Two dimensional ferroelectric domain patterns in Yb3+ optically active LiNbO3 fabricated by direct electron beam writing

The following article appeared in Applied Physics Letters 102.4 (2013): 042910 and may be found at http://scitation.aip.org/content/aip/journal/apl/102/4/10.1063/1.4790149We report on highly controllable ferroelectric domain inversion in Yb 3+ doped LiNbO3 laser crystal. The ferroelectric domain patterns are fabricated by direct electron beam writing without any previous masking process. Square lattices of inverted domains with diameters and distance between domains as low as 1 μm are demonstrated. The lateral growth of the inverted domains is analyzed as a function of the applied charge and the threshold values for domains in the 1-10 μm length scale are determined. Spatially resolved low temperature fluorescence spectroscopy and non-collinear second harmonic generation experiments are also employed to evaluate the optical properties of the system.This work has been supported by Spanish Government under Project No. MAT2010-17443 and Comunidad de Madrid under Grant No. S2009/1756

Field enhancement and spectral features of hexagonal necklaces of silver nanoparticles for enhanced nonlinear optical processes

Access to the online abstract in the journal: https://doi.org/10.1364/OE.26.022394 © 2018 Optical Society of America. Users may use, reuse, and build upon the article, or use the article for text or data mining, so long as such uses are for non-commercial purposes and appropriate attribution is maintained. All other rights are reservedThe 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 nanoscaleSpanish Ministry of Economy and Competitiveness (MINECO) under project MAT2016- 76106-R and the Comunidad de Madrid (grant S2013/MIT-2740). C.T. acknowledges funding from the VILLUM Foundation (Villum Investigator, grant no. 16498). L.E.B and M.O.R also acknowledges financial support from the Spanish Ministry of Economy and Competitiveness, through The “María de Maeztu” Programme for Units of Excellence in R&D (MDM-2014-0377

Enhancing nonlinear interactions by the superposition of plasmonic lattices on ꭕ(2)-nonlinear photonic crystals

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 ꭕ(2) modulated dielectric crystals have been scarcely addressed, mainly due to the complexity in manufacturing appropriate periodic plasmonic structures overlying the ꭕ(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 ꭕ(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 ꭕ(2) structure. The superposition of the plasmonic and the ꭕ(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 technologiesThis work has been supported by the Spanish Government (Contracts MAT2016-76106-R and PID2019-108257GB-I00/ AEI/10.13039/501100011033 and María de Maeztu “Pro gramme for Units of Excellence in R&D CEX2018-000805-M) and Comunidad de Madrid (Grant SI1/PJI/2019-00105

Multiline operation from a single plasmon-assisted laser

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 μm, 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 radiationThis work has been supported by the Spanish Ministry of Economy and Competitiveness (MINECO) under Projects MAT201343301-R, MAT2015-66128-R and MAT2016-76106-R and by Comunidad de Madrid under Grant S2013/MIT-274

Plasmon assisted Nd3+-based solid-state nanolaser

Solid-state lasers constitute essential tools in a variety of scientific and technological areas, being available in many different designs. However, although nanolasing has been successfully achieved for dyes and semiconductor gain media associated with plasmonic structures, the operation of solid-state lasers beyond the diffraction limit has not been reported yet. Here, we demonstrate room temperature laser action with subwavelength confinement in a Nd3+-based solid-state laser by means of the localized surface plasmon resonances supported by chains of metallic nanoparticles. We show a 50% reduction of the pump power at threshold and a remarkable 15-fold improvement of the slope efficiency with respect to the bulk laser operation. The results can be extended to the large diversity of solid-state lasers with the subsequent impact on their applicationsThis work has been supported by the Spanish Ministry of Economy and Competitiveness (MINECO) under projects MAT2013-43301-R and FIS2013-41184-P and Comunidad de Madrid under grant S2013/MIT-2740

Plasmonic enhancement of second harmonic generation from nonlinear RbTiOPO4 crystals by aggregates of silver nanostructures

We demonstrate a 60–fold enhancement of the second harmonic generation (SHG) response at the nanoscale in a hybrid metal-dielectric system. By using complex silver nanostructures photochemically deposited on the polar surface of a ferroelectric crystal, we tune the plasmonic resonances from the visible to the near-infrared (NIR) spectral region, matching either the SH or the fundamental frequency. In both cases the SHG signal at the metal-dielectric interface is enhanced, although with substantially different enhancement values: around 5 times when the plasmonic resonance is at the SH frequency or up to 60 times when it matches the fundamental NIR radiation. The results are consistent with the more spatially-extended near-field response of complex metallic nanostructures and can be well explained by taking into account the quadratic character of the SHG process. The work points out the potential of aggregates of silver nanostructures for enhancing optical nonlinearities at the nanoscale and provides an alternative approach for the development of nanometric nonlinear photonic devices in a scalable way.This work has been supported by the Spanish Ministry of Economy and Competitiveness (MINECO) under projects MAT2013-43301-R, FIS2013-41184-P, MAT2013-47395-C4-4-R and TEC2014-55948-R. The authors also acknowledge Comunidad de Madrid under grant S2013/MIT-2740, Dept. of Industry of the Basque Country under project nanoGUNE’14, and Catalan Authority under project 2014SGF1358. F.D. acknowledges additional support through the ICREA Academia awards 2010ICREA-02 for excellence in research. LSG acknowledges FPU13/02476 grant from the Spanish Ministry of Education.Peer reviewe

Experimental evidence of charged domain walls in lead-free ferroelectric ceramics: Light-driven nanodomain switching

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)NbO 3 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)NbO 3 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 ferroelectricsThis work was supported by the Spanish Ministry of Economy and Competitiveness (MINECO) under the projects MAT201348009-C4-1-P, MAT2013-43301-R and MAT2016-76106-R, the Spanish National Research Council (CSIC) under the project NANOMIND CSIC 201560E068 and the Comunidad de Madrid under the grant S2013/MIT-274

Blue SHG enhancement by silver nanocubes photochemically prepared on a RbTiOPO4 ferroelectric crystal

This is the peer reviewed version of the following article: Blue SHG enhancement by silver nanocubes photochemically prepared on a RbTiOPO4 ferroelectric crystal, which has been published in final form at http://doi.org/10.1002/adma.201401603. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived VersionsSilver nanocubes with low size dispersion have been selectively photo-deposited on the positive surface of a periodically poled RbTiOPO 4 ferroelectric crystal. The obtained nanocubes show preferential orientations with respect to the substrate suggesting ep itaxial growth. The plasmonic resonances supported by the nanocubes are exploited to enhance blue SHG at the domain wallsThis work has been supported by the Spanish Government under projects MAT2010–17443, MAT2011–29255-C02–02 and MAT2013– 43301-R, Comunidad de Madrid under grant S2009/1756 and Generalitat de Catalunya under project 2009SGR23

Anisotropic enhancement of Yb3+ luminescence by disordered plasmonic networks self-assembled on RbTiOPO4 ferroelectric crystals

Disordered plasmonic networks of Ag nanoparticles assembled on Yb3+:RTP crystals produce a remarkable enhancement of the Yb3+ excitation rate increasing the photoluminescence 5-times.</p

Giant Second Harmonic Generation Enhancement by Ag Nanoparticles Compactly Distributed on Hexagonal Arrangements

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