High-Resolution Photonic Force Microscopy Based on Sharp Nanofabricated Tips.

Although near-field imaging techniques reach sub-nanometer resolution on rigid samples, it remains extremely challenging to image soft interfaces, such as biological membranes, due to the deformations induced by the probe. In photonic force microscopy, optical tweezers are used to manipulate and measure the scanning probe, allowing imaging of soft materials without force-induced artifacts. However, the size of the optically trapped probe still limits the maximum resolution. Here, we show a novel and simple nanofabrication protocol to massively produce optically trappable quartz particles which mimic the sharp tips of atomic force microscopy. Imaging rigid nanostructures with our tips, we resolve features smaller than 80 nm. Scanning the membrane of living malaria-infected red blood cells reveals, with no visible artifacts, submicron features termed knobs, related to the parasite activity. The use of nanoengineered particles in photonic force microscopy opens the way to imaging soft samples at high resolution.

Optical Trapping, Optical Binding, and Rotational Dynamics of Silicon Nanowires in Counter-Propagating Beams.

Silicon nanowires are held and manipulated in controlled optical traps based on counter-propagating beams focused by low numerical aperture lenses. The double-beam configuration compensates light scattering forces enabling an in-depth investigation of the rich dynamics of trapped nanowires that are prone to both optical and hydrodynamic interactions. Several polarization configurations are used, allowing the observation of optical binding with different stable structure as well as the transfer of spin and orbital momentum of light to the trapped silicon nanowires. Accurate modeling based on Brownian dynamics simulations with appropriate optical and hydrodynamic coupling confirms that this rich scenario is crucially dependent on the non-spherical shape of the nanowires. Such an increased level of optical control of multiparticle structure and dynamics open perspectives for nanofluidics and multi-component light-driven nanomachines.

Raman Tweezers for Small Microplastics and Nanoplastics Identification in Seawater.

Our understanding of the fate and distribution of micro- and nano- plastics in the marine environment is limited by the intrinsic difficulties of the techniques currently used for the detection, quantification, and chemical identification of small particles in liquid (light scattering, vibrational spectroscopies, and optical and electron microscopies). Here we introduce Raman Tweezers (RTs), namely optical tweezers combined with Raman spectroscopy, as an analytical tool for the study of micro- and nanoplastics in seawater. We show optical trapping and chemical identification of sub-20 µm plastics, down to the 50 nm range. Analysis at the single particle level allows us to unambiguously discriminate plastics from organic matter and mineral sediments, overcoming the capacities of standard Raman spectroscopy in liquid, intrinsically limited to ensemble measurements. Being a microscopy technique, RTs also permits one to assess the size and shapes of particles (beads, fragments, and fibers), with spatial resolution only limited by diffraction. Applications are shown on both model particles and naturally aged environmental samples, made of common plastic pollutants, including polyethylene, polypropylene, nylon, and polystyrene, also in the presence of a thin eco-corona. Coupled to suitable extraction and concentration protocols, RTs have the potential to strongly impact future research on micro and nanoplastics environmental pollution, and enable the understanding of the fragmentation processes on a multiscale level of aged polymers.

Nanoscale Discrimination between Toxic and Nontoxic Protein Misfolded Oligomers with Tip-Enhanced Raman Spectroscopy.

Highly toxic protein misfolded oligomers associated with neurological disorders such as Alzheimer's and Parkinson's diseases are nowadays considered primarily responsible for promoting synaptic failure and neuronal death. Unraveling the relationship between structure and neurotoxicity of protein oligomers appears pivotal in understanding the causes of the pathological process, as well as in designing novel diagnostic and therapeutic strategies tuned toward the earliest and presymptomatic stages of the disease. Here, it is benefited from tip-enhanced Raman spectroscopy (TERS) as a surface-sensitive tool with spatial resolution on the nanoscale, to inspect the spatial organization and surface character of individual protein oligomers from two samples formed by the same polypeptide sequence and different toxicity levels. TERS provides direct assignment of specific amino acid residues that are exposed to a large extent on the surface of toxic species and buried in nontoxic oligomers. These residues, thanks to their outward disposition, might represent structural factors driving the pathogenic behavior exhibited by protein misfolded oligomers, including affecting cell membrane integrity and specific signaling pathways in neurodegenerative conditions.

Optical Binding of Nanowires.

