The development of 3D structural composites with electromagnetic(EM)wave absorption could attenuate EM waves.Herein,magnetized flower-like Cu_(9)S_(5)/ZnFe_(2)O_(4)composites were fabricated through a multistep hydrot...The development of 3D structural composites with electromagnetic(EM)wave absorption could attenuate EM waves.Herein,magnetized flower-like Cu_(9)S_(5)/ZnFe_(2)O_(4)composites were fabricated through a multistep hydrothermal method.The crystallographic and surface phase chemical information,morphological structure,and magnetic and EM parameters of the composites were analyzed.The prepared Cu_(9)S_(5)/ZnFe_(2)O_(4)composites have multiple loss paths for EM waves and present an overall 3D flower-like structure.The Cu_(9)S_(5)/ZnFe_(2)O_(4)composites exhibit a minimum reflection loss of-54.38 dB and a broad effective absorption bandwidth of 5.92 GHz.Through magnetization,ZnFe_(2)O_(4)particles are self-assembled and grown on the surfaces of Cu_(9)S_(5).Such a modification is conducive to the generation of additional cross-linking contact sites and the effective introduction of a large number of phase interfaces,crystalline defects,special three-dimensional flower-like structures,and magneto-electrical coupling loss effects.Moreover,the synergistic effect of multiple loss strategies effectively improves EM wave absorption by the material.This work can provide a strategy for the use of magnetizationmodified sulfide composite functional materials in EM wave absorption.展开更多
Although many dielectric polymers exhibit high energy storage density(Ue)with enhanced dipolar polarization at room temperature,the substantially increased electric conduction loss at high applied electric fields and ...Although many dielectric polymers exhibit high energy storage density(Ue)with enhanced dipolar polarization at room temperature,the substantially increased electric conduction loss at high applied electric fields and high temperatures remains a great challenge.Here,we report a strategy that high contents of medium-polar ester group and end-group(St)modification are introduced into a biode-gradable polymer polylactic acid(PLA)to synergistically reduce the loss and enhance Ue and charge-discharge efficiency(h).The resultant St-modified PLA polymer(PLA-St)exhibits an Ue of 6.5 J/cm^(3)with an ultra-high h(95.4%),far outperforming the best reported dielectric polymers.It is worth noting that the modified molecular structures can generate deep trap centers and restrict the local dipole motions in the polymer,which are responsible for the reduction of conduction loss and improvements in high-temperature capacitive performance.In addition,the PLA-St polymer shows intrinsically excellent self-healing ability and cyclic stability surviving over 500000 charge-discharge cycles.This work offers an efficient route to next-generation eco-friendly dielectric polymers with high energy density,low loss,and long-term stability.展开更多
Lanthanide-doped upconversion nanocrystals(UCNCs)have recently become an attractive nonlinear fluorescence material for use in bioimaging because of their tunable spectral characteristics and exceptional photostabilit...Lanthanide-doped upconversion nanocrystals(UCNCs)have recently become an attractive nonlinear fluorescence material for use in bioimaging because of their tunable spectral characteristics and exceptional photostability.Plasmonic materials are often introduced into the vicinity of UCNCs to increase their emission intensity by means of enlarging the absorption cross-section and accelerating the radiative decay rate.Moreover,plasmonic nanostructures(e.g.,gold nanorods,GNRs)can also influence the polarization state of the UC fluorescence—an effect that is of fundamental importance for fluorescence polarization-based imaging methods yet has not been discussed previously.To study this effect,we synthesized GNR@SiO_(2)@CaF2:Yb^(3+),Er^(3+)hybrid core–shell–satellite nanostructures with precise control over the thickness of the SiO_(2) shell.We evaluated the shell thicknessdependent plasmonic enhancement of the emission intensity in ensemble and studied the plasmonic modulation of the emission polarization at the single-particle level.The hybrid plasmonic UC nanostructures with an optimal shell thickness exhibit an improved bioimaging performance compared with bare UCNCs,and we observed a polarized nature of the light at both UC emission bands,which stems from the relationship between the excitation polarization and GNR orientation.We used electrodynamic simulations combined with Förster resonance energy transfer theory to fully explain the observed effect.Our results provide extensive insights into how the coherent interaction between the emission dipoles of UCNCs and the plasmonic dipoles of the GNR determines the emission polarization state in various situations and thus open the way to the accurate control of the UC emission anisotropy for a wide range of bioimaging and biosensing applications.展开更多
