Circularly polarized luminescence(CPL)and two-photon absorption(TPA)materials have garnered considerable attentions due to their minimal energy loss and superior optical penetration[1,2].However,the current challenge ...Circularly polarized luminescence(CPL)and two-photon absorption(TPA)materials have garnered considerable attentions due to their minimal energy loss and superior optical penetration[1,2].However,the current challenge lies in the absence of well-developed strategies for designing materials that combine these two exceptional optical properties.展开更多
Strong feld-induced nonsequential double ionization(NSDI)is a signifcant multi-electron phenomenon that provides crucial insights into understanding electron correlation and multiple ionization of atoms and molecules,...Strong feld-induced nonsequential double ionization(NSDI)is a signifcant multi-electron phenomenon that provides crucial insights into understanding electron correlation and multiple ionization of atoms and molecules,but it is typically unattainable in a circularly polarized laser pulse,especially for long-wavelength lasers.We present evidence that NSDI can occur in the presence of a near-infrared or beyond laser pulse by introducing a bowtie-nanotip.The laser-induced local plasmon can alter the local ellipticity of the feld,thereby enabling NSDI through elliptical trajectories that facilitate recollisions with parent atoms.An oval-shaped momentum distribution of recoiled ions provides evidence for the modifcation of trajectories by the aligned nanotips.Our study introduces an innovative control knob to manipulate NSDI and electron dynamics through the utilization of nanostructures.展开更多
Symmetry breaking,a critical phenomenon in both natural and artificial systems,is pivotal in constructing chiral structures from achiral building units.This study focuses on the achiral molecule 8,8',8'',8...Symmetry breaking,a critical phenomenon in both natural and artificial systems,is pivotal in constructing chiral structures from achiral building units.This study focuses on the achiral molecule 8,8',8'',8'''-((pyrazine-2,3,5,6-tetrayltetrakis(benzene-4,1-iyl))tetrakis(oxy))tetrakis(octan-1-ol)(TPP-C8OH),an aggregation-induced emission(AIE)molecule,to explore its symmetry breaking behavior in supramolecular assembly.By analyzing TPP-C8OH in various solvents—both non-chiral and chiral—we find that chiral solvents significantly enhance the molecule's symmetry breaking and chiroptical properties.Specially,alcohol solvents,particularly dodecyl alcohol,facilitate the formation of helical structures with both left-handed(M)and right-handed(P)helices within single twisted nanoribbons.This observation contrasts with previously reported symmetry breaking phenomena in assembly systems.Chiral solvents induce assemblies with distinct helical orientations,resulting in notable circularly polarized luminescence(CPL)and circular dichroism(CD)signals.This study elucidates the impact of solvent choice on symmetry breaking and chiral assembly,offering insights into the design of advanced chiral materials with tailored self-assembly processes.展开更多
Perovskites showcased potential promise for innovative circularly polarized luminescence (CPL)-active multi-channelinformation encryption, owing to the exceptional luminescence brightness. It was still a formidablecha...Perovskites showcased potential promise for innovative circularly polarized luminescence (CPL)-active multi-channelinformation encryption, owing to the exceptional luminescence brightness. It was still a formidablechallenge to fabricate CPL-active perovskites with significant luminescent asymmetry factor (glum) and full-colour-tailorableCPL properties. Indeed, compared to isotropic perovskites, anisotropic perovskite nanowires (NWs)were conducive to carrier separation and transport for polarization enhancement. Herein, three types of CsPb(Br/I)3 NWs with green, orange, red fluorescence (FL) were respectively synthesized and assembled into chiral NWfilms. The right-handed/left-handed chiral NW films constructed by 4+4 layers and 45° inter-angles exhibitshighly symmetric and mirror-like chiral signals. The strongest chiral intensity is more than 3000 medg. CPLsignals with wide colour gamut produce ranging from 480 nm to 800 nm, and tailorable CPL wavelengths aremanipulated by the emission wavelength of perovskite NWs. A giant CPL signal with a maximum glum of up to 10^(-1) is achieved. The polarization imaging of chiral NW films produces brilliant differential circularly polarizedstructural colours, making it more widely used in multilevel anti-counterfeiting systems. A significant break-throughlies in the development of advanced chiral perovskite materials with remarkable glum and tailorable CPLproperties, which sheds new light on optical anti-counterfeiting and intelligent information encryption.展开更多
The development of circularly polarized luminescence (CPL) materials from simple organic molecules is of critical importance for advancing their practical applications, yet it remains hindered by challenges such as lo...The development of circularly polarized luminescence (CPL) materials from simple organic molecules is of critical importance for advancing their practical applications, yet it remains hindered by challenges such as low dissymmetry factors (glum) and complex synthetic process. Herein, we report a facile one-step [2+2] condensation strategy to access a Schiff-base pyrene dimer featuring 1,6-substituted pyrenes and trans-1,2-diaminocyclohexane units in 77% yield. Taking advantages of face-to-face π-π stacking of pyrene rings in the constrained D_(2) symmetric structure, intense excimer CPL was successfully realized with a |glum| value of 0.021 and a CPL brightness, BCPL, value of 154.5 M-1·cm-1. The optimized excited state structures reveal that the high |glum| value arises from the parallel arrangement of electric and magnetic dipole transition moments. Importantly, the rigid pyrene dimer architecture ensures robust CPL performance invariant under diverse conditions, including changes in temperature, concentration, and solvents, as well as in polymer films.展开更多
