A series of isostructural d/f molecular compounds Zn（H2L）Ln（NO3）3·CH3OH（Ln = Dy（1）, Tb（2） and Sm（3）） were synthesized by the introduction of a designed multifunctional ligand N,N？,N？？,N？？？-tetra...A series of isostructural d/f molecular compounds Zn（H2L）Ln（NO3）3·CH3OH（Ln = Dy（1）, Tb（2） and Sm（3）） were synthesized by the introduction of a designed multifunctional ligand N,N？,N？？,N？？？-tetra（2-hydroxy-3-methoxy-5-methylbenzyl）-1,4,7,10-tetraazacyclododecan（H4L = C（44）H（60）N4O8）. In the isostructural molecules, each crystallographically independent Zn2＋ and Ln3＋ centers are connected by two phenolic oxygen atoms. For the six-coordinate Zn-（2＋） ion, the coordination geometry can be viewed as a regular bicapped square pyramid. While for the ten-coordinate Ln-（3＋） ion, if each O,O？-chelated nitrate ligand is seen as a single coordination site, the coordination geometry can be viewed as a distorted pentagonal bipyramid. The fluorescent spectra show that compounds 2 and 3 exhibited characteristic sharp emissions of Tb-（3＋） and Sm-（3＋）, respectively, while compound 1 was found to be a single-component white-light-emitting complex in the solid state. Thermal stabilities of the three compounds were investigated by using thermal gravimetric analysis. In addition, the thermal decomposition of compound 1 was confirmed by temperature-dependent powder X-ray diffraction technique.展开更多
We present a digital micromirror device（DMD） based superpixel method for focusing light through scattering media by modulating the complex field of incident light. Firstly, we numerically and experimentally investig...We present a digital micromirror device（DMD） based superpixel method for focusing light through scattering media by modulating the complex field of incident light. Firstly, we numerically and experimentally investigate focusing light through a scattering sample using the superpixel methods with different target complex fields.Then, single-point and multiple-point focusing experiments are performed using this superpixel-based complex modulation method. In our experiment, up to 71.5% relative enhancement is realized. The use of the DMDbased superpixel method for the control of the complex field of incident light opens an avenue to improve the enhancement of focusing light through scattering media.展开更多
Energy transfers in two kinds of peripheral light-harvesting complexes （LH2） of Rhodobacter sphaeroides （RS） 601 are studied by using femtosecond pump^probe spectroscopy with tunable laser wavelength at room tempe...Energy transfers in two kinds of peripheral light-harvesting complexes （LH2） of Rhodobacter sphaeroides （RS） 601 are studied by using femtosecond pump^probe spectroscopy with tunable laser wavelength at room temperature. These two complexes are native LH2 （RS601） and green carotenoid mutated LH2 （GM309）. The obtained results demonstrate that, compared with spheroidenes with ten conjugated double bonds in native RS601, carotenoid in GM309 containing neurosporenes with nine conjugated double bonds can lead to a reduction in energy transfer rate in the B800-to-B850 band and the disturbance in the energy relaxation processes within the excitonic B850 band.展开更多
Thermo-responsive light-emitting materials have wide potential applications in temperature sensing,bioimaging,optoelectronic devices and information security,due to their intriguing luminescence property changes in re...Thermo-responsive light-emitting materials have wide potential applications in temperature sensing,bioimaging,optoelectronic devices and information security,due to their intriguing luminescence property changes in response to temperature.Among them,light-emitting metal complexes and related coordination materials are appealing in possessing enormous structural diversity and excellent luminescence properties.The general thermo-responsive types and the underlying mechanism of these materials and recent progress in the development of thermo-responsive metal complexes and related materials are surveyed in this critical review,including small molecular metal complexes with different electronic configurations (d^(6),d^(8),d^(10),among others),metal clusters,coordination polymers,metal–organic frameworks (MOFs),and multicomponent coordination polymers and assemblies.A particular focus is given on how to build systems showing ratiometric luminescence changes in response to temperature,including molecular dyads containing two chromophores,heterodimetallic clusters,mixed-metal MOFs,and energy donor–acceptor assemblies.In addition,the applications of these materials in temperature sensing,bioimaging,and information security are briefly discussed.A perspective is given in the Conclusion section to reflect potential guidelines for future research in this field.展开更多
Complex field modulation(CFM)has found a plethora of applications in physics,biomedicine,and instrumentation.Among existing methods,superpixel-based CFM has been increasingly featured because of its advantages in high...Complex field modulation(CFM)has found a plethora of applications in physics,biomedicine,and instrumentation.Among existing methods,superpixel-based CFM has been increasingly featured because of its advantages in high modulation accuracy and its compatibility with high-speed spatial light modulators(SLMs).Nonetheless,the mainstream approach based on binary-amplitude modulation confronts limitations in optical efficiency and dynamic range.To surmount these challenges,we develop binary phase-engraved(BiPE)superpixel-based CFM and implement it using the phase light modulator(PLM)—a new micro-electromechanical system-based SLM undergoing development by Texas Instruments in recent years.Using BiPE superpixels,we demonstrate highaccuracy spatial amplitude and phase modulation at up to 1.44 kHz.To showcase its broad utility,we apply BiPEsuperpixel-based CFM to beam shaping,high-speed projection,and augmented-reality display.展开更多
