We report on the fabrication and optical characterization of a new hybrid material consisting of Nd3+ doped Y2O3 submicron particles associated with linear chains of plasmonic nanostructures. By drop-casting deposition, single Nd3+ doped Y2O3 polycrystalline particles are dispersed and located in the vicinities of plasmonic chains of silver nanoparticles formed on the surface a LiNbO3 substrate. The interaction between the plasmonic modes of the chain with the fluorescent yttria submicron particles is analyzed by micro-luminescence experiments. Orthogonal polarization configurations of the excitation radiation, namely, perpendicular and parallel to plasmonic chain axis, are employed to study the effect of the longitudinal and transverse chain plasmonic modes on the luminescence of the particles. A remarkable dependence of the emission intensity of the Nd3+:Y2O3 submicron particles on the excitation polarization is observed, showing the capability of plasmonic chains to modulate the emission of fluorescent submicron particles in contact with the chain. Numerical simulations evidence a different distribution of the excitation radiation field within the Nd3+:Y2O3 particle depending on the type of excited plasmonic mode, longitudinal or transversal, of the chain, and hence, the ability of plasmonic chains for controlling the emission of Rare Earth doped submicron particles.

The association of 2D materials and ferroelectrics offers a promising approach to tune the optoelectronic properties of atomically thin Transition Metal Dichalcogenides (TMDs). In this work, the combined effect of ferroelectricity and light on the optoelectronic properties of monolayer (1L)-MoS2 deposited on periodically poled lithium niobate crystals is explored. Using scanning micro-photoluminescence, the effect of excitation intensity, scanning direction, and domain walls on the 1L-MoS2 photoluminescence properties is analyzed, offering insights into charge modulation of MoS2. The findings unveil a photoinduced charging process dependent on the ferroelectric domain orientation, in which light induces charge generation and transfer at the monolayer-substrate interface. This highlights the substantial role of light excitation in ferroelectrically-driven electrostatic doping in MoS2. Additionally, the work provides insights into the effect of the strong, nanometrically confined electric fields on LiNbO3 domain wall surfaces, demonstrating precise control over charge carriers in MoS2, and enabling the creation of deterministic p-n homojunctions with exceptional precision. The results suggest prospects for novel optoelectronic and photonic application involving monolayer TMDs by combining light-matter interaction processes and the surface selectivity provided by ferroelectric domain structures.

The current need for coherent light sources for integrated (nano)photonics motivates the search for novel laser designs emitting at technologically relevant wavelengths with high‐frequency stability and low power consumption. Here, a new monolithic architecture that integrates monolayer MoS2 and chains of silver nanoparticles on a rare‐earth (Nd3+) doped LiNbO3 platform is developed to demonstrate Q‐switched lasing operation at the nanoscale. The localized surface plasmons provided by the nanoparticle chains spatially confine the gain generated by Nd3+ ions at subwavelength scales, and large‐area monolayer MoS2 acts as saturable absorber. As a result, an ultra‐compact coherent pulsed light source delivering stable train pulses with repetition rates of hundreds of kHz and pulse duration of 1 µs is demonstrated without the need of any voltage‐driven optical modulation. Moreover, the monolithic integration of the different elements is achieved without sophisticated processing, and it is compatible with LiNbO3‐based photonics. The results highlight the robustness of the approach, which can be extended to other 2D materials and solid‐state gain media. Potential applications in communications, quantum computing, or ultra‐sensitive sensing can benefit from the synergy of the materials involved in this approach, which provides a wealth of opportunities for light control at reduced scales.

Plasmonic waveguides have been shown to be a promising approach to confine and transport electromagnetic energy beyond the diffraction limit. However, ohmic losses generally prevent their integration at micrometric or millimetric scales. Here, we present a gain-compensated plasmonic waveguide based on the integration of linear chains of Ag nanoparticles on an optically active Nd3+-doped solid-state gain medium. By means of dual confocal fluorescence microscopy, we demonstrate long-range optical energy propagation due to the near-field coupling between the plasmonic nanostructures and the Nd3+ ions. The subwavelength fluorescence guiding is monitored at distances of around 100 µm from the excitation source for two different emission ranges centered at around 900 nm and 1080 nm. In both cases, the guided fluorescence exhibits a strong polarization dependence, consistent with the polarization behavior of the plasmon resonance supported by the chain. The experimental results are interpreted through numerical simulations in quasi-infinite long chains, which corroborate the propagation features of the Ag nanoparticle chains at both excitation (λexc = 590 nm) and emission wavelengths. The obtained results exceed by an order of magnitude that of previous reports on electromagnetic energy transport using linear plasmonic chains. The work points out the potential of combining Ag nanoparticle chains with a small interparticle distance (~2 nm) with rare-earth-based optical gain media as ultra-long-range waveguides with extreme light confinement. The results offer new perspectives for the design of integrated hybrid plasmonic–photonic circuits based on rare-earth-activated solid-state platforms.

