Singular-phase nanooptics: towards label-free single molecule detection

Non-trivial topology of phase is crucial for many important physics phenomena such as, for example, the Aharonov-Bohm effect 1 and the Berry phase 2. Light phase allows one to create "twisted" photons 3, 4 , vortex knots 5, dislocations 6 which has led to an emerging field of singular optics relying on abrupt phase changes 7. Here we demonstrate the feasibility of singular visible-light nanooptics which exploits the benefits of both plasmonic field enhancement and non-trivial topology of light phase. We show that properly designed plasmonic nanomaterials exhibit topologically protected singular phase behaviour which can be employed to radically improve sensitivity of detectors based on plasmon resonances. By using reversible hydrogenation of graphene 8 and a streptavidin-biotin test 9, we demonstrate areal mass sensitivity at a level of femto-grams per mm2 and detection of individual biomolecules, respectively. Our proof-of-concept results offer a way towards simple and scalable single-molecular label-free biosensing technologies.Comment: 19 pages, 4 figure

Nanofabrication with Pulsed Lasers

An overview of pulsed laser-assisted methods for nanofabrication, which are currently developed in our Institute (LP3), is presented. The methods compass a variety of possibilities for material nanostructuring offered by laser–matter interactions and imply either the nanostructuring of the laser-illuminated surface itself, as in cases of direct laser ablation or laser plasma-assisted treatment of semiconductors to form light-absorbing and light-emitting nano-architectures, as well as periodic nanoarrays, or laser-assisted production of nanoclusters and their controlled growth in gaseous or liquid medium to form nanostructured films or colloidal nanoparticles. Nanomaterials synthesized by laser-assisted methods have a variety of unique properties, not reproducible by any other route, and are of importance for photovoltaics, optoelectronics, biological sensing, imaging and therapeutics

Topological Darkness: How to Design a Metamaterial for Optical Biosensing with Virtually Unlimited Sensitivity

Due to the absence of labels and fast analyses, optical biosensors promise major advances in biomedical diagnostics, security, environmental and food safety applications. However, sensitivity of the most advanced plasmonic biosensor implementations has a fundamental limitation caused by losses in the system and or geometry of biochips. Here, we report a scissor effect in topologically dark metamaterials which is capable of providing virtually unlimited bona fide sensitivity to biosensing thus solving the bottleneck sensitivity limitation problem. We explain how the scissor effect can be realized via a proper design of topologically dark metamaterials and describe strategies for their fabrication. To validate the applicability of this effect in biosensing, we demonstrate the detection of folic acid (vitamin important for human health) in the wide 3-log linear dynamic range with the limit of detection of 0.125 nM, which is orders of magnitude better than previously reported for all optical counterparts. Our work opens possibilities for designing and realising plasmonic, semiconductor and dielectric metamaterials with ultra-sensitivity to binding events.Comment: 22 pages, 4 figure

Boosting the Figure Of Merit of LSPR-based refractive index sensing by phase-sensitive measurements

Localized surface plasmon resonances possess very interesting properties for a wide variety of sensing applications. In many of the existing applications only the intensity of the reflected or transmitted signals is taken into account, while the phase information is ignored. At the center frequency of a (localized) surface plasmon resonance, the electron cloud makes the transition between in- and out-of-phase oscillation with respect to the incident wave. Here we show that this information can experimentally be extracted by performing phase-sensitive measurements, which result in linewidths that are almost one order of magnitude smaller than those for intensity based measurements. As this phase transition is an intrinsic property of a plasmon resonance, this opens up many possibilities for boosting the figure of merit (FOM) of refractive index sensing by taking into account the phase of the plasmon resonance. We experimentally investigated this for two model systems: randomly distributed gold nanodisks and gold nanorings on top of a continuous gold layer and a dielectric spacer and observed FOM values up to 8.3 and 16.5 for the respective nanoparticles

Biocompatibility of Bare Nanoparticles Based on Silicon and Gold for Nervous Cells

This work aimed to investigate the biocompatibility of bare (ligand-free) lasersynthesized nanoparticles (NPs) based on silicon (Si) and gold (Au) with primary hippocampal cultures. 1%, 5% and 7% of culture medium were replaced by 0.1 mg/mL NP solution on day 14 of culture development in vitro. Our studies revealed that the NPs caused a dose-dependent cytotoxic effect, which was manifested by an increase the number of dead cells and a decrease of the spontaneous functional calcium activity of neural networks. Au NPs revealed less pronounced cytotoxic effect than Si ones and it can be explained by larger size and better solubility of Si NPs. Keywords: bare nanoparticles, primary hippocampal cultures, neurotoxicit

Concave Plasmonic Particles: Broad-Band Geometrical Tunability in the Near Infra-Red

Optical resonances spanning the Near and Short Infra-Red spectral regime were exhibited experimentally by arrays of plasmonic nano-particles with concave cross-section. The concavity of the particle was shown to be the key ingredient for enabling the broad band tunability of the resonance frequency, even for particles with dimensional aspect ratios of order unity. The atypical flexibility of setting the resonance wavelength is shown to stem from a unique interplay of local geometry with surface charge distributions

Analysis of the structure, configuration, and sizing of Cu and Cu oxide nanoparticles generated by fs laser ablation of solid target in liquids