Appressed and non-appressed lamella membranes of Castor bean leaf chloroplasts were separated by non-ionic detergent Triton-X 100.Appressed membranes showed a high oxygen-evolving activity and low chl a/b ratio. Exami...Appressed and non-appressed lamella membranes of Castor bean leaf chloroplasts were separated by non-ionic detergent Triton-X 100.Appressed membranes showed a high oxygen-evolving activity and low chl a/b ratio. Examining with SDS-PTGE and liquid nitrogen temperature fluorescence measurement showed that they contained only PSII and light-harvesting pigment-protein complexes (LHCP),and there was no detectable amount of PSI. Freeze-fracture electromicroscopic observation confirmed that this part was really an appressed lamella membrane. Through divalent cation Mg^(++), the thylakoid membranes were induced to unstack and restack.With the addition of Mg^(++), the fluorescence intensity was changed instantly. We realized that there existed two processes:One was a rapid process which was accomplished within 30 s. The other was a slow process of which the time duration was about 60 min. This dual effects of Mg^(++) had not been reported before.We had analyzed the change of F685/F730 and discussed the possible rneehanis ms of light energy distribution between photosystems.展开更多
Structured light,where light is tailored in all its degrees of freedom,has shown tremendous power in unlocking new modalities of light,with its impact felt across dimensions,disciplines,and applications.This richly te...Structured light,where light is tailored in all its degrees of freedom,has shown tremendous power in unlocking new modalities of light,with its impact felt across dimensions,disciplines,and applications.This richly textured light comes with deeply embedded complexity,making the design,analysis,and recognition of such complex light patterns highly non-trivial.In recent years artificial intelligence(AI)has come to the fore,not only for the design,characterization,and optimization of structured light but also for increasingly important roles in adding new functionalities and breaking old paradigms.An exciting twist is the flip side of the coin,where complex light in complex media acts as a light-speed neural network,ushering in a new era of ultrafast optical-based“machines”for intelligence and learning.In this review,we focus on how AI has enhanced structured light technologies,and vice versa,touching on imaging,microscopy,sensing,communication,and optical neural networks as topical application areas,while covering scales from the macroscopic to the microscopic,and from classical to quantum.We highlight the symbiotic relationship between intelligence and light in these processes and offer a perspective on the open challenges and future prospects of this emerging research direction.展开更多
It is well known that the entanglement of a quantum state is invariant under local unitary transformations.This rule dictates,for example,that the entanglement of internal degrees of freedom of a photon remains invari...It is well known that the entanglement of a quantum state is invariant under local unitary transformations.This rule dictates,for example,that the entanglement of internal degrees of freedom of a photon remains invariant during free-space propagation.Here,we outline a scenario in which this paradigm does not hold.Using local Bell states engineered from classical vector vortex beams with non-separable degrees of freedom,the so-called classically entangled states,we demonstrate that the entanglement evolves during propagation,oscillating between maximally entangled(purely vector)and product states(purely scalar).We outline the spin–orbit interaction behind these novel propagation dynamics and confirm the results experimentally,demonstrating spin–orbit coupling in paraxial beams.This demonstration highlights a hitherto unnoticed property of classical entanglement and simultaneously offers a device for the on-demand delivery of vector states to targets,for example,for dynamic laser materials processing,switchable resolution within stimulated emission depletion(STED)systems,and a tractor beam for entanglement.展开更多
基金supported by the Natural Science Foundation of China(No.21171165,21201165 and 91122015)
文摘A series of isostructural d/f molecular compounds Zn（H2L）Ln（NO3）3·CH3OH（Ln = Dy（1）, Tb（2） and Sm（3）） were synthesized by the introduction of a designed multifunctional ligand N,N？,N？？,N？？？-tetra（2-hydroxy-3-methoxy-5-methylbenzyl）-1,4,7,10-tetraazacyclododecan（H4L = C（44）H（60）N4O8）. In the isostructural molecules, each crystallographically independent Zn2＋ and Ln3＋ centers are connected by two phenolic oxygen atoms. For the six-coordinate Zn-（2＋） ion, the coordination geometry can be viewed as a regular bicapped square pyramid. While for the ten-coordinate Ln-（3＋） ion, if each O,O？-chelated nitrate ligand is seen as a single coordination site, the coordination geometry can be viewed as a distorted pentagonal bipyramid. The fluorescent spectra show that compounds 2 and 3 exhibited characteristic sharp emissions of Tb-（3＋） and Sm-（3＋）, respectively, while compound 1 was found to be a single-component white-light-emitting complex in the solid state. Thermal stabilities of the three compounds were investigated by using thermal gravimetric analysis. In addition, the thermal decomposition of compound 1 was confirmed by temperature-dependent powder X-ray diffraction technique.
