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Nanofabrication of flat optic silica gratings conformally layered with two-dimensional (2D) MoS2 is demonstrated over large area (cm2), achieving a strong amplification of the photon absorption in ...

Bidirectional nanoantennas are of key relevance for advanced functionalities to be implemented at the nanoscale, and in particular for color routing in an ultracompact flat-optics configuration. Here we demonstrate a novel approach avoiding complex collective geometries and/or restrictive morphological parameters, based on cross-polarized detuned plasmonic nanoantennas in a uniaxial (quasi-1D) bimetallic configuration. The nanofabrication of such a flat-optics system is controlled over a large-area (cm^2) by a novel self-organized technique exploiting ion-induced nanoscale wrinkling instability on glass templates to engineer tilted bimetallic nanostrip dimers. These nanoantennas feature broadband color routing with superior light scattering directivity figures, which are well described by numerical simulations and turn out to be competitive with the response of lithographic nanoantennas. These results demonstrate that our large-area self-organized metasurfaces can be implemented in real world applications of flat optics color routing from telecom photonics to optical nanosensing., 25+8 pages, 5+4 figures

Substrates with engineered roughness are studied with the aim of achieving broadband and omnidirectional photon harvesting in thin film devices. Light coupling across the interfaces of a photonic device is induced by uniaxial pseudo-periodic gratings formed in a self-organised fashion via de-focused ion beam sputtering (IBS). The optical properties of the textured interfaces are assessed both experimentally and numerically using finite difference time domain (FDTD) algorithm, quantitatively demonstrating the optimal geometries which favour broadband diffuse scattering of radiation across the Vis-NIR spectral range. Thin film amorphous silicon solar cells based on the nanostructured patterns have been numerically studied via FDTD to assess absorption enhancement in comparison to flat reference devices, finding a 25% increase of short-circuit current, in good agreement with the experiment. Similar light trapping experiments performed on prototypical solar cells employing a PTB7:PC61BM organic absorber, allow to extend the general validity of the results to a relevant class of materials in the view of photovoltaic applications.

Flat-optics microfluidic sensor based on one-dimensional (1D) Au nanostrip lattices are homogeneously fabricated over large area (cm2), demonstrating a cost-effective approach able to combine scala...

Plasmonic metasurfaces based on quasi-one-dimensional (1D) nanostripe arrays are homogeneously prepared over large-area substrates (cm2), exploiting a novel self-organized nanofabrication method. Glass templates are nanopatterned by ion beam-induced anisotropic nanoscale wrinkling, enabling the maskless confinement of quasi-1D arrays of out-of-plane tilted gold nanostripes, behaving as transparent wire-grid polarizer nanoelectrodes. These templates enable the dichroic excitation of localized surface plasmon resonances, easily tunable over a broadband spectrum from the visible to the near- and mid-infrared, by tailoring the nanostripes’ shape and/or changing the illumination conditions. The controlled self-organized method allows the engineering of the nanoantennas’ morphology in the form of Au-SiO2-Au nanostripe dimers, which show hybridized plasmonic resonances with enhanced tunability. Under this condition, superior near-field amplification is achievable for the excitation of the hybridized magnetic dipole mode, as pointed out by numerical simulations. The high efficiency of these plasmonic nanoantennas, combined with the controlled tuning of the resonant response, opens a variety of applications for these cost-effective templates, ranging from biosensing and optical spectroscopies to high-resolution molecular imaging and nonlinear optics.

We report on the optical photomodulation properties of all-polymer planar microcavities in which the photochromic poly((4-pentyloxy-3’-methyl-4’-(6-methacryloxyhexyloxy))azobenzene) (PMA4) acts as photoresponsive cavity layer. We induce the trans-cis isomerization process of the azobenzene group by polarized 405 nm CW-laser irradiation, while the backward process is driven by unpolarized CW-laser irradiation at 442 nm. The all-optical photoisomerization process induces a remarkable in-plane anisotropic spectral shift of the cavity modes for the first and second order photonic band gaps. The spectral and intensity modulation effects for these flexible all-polymer microcavities are discussed with respect to those so far reported in literature for analogous systems.