Multiple scattering of light induces structured interactions, or optical binding forces, between collections of small particles. This has been extensively studied in the case of microspheres. However, binding forces are strongly shape dependent: here, we turn our attention to dielectric nanowires. Using a novel numerical model we uncover rich behavior. The extreme geometry of the nanowires produces a sequence of stationary and dynamic states. In linearly polarized light, thermally stable ladder-like structures emerge. Lower symmetry, sagittate arrangements can also arise, whose configurational asymmetry unbalances the optical forces leading to nonconservative, translational motion. Finally, the addition of circular polarization drives a variety of coordinated rotational states whose dynamics expose fundamental properties of optical spin. These results suggest that optical binding can provide an increased level of control over the positions and motions of nanoparticles, opening new possibilities for driven self-organization and heralding a new field of self-assembling optically driven micromachines.

Photonic Torque Microscopy of the Nonconservative Force Field for Optically Trapped Silicon Nanowires.

We measure, by photonic torque microscopy, the nonconservative rotational motion arising from the transverse components of the radiation pressure on optically trapped, ultrathin silicon nanowires. Unlike spherical particles, we find that nonconservative effects have a significant influence on the nanowire dynamics in the trap. We show that the extreme shape of the trapped nanowires yields a transverse component of the radiation pressure that results in an orbital rotation of the nanowire about the trap axis. We study the resulting motion as a function of optical power and nanowire length, discussing its size-scaling behavior. These shape-dependent nonconservative effects have implications for optical force calibration and optomechanics with levitated nonspherical particles.

Surface-enhanced Raman spectroscopy in 3D electrospun nanofiber mats coated with gold nanorods.

Nanofibers functionalized by metal nanostructures and particles are exploited as effective flexible substrates for surface-enhanced Raman scattering (SERS) analysis. Their complex three-dimensional structure may provide Raman signals enhanced by orders of magnitude compared to untextured surfaces. Understanding the origin of such improved performances is therefore very important for pushing nanofiber-based analytical technologies to their upper limit. Here, we report on polymer nanofiber mats which can be exploited as substrates for enhancing the Raman spectra of adsorbed probe molecules. The increased surface area and the scattering of light in the nanofibrous system are individually analyzed as mechanisms to enhance Raman scattering. The deposition of gold nanorods on the fibers further amplifies Raman signals due to SERS. This study suggests that Raman signals can be finely tuned in intensity and effectively enhanced in nanofiber mats and arrays by properly tailoring the architecture, composition, and light-scattering properties of the complex networks of filaments.

Focus issue introduction: optical cooling and trapping.

The year 2015 is an auspicious year for optical science, as it is being celebrated as the International Year of Light and Light-Based Technologies. This Focus Issue of the journals Optics Express and Journal of the Optical Society of America B has been organized by the OSA Technical Group on Optical Cooling and Trapping to mark this occasion, and to highlight the most recent and exciting developments in the topics covered by the group. Together this joint Focus Issue features 32 papers, including both experimental and theoretical works, which span this wide range of activities.

Faster and More Accurate Geometrical-Optics Optical Force Calculation Using Neural Networks.

Optical forces are often calculated by discretizing the trapping light beam into a set of rays and using geometrical optics to compute the exchange of momentum. However, the number of rays sets a trade-off between calculation speed and accuracy. Here, we show that using neural networks permits overcoming this limitation, obtaining not only faster but also more accurate simulations. We demonstrate this using an optically trapped spherical particle for which we obtain an analytical solution to use as ground truth. Then, we take advantage of the acceleration provided by neural networks to study the dynamics of ellipsoidal particles in a double trap, which would be computationally impossible otherwise.

Optically Driven Janus Microengine with Full Orbital Motion Control.

Microengines have shown promise for a variety of applications in nanotechnology, microfluidics, and nanomedicine, including targeted drug delivery, microscale pumping, and environmental remediation. However, achieving precise control over their dynamics remains a significant challenge. In this study, we introduce a microengine that exploits both optical and thermal effects to achieve a high degree of controllability. We find that in the presence of a strongly focused light beam, a gold-silica Janus particle becomes confined at the stationary point where the optical and thermal forces balance. By using circularly polarized light, we can transfer angular momentum to the particle, breaking the symmetry between the two forces and resulting in a tangential force that drives directed orbital motion. We can simultaneously control the velocity and direction of rotation of the particle changing the ellipticity of the incoming light beam while tuning the radius of the orbit with laser power. Our experimental results are validated using a geometrical optics phenomenological model that considers the optical force, the absorption of optical power, and the resulting heating of the particle. The demonstrated enhanced flexibility in the control of microengines opens up new possibilities for their utilization in a wide range of applications, including microscale transport, sensing, and actuation.

