, resulting in broadband near‐infrared (NIR) absorption and efficient hot‐electron transfer via an all‐around Schottky emission path. Meanwhile, time and spectral‐resolved photoresponse measurements reveal that embedded NPs with superior absorption resembling plasmonic local heating sources can transfer their energy to electricity via the photothermal mechanism, which until now has not been adequately assessed or rigorously differentiated from the photoelectric process in plasmon‐mediated photon harvesting nano‐systems.     

Ultrafast optical switching of terahertz metamaterials fabricated on ErAs/GaAs nanoisland superlattices

We demonstrate optical switching of electrically resonant terahertz planar metamaterials fabricated on ErAs/GaAs nanoisland superlattice substrates. Photoexcited charge carriers in the superlattice shunt the capacitive regions of the constituent elements, thereby modulating the resonant response of the metamaterials. A switching recovery time of 20 ps results from fast carrier recombination in the ErAs/GaAs superlattice substrates.     

Intra‐laser‐cavity microparticle sensing with a dual‐wavelength distributed‐feedback laser

An integrated intra‐laser‐cavity microparticle sensor based on a dual‐wavelength distributed‐feedback channel waveguide laser in ytterbium‐doped amorphous aluminum oxide on a silicon substrate is demonstrated. Real‐time detection and accurate size measurement of single micro‐particles with diameters ranging between 1 µm and 20 µm are achieved, which represent the typical sizes of many fungal and bacterial pathogens as well as a large variety of human cells. A limit of detection of ∼500 nm is deduced. The sensing principle relies on measuring changes in the frequency difference between the two longitudinal laser modes as the evanescent field of the dual‐wavelength laser interacts with micro‐sized particles on the surface of the waveguide. Improvement in sensitivity far down to the nanometer range can be expected upon stabilizing the pump power, minimizing back reflections, and optimizing the grating geometry to increase the evanescent fraction of the guided modes.