Optical trapping and manipulation of micrometre-sized particles was first reported in 1970. Since then, it has been successfully implemented in two size ranges: the subnanometre scale, where light-matter mechanical coupling enables cooling of atoms, ions and molecules, and the micrometre scale, where the momentum transfer resulting from light scattering allows manipulation of microscopic objects such as cells. But it has been difficult to apply these techniques to the intermediate - nanoscale - range that includes structures such as quantum dots, nanowires, nanotubes, graphene and two-dimensional crystals, all of crucial importance for nanomaterials-based applications. Recently, however, several new approaches have been developed and demonstrated for trapping plasmonic nanoparticles, semiconductor nanowires and carbon nanostructures. Here we review the state-of-the-art in optical trapping at the nanoscale, with an emphasis on some of the most promising advances, such as controlled manipulation and assembly of individual and multiple nanostructures, force measurement with femtonewton resolution, and biosensors.
We study the Brownian motion (BM) of optically trapped graphene flakes. These orient orthogonal to the light polarization, due to the optical constants anisotropy. We explain the flake dynamics, measure force and torque constants and derive a full electromagnetic theory of optical trapping. The understanding of two dimensional BM paves the way to light-controlled manipulation and all-optical sorting of biological membranes and anisotropic macromolecules.The random motion of microscopic particles in a fluid was first observed in the late eighteenth century, and goes by the name of Brownian motion(BM) [1]. This was ascribed to thermal agitation[2], leading to Einstein's predictions of the resulting particle displacements [3]. BM is ubiquitous throughout physics, chemistry, biology, and even finance. It can be harnessed to produce directed motion [4]. It was also suggested that thermally activated BM may be responsible for the movement of molecular motors, such as myosin and kinesin [5]. When a Brownian particle (BP), i.e. a particle undergoing BM, is subject to an external field, e.g. a confining potential, the fluid damps the BM and, in a high damping regime, such as for a BP in water, the confining potential acts as a cut-off to the BM dynamics. This is free for short times (high frequency limit), while is frozen at longer times (low frequency limit) [8]. These processes have perfect ground in experiments with optical traps, where a BP is held by a focused laser beam, i.e. an optical tweezers [9]. In this context, BM can be utilized to investigate the properties of the surrounding environment [10,11], as well as of the trapped particle, and for accurate calibration of the spring constants of the optical harmonic potential [12,13].Dimensionality plays a special role in nature. From phase transitions [14], to transport phenomena[15], twodimensional (2d) systems often exhibit a strikingly different behavior [14]. Nanomaterials are an attractive target for optical trapping [16][17][18]. This can lead to top-down organization of composite nano-assemblies[16], sub-wavelength imaging by the excitation and scanning of nano-optical probes [17], photonic force microscopy with increased space and force resolution [18]. Graphene[19] is the prototype 2d material, and, as such, has unique mechanical, thermal, electronic and optical properties [20]. Here, we use graphene as prototype material to unravel the consequences of BM in 2d.Graphene is dispersed by processing graphite in a water-surfactant solution, Fig.1a. We do not use any functionalization nor oxidation, to retain the pristine electronic structure in the exfoliated monolayers [21][22][23]. We use di-hydroxy sodium deoxycholate surfactant. High resolution Transmission Electron Microscopy (HRTEM) shows∼10-40nm flakes. Fig.1b is an image of one such flake, with the typical honeycomb lattice. By analyzing over a hundred flakes, we find∼ 60% single-layer (SLG), much higher than previous aqueous [22] and nonaqueous dispersions [21], and the remainder bi-and trilayers (Fi...
In this article we show that linear nanoantennas can be used as shared substrates for surface-enhanced Raman and infrared spectroscopy (SERS and SEIRS, respectively). This is done by engineering the plasmonic properties of the nanoantennas, so to make them resonant in both the visible (transversal resonance) and the infrared (longitudinal resonance), and by rotating the excitation field polarization to selectively take advantage of each resonance and achieve SERS and SEIRS on the same nanoantennas. As a proof of concept, we have fabricated gold nanoantennas by electron beam lithography on calcium difluoride (1-2 μm long, 60 nm wide, 60 nm high) that exhibit a transverse plasmonic resonance in the visible (640 nm) and a particularly strong longitudinal dipolar resonance in the infrared (tunable in the 1280-3100 cm(-1) energy range as a function of the length). SERS and SEIRS detection of methylene blue molecules adsorbed on the nanoantenna's surface is accomplished, with signal enhancement factors of 5×10(2) for SERS (electromagnetic enhancement) and up to 10(5) for SEIRS. Notably, we find that the field enhancement provided by the transverse resonance is sufficient to achieve SERS from single nanoantennas. Furthermore, we show that by properly tuning the nanoantenna length the signals of a multitude of vibrational modes can be enhanced with SEIRS. This simple concept of plasmonic nanosensor is highly suitable for integration on lab-on-a-chip schemes for label-free chemical and biomolecular identification with optimized performances.