The lack of cost-effective systems for the assessment of air pollutants is a concern for health and safety in urban and industrial areas. The use of polymer thin films as label-free colorimetric sensors featuring specific interactions with pollutants would then represent a paradigm shift in environmental monitoring and packaging technologies, allowing to assess air quality, formation of byproducts in closed environment, and the barrier properties of the polymers. To this end, all-polymer distributed Bragg reflectors represent a promising approach toward a reliable and cost-effective transduction of chemical stimuli and effective colorimetric label-free selective detectors. We show selectivity attained by specific interactions between the polymer and analytes. Such interactions drive the analyte intercalation through the polymer structure and its kinetics, converting it in a dynamic optical response which is at the basis of the Flory-Huggins photonic sensors. The multivariate analyses of the response kinetics also allow distinguishing binary mixtures. Additionally, we demonstrate that such optical responses can be used to esteem the diffusion coefficients of small molecules within polymer media via simple UV-vis spectroscopy retrieving data comparable to those obtained with state-of-the-art gravimetric procedures. Last, we assess the figures of merit of the sensors in terms of lower detection limit, sensitivity, and reversibility, demonstrating that such devices can pave the way to an innovative, simple, and low-cost detection method integrable to in situ assessment of barrier polymers used for the encapsulation of optoelectronic devices, food packaging, and goods storage in general.

Pentacene is known to grow on isotropic silicon oxide surfaces in a substrate-induced phase with fiber textured crystallites. This growth study reports on the growth of pentacene crystallites on uniaxially oriented surfaces. Silica substrates have been treated by ion beam sputtering so that ripples with a lateral corrugation length of 38 nm and a surface roughness of 1.3 nm are formed. Pentacene thin films with a nominal thickness in the range from 20 nm up to 300 nm are deposited on top of the rippled surfaces. The films are characterized by atomic force microscopy and grazing incidence X-ray diffraction. Bi-axially oriented crystals are formed due to the grooves of the substrate surface opening up the possibility of a defined in-plane alignment of the crystals. In a first stage of thin film growth, the thin film phase (TFP) of pentacene is formed, while in the later stage the bulk crystal structure (C, Campbell phase) also appears. Due to the bi-axial alignment of the crystallites the transition from the thin film phase to the bulk crystal structure can be directly investigated. An epitaxial relationship with (1 2 0)TFP || (2 1 0)C and [−2 1 0]TFP ||[1 −2 0]C is observed which can be explained by an adaption of the herringbone layers of both crystal structures. This work reveals one possible microscopic mechanism for the transition from the metastable substrate-induced phase of pentacene to its equilibrium bulk structure.

Pattern formation induced by wrinkling is a very common phenomenon exhibited in soft-matter substrates. In all these systems wrinkles develop in presence of compressively stressed thin films lying on compliant substrates. Here we demonstrate the controlled growth of self-organized nanopatterns exploiting a wrinkling instability on a solid-state substrate. Soda-lime glasses are modified in the surface layers by a defocused ion beam which triggers the formation of a compressively stressed surface layer deprived of alkali ions. When the substrate is heated up near its glass transition temperature, the wrinkling instability boosts the growth rate of the pattern by about two orders of magnitude. High aspect ratio anisotropic ripples bound by faceted ridges are thus formed which represent an optimal template for guiding the growth of large area arrays of functional nanostructures. We demonstrate the engineering over large square cm areas of quasi-1D arrays of Au nanostripe dimers endowed with tunable plasmonic response, strong optical dichroism and high electrical conductivity. These peculiar functionalities allow to exploit these large area substrates as active metamaterials in nanophotonics, biosensing and optoelectronics., Comment: Manuscript: 18 pages, 4 figures. Supporting Info: 6 pages, 5 figures

MoS2 and generally speaking, the wide family of transition-metal dichalcogenides represents a solid nanotechnology platform on which to engineer a wealth of new and outperforming applications involving 2D materials. An even richer flexibility can be gained by extrinsically inducing an in-plane shape anisotropy of the nanosheets. Here, the synthesis of anisotropic MoS2 nanosheets is proposed as a prototypical example in this respect starting from a highly conformal chemical vapor deposition on prepatterend substrates and aiming at the more general purpose of tailoring anisotropy of 2D nanosheets by design. This is envisioned to be a suitable configuration for strain engineering as far as strain can be spatially redistributed in morphologically different regions. With a similar approach, both the optical and electronic properties of the 2D transition-metal dichalcogenides can be tailored over macroscopic sample areas in a self-organized fashion, thus paving the way for new applications in the field of optical metasurfaces, light harvesting, and catalysis.

The engineering of self-organized plasmonic metasurfaces is demonstrated using a maskless technique with defocused ion-beam sputtering and kinetically controlled deposition. The proposed reliable, cost-effective, and controllable approach enables large-area (order of square centimeter) sub-wavelength periodic patterning with close-packed gold nanostrips. A multi-level variant of the method leads to high-resolution manufacturing of vertically stacked nanostrip dimer arrays, without resorting to lithographic approaches. The design of these self-organized metasurfaces is optimized by employing plasmon hybridization methods. In particular, preliminary results on the so-called gap-plasmon configuration of the nanostrip dimers, implementing magnetic dipole resonance in the near-infrared range, are reported. This resonance offers a superior sensitivity and field enhancement, compared with the more conventional electric dipole resonance. The translational invariance of the nanostrip configuration leads to a high filling factor of the hot spots. These advanced features make the large-area metasurface based on gap-plasmon nanostrip dimers very attractive for surface-enhanced linear and nonlinear spectroscopy (e.g., surface-enhanced Raman scattering) and plasmon-enhanced photon harvesting in solar and photovoltaic cells. [Figure not available: see fulltext.].