The association of plasmonic nanostructures with nonlinear dielectric systems has been shown to provide useful platforms for boosting frequency conversion processes at metal-dielectric interfaces. Here, we report on an efficient route for engineering light–matter interaction processes in hybrid plasmonic-χ(2) dielectric systems to enhance second harmonic generation (SHG) processes confined in small spatial regions. By means of ferroelectric lithography, we have fabricated scalable micrometric arrangements of interacting silver nanoparticles compactly distributed on hexagonal regions. The fabricated polygonal microstructures support both localized and extended plasmonic modes, providing large spatial regions of field enhancement at the optical frequencies involved in the SHG process. We experimentally demonstrate that the resonant excitation of the plasmonic modes supported by the Ag nanoparticle-filled hexagons in the near infrared region produces an extraordinary 104-fold enhancement of the blue second harmonic intensity generated in the surface of a LiNbO3 crystal. The results open new perspectives for the design of efficient hybrid plasmonic frequency converters in miniaturized devices.

Plasmonic structures have been revealed as efficient units to enhance localized nonlinear phenomena generated at dielectric-metal interfaces. However, their effect on the nonlinear interactions provided by quasi-phase matching processes in AP modulated dielectric crystals have been scarcely addressed, mainly due to the complexity in manufacturing appropriate periodic plasmonic structures overlying the chi((2)) dielectric structure. Here, by a simple method we have fabricated a periodic structure based on the combination of two commensurate lattices: a periodic lattice of chains of Ag nanoparticles and a periodic lattice of chi((2))-modulation based on a ferroelectric domains structure. The hybrid system supports multiple surface plasmon lattice resonances (SLRs) at the technologically relevant NIR spectral region, which yield the enhancement of the nonlinear diffraction pattern generated by the chi((2)) structure. The superposition of the plasmonic and the chi((2))-modulation lattice results in a 20-fold enhancement of the directional SHG due to the excitation of SLRs by the interacting waves involved in the nonlinear process. The results are obtained in lithium niobate, a widely used crystal in optoelectronics, and demonstrate the potential of the approach to design integrated solid-state platforms for on-chip optical steering, multiplexing or quantum technologies.

Controlling the coherence properties of rare earth emitters in solid-state platforms in the absence of an optical cavity is highly desirable for quantum light-matter interfaces and photonic networks. Here, we demonstrate the possibility of generating directional and spatially coherent light from Nd3+ ions coupled to the longitudinal plasmonic mode of a chain of interacting Ag nanoparticles. The effect of the plasmonic chain on the Nd3+ emission is analyzed by Fourier microscopy. The results reveal the presence of an interference pattern in which the Nd3+ emission is enhanced at specific directions, as a distinctive signature of spatial coherence. Numerical simulations corroborate the need of near-field coherent coupling of the emitting ions with the plasmonic chain mode. The work provides fundamental insights for controlling the coherence properties of quantum emitters at room temperature and opens new avenues towards rare earth based nanoscale hybrid devices for quantum information or optical communication in nanocircuits.

Controlling and manipulating light-matter interaction phenomena at the nanoscale leads to a variety of fascinating effects that are currently the focus of an intense research from both a fundamental and technological perspectives. In this talk, I will summarize the most recent advances on the fabrication and performance features of coherent light sources operating at the nanoscale, which are attained by the interaction of localized surface plasmons with optical gain nonlinear dielectric media [1]. The optical gain is provided by functional ferroelectric platforms, either by stimulated emission [2] or by nonlinear frequency conversion processes [3]. The mechanisms responsible for the intensification of the radiation–matter interaction processes are discussed in each case.