基金Supported by the Natural Science Foundation of Beijing under Grant Nos 2162033 and 7182091the National Natural Science Foundation of China under Grant No 21627813
文摘We present a digital micromirror device（DMD） based superpixel method for focusing light through scattering media by modulating the complex field of incident light. Firstly, we numerically and experimentally investigate focusing light through a scattering sample using the superpixel methods with different target complex fields.Then, single-point and multiple-point focusing experiments are performed using this superpixel-based complex modulation method. In our experiment, up to 71.5% relative enhancement is realized. The use of the DMDbased superpixel method for the control of the complex field of incident light opens an avenue to improve the enhancement of focusing light through scattering media.
基金the National Natural Science Foundation of China，the National Basic Research Program，the Strategic Priority Research Program of Chinese Academy of Sciences
基金Project supported by the National Natural Science Foundation of China （Grant No 10274013）.
文摘Energy transfers in two kinds of peripheral light-harvesting complexes （LH2） of Rhodobacter sphaeroides （RS） 601 are studied by using femtosecond pump^probe spectroscopy with tunable laser wavelength at room temperature. These two complexes are native LH2 （RS601） and green carotenoid mutated LH2 （GM309）. The obtained results demonstrate that, compared with spheroidenes with ten conjugated double bonds in native RS601, carotenoid in GM309 containing neurosporenes with nine conjugated double bonds can lead to a reduction in energy transfer rate in the B800-to-B850 band and the disturbance in the energy relaxation processes within the excitonic B850 band.
基金support from the National Science Fund for Distinguished Young Scholars(No.21925112)the National Natural Science Foundation of China(grants 21601194 and 21872154)the Beijing Natural Science Foundation(grant 2191003).
文摘Thermo-responsive light-emitting materials have wide potential applications in temperature sensing,bioimaging,optoelectronic devices and information security,due to their intriguing luminescence property changes in response to temperature.Among them,light-emitting metal complexes and related coordination materials are appealing in possessing enormous structural diversity and excellent luminescence properties.The general thermo-responsive types and the underlying mechanism of these materials and recent progress in the development of thermo-responsive metal complexes and related materials are surveyed in this critical review,including small molecular metal complexes with different electronic configurations (d^(6),d^(8),d^(10),among others),metal clusters,coordination polymers,metal–organic frameworks (MOFs),and multicomponent coordination polymers and assemblies.A particular focus is given on how to build systems showing ratiometric luminescence changes in response to temperature,including molecular dyads containing two chromophores,heterodimetallic clusters,mixed-metal MOFs,and energy donor–acceptor assemblies.In addition,the applications of these materials in temperature sensing,bioimaging,and information security are briefly discussed.A perspective is given in the Conclusion section to reflect potential guidelines for future research in this field.
基金supported in part by the Natural Sciences and Engineering Research Council of Canada(Grant Nos.RGPIN-2024-05551,ALLRP 592389-23)the Canada Research Chairs Program(Grant No.CRC-2022-00119)the Fonds de Recherche du Québec–Nature et Technologies(Grant Nos.203345–Centre d’Optique,Photonique,et Lasers).