Generally,most materials expand when heated and contract when cooled,whereas negative thermal expansion(NTE)materials are very rare.As a typical NTE material,PbTiO_(3) and related compounds have drawn particular inter...Generally,most materials expand when heated and contract when cooled,whereas negative thermal expansion(NTE)materials are very rare.As a typical NTE material,PbTiO_(3) and related compounds have drawn particular interest in recent years.The discovery of an enhanced NTE system in PbTiO_(3) is beneficial to deepen our understanding of its mechanism and regulate its properties.At present,the method of discriminating an enhanced NTE material based on PbTiO_(3) is not universal.Here,we propose a semi-empirical method through evaluating the average lattice distortion in related systems to estimate the relative coefficient of thermal expansion conveniently.The rationality of the method was verified by the analysis of the 0.6PbTiO_(3)-0.4Bi(Ga_(x)Fe_(1-x))O_(3) system.So far,all PbTiO_(3)-based compounds with enhanced NTE conform well to this method.This method provides the possibility to find more enhanced NTE PbTiO_(3)-based materials.展开更多
Sentinel-1A/B data are crucial for retrieving numerical information about surface phenomena and processes.Coregistration of terrain observation by progressive scans(TOPS)data is a critical step in its application.TOPS...Sentinel-1A/B data are crucial for retrieving numerical information about surface phenomena and processes.Coregistration of terrain observation by progressive scans(TOPS)data is a critical step in its application.TOPS data must be fundamentally co-registered with an accuracy of 0.001 pixels.However,various decorrelation factors due to natural vegetation and seasonal effects affect the coregistration accuracy of TOPS data.This paper proposed an enhanced spectral diversity coregistration method for dual-polarimetric(PolESD)Sentinel-1A/B TOPS data.The PolESD method suppresses speckle noise based on a unified non-local framework in dual-pol Synthetic Aperture Radar(SAR),and extracts the phase of the optimal polarization channel from the denoised polarimetric interferometric coherency matrix.Compared with the traditional ESD method developed for single-polarization data,the PolESD method can obtain more accurate coherence and phase and get more pixels for azimuth-offset estimation.In bare areas covered with low vegetation,the number of pixels selected by PolESD is more than the Boxcar method.It can also correct misregistration more effectively and eliminate phase jumps in the burst edge.Therefore,PolESD will help improve the application of TOPS data in low-coherence scenarios.展开更多
Developing well-defined nanostructures with superior surface-enhanced Raman scattering （SERS） performance is a critical and highly desirable goal for the practical applications of SERS in sensing and analysis. Here,...Developing well-defined nanostructures with superior surface-enhanced Raman scattering （SERS） performance is a critical and highly desirable goal for the practical applications of SERS in sensing and analysis. Here, a SERS-active substrate was fabricated by decorating a MoS2 monolayer with Ag nanowire （NW） and nanoparticle （NP） structures, using a spin-coating method. Both experimental and theoretical results indicate that strong SERS signals of rhodamine 6G （R6G） molecules can be achieved at ＂hotspots＂ formed in the Ag NW-Ag NP-MoS2 hybrid structure, with an enhancement factor of 106. The SERS enhancement is found to be strongly polarization dependent. The fabricated SERS substrate also exhibits ultrasensitive detection capabilities with a detection limit of 10-11 M, as well as reliable reproducibility and good stability.展开更多
