Fully Metal-Coated Scanning Near-Field Optical Microscopy Probes with Spiral Corrugations for Superfocusing under Arbitrarily Oriented Linearly Polarised Excitation

We study the effect of a spiral corrugation on the outer surface of a fully metal-coated scanning near-field optical microscopy (SNOM) probe using the finite element method. The introduction of a novel form of asymmetry, devoid of any preferential spatial direction and covering the whole angular range of the originally axisymmetric tip, allows attaining strong field localization for a linearly polarised mode with arbitrary orientation. Compared to previously proposed asymmetric structures which require linearly polarised excitation properly oriented with respect to the asymmetry, such a configuration enables significant simplification in mode injection. In fact, not only is the need for the delicate procedure to generate radially polarised beams overcome, but also the relative alignment between the linearly polarised beam and the tip modification is no longer critica

Fully Metal-Coated Scanning Near-Field Optical Microscopy Probes with Spiral Corrugations for Superfocusing under Arbitrarily Oriented Linearly Polarised Excitation

We study the effect of a spiral corrugation on the outer surface of a fully metal-coated scanning near-field optical microscopy (SNOM) probe using the finite element method. The introduction of a novel form of asymmetry, devoid of any preferential spatial direction and covering the whole angular range of the originally axisymmetric tip, allows attaining strong field localization for a linearly polarised mode with arbitrary orientation. Compared to previously proposed asymmetric structures which require linearly polarised excitation properly oriented with respect to the asymmetry, such a configuration enables significant simplification in mode injection. In fact, not only is the need for the delicate procedure to generate radially polarised beams overcome, but also the relative alignment between the linearly polarised beam and the tip modification is no longer critical

Playing with sizes and shapes of colloidal particles via dry etching methods

Monolayers of self-assembled quasi-spherical colloidal particles are essential building blocks in the field of materials science and engineering. More typically, they are used as a template for the fabrication of nanostructures if they serve, for instance, as a mask for deposition of new material on the surface on which particles are assembled or for etching of the material underneath; in this case, they are removed afterwards. This is what occurs in colloidal or nanosphere lithography. In some other cases, they are not used as a sacrificial material but they are incorporated in the final structure because they are inherently interesting for their properties. Independently of their specific use and application, different strategies have been devised in order to modify size and shape of colloidal particles, so as to enrich the variety of attainable patterns and to tailor the properties of the final structures and materials. In this review, we will focus on one of the most widespread methods to shape spherical colloidal particles, i.e. dry etching techniques. We will follow the development of such approaches until recent days, so as to trace an extensive panorama of the diverse parameters that can be harnessed to achieve specific morphological changes and highlight the characteristic features of the variants of this method. We will finally discuss how particles modified via dry etching can be used for patterning or can be resuspended in solvents for very diverse applications.ISSN:0001-8686ISSN:1873-372

A Journey Through the Landscapes of Small Particles in Binary Colloidal Assemblies: Unveiling Structural Transitions from Isolated Particles to Clusters upon Variation in Composition

Two-dimensional (2D) amorphous binary colloidal assemblies composed of particles of two different sizes are characterized by the loss of hexagonal close-packing for larger particles, occurring when the size ratio between small (S) and large (L) particles d S / d L exceeds a certain threshold value. For moderately low particle number ratios N S / N L large particles still retain a denser arrangement with transitions from hexagonal symmetry to the coexistence of different types of symmetries as N S / N L progressively departs from 0 to higher values. On the other hand, small particles reveal sparser arrangements: shape identification and quantification of structural transitions in small particle arrangements appear particularly challenging. In this article, we investigate their shapes and transitions for amorphous binary colloidal particles assembled at the air/water interface. For the quantitative characterization of the evolution in particle arrangements for N S / N L variable between 0.5 and 2, we develop an innovative procedure for morphological analysis, combining Minkowski functionals, Voronoi diagrams and ad hoc techniques to recognize and classify specific features. Such a powerful approach has revealed a wide variety of landscapes featuring isolated particles, dimers, chains, small clusters evolving with the colloidal suspension composition. Our method can be applied to the analysis of spatial configurations of sparse colloidal patterns obtained in different conditions

Pattern Formation in Binary Colloidal Assemblies: Hidden Symmetries in a Kaleidoscope of Structures