Although many racemic M4L6cages have been synthesized,little attention has been paid to the resolution of M4L6cages because resolution of these cages is very difficult.To explore the use of optically pure M4L6cages in...Although many racemic M4L6cages have been synthesized,little attention has been paid to the resolution of M4L6cages because resolution of these cages is very difficult.To explore the use of optically pure M4L6cages in chiral applications,it is important to obtain a single enantiomer.In this work,the anionicΛΛΛΛ-Zr_(4)L_(6)andΛΛΛΛ-Zr_(4)L_(6)(L=embonate)cages have been completely separated by introducing chiral organic ligands R/S-BINAP and 1S,2S/1R,2R-DPEN,respectively,and the active vertex of homochiral Zr_(4)L_(6)cage trapsπ-conjugated coordination silver cations(such as[Ag_(2)(DPPM)_(2)]^(2+),chiral[Ag_(2)(PPh_(3))_(2)(DPEN)]^(2+)and[Ag(PPh_(3))(DPEN)]^(+)),obtaining two pair of pure enantiomers(PTC-375(Λ/Λ)and PTC-376(Λ/Λ)).Interestingly,the chiral resolution and surface modification of such zirconium cage endow it with homochirality and significant circularly polarized luminescence(CPL)response,and PTC-376 enantiomers show a CPL output with glumvalues up to~1.4×10^(-2).This work not only provides a new resolution strategy for metal-organic cages,but also expands their chiral application especially in CPL field.展开更多
Recently circularly polarized luminescence(CPL)materials have attracted significant interest.Introducing reversible dynamic property to these materials has been a key focus in cutting-edge fields,such as in high-level...Recently circularly polarized luminescence(CPL)materials have attracted significant interest.Introducing reversible dynamic property to these materials has been a key focus in cutting-edge fields,such as in high-level information encryption.Here,we provided a novel and general strategy involving handednessselective filtration and ground-state chiral self-recovery(CSR)in double film system to address this issue.Based on this strategy,we achieved CPL switch through the reversible modulation of ground-state chirality including absorption and scattering circular dichroism(CD)signals over the full UV-visible wavelength range(365-700 nm)in a single azobenzene polymer(PAzo)film.More importantly,by flexibly changing the type of fluorescent films,it is convenient to achieve general excited-state CSR,that is reversible switching of full-color including ideal white(CIE coordinate(0.33,0.33)),as well as room-temperature phosphorescent CPL.All these CPL signals without almost any intensity decay after three cycles of onand-off switching.Experimental results indicated that the trans-cis isomerization and ordered rearrangement of azobenzene units in PAzo film were the fundamental reasons for realizing CPL switching.Finally,based on this system we achieved dynamic visual encryption and decryption process including multiple decryption methods.This study provides an effective method for constructing a universally applicable chiroptical switch in excited state.展开更多
Non-covalent interactions-driven host-vip assembly based on metallo-tweezers has been used to construct varied optical functional materials with attractive structures and properties.We reported here two pairs of chi...Non-covalent interactions-driven host-vip assembly based on metallo-tweezers has been used to construct varied optical functional materials with attractive structures and properties.We reported here two pairs of chiral gold(Ⅰ)-based metallo-tweezers as hosts to clip Ag^(Ⅰ)or Cu^(Ⅰ)cations for circularly polarized phosphorescence(CPP),driven by the integration of two-fold coordination and heterometallophilic interactions.The Au^(Ⅰ)-based hosts and metal ions-vips formed sandwich structures in 1:1 ratio with high binding affinity.The achieved tweezer/cation adducts exhibited red-shifted absorption bands and circular dichroism signals,which were attributed to the newly formed ligand to metal-metal charge transfer process.Remarkably,the host-vip supramolecular adducts showed turn-on phosphorescence and CPP,which benefited from rigidifying effect of multiple intermolecular interactions and shorter excited-state lifetime.Overall,our findings bring new insights into the feasibility to achieve and modulate CPP performance by fabricating metallo-tweezer-based host-vip complexes.展开更多
A millimeter-wave (mmW) broadband dual circularly polarized (dual-CP) antenna with high port isolation is proposed in this paper. The dual-CP performance is realized based on the symmetrical septum circular polarizer ...A millimeter-wave (mmW) broadband dual circularly polarized (dual-CP) antenna with high port isolation is proposed in this paper. The dual-CP performance is realized based on the symmetrical septum circular polarizer based on the gap waveguide (GWG) technology. Two sets of symmetrical septum circular polarizers are used for common aperture combination,achieving the broadband dual-CP characteristics. Taking advantage of GWG structure without good electrical contact, the antenna can also be fabricated and assembled easily in the mmW band. The principle analysis of the antenna is given, and the antenna is simulated and fabricated. The measured results show that the bandwidth for S11lower than-10.7 dB and the axial ratio (AR) lower than 2.90 dB in 75-110 GHz, with realative bandwidth of 38%. Over the frequency band, the gain is higher than 9.16 dBic, and the dual-CP port isolation is greater than32 dB. The proposed antenna with dual-CP and highly isolated in a wide bandwidth range has broad application prospects in the field of mmW communication.展开更多
Metal-complexed chiral macrocyclic architectures have attracted increasing research interests in circularly polarized luminescence owing to their distinctive structural and functional attributes.The method of metal co...Metal-complexed chiral macrocyclic architectures have attracted increasing research interests in circularly polarized luminescence owing to their distinctive structural and functional attributes.The method of metal coordination has emerged as a robust methodology for chirality induction in many systems.In this work,we engineered two rigid and flexible chiral organic ligands(L_(1) and L_(2))by synergizing the inherent planar chirality of pillar[5]arenes with tailored metal-coordination moieties.They demonstrate versatile coordination capabilities toward both 3d-and 4f-block metals,enabling modulation of luminescent characteristics with blue,green and red emissions.Four planar chiral complexes exhibiting CPL activity were synthesized through systematic coordination of L_(1)/L_(2) with Zn^(2+),Eu^(3+),and Tb^(3+).The coordination processes effectively rigidify molecular conformations,leading to an enhanced CPL performance.Particularly,the Tb-L_(2) complex displays superior lanthanide-centered emission with a fluorescence quantum yield of~55%and an emission dissymmetry factor glum=5.5×10^(-3).By engineering the substitution on pillar[5]arene scaffolds,we have established a metal-coordination platform with CPL characteristics,which paves the way in the design of new metal-based luminescent materials.展开更多
