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The ability to reverse the inherent tendency of noble metals to grow in an uncontrolled three-dimensional (3D) fashion on weakly interacting substrates, including two-dimensional (2D) materials and oxides, is essential for the fabrication of high-quality multifunctional metal contacts in key enabling devices. In this study, we show that this can be effectively achieved by deploying nitrogen (N2) gas with high temporal precision during magnetron sputtering of nanoscale silver (Ag) islands and layers on silicon dioxide (SiO2) substrates. We employ real-time in situ film growth monitoring using spectroscopic ellipsometry, along with optical modeling in the framework of the finite-difference time-domain method, and establish that localized surface plasmon resonance (LSPR) from nanoscale Ag islands can be used to gauge the evolution of surface morphology of discontinuous layers up to a SiO2 substrate area coverage of ∼70%. Such analysis, in combination with data on the evolution of room-temperature resistivity of electrically conductive layers, reveals that presence of N2 in the sputtering gas atmosphere throughout all film-formation stages: (i) promotes 2D growth and smooth film surfaces and (ii) leads to an increase of the continuous-layer electrical resistivity by ∼30% compared to Ag films grown in a pure argon (Ar) ambient atmosphere. Detailed ex situ nanoscale structural analyses suggest that N2 favors 2D morphology by suppressing island coalescence rates during initial growth stages, while it causes interruption of local epitaxial growth on Ag crystals. Using these insights, we deposit Ag layers by deploying N2 selectively, either during the early precoalescence growth stages or after coalescence completion. We show that early N2 deployment leads to 2D morphology without affecting the Ag-layer resistivity, while postcoalescence introduction of N2 in the gas atmosphere further promotes formation of three-dimensional (3D) nanostructures and roughness at the film growth front. In a broader context this study generates knowledge that is relevant for the development of (i) single-step growth manipulation strategies based on selective deployment of surfactant species and (ii) real-time methodologies for tracking film and nanostructure morphological evolution using LSPR.

Nano-structuring of metals is one of the greatest challenges for the future of plasmonic and photonic devices. Such a technological challenge calls for the development of ultra-fast, high-throughput and low-cost fabrication techniques. Laser processing, accounts for the aforementioned properties, representing an unrivalled tool towards the anticipated arrival of modules based in metallic nanostructures, with an extra advantage: the ease of scalability. In the present work we take advantage of the ability to tune the laser wavelength to either match the absorption spectral profile of the metal or to be resonant with the plasma oscillation frequency, and demonstrate the utilization of different optical absorption mechanisms that are size-selective and enable the fabrication of pre-determined patterns of metal nanostructures. Thus, we overcome the greatest challenge of Laser Induced Self Assembly by combining simultaneously large-scale character with atomic-scale precision. The proposed process can serve as a platform that will stimulate further progress towards the engineering of plasmonic devices.

Conductive binary transition metal nitrides, such as TiN and ZrN, have emerged as a category of promising alternative plasmonic materials. In this work, we show that ternary transition metal nitrides such as TixTa1−xN, TixZr1−xN, TixAl1−xN, and ZrxTa1−xN share the important plasmonic features with their binary counterparts, while having the additional asset of the exceptional spectral tunability in the entire visible (400–700 nm) and UVA (315–400 nm) spectral ranges depending on their net valence electrons. In particular, we demonstrate that such ternary nitrides can exhibit maximum field enhancement factors comparable with gold in the aforementioned broadband range. We also critically evaluate the structural features that affect the quality factor of the plasmon resonance and we provide rules of thumb for the selection and growth of materials for nitride plasmonics.

CMOS-compatible, refractory conductors are emerging as the materials that will advance novel concepts into real, practical plasmonic technologies. From the available pallet of materials, those with negative real permittivity at very short wavelengths are extremely rare; importantly they are vulnerable to oxidationupon exposure to far UV radiationand nonrefractory. Epitaxial, substoichiometric, cubic MoN (B1-MoNx) films exhibit resistivity as low as 250 cm and negative real permittivity for experimental wavelengths as short as 155 nm, accompanied with unparalleled chemical and thermal stability, are reported herein. Finite-difference time domain calculations suggest that B1-MoNx operates as an active plasmonic element deeper in the UV (100-200 nm) than any other known material, apart from Al, while being by far more stable and abundant than any other UV plasmonic conductor. Unexpectedly, the unique optical performance of B1-MoNx is promoted by nitrogen vacancies, thus changing the common perception on the role of defects in plasmonic materials.

Laser nanostructuring of pure ultrathin metal layers or ceramic/metal composite thin films has emerged as a 15 promising route for the fabrication of plasmonic patterns with applications in information storage, cryptography, and security tagging. However, the environmental sensitivity of pure Ag layers and the complexity of ceramic/metal composite film growth hinder the implementation of this technology to largescale production, as well as its combination with flexible substrates. In the present work we investigate an alternative pathway, namely, starting from non-plasmonic multilayer metal/dielectric layers, whose growth is 20 compatible with large scale production such as in-line sputtering and roll-to-roll deposition, which are then transformed into plasmonic templates by single-shot UV-laser annealing (LA). This entirely cold, large-scale process leads to a subsurface nanoconstruction involving plasmonic Ag nanoparticles embedded in a hard and inert dielectric matrix on top of both rigid and flexible substrates. The subsurface encapsulation of Ag nanoparticles provides durability and long-term stability, while the cold character of LA suits the use of 25 sensitive flexible substrates. The morphology of the final composite film depends primarily on the

We review different technologies and architectures for neuromorphic photonic accelerators, spanning from bulk optics to photonic-integrated-circuits (PICs), and assess compute efficiency in OPs/Watt through the lens of a comparative study where key technology aspects are analyzed. With an emphasis on PIC neuromorphic accelerators, we shed light onto the latest advances in photonic and plasmonic modulation technologies for the realization of weighting elements in training and inference applications, and present a recently introduced scalable coherent crossbar layout. Finally, we stress that current technologies face challenges endowing photonic accelerators with compute efficiencies in the PetaOPs/W, and discuss future implementation pathways towards improving performance.

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