Second harmonic generation and sum frequency generation(SHG and SFG)provide effective means to realize coherent light at desired frequencies when lasing is not easily achievable.They have found applications from sensi...Second harmonic generation and sum frequency generation(SHG and SFG)provide effective means to realize coherent light at desired frequencies when lasing is not easily achievable.They have found applications from sensing to quantum optics and are of particular interest for integrated photonics at communication wavelengths.Decreasing the footprints of nonlinear components while maintaining their high up-conversion efficiency remains a challenge in the miniaturization of integrated photonics.Here we explore lithographically defined AlGaInP nano(micro)structures/Al_(2)O_(3)/Ag as a versatile platform to achieve efficient SHG/SFG in both waveguide and resonant cavity configurations in both narrow-and broadband infrared(IR)wavelength regimes(1300-1600 nm).The effective excitation of highly confined hybrid plasmonic modes at fundamental wavelengths allows efficient SHG/SFG to be achieved in a waveguide of a cross-section of 113 nm×250 nm,with a mode area on the deep subwavelength scale(λ2/135)at fundamental wavelengths.Remarkably,we demonstrate direct visualization of SHG/SFG phase-matching evolution in the waveguides.This together with mode analysis highlights the origin of the improved SHG/SFG efficiency.We also demonstrate strongly enhanced SFG with a broadband IR source by exploiting multiple coherent SFG processes on 1μm diameter AlGaInP disks/Al_(2)O_(3)/Ag with a conversion efficiency of 14.8%MW^(−1) which is five times the SHG value using the narrowband IR source.In both configurations,the hybrid plasmonic structures exhibit>1000 enhancement in the nonlinear conversion efficiency compared to their photonic counterparts.Our results manifest the potential of developing such nanoscale hybrid plasmonic devices for state-of-the-art on-chip nonlinear optics applications.展开更多
Vectored non-covalent interactions—mainly hydrogen bonding and aromatic interactions—extensively contribute to(bio)-organic self-assembling processes and significantly impact the physicochemical properties of the as...Vectored non-covalent interactions—mainly hydrogen bonding and aromatic interactions—extensively contribute to(bio)-organic self-assembling processes and significantly impact the physicochemical properties of the associated superstructures.However,vectored non-covalent interaction-driven assembly occursmainly along one-dimensional(1D)or three-dimensional(3D)directions,and a two-dimensional(2D)orientation,especially that of multilayered,graphene-like assembly,has been reported less.In this present research,by introducing amino,hydroxyl,and phenyl moieties to the triazine skeleton,supramolecular layered assembly is achieved by vectored non-covalent interactions.The planar hydrogen bonding network results in high stability,with a thermal sustainability of up to about 330°C and a Young’s modulus of up to about 40 GPa.Upon introducing wrinkles by biased hydrogen bonding or aromatic interactions to disturb the planar organization,the stability attenuates.However,the intertwined aromatic interactions prompt a red edge excitation shift effect inside the assemblies,inducing broad-spectrum fluorescence covering nearly the entire visible light region(400–650 nm).We show that bionic,superhydrophobic,pillar-like arrays with contact angles of up to about 170°can be engineered by aromatic interactions using a physical vapor deposition approach,which cannot be realized through hydrogen bonding.Our findings show the feasibility of 2D assembly with engineerable properties by modulating vectored non-covalent interactions.展开更多
Ferroelectricity in biological system has been anticipated both theoretically and experimentally over the past few decades.Claims of ferroelectricity in biological systems have given rise to confusion and methodologic...Ferroelectricity in biological system has been anticipated both theoretically and experimentally over the past few decades.Claims of ferroelectricity in biological systems have given rise to confusion and methodological controversy.Over the years,a“loop”of induced polarization in response to a varying applied electrical field and a consequent polarization reversal has prompted many researchers to claim ferroelectricity in biological structures and their building blocks.Other observers were skeptical about the methodology adopted in generating the data and questioned the validity of the claimed ferroelectricity as such,“loop”can also be obtained from linear capacitors.In a paper with somewhat tongue-in-cheek title,Jim Scott showed that ordinary banana peels could exhibit closed loops of electrical charge which closely resemble and thus could be misinterpreted as ferroelectric hysteresis loops in barium sodium niobate,BNN paraphrasing it as“banana”.In this paper,we critically review ferroelectricity in biological system and argue that knowing the molecular and crystalline structure of biological building blocks and experimenting on such building blocks may be the way forward in revealing the“true”nature of ferroelectricity in biological systems.展开更多
基金the support from the Science Foundation Ireland(SFI)National Access Programme(number 444)SFI 17/CDA/4733+6 种基金the support from the special fund of Wuhan University Graduate Students overseas exchange programthe support from SFI 16/IA/4629,12/RC/2278_P2,12/RC/2302_P2the Irish Research Council under IRCLA/2017/285the funding provided by SFI under grants 12/RC/2276_P2 and 15/IA/2864the support from SFI 13/CDA/2221the support from the National Natural Science Foundation of China(Grants numbers 91850207 and 11674256)the National Key R&D Program of China(Grant number 2017YFA0205800).
