In modern science and technology,on-demand control of the polarization and wavefront of electromagnetic(EM)waves is crucial for compact opto-electronic systems.Metasurfaces composed of subwavelength array structures i...In modern science and technology,on-demand control of the polarization and wavefront of electromagnetic(EM)waves is crucial for compact opto-electronic systems.Metasurfaces composed of subwavelength array structures inject infinite vitality to shape this fantastic concept,which has fundamentally changed the way humans engineer matter–wave interactions.However,achieving full-space arbitrarily polarized beams with independent wavefronts in broadband on a single metasurface aperture still remains challenging.Herein,the authors propose a generic method for broadband transmission-reflection-integrated wavefronts shaping with multichannel arbitrary polarization regulation from 8 to 16 GHz,which is based on the chirality effect of full-space non-interleaved tetrameric meta-molecules.Through superimposing eigen-polarization responses of the two kinds of enantiomers,the possibility for high-efficiency evolution of several typical polarization states with specific wavefronts is demonstrated.As proofs-of-concept,the feasibility of our methodology is validated via implementing miscellaneous functionalities,including circularly polarized(CP)beam splitting,linearly polarized(LP)vortex beams generation,and CP and LP multifoci.Meanwhile,numerous simulated and experimental results are in excellent agreement with the theoretical predictions.Encouragingly,this proposed approach imaginatively merges broadband polarization and phase control into one single full-space and shared-aperture EM device,which can extremely enhance the functional richness and information capacity in advanced integrated systems.展开更多
Traditionally,magic cube configurations,which have been employed to mechanically execute diverse and unconventional structural transformations,are capable of significantly boosting versatile electromagnetic responses ...Traditionally,magic cube configurations,which have been employed to mechanically execute diverse and unconventional structural transformations,are capable of significantly boosting versatile electromagnetic responses of reconfigurable metamaterials.However,this idea is still in the initial exploration stage and faces many constraints.Here,we propose magic cube metamaterials with features of high transparency,multi-gradient phase distribution,full polarization,and high information,which manifest 47.58% optical transmittance,a 6-order phase distribution,a 77% fractional operating bandwidth,and 65.23 times information entropy of their planar counterparts.The reflection phase corresponding to coplanar lattice of the metamaterials can be dynamically and omni-directionally controlled via altering their spatial distributions through individually addressing each rotatable meta-particle while maintaining the polarization states.The optically transparent design allows for real-time visual interaction and sequence mapping of the reconfigurable metamaterials.As two proof-of-concept meta-devices,an achromatic metalens with an unchanged focal length and a switchable multi-functional beam generator is demonstrated by simulations and experiments in an ultra-wide band(8.0-18.0 GHz).This work provides an effective alternative for designing reconfigurable metamaterials with high information-entropy properties,paving a new route toward advanced equipment such as active signal processors and information encryption/decryption systems.展开更多
Surface-enhanced Raman spectroscopy(SERS)-based bioanalytical technique involves the interaction of SERS-active substrate with complex environment,which has aroused intensive research interests.Compared to the commonl...Surface-enhanced Raman spectroscopy(SERS)-based bioanalytical technique involves the interaction of SERS-active substrate with complex environment,which has aroused intensive research interests.Compared to the commonly used Au SERS substrates,Ag nanocrystals have larger optical absorption cross section and acceptable price,but they possess poor oxidation resistance and potential biotoxicity,and the occurrence of unnecessary chemical reactions is inevitable due to the direct contact with probe molecules.Herein,we report a graphene-isolated AuAg nanocrystal(GIAAN)with the SERS-active AuAg core confined in a nanospace of few-layer graphene shell,which possesses unique Raman peaks,high SERS activity,excellent stability,superior fluorescence quenching performance and good biocompatibility.Based on the limited solubility of GIAAN in water and organic solvents,it is able to spontaneously generate interfacial self-assembled GIAAN(ISA-GIAAN)film at immiscible two-phase interfaces without any inducer,and multiphase Raman analysis of both water-and lipid-soluble drug model molecules is further achieved.Moreover,the GIAAN is further non-covalently functionalized with polyoxyethylenestearyl ether(C18-PEG)to acquire GIAAN@PEG with good water-solubility for SERS quantitative analysis in homogeneous system and multimodal Raman imaging of MCF-7 cells.We expect the versatile GIAAN holds great potential to monitor drug metabolism and guide intended drug delivery in clinic trials.展开更多