Separated transmit and receive antennas are employed to improve transmit-receive isolation in conventional short-range radars, which greatly increases the antenna size and misaligns of the transmit/receive radiation p...Separated transmit and receive antennas are employed to improve transmit-receive isolation in conventional short-range radars, which greatly increases the antenna size and misaligns of the transmit/receive radiation patterns. In this paper,a dual circularly polarized(CP) monostatic simultaneous transmit and receive(MSTAR) antenna with enhanced isolation is proposed to alleviate the problem. The proposed antenna consists of one sequentially rotating array(SRA), two beamforming networks(BFN), and a combined decoupling structure. The SRA is shared by the transmit and receive to reduce the size of the antenna and to obtain a consistent transmit and receive pattern.The BFN achieve right-hand CP for transmit and left-hand CP for receive. By exploring the combined decoupling structure of uniplanar compact electromagnetic band gap(UC-EBG) and ringshaped defected ground structure(RS-DGS), good transmitreceive isolation is achieved. The proposed antenna prototype is fabricated and experimentally characterized. The simulated and measured results show good agreement. The demonstrate transmit/receive isolation is height than 33 dB, voltage standing wave ratio is lower than 2, axial ratio is lower than 3 dB, and consistent radiation for both transmit and receive is within4.25-4.35 GHz.展开更多
In this paper,a new compact ultrawideband(UWB)circularly polarized(CP)antenna array for vehicular communications is proposed.The antenna array consists of a 2×2 sequentially rotated T-shaped cross dipole,four par...In this paper,a new compact ultrawideband(UWB)circularly polarized(CP)antenna array for vehicular communications is proposed.The antenna array consists of a 2×2 sequentially rotated T-shaped cross dipole,four parasitic elements,and a feeding network.By loading the T-shaped cross dipoles with parasitic rectangular elements with cut corners,the bandwidth can be expanded.On this basis,the radiation pattern can be improved by the topology with sequential rotation of four T-shaped cross-dipole antennas,and the axial ratio(AR)bandwidth of the antenna also can be further enhanced.In addition,due to the special topology that the vertical arms of all Tshaped cross dipoles are all oriented toward the center of the antenna array,the gain of proposed antenna is improved while the size of the antenna is almost the same as the traditional cross dipole.Simulated and measured results show that the proposed antenna has good CP characteristics,an impedance bandwidth for S11<-10 d B of about 106.1%(3.26:1,1.57-5.12 GHz)and the 3-d B AR bandwidth of about 104.1%(3.17:1,1.57-4.98 GHz),a wide 3-d B gain bandwidth of 73.3%as well as the peak gain of 8.6 d Bic at 3.5 GHz.The overall size of antenna is 0.56λ×0.56λ×0.12λ(λrefers to the wavelength of the lowest operating frequency in free space).The good performance of this compact UWB CP antenna array is promising for applications in vehicular communications.展开更多
For decades,chiral nanomaterials have been extensively studied because of their extraordinary properties.Chiral nanostructures have attracted a lot of interest because of their potential applications including biosens...For decades,chiral nanomaterials have been extensively studied because of their extraordinary properties.Chiral nanostructures have attracted a lot of interest because of their potential applications including biosensing,asymmetric catalysis,optical devices,and negative index materials.Circularly polarized light(CPL)is the most attractive source for chirality owing to its high availability,and now it has been used as a chiral source for the preparation of chiral matter.In this review,the recent progress in the field of CPL-enabled chiral nanomaterials is summarized.Firstly,the recent advancements in the fabrication of chiral materials using circularly polarized light are described,focusing on the unique strategies.Secondly,an overview of the potential applications of chiral nanomaterials driven by CPL is provided,with a particular emphasis on biosensing,catalysis,and phototherapy.Finally,a perspective on the challenges in the field of CPL-enabled chiral nanomaterials is given.展开更多
Circularly polarized light(CPL)has been given great attention because of its extensive application.While several devices for CPL detection have been studied,their performance is affected by the magnitude of photocurre...Circularly polarized light(CPL)has been given great attention because of its extensive application.While several devices for CPL detection have been studied,their performance is affected by the magnitude of photocurrent.In this paper,a self-powered photodetector based on hot electrons in chiral metamaterials is proposed and optimized.CPL can be distinguished by the direction of photocurrent without external bias owing to the interdigital electrodes with asymmetric chiral metamaterials.Distinguished by the direction of photocurrent,the device can easily detect the rotation direction of the CPL electric field,even if it only has a very weak responsivity.The responsivity of the proposed detector is near 1.9 mA/W at the wavelength of 1322 nm,which is enough to distinguish CPL.The detector we proposed has the potential for application in optical communication.展开更多
We present a surface current method to model the graphene rectangular nanoantenna scattering in the terahertz band with Comsol. Compared with the equivalent thin slab method, the results obtained by the surface curren...We present a surface current method to model the graphene rectangular nanoantenna scattering in the terahertz band with Comsol. Compared with the equivalent thin slab method, the results obtained by the surface current method are more accurate and efficient. Then the electromagnetic scattering of circularly polarized terahertz waves on graphene nanoantennas is numerically analyzed by utilizing the surface current method. The depen- dences of the antenna resonant frequency with the circularly polarized wave on width and length are consistent with those for the linear polarized waves. These results are proved to be useful to design et^cient nanoantennas in terahertz wireless communications.展开更多
