Mechanically Tunable Lattice-Plasmon Resonances by Templated Self-Assembled Superlattices for Multi-Wavelength Surface-Enhanced Raman Spectroscopy.

Lattice plasmons, i.e., diffractively coupled localized surface plasmon resonances, occur in long-range ordered plasmonic nanostructures such as 1D and 2D periodic lattices. Such far-field coupled resonances can be employed for ultrasensitive surface-enhanced Raman spectroscopy (SERS), provided they are spectrally matched to the excitation wavelength. The spectral positions of lattice plasmon modes critically depend on the lattice period and uniformity, owing to their pronounced sensitivity to structural disorder. We report the fabrication of superlattices by templated self-assembly of gold nanoparticles on a flexible support, with tunable lattice-plasmon resonances by means of macroscopic strain. We demonstrate that the highest SERS performance is achieved by matching the lattice plasmon mode to the excitation wavelength, by post-assembly fine-tuning of long-range structural parameters. Both asymmetric and symmetric lattice deformations can be used to adapt a single lattice structure to both red-shifted and blue-shifted excitation lines, as exemplified by lattice expansion and contraction, respectively. This proof-of-principle study represents a basis for alternative designs of adaptive functional nanostructures with mechanically tunable lattice resonances using strain as a macroscopic control parameter.

Hydroxypropyl Cellulose Adhesives for Transfer Printing of Carbon Nanotubes and Metallic Nanostructures.

Transfer printing is one of the key nanofabrication techniques for the large-scale manufacturing of complex device architectures. It provides a cost-effective and high-throughput route for the integration of independently processed materials into spatially tailored architectures. Furthermore, this method enables the fabrication of flexible and curvilinear devices, paving the way for the fabrication of a new generation of technologies for optics, electronics, and biomedicine. In this work, hydroxypropyl cellulose (HPC) membranes are used as water soluble adhesives for transfer printing processes with improved performance and versatility compared to conventional silicone alternatives. The high-water solubility and excellent mechanical properties of HPC facilitate transfer printing with high yield for both metal and carbon nanotubes (CNTs) inks. In the case of metal inks, crack-free stripping of silver films and the simple fabrication of Moiré Plasmonic architectures of different geometries are demonstrated. Furthermore, HPC membranes are used to transfer print carbon nanotube films with different thicknesses and up to 77% transparency in the visible and near infrared region with potential applications as transparent conductive substrates. Finally, the use of prepatterned HPC membranes enables nanoscale patterning of CNT with feature resolution down to 1 µm.

Templated-Assembly of CsPbBr3 Perovskite Nanocrystals into 2D Photonic Supercrystals with Amplified Spontaneous Emission.

Perovskite nanocrystals (NCs) have revolutionized optoelectronic devices because of their versatile optical properties. However, controlling and extending these functionalities often requires a light-management strategy involving additional processing steps. Herein, we introduce a simple approach to shape perovskite nanocrystals (NC) into photonic architectures that provide light management by directly shaping the active material. Pre-patterned polydimethylsiloxane (PDMS) templates are used for the template-induced self-assembly of 10 nm CsPbBr3 perovskite NC colloids into large area (1 cm2 ) 2D photonic crystals with tunable lattice spacing, ranging from 400 nm up to several microns. The photonic crystal arrangement facilitates efficient light coupling to the nanocrystal layer, thereby increasing the electric field intensity within the perovskite film. As a result, CsPbBr3 2D photonic crystals show amplified spontaneous emission (ASE) under lower optical excitation fluences in the near-IR, in contrast to equivalent flat NC films prepared using the same colloidal ink. This improvement is attributed to the enhanced multi-photon absorption caused by light trapping in the photonic crystal.

Tunable index metamaterials made by bottom-up approaches.

Despite the exciting optical properties metamaterials exhibit, their implementation in technology is being hampered nowadays by the inherent losses of their metal constituents and the expensive and low-throughput procedures used. As an alternative, we present a new design of double fishnet metamaterials that can be easily realized combining two inexpensive and up-scalable techniques: nanosphere lithography and metallic electrodeposition. A monolayer of polystyrene spheres is used as a template for the infiltration of two symmetric gold layers separated by an air gap. The effective refractive index of the metamaterial can be easily tuned by the appropriate choice of the diameter of the spheres and the gap width between the metallic layers, varying its value from positive to negative. The good agreement between optical measurements and finite-difference time-domain simulations confirms the success of our process. Fishnet metamaterials with refractive index going from 1.5 until -1.0 in the near infrared range are demonstrated and the key parameters for these architectures provided.

Gold Nanoparticle Plasmonic Superlattices as Surface-Enhanced Raman Spectroscopy Substrates.

