Si1-xGex nanoantennas with a tailored Raman response and light-to-heat conversion for advanced sensing applications.

Active light-emitting all-dielectric nanoantennas recently have demonstrated great potential as highly efficient nanoscale light sources owing to their strong luminescent and Raman responses. However, their large-scale fabrication faces a number of problems related to productivity limits of existing lithography techniques. Thus, high-throughput fabrication strategies allowing in a facile way to tailor of the nanoantenna emission and thermal properties in the process of their fabrication are highly desirable for various applications. Here, we propose a cost-effective approach to large-scale fabrication of Si1-xGex alloyed Mie nanoresonators possessing an enhanced inherent Raman response which can be simply tailored via tuning the Ge concentration. Moreover, by tailoring the relative Ge composition one can gradually change a complex refractive index of the produced Si1-xGex alloy, which affects the ratio between radiative and nonradiative losses in Si1-xGex nanoantennas, which is crucial for optimization of their optical heating efficiency. Composition-tunable Si1-xGex nanoantennas with an optimized size, light-to-heat conversion and Raman response are implemented for non-invasive sensing of 4-aminothiophenol molecules with a temperature feedback modality and high subwavelength spatial resolution. The results are important for advanced multichannel optical sensing, providing information on analyte's composition, analyte-nanoantenna temperature response and spatial position.

Ordered arrays of Au catalysts by FIB assisted heterogeneous dewetting.

Synthesizing Au0.8Si0.2 nanocatalysts that are homogeneous in size and have controlled position is becoming a challenging and crucial prequisite for the fabrication of ordered semiconductor nanowires. In this study, Au0.8Si0.2 nanocatalysts are synthesized via dewetting of Au layers on Si(111) during thermal annealing in an ultra-high vacuum. In the first part of the paper, the mechanism of homogeneous dewetting is analyzed as a function of the Au-deposited thickness (h Au). We distinguish three different dewetting regimes: (I) for a low thickness ([Formula: see text]), a submonolyer coverage of Au is stabilized and there is no dewetting. (II) For an intermediate thickness ([Formula: see text]), there is both dewetting and Au0.8Si0.2 phase formation. The size and density of the Au0.8Si0.2 clusters are directly related to h Au. When cooling down to room temperature, the clusters decompose and reject the Si at the Au/Si substrate interface. (III) For a large thickness ([Formula: see text]), only dewetting takes place, without forming AuSi clusters. In this regime, the dewetting is kinetically controlled by the self-diffusion of Au (activation energy ∼0.43 eV) without evidence of an Si-alloying effect. As a practical consequence, when relying solely on the homogeneous dewetting of Au/Si(111) to form the Au0.8Si0.2 catalysts (without a supply of Si atoms from vapor), regime II should be used to obtain good size and density control. In the second part of the paper, a process for ordering the catalysts using focused ion beam-(FIB) assisted dewetting (heterogeneous dewetting) is developed. We show that no matter what the FIB milling conditions and the Au nominal thickness are, dewetting is promoted by ion beam irradiation and is accompanied by the formation of Au0.8Si0.2 droplets. The droplets preferentially form on the patterned areas, while in similar annealing conditions, they do not form on the unpatterned areas. This behavior is attributed to the larger Au-Si interdiffusion in the patterned areas, which results from the Si amorphization induced by the FIB. A systematic analysis of the position of the nanodroplets shows their preferential nucleation inside the patterns, while thicker platelets of almost pure Au are observed between the patterns. The evolutions of the size homogeneity and the occupancy rate of the patterns are quantified as a function of the FIB dose and annealing temperature. Nice arrays of perfectly ordered AuSi catalysts are obtained after optimizing the FIB and dewetting conditions.