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
Solid polymer electrolytes have demonstrated high promise to solve the safety problems caused by conventional liquid electrolytes in lithium ion batteries.However,the inherent flammability of most polymer electrolyte ...Solid polymer electrolytes have demonstrated high promise to solve the safety problems caused by conventional liquid electrolytes in lithium ion batteries.However,the inherent flammability of most polymer electrolyte materials remains unresolved,hence hindering their further industrial application.Addressing this challenge,we designed and constructed a thermal-responsive imide-linked covalent organic framework(COF)bearing ortho-positioned hydroxy groups as precursors,which can conduct a thermal rearrangement to transform into a highly crystalline and robust benzoxazole-linked COF upon heating.Benefiting from the release of carbon dioxide through thermal rearrangement reaction,this COF platform exhibited excellent flame retardant properties.By contrast,classic COFs(e.g.,boronate ester,imine,olefin,imide linked)were all flammable.Moreover,incorpo-rating polyethylene glycol and Li salt into the COF channels can produce solid polymer electrolytes with outstanding flame retardancy,high ionic conductivity(6.42×10^(-4) S cm^(-1))and a high lithium-ion transference number of 0.95.This thermal rearrangement strategy not only opens a new route for the fabrication of ultrastable COFs,but also provides promising perspectives to designing flame-retardant materials for energy-related applications.展开更多
2D materials are considered for applications that require strong light-matter interaction because of the apparently giant oscillator strength of the exciton transitions in the absorbance spectrum.Nevertheless,the effe...2D materials are considered for applications that require strong light-matter interaction because of the apparently giant oscillator strength of the exciton transitions in the absorbance spectrum.Nevertheless,the effective oscillator strengths of these transitions have bee n scarcely reported,nor is there a con sistent interpretati on of the obtained values.Here,we analyse the transition dipole moment and the ensuing oscillator strength of the exciton transition in 2D CdSe nanoplatelets by means of the optically induced Stark effect(OSE).Intriguingly,we find that the exciton absorption line reacts to a high intensity optical field as a transition with an oscillator strength FStark that is 50 times smaller than expected based on the linear absorption coefficient.We propose that the pronounced exciton absorption line should be seen as the sum of multiple,low oscillator strength transitions,rather than a single high oscillator strength one,a feat we assign to strong exciton center-of-mass localization.Within the quantum mechanical description of excitons,this 50-fold difference between both oscillator strengths corresponds to the ratio between the cohere nee area of the exciton's center of mass and the total area,which yields a coherence area of a mere 6.1 nm2.Since we find that the coherence area in creases with reducing temperature,we conclude that thermal effects,related to lattice vibrations,contribute to exciton localization.In further support of this localization model,we show that FStark is in dependent of the n anoplatelet area,correctly predicts the radiative lifetime,and lines up for strongly confined quantum dot 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 Tianjin Natural Science Foundation(20JCJQJC00170)National Natural Science Foundation of China(22001131 and 22175099)+2 种基金Frontiers Science Center for New Organic Matter of Nankai University(63181206)111 Project(B12015)Postdoctoral Science Foundation of China(2019M660974).
文摘Solid polymer electrolytes have demonstrated high promise to solve the safety problems caused by conventional liquid electrolytes in lithium ion batteries.However,the inherent flammability of most polymer electrolyte materials remains unresolved,hence hindering their further industrial application.Addressing this challenge,we designed and constructed a thermal-responsive imide-linked covalent organic framework(COF)bearing ortho-positioned hydroxy groups as precursors,which can conduct a thermal rearrangement to transform into a highly crystalline and robust benzoxazole-linked COF upon heating.Benefiting from the release of carbon dioxide through thermal rearrangement reaction,this COF platform exhibited excellent flame retardant properties.By contrast,classic COFs(e.g.,boronate ester,imine,olefin,imide linked)were all flammable.Moreover,incorpo-rating polyethylene glycol and Li salt into the COF channels can produce solid polymer electrolytes with outstanding flame retardancy,high ionic conductivity(6.42×10^(-4) S cm^(-1))and a high lithium-ion transference number of 0.95.This thermal rearrangement strategy not only opens a new route for the fabrication of ultrastable COFs,but also provides promising perspectives to designing flame-retardant materials for energy-related applications.
基金from FWO-Vlaanderen(12K8216N)Z.H.ack no wledges the Research Foundation Flanders(research projects 17006602 and G0F0920N)+1 种基金Ghent University(GOA no.01G01513)for funding.AJ.H acknowledges the ERC and NWO-TTW.S.Bisschop is acknowledged for SEM imaging of the platelet layers and K.De Nolf for help with the CdSe QD/platelet synthesis respectively.This project has received fun ding from the European Research Council(ERC)under the European Union's Horizon 2020 research and innovation program(grant agreement no.714876 PHOCONA).
文摘2D materials are considered for applications that require strong light-matter interaction because of the apparently giant oscillator strength of the exciton transitions in the absorbance spectrum.Nevertheless,the effective oscillator strengths of these transitions have bee n scarcely reported,nor is there a con sistent interpretati on of the obtained values.Here,we analyse the transition dipole moment and the ensuing oscillator strength of the exciton transition in 2D CdSe nanoplatelets by means of the optically induced Stark effect(OSE).Intriguingly,we find that the exciton absorption line reacts to a high intensity optical field as a transition with an oscillator strength FStark that is 50 times smaller than expected based on the linear absorption coefficient.We propose that the pronounced exciton absorption line should be seen as the sum of multiple,low oscillator strength transitions,rather than a single high oscillator strength one,a feat we assign to strong exciton center-of-mass localization.Within the quantum mechanical description of excitons,this 50-fold difference between both oscillator strengths corresponds to the ratio between the cohere nee area of the exciton's center of mass and the total area,which yields a coherence area of a mere 6.1 nm2.Since we find that the coherence area in creases with reducing temperature,we conclude that thermal effects,related to lattice vibrations,contribute to exciton localization.In further support of this localization model,we show that FStark is in dependent of the n anoplatelet area,correctly predicts the radiative lifetime,and lines up for strongly confined quantum dot systems.