As Interface mediated self-assembly of nanocrystals provide excellent strategy for sensing,catalysis or photonics,the construction of innovative interfaces and development of versatile strategies for nanocrystal synth...As Interface mediated self-assembly of nanocrystals provide excellent strategy for sensing,catalysis or photonics,the construction of innovative interfaces and development of versatile strategies for nanocrystal synthesis are urgently needed.Herein,latent fingerprints(LFPs),the most common markers for human identity,are used as naturally accessible interface for organization of graphene isolated nanocrystals(GINs).Excitingly,the selective adsorption of GINs on lipidic ridge provides a universal approach for the in-situ construction of the plasmonic arrays.Such system with intrinsic chrominance and Raman signal enables the high resolution colorimetric and surfaced-enhanced Raman spectroscopy(SERS)dual-mode imaging,which can detail the structures of the LFPs from 1st to 3rd level even the LFPs are shielded.Furthermore,the interface can be constructed on diverse materials by a simple finger-pressing process and the densely packed arrays can serve as superior SERS substrate for label-free,non-invasive acquisition of molecule information especially residues in LFPs.The combination of chemical composition with detailed structures efficiently recognizes the human identity and could help link it to a crime scene.Overall,the LFPs can act as natural platform for interface mediated localized assembly and personalized information acquisition for forensic science or precise medicine.展开更多
Complex biological environments and multiple physiological barriers significantly impede efficient accumulation and penetration of nanomaterials within tumor tissue for therapy.In situ energy conversion of nanomotors ...Complex biological environments and multiple physiological barriers significantly impede efficient accumulation and penetration of nanomaterials within tumor tissue for therapy.In situ energy conversion of nanomotors features autonomous movements and improves cancer treatment.However,one of the key challenges is to prepare nanomotors with an adequately small size,good biocompatibility,and precise positioning.Herein,we demonstrate a simple,ultrasmall,versatile,and real-time motion guidance strategy for magnetocatalytic CoPt@graphene navigators(MCGNs)that can enable highly efficient propulsion in the presence of H_(2)O_(2) or magnetic actuation.MCGNs act as highly diffusive delivery vehicles to promote tumor tissue targeting,and the amount of drug in the tumor was three times than without navigation.By engaging movements powered through in situ energy conversion,MCGNs gain considerable propulsion to penetrate a cell’s membrane and enhance intracellular delivery.展开更多
Reprogrammable metasurfaces,which establish a fascinating bridge between physical and information domains,can dynamically control electromagnetic(EM)waves in real time and thus have attracted great attentions from res...Reprogrammable metasurfaces,which establish a fascinating bridge between physical and information domains,can dynamically control electromagnetic(EM)waves in real time and thus have attracted great attentions from researchers around the world.To control EM waves with an arbitrary polarization state,it is desirable that a complete set of basis states be controlled independently since incident EM waves with an arbitrary polarization state can be decomposed as a linear sum of these basis states.In this work,we present the concept of complete-basis-reprogrammable coding metasurface(CBR-CM)in reflective manners,which can achieve independently dynamic controls over the reflection phases while maintaining the same amplitude for left-handed circularly polarized(LCP)waves and right-handed circularly polarized(RCP)waves.Since LCP and RCP waves together constitute a complete basis set of planar EM waves,dynamicallycontrolled holograms can be generated under arbitrarily polarized wave incidence.The dynamically reconfigurable metaparticle is implemented to demonstrate the CBR-CM’s robust capability of controlling the longitudinal and transverse positions of holograms under LCP and RCP waves independently.It’s expected that the proposed CBR-CM opens up ways of realizing more sophisticated and advanced devices with multiple independent information channels,which may provide technical assistance for digital EM environment reproduction.展开更多