The enantiomers of carboline-based cryptates were successfully resolved by chiral HPLC.These complexes show high configurational stability under harsh conditions and their absolute configuration was determined by comp...The enantiomers of carboline-based cryptates were successfully resolved by chiral HPLC.These complexes show high configurational stability under harsh conditions and their absolute configuration was determined by comparing theoretical and expe rimental electronic circular dichroism spectra.The e nantiopure cryptates exhibit strong circularly polarized luminescence with a maximum dissymmetry factor glum=0.25 for the f-f transition 5 D0→7 F1(λ=594 nm)under visible light excitation atλgx=400 nm.展开更多
Perylene derivative with circularly polarized luminescence(CPL) at aggregated state was seldom reported due to the strong ACQ(aggregation-caused quench) effect at aggregation. In this work, a novel cholesterol-tetraph...Perylene derivative with circularly polarized luminescence(CPL) at aggregated state was seldom reported due to the strong ACQ(aggregation-caused quench) effect at aggregation. In this work, a novel cholesterol-tetraphenylethylene-perylene derivative(TPE-P) was designed and synthesized in moderate yield. It exhibited liquid crystalline behavior with orderly hexagonal columnar mesophase and good fluorescence emission at long wavelength(600-700 nm) not only in solution but also at aggregated states based on the AIE(aggregation-induced emission)-FRET(fluorescence resonance energy transfer) effect between tetraphenylethylene unit and perylene moiety. Moreover, the circular dichroism(CD) and CPL studies suggested the effective chiral transfer from cholesterol unit to tetraphenylethylene unit and perylene skeleton due to the spiral liquid crystalline self-assembly. The CD and CPL signals showed the order of THF < THF-hexane < solid film < meosphase, indicating that the higher spiral orderly degree resulted in the stronger chiral transfer. The largest |glum| value for mesophase excited at 320 nm was as high as 1.5×10^(−2) based on the combining effect of AIE-FRET and chiral transfer. This research not only reported a novel CPL perylene derivative at aggregated state, but also confirmed that the combination of AIE-FRET effect and chiral transfer of liquid crytalline phase was an effective method to construct normal dye with excellent CPL property in aggregated state.展开更多
It is of great significance to construct organic circularly polarized luminescence systems(CPL) with large luminescence dissymmetry factors(g_(lum)) for practical applications. Here we report organic CPL systems const...It is of great significance to construct organic circularly polarized luminescence systems(CPL) with large luminescence dissymmetry factors(g_(lum)) for practical applications. Here we report organic CPL systems constructed by merging triplet-triplet annihilation upconversion chromophores in cellulose matrices. The chirality of the matrix is transferred to the achiral chromophores of photon upconversion and then the multistep energy transfer processes of upconversion amplify g_(lum). The g_(lum)value of upconversion CPL in the left-handed ethyl cellulose and the right-handed(acetyl) ethyl cellulose are up to +0.1 and -0.15, respectively. The study provides a straightforward approach for constructing solid organic upconversion CPL materials with large g_(lum), which may expand the application potentials of organic chiroptical materials.展开更多
While enol-keto tautomerism has attracted great interest in Schiff bases and related compounds in solution and crystal states,the self-assembly of energy-unfavored keto form were scarcely investigated.Here,we report a...While enol-keto tautomerism has attracted great interest in Schiff bases and related compounds in solution and crystal states,the self-assembly of energy-unfavored keto form were scarcely investigated.Here,we report a keto-form directed self-assembly of a naphthalene-attached enantiomeric N-salicylideneanil analog L/DGG-Nap accompanied with a significantly amplified circularly polarized luminescence(CPL).It was found that LGG-Nap exists as a mixture of enol and keto form in monomer at a diluted toluene solution.The increment of the concentrations leads to the formation of predominated keto form,which subsequently triggers the self-assembly.Cryo-transmission electron microscopy(Cryo-TEM)revealed that a hierarchical assembly process happened upon increasing the concentration of LGG-Nap in toluene.Individual nanofibers formed at 1×10-4 mol/L and transferred into helical nanofiber bundles in 5×10-3 mol/L.Interestingly,while these is nearly no circular dichroism(CD)or CPL in the monomeric solution,the assembly showed strong CD and CPL.Remarkably,the dissymmetry factor(glum)was significantly amplified from zero in solution through the 0.005 in individual nanofiber to 0.1 in nanofiber bundles.This work demonstrates that the enol-keto tautomerism can be broken and trigger the self-assembly upon increasing the concentration,which can subsequently direct the chiral self-assembly and significantly amplify the dissymmetry factor of assembled CPL materials.展开更多
The generation of high-order harmonics and the attosecond pulse of the N2 molecule in two-color circularly polarized laser fields are investigated by the strong-field Lewenstein model. We show that the plateau of spec...The generation of high-order harmonics and the attosecond pulse of the N2 molecule in two-color circularly polarized laser fields are investigated by the strong-field Lewenstein model. We show that the plateau of spectra is dramatically extended and a continuous harmonic spectrum with the bandwidth of 113 eV is obtained. When a static field is added to the x direction, the quantum path control is realized and a supercontinuum spectrum can be obtained, which is beneficial to obtain a shorter attosecond pulse. The underlying physical mechanism is well explained by the time-frequency analysis and the semi-classical three-step model with a finite initial transverse velocity. By superposing several orders of harmonics in the combination of two-color circularly polarized laser fields and a static field, an isolated attosecond pulse with a duration of 30 as can be generated.展开更多
基金supported by NSFC(22271282)the Self-deployment Project Research Program of Haixi Institutes,Chinese Academy of Sciences with the grant number of CXZX-2022-JQ04.
文摘Circularly polarized luminescence(CPL)and two-photon absorption(TPA)materials have garnered considerable attentions due to their minimal energy loss and superior optical penetration[1,2].However,the current challenge lies in the absence of well-developed strategies for designing materials that combine these two exceptional optical properties.