Size-scaling in optical trapping of silicon nanowires.

We investigate size-scaling in optical trapping of ultrathin silicon nanowires showing how length regulates their Brownian dynamics, optical forces, and torques. Force and torque constants are measured on nanowires of different lengths through correlation function analysis of their tracking signals. Results are compared with a full electromagnetic theory of optical trapping developed in the transition matrix framework, finding good agreement.

Optical trapping of porous silicon nanoparticles.

Silicon nanoparticles obtained by ball-milling of a 50% porosity silicon layer have been optically trapped when dispersed in a water-surfactant environment. We measured the optical force constants using linearly and radially polarized trapping beams finding a reshaping of the optical potential and an enhanced axial spring constant for the latter. These measurements open perspectives for the control and handling of silicon nanoparticles as labeling agents in biological analysis and fluorescence imaging techniques.

Rotational dynamics of optically trapped nanofibers.

We report on the experimental evidence of tilted polymer nanofiber rotation, using a highly focused linear polarized Gaussian beam. Torque is controlled by varying trapping power or fiber tilt angle. This suggests an alternative strategy to previously reported approaches for the rotation of nano-objects, to test fundamental theoretical aspects. We compare experimental rotation frequencies to calculations based on T-Matrix formalism, which accurately reproduces measured data, thus providing a comprehensive description of trapping and rotation dynamics of the linear nanostructures.

Intelligent non-colorimetric indicators for the perishable supply chain by non-wovens with photo-programmed thermal response.

Spoiled perishable products, such as food and drugs exposed to inappropriate temperature, cause million illnesses every year. Risks range from intoxication due to pathogen-contaminated edibles, to suboptimal potency of temperature-sensitive vaccines. High-performance and low-cost indicators are needed, based on conformable materials whose properties change continuously and irreversibly depending on the experienced time-temperature profile. However, these systems can be limited by unclear reading, especially for colour-blind people, and are often difficult to be encoded with a tailored response to detect excess temperature over varying temporal profiles. Here we report on optically-programmed, non-colorimetric indicators based on nano-textured non-wovens encoded by their cross-linking degree. This combination allows a desired time-temperature response to be achieved, to address different perishable products. The devices operate by visual contrast with ambient light, which is explained by backscattering calculations for the complex fibrous material. Optical nanomaterials with photo-encoded thermal properties might establish new design rules for intelligent labels.

Optical trapping calculations for metal nanoparticles. Comparison with experimental data for Au and Ag spheres.

We calculate the optical forces on Au and Ag nanospheres through a procedure based on the Maxwell stress tensor. We compare the theoretical and experimental force constants obtained for gold and silver nanospheres finding good agreement for all particles with r < 80 nm. The trapping of the larger particles recently demonstrated in experiments is not foreseen by our purely electromagnetic theory based on fixed dielectric properties. Since the laser power produces a heating that may be large for the largest spheres, we propose a model in which the latter particles are surrounded by a steam bubble. This model foresees the trapping of these particles and the results turn out to be in reasonable agreement with the experimental data.

Intracavity optical trapping of microscopic particles in a ring-cavity fiber laser.

Standard optical tweezers rely on optical forces arising when a focused laser beam interacts with a microscopic particle: scattering forces, pushing the particle along the beam direction, and gradient forces, attracting it towards the high-intensity focal spot. Importantly, the incoming laser beam is not affected by the particle position because the particle is outside the laser cavity. Here, we demonstrate that intracavity nonlinear feedback forces emerge when the particle is placed inside the optical cavity, resulting in orders-of-magnitude higher confinement along the three axes per unit laser intensity on the sample. This scheme allows trapping at very low numerical apertures and reduces the laser intensity to which the particle is exposed by two orders of magnitude compared to a standard 3D optical tweezers. These results are highly relevant for many applications requiring manipulation of samples that are subject to photodamage, such as in biophysics and nanosciences.

Chiral optical tweezers for optically active particles in the T-matrix formalism.