Aggregation plays a critical role in modulating the photophysical process of organicmolecules.However,the rational control of the construction of a functionoriented stacking mode for efficient photothermal(PT)conversi...Aggregation plays a critical role in modulating the photophysical process of organicmolecules.However,the rational control of the construction of a functionoriented stacking mode for efficient photothermal(PT)conversion in the second near-infrared region(NIR-II;1000-1700 nm)remains a challenge.Herein,an H-aggregation of 3,3′,5,5′-Tetramethylbenzidine(TMB)-TMB dication(TMB++)complexes in linear agarose(H-TTC/LAG)with narrowed band gap(0.96 eV)was fabricated through intermolecular hydrogenbonding interactions between the amino groups of TTC and the peripheral hydroxyl groups of LAG.Charge-transfer mechanism and H-aggregation ensured NIR-Ⅱ absorption of the complex at>1400 nm.The H-aggregation also promoted a non-radiation relaxation pathway and improved the thermal stability of TTC,which together favored the constructed H-TTC/LAG with ultra-efficient PT conversion that increased rapidly to 140℃ in 15 s under the NIR-Ⅱ laser(1064 nm,1.0 W cm^(−2))irradiation.Such a unique H-TTC/LAG with good biocompatibility was used to demonstrate a superior PT therapy via high-efficie ncy tumor growth inhibition in mouse mammary carcinoma(4T1)the BALB/c mice tumor-bearing xenografts.This is the first established H-aggregation of charge-transfer complexes in a noncovalent system,which not only provides a new strategy to develop ultra-efficient NIR-Ⅱ PT materials but also paves the way for constructing functional materials with aggregates of charge-transfer complexes.展开更多
Reconfigurable metasurfaces enable dynamic and real-time manipulation of electromagnetic(EM)waves in subwavelength resolution,possessing unparalleled potentials to construct meta-devices.However,most existing reconfig...Reconfigurable metasurfaces enable dynamic and real-time manipulation of electromagnetic(EM)waves in subwavelength resolution,possessing unparalleled potentials to construct meta-devices.However,most existing reconfigurable metasurfaces either operate under single polarization or in limited polarization channels or discretely tailor EM variables within relatively narrow bandwidth,which are hard to adapt to the urgent development requirements of multitask and highly integrated intelligent communication systems.Herein,a reconfigurable metasurface strategy based on continuous amplitude modulation utilizing circularly polarized(CP)basis vectors is proposed and demonstrated,with which the orthogonal component energy proportion of an arbitrarily polarized wave can be tailored,achieving full-polarization customized broadband and versatile function generation and control.Two symmetrically positive–intrinsic–negative diodes embedded into split-ring resonators are employed to simultaneously and independently switch dual-channel co-polarized amplitude with almost unaltered phase,which significantly simplifies control framework and enhances information capacity.In addition,a fullpolarization reconfigurable metasurface prototype of 0.1λ0 thickness is designed and fabricated,which can continuously tune the reflection,polarization conversion,and absorption via loading different external bias voltages from 6 to 8.6 GHz.This inspiring methodology opens up routes for advanced multiplexed equipment and might find applications in future-oriented data storage and multi-input/multi-output systems.展开更多
基金National Key Research and Development Program of China(SQ2022YFB3806200)National Natural Science Foundation of China(62301596,62101588)+1 种基金Young Talent Fund of Association for Science and Technology in Shaanxi(20240129)Postdoctoral Fellowship Program of CPSF(GZC20242285)。