基金supported by the National Key Research and Development Program of China(Grant No.2022YFE0134200)the National Natural Science Foundation of China(Grant Nos.12474343,12174147,and 12074142)the Natural Science Foundation of Jilin Province,China(Grant No.20220101016JC)。
文摘Strong feld-induced nonsequential double ionization(NSDI)is a signifcant multi-electron phenomenon that provides crucial insights into understanding electron correlation and multiple ionization of atoms and molecules,but it is typically unattainable in a circularly polarized laser pulse,especially for long-wavelength lasers.We present evidence that NSDI can occur in the presence of a near-infrared or beyond laser pulse by introducing a bowtie-nanotip.The laser-induced local plasmon can alter the local ellipticity of the feld,thereby enabling NSDI through elliptical trajectories that facilitate recollisions with parent atoms.An oval-shaped momentum distribution of recoiled ions provides evidence for the modifcation of trajectories by the aligned nanotips.Our study introduces an innovative control knob to manipulate NSDI and electron dynamics through the utilization of nanostructures.
基金support from the National Natural Science Foundation of China(Nos.22471198,22101208)the Fundamental Research Funds for the Central Universities.
文摘Symmetry breaking,a critical phenomenon in both natural and artificial systems,is pivotal in constructing chiral structures from achiral building units.This study focuses on the achiral molecule 8,8',8'',8'''-((pyrazine-2,3,5,6-tetrayltetrakis(benzene-4,1-iyl))tetrakis(oxy))tetrakis(octan-1-ol)(TPP-C8OH),an aggregation-induced emission(AIE)molecule,to explore its symmetry breaking behavior in supramolecular assembly.By analyzing TPP-C8OH in various solvents—both non-chiral and chiral—we find that chiral solvents significantly enhance the molecule's symmetry breaking and chiroptical properties.Specially,alcohol solvents,particularly dodecyl alcohol,facilitate the formation of helical structures with both left-handed(M)and right-handed(P)helices within single twisted nanoribbons.This observation contrasts with previously reported symmetry breaking phenomena in assembly systems.Chiral solvents induce assemblies with distinct helical orientations,resulting in notable circularly polarized luminescence(CPL)and circular dichroism(CD)signals.This study elucidates the impact of solvent choice on symmetry breaking and chiral assembly,offering insights into the design of advanced chiral materials with tailored self-assembly processes.
基金supported by the National Natural Science Foundation of China(22278184,22272065)the Natural Science Foundation of Jiangsu Province(BK20211530)+1 种基金the Fundamental Research Funds for the Central Universities(JUSRP622018,JUSRP202404022)the Key Research and Development Special Project of Yichun City,Jiangxi Province,China(2023ZDYFZX06).
文摘Perovskites showcased potential promise for innovative circularly polarized luminescence (CPL)-active multi-channelinformation encryption, owing to the exceptional luminescence brightness. It was still a formidablechallenge to fabricate CPL-active perovskites with significant luminescent asymmetry factor (glum) and full-colour-tailorableCPL properties. Indeed, compared to isotropic perovskites, anisotropic perovskite nanowires (NWs)were conducive to carrier separation and transport for polarization enhancement. Herein, three types of CsPb(Br/I)3 NWs with green, orange, red fluorescence (FL) were respectively synthesized and assembled into chiral NWfilms. The right-handed/left-handed chiral NW films constructed by 4+4 layers and 45° inter-angles exhibitshighly symmetric and mirror-like chiral signals. The strongest chiral intensity is more than 3000 medg. CPLsignals with wide colour gamut produce ranging from 480 nm to 800 nm, and tailorable CPL wavelengths aremanipulated by the emission wavelength of perovskite NWs. A giant CPL signal with a maximum glum of up to 10^(-1) is achieved. The polarization imaging of chiral NW films produces brilliant differential circularly polarizedstructural colours, making it more widely used in multilevel anti-counterfeiting systems. A significant break-throughlies in the development of advanced chiral perovskite materials with remarkable glum and tailorable CPLproperties, which sheds new light on optical anti-counterfeiting and intelligent information encryption.
基金the financial support of the National Natural Science Foundation of China(No.22471057)Natural Science Foundation of Hebei Province(Nos.226Z1501G,B2024205039)+2 种基金Young Scientific and Technological Talents Support Project of Jiangsu Province(JSTJ-2024-426)Jiangsu FundingProgram for Excellent Postdoctoral Talent(2024zB630)We also gratefully acknowledge the support from the National Demonstration Center for Experimental Chemistry Education of Hebei Normal University.
文摘The development of circularly polarized luminescence (CPL) materials from simple organic molecules is of critical importance for advancing their practical applications, yet it remains hindered by challenges such as low dissymmetry factors (glum) and complex synthetic process. Herein, we report a facile one-step [2+2] condensation strategy to access a Schiff-base pyrene dimer featuring 1,6-substituted pyrenes and trans-1,2-diaminocyclohexane units in 77% yield. Taking advantages of face-to-face π-π stacking of pyrene rings in the constrained D_(2) symmetric structure, intense excimer CPL was successfully realized with a |glum| value of 0.021 and a CPL brightness, BCPL, value of 154.5 M-1·cm-1. The optimized excited state structures reveal that the high |glum| value arises from the parallel arrangement of electric and magnetic dipole transition moments. Importantly, the rigid pyrene dimer architecture ensures robust CPL performance invariant under diverse conditions, including changes in temperature, concentration, and solvents, as well as in polymer films.