文摘Complex field modulation(CFM)has found a plethora of applications in physics,biomedicine,and instrumentation.Among existing methods,superpixel-based CFM has been increasingly featured because of its advantages in high modulation accuracy and its compatibility with high-speed spatial light modulators(SLMs).Nonetheless,the mainstream approach based on binary-amplitude modulation confronts limitations in optical efficiency and dynamic range.To surmount these challenges,we develop binary phase-engraved(BiPE)superpixel-based CFM and implement it using the phase light modulator(PLM)—a new micro-electromechanical system-based SLM undergoing development by Texas Instruments in recent years.Using BiPE superpixels,we demonstrate highaccuracy spatial amplitude and phase modulation at up to 1.44 kHz.To showcase its broad utility,we apply BiPEsuperpixel-based CFM to beam shaping,high-speed projection,and augmented-reality display.
文摘Appressed and non-appressed lamella membranes of Castor bean leaf chloroplasts were separated by non-ionic detergent Triton-X 100.Appressed membranes showed a high oxygen-evolving activity and low chl a/b ratio. Examining with SDS-PTGE and liquid nitrogen temperature fluorescence measurement showed that they contained only PSII and light-harvesting pigment-protein complexes (LHCP),and there was no detectable amount of PSI. Freeze-fracture electromicroscopic observation confirmed that this part was really an appressed lamella membrane. Through divalent cation Mg^(++), the thylakoid membranes were induced to unstack and restack.With the addition of Mg^(++), the fluorescence intensity was changed instantly. We realized that there existed two processes:One was a rapid process which was accomplished within 30 s. The other was a slow process of which the time duration was about 60 min. This dual effects of Mg^(++) had not been reported before.We had analyzed the change of F685/F730 and discussed the possible rneehanis ms of light energy distribution between photosystems.
基金National Natural Science Foundation of China(62375015)National Natural Science Foundation of China(U23A20481,62275010)+7 种基金Open Fund of the State Key Laboratory of Precision Space–time Information Sensing Technology No.STL2023-B-03-01(J)Fundamental Research Funds for the Central Universities(2025CX11009)South African Quantum Technology Initiative(SAQuTI),OpticaNanyang Assistant Professorship Start Up Grant,Singapore Ministry of Education(MOE)AcRF Tier 1 grant(RG157/23)MoE AcRF Tier 1 Thematic grant(RT11/23)Imperial-Nanyang Technological University Collaboration Fund(INCF-2024-007)Nanyang Technological University SPMS Collaborative Research Award 2024Singapore Agency for Science,Technology and Research(A*STAR)MTC Individual Research Grants(M24N7c0080).
文摘Structured light,where light is tailored in all its degrees of freedom,has shown tremendous power in unlocking new modalities of light,with its impact felt across dimensions,disciplines,and applications.This richly textured light comes with deeply embedded complexity,making the design,analysis,and recognition of such complex light patterns highly non-trivial.In recent years artificial intelligence(AI)has come to the fore,not only for the design,characterization,and optimization of structured light but also for increasingly important roles in adding new functionalities and breaking old paradigms.An exciting twist is the flip side of the coin,where complex light in complex media acts as a light-speed neural network,ushering in a new era of ultrafast optical-based“machines”for intelligence and learning.In this review,we focus on how AI has enhanced structured light technologies,and vice versa,touching on imaging,microscopy,sensing,communication,and optical neural networks as topical application areas,while covering scales from the macroscopic to the microscopic,and from classical to quantum.We highlight the symbiotic relationship between intelligence and light in these processes and offer a perspective on the open challenges and future prospects of this emerging research direction.
基金support from the German Research Foundation DFG(EXC 1003–CiM,TRR61)CRG from the Claude Leon foundationBN from the National Research Foundation of South Africa.
文摘It is well known that the entanglement of a quantum state is invariant under local unitary transformations.This rule dictates,for example,that the entanglement of internal degrees of freedom of a photon remains invariant during free-space propagation.Here,we outline a scenario in which this paradigm does not hold.Using local Bell states engineered from classical vector vortex beams with non-separable degrees of freedom,the so-called classically entangled states,we demonstrate that the entanglement evolves during propagation,oscillating between maximally entangled(purely vector)and product states(purely scalar).We outline the spin–orbit interaction behind these novel propagation dynamics and confirm the results experimentally,demonstrating spin–orbit coupling in paraxial beams.This demonstration highlights a hitherto unnoticed property of classical entanglement and simultaneously offers a device for the on-demand delivery of vector states to targets,for example,for dynamic laser materials processing,switchable resolution within stimulated emission depletion(STED)systems,and a tractor beam for entanglement.