文摘In modern science and technology,on-demand control of the polarization and wavefront of electromagnetic(EM)waves is crucial for compact opto-electronic systems.Metasurfaces composed of subwavelength array structures inject infinite vitality to shape this fantastic concept,which has fundamentally changed the way humans engineer matter–wave interactions.However,achieving full-space arbitrarily polarized beams with independent wavefronts in broadband on a single metasurface aperture still remains challenging.Herein,the authors propose a generic method for broadband transmission-reflection-integrated wavefronts shaping with multichannel arbitrary polarization regulation from 8 to 16 GHz,which is based on the chirality effect of full-space non-interleaved tetrameric meta-molecules.Through superimposing eigen-polarization responses of the two kinds of enantiomers,the possibility for high-efficiency evolution of several typical polarization states with specific wavefronts is demonstrated.As proofs-of-concept,the feasibility of our methodology is validated via implementing miscellaneous functionalities,including circularly polarized(CP)beam splitting,linearly polarized(LP)vortex beams generation,and CP and LP multifoci.Meanwhile,numerous simulated and experimental results are in excellent agreement with the theoretical predictions.Encouragingly,this proposed approach imaginatively merges broadband polarization and phase control into one single full-space and shared-aperture EM device,which can extremely enhance the functional richness and information capacity in advanced integrated systems.
基金supported by the National Key Research and Development Program of China(SQ2022YFB3806200)the Shaanxi Province Innovation Capability Promotion Plan(2023-CX-TD-48)+2 种基金the National Natural Science Foundation of China(62401614,62401617)the China Postdoctoral Science Foundation(2023M734275)the Postdoctoral Fellowship Program of China Postdoctoral Science Foundation(GZC20233576)。
文摘Traditionally,magic cube configurations,which have been employed to mechanically execute diverse and unconventional structural transformations,are capable of significantly boosting versatile electromagnetic responses of reconfigurable metamaterials.However,this idea is still in the initial exploration stage and faces many constraints.Here,we propose magic cube metamaterials with features of high transparency,multi-gradient phase distribution,full polarization,and high information,which manifest 47.58% optical transmittance,a 6-order phase distribution,a 77% fractional operating bandwidth,and 65.23 times information entropy of their planar counterparts.The reflection phase corresponding to coplanar lattice of the metamaterials can be dynamically and omni-directionally controlled via altering their spatial distributions through individually addressing each rotatable meta-particle while maintaining the polarization states.The optically transparent design allows for real-time visual interaction and sequence mapping of the reconfigurable metamaterials.As two proof-of-concept meta-devices,an achromatic metalens with an unchanged focal length and a switchable multi-functional beam generator is demonstrated by simulations and experiments in an ultra-wide band(8.0-18.0 GHz).This work provides an effective alternative for designing reconfigurable metamaterials with high information-entropy properties,paving a new route toward advanced equipment such as active signal processors and information encryption/decryption systems.
基金the Hunan Provincial Natural Science Foundation of China(Nos.2020RC4017,2018JJ1007)the Science and Technology Development Fund,Macao(No.196/2017/A3).
文摘Surface-enhanced Raman spectroscopy(SERS)-based bioanalytical technique involves the interaction of SERS-active substrate with complex environment,which has aroused intensive research interests.Compared to the commonly used Au SERS substrates,Ag nanocrystals have larger optical absorption cross section and acceptable price,but they possess poor oxidation resistance and potential biotoxicity,and the occurrence of unnecessary chemical reactions is inevitable due to the direct contact with probe molecules.Herein,we report a graphene-isolated AuAg nanocrystal(GIAAN)with the SERS-active AuAg core confined in a nanospace of few-layer graphene shell,which possesses unique Raman peaks,high SERS activity,excellent stability,superior fluorescence quenching performance and good biocompatibility.Based on the limited solubility of GIAAN in water and organic solvents,it is able to spontaneously generate interfacial self-assembled GIAAN(ISA-GIAAN)film at immiscible two-phase interfaces without any inducer,and multiphase Raman analysis of both water-and lipid-soluble drug model molecules is further achieved.Moreover,the GIAAN is further non-covalently functionalized with polyoxyethylenestearyl ether(C18-PEG)to acquire GIAAN@PEG with good water-solubility for SERS quantitative analysis in homogeneous system and multimodal Raman imaging of MCF-7 cells.We expect the versatile GIAAN holds great potential to monitor drug metabolism and guide intended drug delivery in clinic trials.