In this study, we present a detailed investigation of the morphology of binary colloidal structures formed by self-assembly at air/water interface of particles of two different sizes, with a size ratio such that the larger particles do not retain a hexagonal arrangement in the binary assembly. While the structure and symmetry of binary mixtures in which such hexagonal order is preserved has been thoroughly scrutinized, binary colloids in the regime of nonpreservation of the hexagonal order have not been examined with the same level of detail due also to the difficulty in finding analysis tools suitable to recognize hidden symmetries in seemingly amorphous and disordered arrangements. For this purpose, we resorted to a combination of different analysis tools based on computational geometry and computational topology to get a comprehensive picture of the morphology of the assemblies. By carrying out an extensive investigation of binary assemblies in this regime with variable concentration of smaller particles with respect to larger particles, we identify the main patterns that coexist in the apparently disordered assemblies and detect transitions in the symmetries upon increase in the number of small particles. As the concentration of small particles increases, large particle arrangements become more dilute and a transition from hexagonal to rhombic and square symmetries occurs, accompanied also by an increase in clusters of small particles; the relative weight of each specific symmetry can be controlled by varying the composition of the assemblies. The demonstration of the possibility to control the morphology of apparently disordered binary colloidal assemblies by varying experimental conditions and the definition of a route for the investigation of disordered assemblies are important for future studies of complex colloidal patterns to understand self-assembly mechanisms and to tailor the physical properties of colloidal assemblies

Self-assembly of single-sized and binary colloidal particles at air/water interface by surface confinement and water discharge

We present an innovative apparatus allowing self-assembly at air/water interface in a smooth and reproducible way. The combination of water discharge and surface confinement of the area over which self-assembly takes place allows transfer of the assembled monolayer without any risk of damage to the colloidal crystal. As we demonstrate, the designed approach offers remarkable advantages in terms of cost and robustness compared to state-of-the art methods and is suitable for the fabrication of highly ordered monolayers even for more challenging assembly experiments such as transfer on rough substrates or assembly of binary colloids. Hence, our apparatus represents a significant headway toward high scale production of large area colloidal crystals. For the binary colloid assembly experiments, we also report the first experimental demonstration of a morphology based on the alternation of three and four small particles in the interstices between large particles

Self-assembly and nanosphere lithography for large-area plasmonic patterns on graphene

Plasmonic structures on graphene can tailor its optical properties, which is essential for sensing and optoelectronic applications, e.g. for the enhancement of photoresponsivity of graphene photodetectors. Control over their structural and, hence, spectral properties can be attained by using electron beam lithography, which is not a viable solution for the definition of patterns over large areas. For the fabrication of large-area plasmonic nanostructures, we propose to use self-assembled monolayers of nanospheres as a mask for metal evaporation and etching processes. An optimized approach based on self-assembly at air/water interface with a properly designed apparatus allows the attainment of monolayers of hexagonally closely packed patterns with high long-range order and large area coverage; special strategies are devised in order to protect graphene against damage resulting from surface treatment and further processing steps such as reactive ion etching, which could potentially impair graphene properties. Therefore we demonstrate that nanosphere lithography is a cost-effective solution to create plasmonic patterns on graphene

Pattern detection in colloidal assembly: A mosaic of analysis techniques

Characterization of the morphology, identification of patterns and quantification of order encountered in colloidal assemblies is essential for several reasons. First of all, it is useful to compare different self-assembly methods and assess the influence of different process parameters on the final colloidal pattern. In addition, casting light on the structures formed by colloidal particles can help to get better insight into colloidal interactions and understand phase transitions. Finally, the growing interest in colloidal assemblies in materials science for practical applications going from optoelectronics to biosensing imposes a thorough characterization of the morphology of colloidal assemblies because of the intimate relationship between morphology and physical properties (e.g. optical and mechanical) of a material. Several image analysis techniques developed to investigate images (acquired via scanning electron microscopy, digital video microscopy and other imaging methods) provide variegated and complementary information on the colloidal structures under scrutiny. However, understanding how to use such image analysis tools to get information on the characteristics of the colloidal assemblies may represent a non-trivial task, because it requires the combination of approaches drawn from diverse disciplines such as image processing, computational geometry and computational topology and their application to a primarily physico-chemical process. Moreover, the lack of a systematic description of such analysis tools makes it difficult to select the ones more suitable for the features of the colloidal assembly under examination. In this review we provide a methodical and extensive description of real-space image analysis tools by explaining their principles and their application to the investigation of two-dimensional colloidal assemblies with different morphological characteristics.ISSN:0001-8686ISSN:1873-372