Coherent light sources providing sub-wavelength confined modes are in ever more demand to face new challenges in a variety of disciplines. Scalability and cost-effective production of these systems are also highly desired. The use of ferroelectrics in functional optical platforms, on which plasmonic arrangements can be formed, is revealed as a simple and powerful method to develop coherent light sources with improved and novel functionalities at the nanoscale. Two types of sources with sub-diffraction spatial confinement and improved performances are presented: i) plasmon-assisted solid-state nanolasers based on the interaction between metallic nanostructures and optically active rare earth doped ferroelectric crystals and ii) nonlinear radiation sources based on quadratic frequency mixing processes that are enhanced by means of localized surface plasmon (LSP) resonances. The mechanisms responsible for the intensification of the radiation-matter interaction processes by LSP resonances are discussed in each case. The challenges, potential applications, and future perspectives of the field are highlighted.

The association of metallic nanostructures and solid-state gain media has recently led to the emergence of functional platforms for nanolasing with relevant features such as chemical and thermal stability and the absence of photobleaching. In this work, we demonstrate that the incorporation of plasmonic nanoparticle chains on a Nd3+-doped solid-state laser platform enables nanoscale laser emission at the technologically relevant spectral region of telecom (lambda(e) = 1385 nm), outside the spectral response of the plasmonic resonance of the nanoparticle chains. In addition, we experimentally show that the plasmonic chains improve the monochromaticity of the solid-state laser, thus, attaining spectral narrowing of the laser line by up to 38% depending on the pump wavelength. The effect of the plasmon driven absorption enhancement in the vicinities of the Ag nanoparticle chains is analyzed by tuning the optical pump in a broad spectral range (580-890 nm) at different Nd3+ transitions that overlap the spectral response of the longitudinal plasmonic mode of the chain. Theoretical insight shows that the plasmon-induced narrowing of the laser linewidth close to the nanoparticle chains can be related to the modification of the effective pump rate within the active medium, which is produced by the excitation of the localized plasmonic mode. The work constitutes a step forward in the development of high-quality and highly integrated photonic devices featuring narrowband laser emission in ultrasmall volumes operating in a technologically relevant spectral range.

Polar instabilities are well known to be suppressed on scaling materials down to the nanoscale, when the electrostatic energy increase at surfaces exceeds lowering of the bulk polarization energy. Surprisingly, here we report an emergent low symmetry polar phase arising in nanoscale powders of CaTiO3, the original mineral named perovskite discovered in 1839 and considered nominally nonpolar at any finite temperature in the bulk. Using nonlinear optics and spectroscopy, X-ray diffraction, and microscopy studies, we discover a well-defined polar to non-polar transition at a TC = 350 K in these powders. The same polar phase is also seen as a surface layer in bulk CaTiO3 single crystals, forming striking domains with in-plane polarization orientations. Density functional theory reveals that oxygen octahedral distortions in the surface layer lead to the stabilization of the observed monoclinic polar phase. These results reveal new ways of overcoming the scaling limits to polarization in perovskites.

Expanding the functionalities of plasmon-assisted lasers is essential for emergent applications in nanoscience and nanotechnology. Here, we report on a novel ability of plasmonic structures to induce dual-wavelength lasing in the near-infrared region in a Yb3+ solid-state laser. By means of the effects of disordered plasmonic networks deposited on the surface of a Yb3+-doped nonlinear RTP crystal, room-temperature dual-wavelength lasing, with a frequency difference between the lines in the THz range, is realized. The dual-wavelength laser is produced by the simultaneous activation of two lasing channels, namely, an electronic- and a phonon-terminated laser transition. The latter is enabled by the out-of-plane field components that are generated by the plasmonic structures, which excite specific Raman modes. Additionally, multiline radiation at three different wavelengths is demonstrated in the visible spectral region via two self-frequency conversion processes, which occur in the vicinities of the plasmonic structures. The results demonstrate the potential of plasmonic nanostructures for inducing drastic modifications in the operational mode of a solid-state laser and hold promise for applications in a variety of fields, including multiplexing, precise spectroscopies, and THz radiation generation via a simple and cost-effective procedure.