Surface-enhanced resonance Raman scattering （SERRS） of Rhodamine 6G （R6G） adsorbed on colloidal silver clusters has been studied. Based on the great enhancement of the Raman signal and the quench of the fluorescen...Surface-enhanced resonance Raman scattering （SERRS） of Rhodamine 6G （R6G） adsorbed on colloidal silver clusters has been studied. Based on the great enhancement of the Raman signal and the quench of the fluorescence, the SERRS spectra of R6G were recorded for the samples of dye colloidal solution with different concentrations. Spectral inhomogeneity behaviours from single molecules in the dried sample films were observed with complementary evidences, such as spectral polarization, spectral diffusion, intensity fluctuation of vibrational lines and even ＂breathing＂ of the molecules. Sequential spectra observed from a liquid sample with an average of 0.3 dye molecules in the probed volume exhibited the expected Poisson distribution for actually measuring 0, 1 or 2 molecules. Difference between the SERRS spectra of R6G excited by linearly and circularly polarized light were experimentally measured.展开更多
A novel approach of combining conventional infrared spectroscopy （IR） and atomic force microscopy （AFM） is presented to better understand the behavior of a drug adsorbed on a metal substrate at the nanoscale level...A novel approach of combining conventional infrared spectroscopy （IR） and atomic force microscopy （AFM） is presented to better understand the behavior of a drug adsorbed on a metal substrate at the nanoscale level. Tip-enhanced infrared nanospectroscopy （TEIRA） was used for the first time to investigate Lu AA33810, a selective brain-penetrating Y5 receptor antagonist, after immobilization on gold nanopartides （GNPs）. Here, a gold coated AFM tip and gold substrate were used to obtain the near-field electromagnetic field trapping effect. Because of the huge signal enhancement, it was possible to obtain the spectral information regarding the self-assembled monolayer of the investigated molecule. The effect of two orthogonal polarizations （p- and s-polarization modulations） of the excitation laser beam on the spectral patterns is also discussed. The results show that there is a strong relationship between the state of polarization of the incident radiation and the relative infrared band intensities. Another factor affecting the observed spectral differences is the topology of the metal substrate, which may result in the induction of a cross-polarization effect. The performed analysis indicates that the C--C bond from the cyclohexyl group is oriented almost parallel to the metal surface. Conversely, the p- and s-polarized spectral variations suggest that the O=S---O angle is high enough to enable the simultaneous interaction of both oxygen atoms with the GNPs.展开更多
基金This work was supported by the National Natural Science Foundation of China(No.51477002)the University Synergy Innovation Program of Anhui Province,China(No.GXXT-2019-028).
文摘The development of 3D structural composites with electromagnetic(EM)wave absorption could attenuate EM waves.Herein,magnetized flower-like Cu_(9)S_(5)/ZnFe_(2)O_(4)composites were fabricated through a multistep hydrothermal method.The crystallographic and surface phase chemical information,morphological structure,and magnetic and EM parameters of the composites were analyzed.The prepared Cu_(9)S_(5)/ZnFe_(2)O_(4)composites have multiple loss paths for EM waves and present an overall 3D flower-like structure.The Cu_(9)S_(5)/ZnFe_(2)O_(4)composites exhibit a minimum reflection loss of-54.38 dB and a broad effective absorption bandwidth of 5.92 GHz.Through magnetization,ZnFe_(2)O_(4)particles are self-assembled and grown on the surfaces of Cu_(9)S_(5).Such a modification is conducive to the generation of additional cross-linking contact sites and the effective introduction of a large number of phase interfaces,crystalline defects,special three-dimensional flower-like structures,and magneto-electrical coupling loss effects.Moreover,the synergistic effect of multiple loss strategies effectively improves EM wave absorption by the material.This work can provide a strategy for the use of magnetizationmodified sulfide composite functional materials in EM wave absorption.
基金supported by National Key Research&Development Program(No.2021YFB3800603)National Natural Science Foundation of China(No.92066208)+1 种基金Shenzhen Science and Technology Program(Nos.KQTD20180411143514543,JCYJ20180504165831308)Guangdong Natural Science Foundation(No.2020A1515011043).