Modeling optical tweezers in the T-matrix formalism has been of key importance for accurate and efficient calculations of optical forces and their comparison with experiments. Here we extend this formalism to the modeling of chiral optomechanics and optical tweezers where chiral light is used for optical manipulation and trapping of optically active particles. We first use the Bohren decomposition to deal with the light scattering of chiral light on optically active particles. Thus, we show analytically that all the observables (cross sections, asymmetry parameters) are split into a helicity dependent and independent part and study a practical example of a complex resin particle with inner copper-coated stainless steel helices. Then, we apply this chiral T-matrix framework to optical tweezers where a tightly focused chiral field is used to trap an optically active spherical particle, calculate the chiral behaviour of optical trapping stiffnesses and their size scaling, and extend calculations to chiral nanowires and clusters of astrophysical interest. Such general light scattering framework opens perspectives for modeling optical forces on biological materials where optically active amino acids and carbohydrates are present.

Optical Aggregation of Gold Nanoparticles for SERS Detection of Proteins and Toxins in Liquid Environment: Towards Ultrasensitive and Selective Detection.

Optical forces are used to aggregate plasmonic nanoparticles and create SERS-active hot spots in liquid. When biomolecules are added to the nanoparticles, high sensitivity SERS detection can be accomplished. Here, we pursue studies on Bovine Serum Albumin (BSA) detection, investigating the BSA-nanorod aggregations in a range from 100 µM to 50 nM by combining light scattering, plasmon resonance and SERS, and correlating the SERS signal with the concentration. Experimental data are fitted with a simple model describing the optical aggregation process. We show that BSA-nanorod complexes can be optically printed on non-functionalized glass surfaces, designing custom patterns stable with time. Furthermore, we demonstrate that this methodology can be used to detect catalase and hemoglobin, two Raman resonant biomolecules, at concentrations of 10 nM and 1 pM, respectively, i.e., well beyond the limit of detection of BSA. Finally, we show that nanorods functionalized with specific aptamers can be used to capture and detect Ochratoxin A, a fungal toxin found in food commodities and wine. This experiment represents the first step towards the addition of molecular specificity to this novel biosensor strategy.

Electrospun Conjugated Polymer/Fullerene Hybrid Fibers: Photoactive Blends, Conductivity through Tunneling-AFM, Light Scattering, and Perspective for Their Use in Bulk-Heterojunction Organic Solar Cells.

Hybrid conjugated polymer/fullerene filaments based on MEH-PPV/PVP/PCBM were prepared by electrospinning, and their properties were assessed by scanning electron, atomic and lateral-force, tunneling, and confocal microscopies, as well as by attenuated-total-reflection Fourier transform infrared spectroscopy, photoluminescence quantum yield, and spatially resolved fluorescence. Highlighted features include the ribbon shape of the realized fibers and the persistence of a network serving as a template for heterogeneous active layers in solar cell devices. A set of favorable characteristics is evidenced in this way in terms of homogeneous charge-transport behavior and formation of effective interfaces for diffusion and dissociation of photogenerated excitons. The interaction of the organic filaments with light, exhibiting specific light-scattering properties of the nanofibrous mat, might also contribute to spreading incident radiation across the active layers, thus potentially enhancing photovoltaic performance. This method might be applied to other electron donor-electron acceptor material systems for the fabrication of solar cell devices enhanced by nanofibrillar morphologies embedding conjugated polymers and fullerene compounds.

Surface plasmon resonance in gold nanoparticles: a review.

In the last two decades, plasmon resonance in gold nanoparticles (Au NPs) has been the subject of intense research efforts. Plasmon physics is intriguing and its precise modelling proved to be challenging. In fact, plasmons are highly responsive to a multitude of factors, either intrinsic to the Au NPs or from the environment, and recently the need emerged for the correction of standard electromagnetic approaches with quantum effects. Applications related to plasmon absorption and scattering in Au NPs are impressively numerous, ranging from sensing to photothermal effects to cell imaging. Also, plasmon-enhanced phenomena are highly interesting for multiple purposes, including, for instance, Raman spectroscopy of nearby analytes, catalysis, or sunlight energy conversion. In addition, plasmon excitation is involved in a series of advanced physical processes such as non-linear optics, optical trapping, magneto-plasmonics, and optical activity. Here, we provide the general overview of the field and the background for appropriate modelling of the physical phenomena. Then, we report on the current state of the art and most recent applications of plasmon resonance in Au NPs.