基金supported by the National Key Research and Development Program of China(No.2020YFA0210800)the National Natural Science Foundation of China(No.21522501)+1 种基金the Science and Technology Innovation Program of Hunan Province(No.2020RC4017)the Science and Technology Development Fund,Macao(No.196/2017/A3).
文摘As Interface mediated self-assembly of nanocrystals provide excellent strategy for sensing,catalysis or photonics,the construction of innovative interfaces and development of versatile strategies for nanocrystal synthesis are urgently needed.Herein,latent fingerprints(LFPs),the most common markers for human identity,are used as naturally accessible interface for organization of graphene isolated nanocrystals(GINs).Excitingly,the selective adsorption of GINs on lipidic ridge provides a universal approach for the in-situ construction of the plasmonic arrays.Such system with intrinsic chrominance and Raman signal enables the high resolution colorimetric and surfaced-enhanced Raman spectroscopy(SERS)dual-mode imaging,which can detail the structures of the LFPs from 1st to 3rd level even the LFPs are shielded.Furthermore,the interface can be constructed on diverse materials by a simple finger-pressing process and the densely packed arrays can serve as superior SERS substrate for label-free,non-invasive acquisition of molecule information especially residues in LFPs.The combination of chemical composition with detailed structures efficiently recognizes the human identity and could help link it to a crime scene.Overall,the LFPs can act as natural platform for interface mediated localized assembly and personalized information acquisition for forensic science or precise medicine.
基金financially supported by the National Natural Science Foundation of China(grant no.21522501)Hunan Provincial Natural Science Foundation of China(grant no.2020RC4017)+1 种基金National Postdoctoral Program for Innovative Talents of China(grant no.BX20190111)the Science and Technology Development Fund,Macao(no.196/2017/A3).
文摘Complex biological environments and multiple physiological barriers significantly impede efficient accumulation and penetration of nanomaterials within tumor tissue for therapy.In situ energy conversion of nanomotors features autonomous movements and improves cancer treatment.However,one of the key challenges is to prepare nanomotors with an adequately small size,good biocompatibility,and precise positioning.Herein,we demonstrate a simple,ultrasmall,versatile,and real-time motion guidance strategy for magnetocatalytic CoPt@graphene navigators(MCGNs)that can enable highly efficient propulsion in the presence of H_(2)O_(2) or magnetic actuation.MCGNs act as highly diffusive delivery vehicles to promote tumor tissue targeting,and the amount of drug in the tumor was three times than without navigation.By engaging movements powered through in situ energy conversion,MCGNs gain considerable propulsion to penetrate a cell’s membrane and enhance intracellular delivery.
基金supported by the National Natural Science Foundation of China (62101588)the National Key Research and Development Program of China (SQ2022YFB3806200)+1 种基金the Young Talent Fund of Association for Science and Technology in Shaanxi (20240129)the Postdoctoral Fellowship Program of CPSF (GZC20242285)
文摘Reprogrammable metasurfaces,which establish a fascinating bridge between physical and information domains,can dynamically control electromagnetic(EM)waves in real time and thus have attracted great attentions from researchers around the world.To control EM waves with an arbitrary polarization state,it is desirable that a complete set of basis states be controlled independently since incident EM waves with an arbitrary polarization state can be decomposed as a linear sum of these basis states.In this work,we present the concept of complete-basis-reprogrammable coding metasurface(CBR-CM)in reflective manners,which can achieve independently dynamic controls over the reflection phases while maintaining the same amplitude for left-handed circularly polarized(LCP)waves and right-handed circularly polarized(RCP)waves.Since LCP and RCP waves together constitute a complete basis set of planar EM waves,dynamicallycontrolled holograms can be generated under arbitrarily polarized wave incidence.The dynamically reconfigurable metaparticle is implemented to demonstrate the CBR-CM’s robust capability of controlling the longitudinal and transverse positions of holograms under LCP and RCP waves independently.It’s expected that the proposed CBR-CM opens up ways of realizing more sophisticated and advanced devices with multiple independent information channels,which may provide technical assistance for digital EM environment reproduction.