文摘Although many dielectric polymers exhibit high energy storage density(Ue)with enhanced dipolar polarization at room temperature,the substantially increased electric conduction loss at high applied electric fields and high temperatures remains a great challenge.Here,we report a strategy that high contents of medium-polar ester group and end-group(St)modification are introduced into a biode-gradable polymer polylactic acid(PLA)to synergistically reduce the loss and enhance Ue and charge-discharge efficiency(h).The resultant St-modified PLA polymer(PLA-St)exhibits an Ue of 6.5 J/cm^(3)with an ultra-high h(95.4%),far outperforming the best reported dielectric polymers.It is worth noting that the modified molecular structures can generate deep trap centers and restrict the local dipole motions in the polymer,which are responsible for the reduction of conduction loss and improvements in high-temperature capacitive performance.In addition,the PLA-St polymer shows intrinsically excellent self-healing ability and cyclic stability surviving over 500000 charge-discharge cycles.This work offers an efficient route to next-generation eco-friendly dielectric polymers with high energy density,low loss,and long-term stability.
基金support by the Hong Kong Research Grants Council(GRF Grant No.15301414)the support by the Ministry of Education,Youth and Sports of the Czech Republic under project CEITEC 2020(LQ1601)+2 种基金the Hong Kong Polytechnic Universitythe financial support by the NSFC(Nos.U1305244,21325104,11304314)the CAS/SAFEA International Partnership Program for Creative Research Teams.
文摘Lanthanide-doped upconversion nanocrystals(UCNCs)have recently become an attractive nonlinear fluorescence material for use in bioimaging because of their tunable spectral characteristics and exceptional photostability.Plasmonic materials are often introduced into the vicinity of UCNCs to increase their emission intensity by means of enlarging the absorption cross-section and accelerating the radiative decay rate.Moreover,plasmonic nanostructures(e.g.,gold nanorods,GNRs)can also influence the polarization state of the UC fluorescence—an effect that is of fundamental importance for fluorescence polarization-based imaging methods yet has not been discussed previously.To study this effect,we synthesized GNR@SiO_(2)@CaF2:Yb^(3+),Er^(3+)hybrid core–shell–satellite nanostructures with precise control over the thickness of the SiO_(2) shell.We evaluated the shell thicknessdependent plasmonic enhancement of the emission intensity in ensemble and studied the plasmonic modulation of the emission polarization at the single-particle level.The hybrid plasmonic UC nanostructures with an optimal shell thickness exhibit an improved bioimaging performance compared with bare UCNCs,and we observed a polarized nature of the light at both UC emission bands,which stems from the relationship between the excitation polarization and GNR orientation.We used electrodynamic simulations combined with Förster resonance energy transfer theory to fully explain the observed effect.Our results provide extensive insights into how the coherent interaction between the emission dipoles of UCNCs and the plasmonic dipoles of the GNR determines the emission polarization state in various situations and thus open the way to the accurate control of the UC emission anisotropy for a wide range of bioimaging and biosensing applications.
基金financially supported by the National Key R&D Program of China(No.2020YFA0406202)the National Natural Science Foundation of China(Nos.22090042 and 21731001)。
文摘Generally,most materials expand when heated and contract when cooled,whereas negative thermal expansion(NTE)materials are very rare.As a typical NTE material,PbTiO_(3) and related compounds have drawn particular interest in recent years.The discovery of an enhanced NTE system in PbTiO_(3) is beneficial to deepen our understanding of its mechanism and regulate its properties.At present,the method of discriminating an enhanced NTE material based on PbTiO_(3) is not universal.Here,we propose a semi-empirical method through evaluating the average lattice distortion in related systems to estimate the relative coefficient of thermal expansion conveniently.The rationality of the method was verified by the analysis of the 0.6PbTiO_(3)-0.4Bi(Ga_(x)Fe_(1-x))O_(3) system.So far,all PbTiO_(3)-based compounds with enhanced NTE conform well to this method.This method provides the possibility to find more enhanced NTE PbTiO_(3)-based materials.
基金supported by Jilin Changbaishan Volcano National Observation and Research Station(Project No.NORSCBS20-04)National Natural Science Foundation of China(42174023)the Fundamental Research Fund for the Central Universities of Central South University(No.506021722).