基金supported by the National Natural Science Foundation of China(Nos.92261108 and 2022YFA1503303)the STS Project of Fujian-CAS(No.2023T3054)。
文摘Although many racemic M4L6cages have been synthesized,little attention has been paid to the resolution of M4L6cages because resolution of these cages is very difficult.To explore the use of optically pure M4L6cages in chiral applications,it is important to obtain a single enantiomer.In this work,the anionicΛΛΛΛ-Zr_(4)L_(6)andΛΛΛΛ-Zr_(4)L_(6)(L=embonate)cages have been completely separated by introducing chiral organic ligands R/S-BINAP and 1S,2S/1R,2R-DPEN,respectively,and the active vertex of homochiral Zr_(4)L_(6)cage trapsπ-conjugated coordination silver cations(such as[Ag_(2)(DPPM)_(2)]^(2+),chiral[Ag_(2)(PPh_(3))_(2)(DPEN)]^(2+)and[Ag(PPh_(3))(DPEN)]^(+)),obtaining two pair of pure enantiomers(PTC-375(Λ/Λ)and PTC-376(Λ/Λ)).Interestingly,the chiral resolution and surface modification of such zirconium cage endow it with homochirality and significant circularly polarized luminescence(CPL)response,and PTC-376 enantiomers show a CPL output with glumvalues up to~1.4×10^(-2).This work not only provides a new resolution strategy for metal-organic cages,but also expands their chiral application especially in CPL field.
基金the financial support from the National Natural Science Foundation of China(Nos.22301206,92356305 and 22301208)Natural Science Foundation of Anhui Province(No.2308085J15)+5 种基金Natural Science Foundation of Anhui Provincial Higher Education Institutions(No.2023AH010012)China Post-doctoral Science Foundation(No.2022M722312)the Key Laboratory of Polymeric Material Design and Synthesis for Biomedical Functionthe Priority Academic Program Development(PAPD)of Jiangsu Higher Education InstitutionsJiangsu Funding Program for Excellent Postdoctoral Talentthe Program of Innovative Research Team of Soochow University。
文摘Recently circularly polarized luminescence(CPL)materials have attracted significant interest.Introducing reversible dynamic property to these materials has been a key focus in cutting-edge fields,such as in high-level information encryption.Here,we provided a novel and general strategy involving handednessselective filtration and ground-state chiral self-recovery(CSR)in double film system to address this issue.Based on this strategy,we achieved CPL switch through the reversible modulation of ground-state chirality including absorption and scattering circular dichroism(CD)signals over the full UV-visible wavelength range(365-700 nm)in a single azobenzene polymer(PAzo)film.More importantly,by flexibly changing the type of fluorescent films,it is convenient to achieve general excited-state CSR,that is reversible switching of full-color including ideal white(CIE coordinate(0.33,0.33)),as well as room-temperature phosphorescent CPL.All these CPL signals without almost any intensity decay after three cycles of onand-off switching.Experimental results indicated that the trans-cis isomerization and ordered rearrangement of azobenzene units in PAzo film were the fundamental reasons for realizing CPL switching.Finally,based on this system we achieved dynamic visual encryption and decryption process including multiple decryption methods.This study provides an effective method for constructing a universally applicable chiroptical switch in excited state.
基金financially supported by the National Natural Science Foundation of China(Nos.92356304,92061201,and 22105177)the National Key R&D Program of China(No.2021YFA1200301)+1 种基金the China Postdoctoral Science Foundation(No.2021TQ0294)the Zhongyuan Thousand Talents(Zhongyuan Scholars)Program of Henan Province(No.234000510007)。
文摘Non-covalent interactions-driven host-vip assembly based on metallo-tweezers has been used to construct varied optical functional materials with attractive structures and properties.We reported here two pairs of chiral gold(Ⅰ)-based metallo-tweezers as hosts to clip Ag^(Ⅰ)or Cu^(Ⅰ)cations for circularly polarized phosphorescence(CPP),driven by the integration of two-fold coordination and heterometallophilic interactions.The Au^(Ⅰ)-based hosts and metal ions-vips formed sandwich structures in 1:1 ratio with high binding affinity.The achieved tweezer/cation adducts exhibited red-shifted absorption bands and circular dichroism signals,which were attributed to the newly formed ligand to metal-metal charge transfer process.Remarkably,the host-vip supramolecular adducts showed turn-on phosphorescence and CPP,which benefited from rigidifying effect of multiple intermolecular interactions and shorter excited-state lifetime.Overall,our findings bring new insights into the feasibility to achieve and modulate CPP performance by fabricating metallo-tweezer-based host-vip complexes.
文摘A millimeter-wave (mmW) broadband dual circularly polarized (dual-CP) antenna with high port isolation is proposed in this paper. The dual-CP performance is realized based on the symmetrical septum circular polarizer based on the gap waveguide (GWG) technology. Two sets of symmetrical septum circular polarizers are used for common aperture combination,achieving the broadband dual-CP characteristics. Taking advantage of GWG structure without good electrical contact, the antenna can also be fabricated and assembled easily in the mmW band. The principle analysis of the antenna is given, and the antenna is simulated and fabricated. The measured results show that the bandwidth for S11lower than-10.7 dB and the axial ratio (AR) lower than 2.90 dB in 75-110 GHz, with realative bandwidth of 38%. Over the frequency band, the gain is higher than 9.16 dBic, and the dual-CP port isolation is greater than32 dB. The proposed antenna with dual-CP and highly isolated in a wide bandwidth range has broad application prospects in the field of mmW communication.
基金supported by the Beijing Natural Science Foundation(No.2232024)the Analysis&Testing Centre at Beijing Institute of Technology for advanced facilities.