We report on the analysis of structure, configuration, and sizing of Cu and Cu oxide nanoparticles (Nps) produced by femtosecond (fs) laser ablation of solid copper target in liquids. Laser pulse energy ranged between 500 µJ and 50 µJ. Water and acetone were used to produce the colloidal suspensions. The study was performed through optical extinction spectroscopy using Mie theory to fit the full experimental spectra, considering free and bound electrons size dependent contributions to the metal dielectric function. Raman spectroscopy and AFM technique were also used to characterize the sample. Considering the possible oxidation of copper during the fabrication process, two species (Cu and Cu2O) arranged in two structures (bare core or core-shell) and in two configuration types (Cu-Cu2O or Cu2O-Cu) were considered for the fitting depending on the laser pulse energy and the surrounding media. For water at high energy, it can be observed that a Cu-Cu2O configuration fits the experimental spectra of the colloidal suspension, while for decreasingenergy and below a certain threshold, a Cu2O-Cu configuration needs to be included for theoptimum fit. Both species coexist for energies below 170 µJ for water. On the other hand, for acetone at high energy, optimum fit of the full spectrum suggests the presence a bimodal Cu-Cu2O core-shell Nps distribution while for decreasing energy and below a 70 µJ threshold energy value, Cu2O-Cu core-shell Nps must be included, together with the former configuration, for the fit of the full spectrum. We discuss possible reasons for the changes in the structural configuration of the core-shell Nps.Fil: Schinca, Daniel Carlos. Universidad Nacional de la Plata. Facultad de Cs.exactas. Instituto de Fisica de la Plata; ArgentinaFil: Videla, Fabian Alfredo. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico la Plata. Centro de Investigaciones Opticas (i); ArgentinaFil: Fernández van Raap, Marcela Beatriz. Universidad Nacional de la Plata. Facultad de Ingenieria; ArgentinaFil: Scaffardi, Lucia Beatriz. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico la Plata. Centro de Investigaciones Opticas (i); ArgentinaFil: Santillán, Jesica María José. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico la Plata. Centro de Investigaciones Opticas (i); Argentin

Transition metal dichalcogenide nanospheres for high-refractive-index nanophotonics and biomedical theranostics

Recent developments in the area of resonant dielectric nanostructures have created attractive opportunities for concentrating and manipulating light at the nanoscale and the establishment of the new exciting field of all-dielectric nanophotonics. Transition metal dichalcogenides (TMDCs) with nanopatterned surfaces are especially promising for these tasks. Still, the fabrication of these structures requires sophisticated lithographic processes, drastically complicating application prospects. To bridge this gap and broaden the application scope of TMDC nanomaterials, we report here femtosecond laser-ablative fabrication of water-dispersed spherical TMDC (MoS2 and WS2) nanoparticles (NPs) of variable size (5 to 250 nm). Such NPs demonstrate exciting optical and electronic properties inherited from TMDC crystals, due to preserved crystalline structure, which offers a unique combination of pronounced excitonic response and high refractive index value, making possible a strong concentration of electromagnetic field in the NPs. Furthermore, such NPs offer additional tunability due to hybridization between the Mie and excitonic resonances. Such properties bring to life a number of nontrivial effects, including enhanced photoabsorption and photothermal conversion. As an illustration, we demonstrate that the NPs exhibit a very strong photothermal response, much exceeding that of conventional dielectric nanoresonators based on Si. Being in a mobile colloidal state and exhibiting superior optical properties compared to other dielectric resonant structures, the synthesized TMDC NPs offer opportunities for the development of next-generation nanophotonic and nanotheranostic platforms, including photothermal therapy and multimodal bioimaging

Resonances On-Demand for Plasmonic Nano-Particles

A method for designing plasmonic particles with desired resonance spectra is presented. The method is based on repetitive perturbations of an initial particle shape while calculating the eigenvalues of the various quasistatic resonances. The method is rigorously proved, assuring a solution exists for any required spectral resonance location. Resonances spanning the visible and the near-infrared regimes, as designed by our method, are verified using finite-difference time-domain simulations. A novel family of particles with collocated dipole-quadrupole resonances is designed, demonstrating the unique power of the method. Such on-demand engineering enables strict realization of nano-antennas and metamaterials for various applications requiring specific spectral functions

From Cleanroom to Desktop: Emerging Micro-Nanofabrication Technology for Biomedical Applications

This review is motivated by the growing demand for low-cost, easy-to-use, compact-size yet powerful micro-nanofabrication technology to address emerging challenges of fundamental biology and translational medicine in regular laboratory settings. Recent advancements in the field benefit considerably from rapidly expanding material selections, ranging from inorganics to organics and from nanoparticles to self-assembled molecules. Meanwhile a great number of novel methodologies, employing off-the-shelf consumer electronics, intriguing interfacial phenomena, bottom-up self-assembly principles, etc., have been implemented to transit micro-nanofabrication from a cleanroom environment to a desktop setup. Furthermore, the latest application of micro-nanofabrication to emerging biomedical research will be presented in detail, which includes point-of-care diagnostics, on-chip cell culture as well as bio-manipulation. While significant progresses have been made in the rapidly growing field, both apparent and unrevealed roadblocks will need to be addressed in the future. We conclude this review by offering our perspectives on the current technical challenges and future research opportunities