文摘Sentinel-1A/B data are crucial for retrieving numerical information about surface phenomena and processes.Coregistration of terrain observation by progressive scans(TOPS)data is a critical step in its application.TOPS data must be fundamentally co-registered with an accuracy of 0.001 pixels.However,various decorrelation factors due to natural vegetation and seasonal effects affect the coregistration accuracy of TOPS data.This paper proposed an enhanced spectral diversity coregistration method for dual-polarimetric(PolESD)Sentinel-1A/B TOPS data.The PolESD method suppresses speckle noise based on a unified non-local framework in dual-pol Synthetic Aperture Radar(SAR),and extracts the phase of the optimal polarization channel from the denoised polarimetric interferometric coherency matrix.Compared with the traditional ESD method developed for single-polarization data,the PolESD method can obtain more accurate coherence and phase and get more pixels for azimuth-offset estimation.In bare areas covered with low vegetation,the number of pixels selected by PolESD is more than the Boxcar method.It can also correct misregistration more effectively and eliminate phase jumps in the burst edge.Therefore,PolESD will help improve the application of TOPS data in low-coherence scenarios.
基金This work was supported by the National Natural Science Foundation of China （No. 11274,395）, the Program for Changjiang Scholars and Innovative Research Team in University （No. IRT13042） and the Open Fund of the Guangdong Provincial Key Laboratory of Optical Fiber Sensing and Communications （Jinan University）.
文摘Developing well-defined nanostructures with superior surface-enhanced Raman scattering （SERS） performance is a critical and highly desirable goal for the practical applications of SERS in sensing and analysis. Here, a SERS-active substrate was fabricated by decorating a MoS2 monolayer with Ag nanowire （NW） and nanoparticle （NP） structures, using a spin-coating method. Both experimental and theoretical results indicate that strong SERS signals of rhodamine 6G （R6G） molecules can be achieved at ＂hotspots＂ formed in the Ag NW-Ag NP-MoS2 hybrid structure, with an enhancement factor of 106. The SERS enhancement is found to be strongly polarization dependent. The fabricated SERS substrate also exhibits ultrasensitive detection capabilities with a detection limit of 10-11 M, as well as reliable reproducibility and good stability.
文摘Surface-enhanced resonance Raman scattering （SERRS） of Rhodamine 6G （R6G） adsorbed on colloidal silver clusters has been studied. Based on the great enhancement of the Raman signal and the quench of the fluorescence, the SERRS spectra of R6G were recorded for the samples of dye colloidal solution with different concentrations. Spectral inhomogeneity behaviours from single molecules in the dried sample films were observed with complementary evidences, such as spectral polarization, spectral diffusion, intensity fluctuation of vibrational lines and even ＂breathing＂ of the molecules. Sequential spectra observed from a liquid sample with an average of 0.3 dye molecules in the probed volume exhibited the expected Poisson distribution for actually measuring 0, 1 or 2 molecules. Difference between the SERRS spectra of R6G excited by linearly and circularly polarized light were experimentally measured.
文摘A novel approach of combining conventional infrared spectroscopy （IR） and atomic force microscopy （AFM） is presented to better understand the behavior of a drug adsorbed on a metal substrate at the nanoscale level. Tip-enhanced infrared nanospectroscopy （TEIRA） was used for the first time to investigate Lu AA33810, a selective brain-penetrating Y5 receptor antagonist, after immobilization on gold nanopartides （GNPs）. Here, a gold coated AFM tip and gold substrate were used to obtain the near-field electromagnetic field trapping effect. Because of the huge signal enhancement, it was possible to obtain the spectral information regarding the self-assembled monolayer of the investigated molecule. The effect of two orthogonal polarizations （p- and s-polarization modulations） of the excitation laser beam on the spectral patterns is also discussed. The results show that there is a strong relationship between the state of polarization of the incident radiation and the relative infrared band intensities. Another factor affecting the observed spectral differences is the topology of the metal substrate, which may result in the induction of a cross-polarization effect. The performed analysis indicates that the C--C bond from the cyclohexyl group is oriented almost parallel to the metal surface. Conversely, the p- and s-polarized spectral variations suggest that the O=S---O angle is high enough to enable the simultaneous interaction of both oxygen atoms with the GNPs.