Metal colloids are of great interest in the field of nanophotonics, mainly due to their morphology-dependent optical properties, but also because they are high-quality building blocks for complex plasmonic architectures. Close-packed colloidal supercrystals not only serve for investigating the rich plasmonic resonances arising in strongly coupled arrangements but also enable tailoring the optical response, on both the nano- and the macroscale. Bridging these vastly different length scales at reasonable fabrication costs has remained fundamentally challenging, but is essential for applications in sensing, photovoltaics or optoelectronics, among other fields. We present here a scalable approach to engineer plasmonic supercrystal arrays, based on the template-assisted assembly of gold nanospheres with topographically patterned polydimethylsiloxane molds. Regular square arrays of hexagonally packed supercrystals were achieved, reaching periodicities down to 400 nm and feature sizes around 200 nm, over areas up to 0.5 cm2. These two-dimensional supercrystals exhibit well-defined collective plasmon modes that can be tuned from the visible through the near-infrared by simple variation of the lattice parameter. We present electromagnetic modeling of the physical origin of the underlying hybrid modes and demonstrate the application of superlattice arrays as surface-enhanced Raman scattering (SERS) spectroscopy substrates which can be tailored for a specific probe laser. We therefore investigated the influence of the lattice parameter, local degree of order, and cluster architecture to identify the optimal configuration for highly efficient SERS of a nonresonant Raman probe with 785 nm excitation.

Ultrathin Semiconductor Superabsorbers from the Visible to the Near-Infrared.

The design of ultrathin semiconducting materials that achieve broadband absorption is a long-sought-after goal of crucial importance for optoelectronic applications. To date, attempts to tackle this problem consisted either of the use of strong-but narrowband-or broader-but moderate-light-trapping mechanisms. Here, a strategy that achieves broadband optimal absorption in arbitrarily thin semiconductor materials for all energies above their bandgap is presented. This stems from the strong interplay between Brewster modes, sustained by judiciously nanostructured thin semiconductors on metal films, and photonic crystal modes. Broadband near-unity absorption in Ge ultrathin films is demonstrated, which extends from the visible to the Ge bandgap in the near-infrared and is robust against angle of incidence variation. The strategy follows an easy and scalable fabrication route enabled by soft nanoimprinting lithography, a technique that allows seamless integration in many optoelectronic fabrication procedures.

Scattering of graphene plasmons by defects in the graphene sheet.

A theoretical study is presented on the scattering of graphene surface plasmons (GSPs) by defects in the graphene sheet they propagate in. These defects can be either natural (as domain boundaries, ripples, and cracks, among others) or induced by an external gate. The scattering is shown to be governed by an integral equation, derived from a plane wave expansion of the fields, which in general must be solved numerically, but it provides useful analytical results for small defects. Two main cases are considered: smooth variations of the graphene conductivity (characterized by a Gaussian conductivity profile) and sharp variations (represented by islands with different conductivity). In general, reflection largely dominates over radiation out of the graphene sheet. However, in the case of sharply defined conductivity islands, there are some values of island size and frequency where the reflectance vanishes and, correspondingly, the radiation out-of-plane is the main scattering process. For smooth defects, the reflectance spectra present a single maximum at the condition k(p)a ≈ √2, where k(p) is the GSP wavevector and a is the spatial width of the defect. In contrast, the reflectance spectra of sharp defects present periodic oscillations with period k(p)'a, where k(p)' is the GSP wavelength inside the defect. Finally, the case of cracks (gaps in the graphene conductivity) is considered, showing that the reflectance is practically unity for gap widths larger than one-tenth of the GSP wavelength.

Hybridization induced transparency in composites of metamaterials and atomic media.

We report hybridization induced transparency (HIT) in a composite medium consisting of a metamaterial and a dielectric. We develop an analytic model that explains HIT by coherent coupling between the hybridized local fields of the metamaterial and the dielectric or an atomic system in general. In a proof-of-principle experiment, we evidence HIT in a split ring resonator metamaterial that is coupled to α-lactose monohydrate. Both, the analytic model and numerical calculations confirm and explain the experimental observations. HIT can be considered as a hybrid analogue to electromagnetically induced transparency (EIT) and plasmon-induced transparency (PIT).

Toy model for plasmonic metamaterial resonances coupled to two-level system gain.

We propose, solve, and discuss a simple model for a metamaterial incorporating optical gain: A single bosonic resonance is coupled to a fermionic (inverted) two-level-system resonance via local-field interactions. For given steady-state inversion, this model can be solved analytically, revealing a rich variety of (Fano) absorption/gain lineshapes. We also give an analytic expression for the fixed inversion resulting from gain pinning under steady-state conditions. Furthermore, the dynamic response of the "lasing SPASER", i.e., its relaxation oscillations, can be obtained by simple numerical calculations within the same model. As a result, this toy model can be viewed as the near-field-optical counterpart of the usual LASER rate equations.