Two-dimensional transition metal dichalcogenide (MX 2 ) are receiving lot of attention in recent years due to their excellent electronic and optical properties which make them feasible for advanced photonics applications [1]. In particular Molybdenum-Disulfide (MoS 2 ) has shown large exciton binding energy, strong spin-orbit interaction, and high carrier mobilities.

We present a self-organizedmethod based on defocused ion beamsputtering for nanostructuring glass substrates which feature antireflective and light trapping effects. By irradiating the substrate, capped with a thin gold (Au) film, a self-organized Au nanowire stencil mask is firstly created. The morphology of the mask is then transferred to the glass surface by further irradiating the substrate, finally producing high aspect ratio, uniaxial ripple-like nanostructures whose morphological parameters can be tailored by varying the ion fluence. The effect of a Ti adhesion layer, interposed between glass and Au with the role of inhibiting nanowire dewetting, has also been investigated in order to achieve an improved morphological tunability of the templates. Morphological and optical characterization have been carried out, revealing remarkable light trapping performance for the largest ion fluences. The photon harvesting capability of the nanostructured glass has been tested for different preparation conditions by fabricating thin film amorphous Si solar cells. The comparison of devices grown on textured and flat substrates reveals a relative increase of the short circuit current up to 25%. However, a detrimental impact on the electrical performance is observed with the rougher morphologies endowed with steep v-shaped grooves. We finally demonstrate that post-growth ion beam restructuring of the glass template represents a viable approach toward improved electrical performance. © 2017 by the authors.

Manipulating the anisotropy in 2D nanosheets is a promising way to tune or trigger functional properties at the nanoscale. Here, a novel approach is presented to introduce a one-directional anisotropy in MoS2 nanosheets via chemical vapor deposition (CVD) onto rippled patterns prepared on ion-sputtered SiO2 /Si substrates. The optoelectronic properties of MoS2 are dramatically affected by the rippled MoS2 morphology both at the macro- and the nanoscale. In particular, strongly anisotropic phonon modes are observed depending on the polarization orientation with respect to the ripple axis. Moreover, the rippled morphology induces localization of strain and charge doping at the nanoscale, thus causing substantial redshifts of the phonon mode frequencies and a topography-dependent modulation of the MoS2 workfunction, respectively. This study paves the way to a controllable tuning of the anisotropy via substrate pattern engineering in CVD-grown 2D nanosheets.

Self-organized nanowire arrays are confined by glancing-angle Au deposition on nanopatterned glass templates prepared by ion beam sputtering. The semi-transparent 1D nanowire arrays are extended over large cm2 areas and are endowed with excellent electrical conductivity competitive with the best transparent conductive oxides (sheet resistance in the range of 5-20 Ohm sq-1). In addition, the nanowires support localized surface plasmon (LSP) resonances, which are easily tunable into the visible and near infrared spectrum and are selectively excited with incident light polarized perpendicularly to the wires. Such substrates, thus, behave as multifunctional nanoelectrodes, which combine good optoelectronic performance with dichroic plasmonic excitation. The electrical percolation process of the Au nanoelectrodes was monitored in situ during growth at glancing angle, both on flat and nanopatterned glass templates. In the first case, we observed a universal scaling of the differential percolation rate, independently of the glancing deposition angle, while deviations from the universal scaling were observed when Au was confined on nanopatterned templates. In the latter case, the pronounced shadowing effect promotes the growth of locally connected 1D Au nanosticks on the 'illuminated' ripple ridges, thus, introducing strong anisotropies with respect to the case of a 2D percolating network.

A tetrairon(III) single-molecule magnet is deposited using a thermal evaporation technique in high vacuum. The chemical integrity is demonstrated by time-of-flight secondary ion mass spectrometry on a film deposited on Al foil, while superconducting quantum interference device magnetometry and alternating current susceptometry of a film deposited on a kapton substrate show magnetic properties identical to the pristine powder. High-frequency electron paramagnetic resonance spectra confirm the characteristic behavior for a system with S = 5 and a large Ising-type magnetic anisotropy. All these results indicate that the molecules are not damaged during the deposition procedure keeping intact the single-molecule magnet behavior.