基金financially supported by the National Natural Science Foundation of China(grant nos.91953000 and 21827811)the Science and Technology Innovation Program of Hunan Province(grant nos.2019SK2201 and 2020RC4017)the Science and Technology Development Fund,Macao(grant no.196/2017/A3).
文摘Aggregation plays a critical role in modulating the photophysical process of organicmolecules.However,the rational control of the construction of a functionoriented stacking mode for efficient photothermal(PT)conversion in the second near-infrared region(NIR-II;1000-1700 nm)remains a challenge.Herein,an H-aggregation of 3,3′,5,5′-Tetramethylbenzidine(TMB)-TMB dication(TMB++)complexes in linear agarose(H-TTC/LAG)with narrowed band gap(0.96 eV)was fabricated through intermolecular hydrogenbonding interactions between the amino groups of TTC and the peripheral hydroxyl groups of LAG.Charge-transfer mechanism and H-aggregation ensured NIR-Ⅱ absorption of the complex at>1400 nm.The H-aggregation also promoted a non-radiation relaxation pathway and improved the thermal stability of TTC,which together favored the constructed H-TTC/LAG with ultra-efficient PT conversion that increased rapidly to 140℃ in 15 s under the NIR-Ⅱ laser(1064 nm,1.0 W cm^(−2))irradiation.Such a unique H-TTC/LAG with good biocompatibility was used to demonstrate a superior PT therapy via high-efficie ncy tumor growth inhibition in mouse mammary carcinoma(4T1)the BALB/c mice tumor-bearing xenografts.This is the first established H-aggregation of charge-transfer complexes in a noncovalent system,which not only provides a new strategy to develop ultra-efficient NIR-Ⅱ PT materials but also paves the way for constructing functional materials with aggregates of charge-transfer complexes.
基金National Natural Science Foundation of China(62101588,62301596)National Key Research and Development Program of China(SQ2022YFB3806200).
文摘Reconfigurable metasurfaces enable dynamic and real-time manipulation of electromagnetic(EM)waves in subwavelength resolution,possessing unparalleled potentials to construct meta-devices.However,most existing reconfigurable metasurfaces either operate under single polarization or in limited polarization channels or discretely tailor EM variables within relatively narrow bandwidth,which are hard to adapt to the urgent development requirements of multitask and highly integrated intelligent communication systems.Herein,a reconfigurable metasurface strategy based on continuous amplitude modulation utilizing circularly polarized(CP)basis vectors is proposed and demonstrated,with which the orthogonal component energy proportion of an arbitrarily polarized wave can be tailored,achieving full-polarization customized broadband and versatile function generation and control.Two symmetrically positive–intrinsic–negative diodes embedded into split-ring resonators are employed to simultaneously and independently switch dual-channel co-polarized amplitude with almost unaltered phase,which significantly simplifies control framework and enhances information capacity.In addition,a fullpolarization reconfigurable metasurface prototype of 0.1λ0 thickness is designed and fabricated,which can continuously tune the reflection,polarization conversion,and absorption via loading different external bias voltages from 6 to 8.6 GHz.This inspiring methodology opens up routes for advanced multiplexed equipment and might find applications in future-oriented data storage and multi-input/multi-output systems.