The control of ferroelectric domain walls at the nanometric level leads to novel interfacial properties and functionalities. In particular, the comprehension of charged domain walls, CDWs, lies at the frontier of future nanoelectronic research. Whereas many of the effects have been demonstrated for ideal archetypes, such as single crystals, and/or thin films, a similar control of CDWs on polycrystalline ferroelectrics has not been achieved. Here, we unambiguously show the presence of charged domain walls on a lead-free (K,Na)NbO3 polycrystalline system. The appearance of CDWs is observed in situ by confocal Raman microscopy and second harmonic generation microscopy. CDWs produce an internal strain gradient within each domain. Specifically, the anisotropic strain develops a crucial piece in the ferroelectric domain switching due to the coupling between the polarization of light and the ferroelectric polarization of the nanodomain in the (K,Na)NbO3 ceramic. This effect leads to the tuning of the ferroelectric domain switching by means of the light polarization angle. Our results will help to understand the relevance of charged domain walls on the ferroelectric domain switching process and may facilitate the development of domain wall nanoelectronics by remote light control utilizing polycrystalline ferroelectrics.

The demonstration of plasmon-assisted lasing by associating optical gain media with plasmonic nanostructures has led to a new generation of nanophotonic devices with unprecedented performances. However, despite the variety of designs demonstrated so far, the operation of these systems is in most cases limited to a single output wavelength, and some reports on multiline emission refer to mixing single nanolasers with the subsequent limitation in compactness. Here, we show multiline operation from a single plasmon-assisted nonlinear solid-state laser on which a linear chain of Ag nanoparticles is deposited. The system provides lasing at 1.08 mu m, which is self converted to the visible range through different parametric frequency-mixing processes generated at metal-dielectric interfaces. Near infrared and simultaneously green and tunable blue radiation with a subwavelength confinement in the direction perpendicular to the nanoparticle chain, are obtained at room temperature in CW regime. The results demonstrate the possibility of multifunctional operation from a single plasmon-assisted laser and offer new avenues for the development of highly integrable sources of coherent radiation.

The nonlinear properties of hybrid metallic-dielectric systems are attracting great interest due to their potential for the enhancement of frequency conversion processes at nanoscale dimensions. In this work, we theoretically and experimentally address the correlation between the near field distribution of hexagonal plasmonic necklaces of silver nanoparticles formed on the surface of a LiNbO3 crystal and the second harmonic generation (SHG) produced by this nonlinear crystal in the vicinities of the necklaces. The spectral response of the hexagonal necklaces does not depend on the polarization direction and is characterized by two main modes, the absorptive high-energy mode located in the UV spectral region and the lower energy mode, which is strongly radiant and extends from the visible to the near infrared region. We show that the spatial distribution of the enhanced SHG is consistent with the local field related to the low energy plasmon mode, which spectrally overlaps the fundamental beam. The results are in agreement with the low absorption losses of this mode and the two-photon character of the nonlinear process and provide deeper insight in the connection between the linear and nonlinear optical properties of the hybrid plasmonic-ferroelectric system. The study also highlights the potential of hexagonal necklaces as useful plasmonic platforms for enhanced optical processes at the nanoscale.

Emergent phenomena driven by light – matter interaction may have potential applications in next-generation domain wall nanoelectronics utilizing polycrystalline ferroelectrics

2D of hexagonal plasmonic necklaces for enhanced second harmonic generation Hexagonal plasmonic necklaces of silver nanoparticles organized in 2D superlattices on functional ferroelectric templates are fabricated in large-scale spatial regions by using a surfactant-free photo-deposition process. The plasmonic necklaces support broad radiative plasmonic resonances allowing the enhancement of second harmonic generation (SHG) at the ferroelectric domain boundaries. A 400-fold SHG enhancement is achieved at the near-UV spectral region with subsequent interest for technological applications.

Increasing Yb3+ absorption efficiency is currently desired in a number of applications including bio-imaging, photovoltaics, near infrared driven photocatalysis or ultra-short pulsed solid-state lasers. In this work, silver nanoparticles, which are connected forming disordered networks, have been self-assembled on Yb3+ doped RbTiOPO4 crystals to produce a remarkable enhancement of Yb3+ absorption, and hence in the photoluminescence of this ion. The results are interpreted taking into account the near-field response of the plasmonic networks, which display strong amplification of the electric field at the maximum of Yb3+ excitation at around 900 nm, together with the anisotropic character of the Yb3+ transitions in RbTiOPO4. We show that in the near field regime, the scattering of the plasmonic networks produces additional polarization field components to those of the incident field, which allows access to the largest transition dipolar moment of Yb3+ ions in RbTiOPO4. As a result, a much more efficient route for Yb3+ excitation takes place at the immediacy of the plasmonic networks. This work provides fundamental insights for improving the optical properties of rare earth ions by the suitable design of metallic nanoparticle arrangements, and constitutes a promising step towards the development of new multifunctional solid-state lasers.