文摘Metal-complexed chiral macrocyclic architectures have attracted increasing research interests in circularly polarized luminescence owing to their distinctive structural and functional attributes.The method of metal coordination has emerged as a robust methodology for chirality induction in many systems.In this work,we engineered two rigid and flexible chiral organic ligands(L_(1) and L_(2))by synergizing the inherent planar chirality of pillar[5]arenes with tailored metal-coordination moieties.They demonstrate versatile coordination capabilities toward both 3d-and 4f-block metals,enabling modulation of luminescent characteristics with blue,green and red emissions.Four planar chiral complexes exhibiting CPL activity were synthesized through systematic coordination of L_(1)/L_(2) with Zn^(2+),Eu^(3+),and Tb^(3+).The coordination processes effectively rigidify molecular conformations,leading to an enhanced CPL performance.Particularly,the Tb-L_(2) complex displays superior lanthanide-centered emission with a fluorescence quantum yield of~55%and an emission dissymmetry factor glum=5.5×10^(-3).By engineering the substitution on pillar[5]arene scaffolds,we have established a metal-coordination platform with CPL characteristics,which paves the way in the design of new metal-based luminescent materials.
基金supported by Guangdong Natural Science Foundation(2019A1515011622)Guangdong Provincial Laboratory of Southern Marine Science and Engineering (Zhuhai)(SML2021SP407)。
文摘Separated transmit and receive antennas are employed to improve transmit-receive isolation in conventional short-range radars, which greatly increases the antenna size and misaligns of the transmit/receive radiation patterns. In this paper,a dual circularly polarized(CP) monostatic simultaneous transmit and receive(MSTAR) antenna with enhanced isolation is proposed to alleviate the problem. The proposed antenna consists of one sequentially rotating array(SRA), two beamforming networks(BFN), and a combined decoupling structure. The SRA is shared by the transmit and receive to reduce the size of the antenna and to obtain a consistent transmit and receive pattern.The BFN achieve right-hand CP for transmit and left-hand CP for receive. By exploring the combined decoupling structure of uniplanar compact electromagnetic band gap(UC-EBG) and ringshaped defected ground structure(RS-DGS), good transmitreceive isolation is achieved. The proposed antenna prototype is fabricated and experimentally characterized. The simulated and measured results show good agreement. The demonstrate transmit/receive isolation is height than 33 dB, voltage standing wave ratio is lower than 2, axial ratio is lower than 3 dB, and consistent radiation for both transmit and receive is within4.25-4.35 GHz.
基金supported in part by the National Natural Science Foundation of China(NSFC)under Grant No.62071306in part by Shenzhen Science and Technology Program under Grants JCYJ202001091-13601723,JSGG20210802154203011 and JSGG-20210420091805014。
文摘In this paper,a new compact ultrawideband(UWB)circularly polarized(CP)antenna array for vehicular communications is proposed.The antenna array consists of a 2×2 sequentially rotated T-shaped cross dipole,four parasitic elements,and a feeding network.By loading the T-shaped cross dipoles with parasitic rectangular elements with cut corners,the bandwidth can be expanded.On this basis,the radiation pattern can be improved by the topology with sequential rotation of four T-shaped cross-dipole antennas,and the axial ratio(AR)bandwidth of the antenna also can be further enhanced.In addition,due to the special topology that the vertical arms of all Tshaped cross dipoles are all oriented toward the center of the antenna array,the gain of proposed antenna is improved while the size of the antenna is almost the same as the traditional cross dipole.Simulated and measured results show that the proposed antenna has good CP characteristics,an impedance bandwidth for S11<-10 d B of about 106.1%(3.26:1,1.57-5.12 GHz)and the 3-d B AR bandwidth of about 104.1%(3.17:1,1.57-4.98 GHz),a wide 3-d B gain bandwidth of 73.3%as well as the peak gain of 8.6 d Bic at 3.5 GHz.The overall size of antenna is 0.56λ×0.56λ×0.12λ(λrefers to the wavelength of the lowest operating frequency in free space).The good performance of this compact UWB CP antenna array is promising for applications in vehicular communications.
基金financially the National Natural Science Foundation of China(51902136)the Fundamental Research Funds for the Central Universities(JUSRP12003,JUSRP622026)Natural Science Foundation of Jiangsu Province(BK20211236)。
文摘For decades,chiral nanomaterials have been extensively studied because of their extraordinary properties.Chiral nanostructures have attracted a lot of interest because of their potential applications including biosensing,asymmetric catalysis,optical devices,and negative index materials.Circularly polarized light(CPL)is the most attractive source for chirality owing to its high availability,and now it has been used as a chiral source for the preparation of chiral matter.In this review,the recent progress in the field of CPL-enabled chiral nanomaterials is summarized.Firstly,the recent advancements in the fabrication of chiral materials using circularly polarized light are described,focusing on the unique strategies.Secondly,an overview of the potential applications of chiral nanomaterials driven by CPL is provided,with a particular emphasis on biosensing,catalysis,and phototherapy.Finally,a perspective on the challenges in the field of CPL-enabled chiral nanomaterials is given.
基金This work was supported by the National Natural Science Foundation of China(No.61705065)Hunan Provincial Natural Science Foundation of China(No.2017JJ3034)+1 种基金Technology Program of Changsha(No.kq1804001)National Training Program of Innovation and Entrepreneurship for undergraduates(No.S201910532166).
文摘Circularly polarized light(CPL)has been given great attention because of its extensive application.While several devices for CPL detection have been studied,their performance is affected by the magnitude of photocurrent.In this paper,a self-powered photodetector based on hot electrons in chiral metamaterials is proposed and optimized.CPL can be distinguished by the direction of photocurrent without external bias owing to the interdigital electrodes with asymmetric chiral metamaterials.Distinguished by the direction of photocurrent,the device can easily detect the rotation direction of the CPL electric field,even if it only has a very weak responsivity.The responsivity of the proposed detector is near 1.9 mA/W at the wavelength of 1322 nm,which is enough to distinguish CPL.The detector we proposed has the potential for application in optical communication.