We extract the distribution of both center-of-mass and angular fluctuations from three-dimensional tracking of optically trapped nanotubes. We measure the optical force and torque constants from autocorrelation and cross-correlation of the tracking signals. This allows us to isolate the angular Brownian motion. We demonstrate that nanotubes enable nanometer spatial and femtonewton force resolution in photonic force microscopy, the smallest to date. This has wide implications in nanotechnology, biotechnology, nanofluidics, and material science.
Density gradient ultracentrifugation (DGU) has emerged as a promising tool to prepare chirality enriched nanotube samples. Here, we assess the performance of different surfactants for DGU. Bile salts (e.g., sodium cholate (SC), sodium deoxycholate (SDC), and sodium taurodeoxycholate (TDC)) are more effective in individualizing Single Wall Carbon Nanotubes (SWNTs) compared to linear chain surfactants (e.g., sodium dodecylbenzene sulfonate (SDBS) and sodium dodecylsulfate (SDS)) and better suited for DGU. Using SC, a narrower diameter distribution (0.69-0.81 nm) is achieved through a single DGU step on CoMoCAT tubes, when compared to SDC and TDC (0.69-0.89 nm). No selectivity is obtained using SDBS, due to its ineffectiveness in debundling. We assign the reduced selectivity of dihydroxy bile salts (SDC and TDC) in comparison with trihydroxy SC to the formation of secondary micelles. This is determined by the number and position of hydroxyl (-OH) groups on the R-side of the steroid backbone. We also enrich CoMoCAT SWNTs in the 0.84-0.92 nm range using the Pluronic F98 triblock copolymer. Mixtures of bile salts (SC) and linear chain surfactants (SDS) are used to enrich metallic and semiconducting laser-ablation grown SWNTs. We demonstrate enrichment of a single chirality, (6,5), combining diameter and metallic versus semiconducting separation on CoMoCAT samples.
Optical tweezers, tools based on strongly focused light, enable optical trapping, manipulation, and characterisation of a wide range of microscopic and nanoscopic materials. In the limiting cases of spherical particles either much smaller or much larger than the trapping wavelength, the force in optical tweez
Strategies for in-liquid molecular detection via Surface Enhanced Raman Scattering (SERS) are currently based on chemically-driven aggregation or optical trapping of metal nanoparticles in presence of the target molecules. Such strategies allow the formation of SERS-active clusters that efficiently embed the molecule at the “hot spots” of the nanoparticles and enhance its Raman scattering by orders of magnitude. Here we report on a novel scheme that exploits the radiation pressure to locally push gold nanorods and induce their aggregation in buffered solutions of biomolecules, achieving biomolecular SERS detection at almost neutral pH. The sensor is applied to detect non-resonant amino acids and proteins, namely Phenylalanine (Phe), Bovine Serum Albumin (BSA) and Lysozyme (Lys), reaching detection limits in the μg/mL range. Being a chemical free and contactless technique, our methodology is easy to implement, fast to operate, needs small sample volumes and has potential for integration in microfluidic circuits for biomarkers detection.
We analyze the rotational dynamics of light driven nanorotors, made of nanotube bundles and gold nanorods aggregates, with nonsymmetric shapes, trapped in optical tweezers. We identify two different regimes depending on dimensions and optical properties of the nanostructures. These correspond to alignment with either the laser propagation axis or the dominant polarization direction, or rotational motions caused by either unbalanced radiation pressure or polarization torque. By analyzing the motion correlations of the trapped nanostructures, we measure with high accuracy both the optical trapping parameters and the rotation frequency induced by the radiation pressure. Our results pave the way to improved all-optical detection, control over rotating nanomachines, and rotation detection in nano-optomechanics.
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