文摘Second harmonic generation and sum frequency generation(SHG and SFG)provide effective means to realize coherent light at desired frequencies when lasing is not easily achievable.They have found applications from sensing to quantum optics and are of particular interest for integrated photonics at communication wavelengths.Decreasing the footprints of nonlinear components while maintaining their high up-conversion efficiency remains a challenge in the miniaturization of integrated photonics.Here we explore lithographically defined AlGaInP nano(micro)structures/Al_(2)O_(3)/Ag as a versatile platform to achieve efficient SHG/SFG in both waveguide and resonant cavity configurations in both narrow-and broadband infrared(IR)wavelength regimes(1300-1600 nm).The effective excitation of highly confined hybrid plasmonic modes at fundamental wavelengths allows efficient SHG/SFG to be achieved in a waveguide of a cross-section of 113 nm×250 nm,with a mode area on the deep subwavelength scale(λ2/135)at fundamental wavelengths.Remarkably,we demonstrate direct visualization of SHG/SFG phase-matching evolution in the waveguides.This together with mode analysis highlights the origin of the improved SHG/SFG efficiency.We also demonstrate strongly enhanced SFG with a broadband IR source by exploiting multiple coherent SFG processes on 1μm diameter AlGaInP disks/Al_(2)O_(3)/Ag with a conversion efficiency of 14.8%MW^(−1) which is five times the SHG value using the narrowband IR source.In both configurations,the hybrid plasmonic structures exhibit>1000 enhancement in the nonlinear conversion efficiency compared to their photonic counterparts.Our results manifest the potential of developing such nanoscale hybrid plasmonic devices for state-of-the-art on-chip nonlinear optics applications.
基金supported by the Fund for Creative Research Groups of National Natural Science Foundation of China (No. 51821093)the National Natural Science Foundation of China (Nos. 52175551, 52075484)(KT and DM)+2 种基金the National Key Research and Development Program (SQ2021YFE010405)(KT)Science Foundation Ireland (SFI) through awards Nos. 15/CDA/3491and 12/RC/2275_P2 (DT)computing resources at the SFI/Higher Education Authority Irish Center for High-End Computing (ICHEC)(SG and DT)
文摘Vectored non-covalent interactions—mainly hydrogen bonding and aromatic interactions—extensively contribute to(bio)-organic self-assembling processes and significantly impact the physicochemical properties of the associated superstructures.However,vectored non-covalent interaction-driven assembly occursmainly along one-dimensional(1D)or three-dimensional(3D)directions,and a two-dimensional(2D)orientation,especially that of multilayered,graphene-like assembly,has been reported less.In this present research,by introducing amino,hydroxyl,and phenyl moieties to the triazine skeleton,supramolecular layered assembly is achieved by vectored non-covalent interactions.The planar hydrogen bonding network results in high stability,with a thermal sustainability of up to about 330°C and a Young’s modulus of up to about 40 GPa.Upon introducing wrinkles by biased hydrogen bonding or aromatic interactions to disturb the planar organization,the stability attenuates.However,the intertwined aromatic interactions prompt a red edge excitation shift effect inside the assemblies,inducing broad-spectrum fluorescence covering nearly the entire visible light region(400–650 nm).We show that bionic,superhydrophobic,pillar-like arrays with contact angles of up to about 170°can be engineered by aromatic interactions using a physical vapor deposition approach,which cannot be realized through hydrogen bonding.Our findings show the feasibility of 2D assembly with engineerable properties by modulating vectored non-covalent interactions.
基金supported by the European Union’s Horizon 2020 Research and Innovation Programme under the Marie Sklodowska-Curie grant agreement(801165),with co-funding through Science Foundation Ireland,Career Development Award(17/CDA/4733)supported by the National Natural Science Foundation of China(12204088,11974069 and U21A2074)+1 种基金Liaoning Revitalization Talents Program(XLYC1902113)the Science and Technology Project of Liaoning Province(2020JH2/10100012)。
文摘Ferroelectricity in biological system has been anticipated both theoretically and experimentally over the past few decades.Claims of ferroelectricity in biological systems have given rise to confusion and methodological controversy.Over the years,a“loop”of induced polarization in response to a varying applied electrical field and a consequent polarization reversal has prompted many researchers to claim ferroelectricity in biological structures and their building blocks.Other observers were skeptical about the methodology adopted in generating the data and questioned the validity of the claimed ferroelectricity as such,“loop”can also be obtained from linear capacitors.In a paper with somewhat tongue-in-cheek title,Jim Scott showed that ordinary banana peels could exhibit closed loops of electrical charge which closely resemble and thus could be misinterpreted as ferroelectric hysteresis loops in barium sodium niobate,BNN paraphrasing it as“banana”.In this paper,we critically review ferroelectricity in biological system and argue that knowing the molecular and crystalline structure of biological building blocks and experimenting on such building blocks may be the way forward in revealing the“true”nature of ferroelectricity in biological systems.