文摘We present a surface current method to model the graphene rectangular nanoantenna scattering in the terahertz band with Comsol. Compared with the equivalent thin slab method, the results obtained by the surface current method are more accurate and efficient. Then the electromagnetic scattering of circularly polarized terahertz waves on graphene nanoantennas is numerically analyzed by utilizing the surface current method. The depen- dences of the antenna resonant frequency with the circularly polarized wave on width and length are consistent with those for the linear polarized waves. These results are proved to be useful to design et^cient nanoantennas in terahertz wireless communications.
基金Project supported by the German Research Foundation(DFG,research grant SE1448/7-1 for M.S.)German Academic Scholarship Foundation(Studienstiftung des deutsches Volkes,predoctoral fellowship for E.K.)。
文摘The enantiomers of carboline-based cryptates were successfully resolved by chiral HPLC.These complexes show high configurational stability under harsh conditions and their absolute configuration was determined by comparing theoretical and expe rimental electronic circular dichroism spectra.The e nantiopure cryptates exhibit strong circularly polarized luminescence with a maximum dissymmetry factor glum=0.25 for the f-f transition 5 D0→7 F1(λ=594 nm)under visible light excitation atλgx=400 nm.
基金support from the National Natural Science Foundation of China(No.21406036)Fujian Science and Technology Project(No.2019N0010)the National Undergraduate Innovation Program in Fujian Normal University(No.cxxl-2021300)were greatly acknowledged.
文摘Perylene derivative with circularly polarized luminescence(CPL) at aggregated state was seldom reported due to the strong ACQ(aggregation-caused quench) effect at aggregation. In this work, a novel cholesterol-tetraphenylethylene-perylene derivative(TPE-P) was designed and synthesized in moderate yield. It exhibited liquid crystalline behavior with orderly hexagonal columnar mesophase and good fluorescence emission at long wavelength(600-700 nm) not only in solution but also at aggregated states based on the AIE(aggregation-induced emission)-FRET(fluorescence resonance energy transfer) effect between tetraphenylethylene unit and perylene moiety. Moreover, the circular dichroism(CD) and CPL studies suggested the effective chiral transfer from cholesterol unit to tetraphenylethylene unit and perylene skeleton due to the spiral liquid crystalline self-assembly. The CD and CPL signals showed the order of THF < THF-hexane < solid film < meosphase, indicating that the higher spiral orderly degree resulted in the stronger chiral transfer. The largest |glum| value for mesophase excited at 320 nm was as high as 1.5×10^(−2) based on the combining effect of AIE-FRET and chiral transfer. This research not only reported a novel CPL perylene derivative at aggregated state, but also confirmed that the combination of AIE-FRET effect and chiral transfer of liquid crytalline phase was an effective method to construct normal dye with excellent CPL property in aggregated state.
基金financial support from the National Natural Science Foundation of China(Nos.21673264,21573266,21672226 and 22090012)the Youth Innovation Promotion Association of the Chinese Academy of Sciences(Nos.2017032 and 2020035)。
文摘It is of great significance to construct organic circularly polarized luminescence systems(CPL) with large luminescence dissymmetry factors(g_(lum)) for practical applications. Here we report organic CPL systems constructed by merging triplet-triplet annihilation upconversion chromophores in cellulose matrices. The chirality of the matrix is transferred to the achiral chromophores of photon upconversion and then the multistep energy transfer processes of upconversion amplify g_(lum). The g_(lum)value of upconversion CPL in the left-handed ethyl cellulose and the right-handed(acetyl) ethyl cellulose are up to +0.1 and -0.15, respectively. The study provides a straightforward approach for constructing solid organic upconversion CPL materials with large g_(lum), which may expand the application potentials of organic chiroptical materials.
基金National Natural Science foundation of China(Nos.21861132002,21773043,21973020 and 21890734).
文摘While enol-keto tautomerism has attracted great interest in Schiff bases and related compounds in solution and crystal states,the self-assembly of energy-unfavored keto form were scarcely investigated.Here,we report a keto-form directed self-assembly of a naphthalene-attached enantiomeric N-salicylideneanil analog L/DGG-Nap accompanied with a significantly amplified circularly polarized luminescence(CPL).It was found that LGG-Nap exists as a mixture of enol and keto form in monomer at a diluted toluene solution.The increment of the concentrations leads to the formation of predominated keto form,which subsequently triggers the self-assembly.Cryo-transmission electron microscopy(Cryo-TEM)revealed that a hierarchical assembly process happened upon increasing the concentration of LGG-Nap in toluene.Individual nanofibers formed at 1×10-4 mol/L and transferred into helical nanofiber bundles in 5×10-3 mol/L.Interestingly,while these is nearly no circular dichroism(CD)or CPL in the monomeric solution,the assembly showed strong CD and CPL.Remarkably,the dissymmetry factor(glum)was significantly amplified from zero in solution through the 0.005 in individual nanofiber to 0.1 in nanofiber bundles.This work demonstrates that the enol-keto tautomerism can be broken and trigger the self-assembly upon increasing the concentration,which can subsequently direct the chiral self-assembly and significantly amplify the dissymmetry factor of assembled CPL materials.
基金supported by the National Natural Science Foundation of China(Grant Nos.61575077,11271158,and 11574117)
文摘The generation of high-order harmonics and the attosecond pulse of the N2 molecule in two-color circularly polarized laser fields are investigated by the strong-field Lewenstein model. We show that the plateau of spectra is dramatically extended and a continuous harmonic spectrum with the bandwidth of 113 eV is obtained. When a static field is added to the x direction, the quantum path control is realized and a supercontinuum spectrum can be obtained, which is beneficial to obtain a shorter attosecond pulse. The underlying physical mechanism is well explained by the time-frequency analysis and the semi-classical three-step model with a finite initial transverse velocity. By superposing several orders of harmonics in the combination of two-color circularly polarized laser fields and a static field, an isolated attosecond pulse with a duration of 30 as can be generated.
