Monolayer graphene has attracted enormous attention owing to its unique electronic and optical properties.However,achieving an effective approach without applying electrical bias for manipulating the charge transfer b...Monolayer graphene has attracted enormous attention owing to its unique electronic and optical properties.However,achieving an effective approach without applying electrical bias for manipulating the charge transfer based on graphene is elusive to date.Herein,we realized the manipulation of excitons’transition from emitter to the graphene surface with plasmonic engineering nanostructures and firstly obtained large enhancements for photon emission on the graphene surface.The localized plasmons generated from the plasmonic nanostructures of shell-isolated nanoparticle coupling to ultra-flat Au substrate would dictate a consistent junction geometry while enhancing the optical field and dominating the electron transition pathways,which may cause obvious perturbations for molecular radiation behaviors.Additionally,the three-dimensional finite-difference time-domain and time-dependent density functional theory were also carried out to simulate the distributions of electromagnetic field and energy levels of hybrid nanostructure respectively and the results agreed well with the experimental data.Therefore,this work paves a novel approach for tunning graphene charge/energy transfer processes,which may hold great potential for applications in photonic devices based on graphene.展开更多
Lithium-sulfur batteries are recognized as one of the most promising next-generation high-performance energy storage systems. However, obstacles like the irreversible capacity loss hinder its broad application. Herein...Lithium-sulfur batteries are recognized as one of the most promising next-generation high-performance energy storage systems. However, obstacles like the irreversible capacity loss hinder its broad application. Herein,we fabricated an interconnected three-dimensional MoS_(2)-MoN heterostructure(3D-MoS_(2)-MoN) via a facile salttemplate method, overcoming the intrinsic shortcomings such as poor conductivity and compact morphology of traditionally-synthesized transition metal sulfides(TMSs).Furthermore, excellent electrocatalysis ability and hierarchical pore structure effectively accelerate the sluggish lithium polysulfides conversions during cycling. As a result, 3D-MoS_(2)-MoN showed a high initial specific capacity of 1466 mAh·g^(-1)and excellent high-rate capability up to 4℃. A stable cycling performance with a sulfur loading of 2 mg·cm^(-2) was realized with a low decay rate of 0.069% per cycle. This work introduced a rational design route for the appliance of TMSs in the lithiumsulfur batteries.展开更多
The light-matter interaction between plasmonic nanocavity and exciton at the sub-diffraction limit is a central research field in nanophotonics.Here,we demonstrated the vertical distribution of the light-matter intera...The light-matter interaction between plasmonic nanocavity and exciton at the sub-diffraction limit is a central research field in nanophotonics.Here,we demonstrated the vertical distribution of the light-matter interactions at~1 nm spatial resolution by coupling A excitons of MoS2 and gap-mode plasmonic nanocavities.Moreover,we observed the significant photoluminescence(PL)enhancement factor reaching up to 2800 times,which is attributed to the Purcell effect and large local density of states in gap-mode plasmonic nanocavities.Meanwhile,the theoretical calculations are well reproduced and support the experimental results.展开更多
Hierarchical chiral self-assembly is of profound significance for biomolecules for their biological functions.Atom-precise metal nanoclusters(NCs)offer better opportunities to construct hierarchical superlattices.Neve...Hierarchical chiral self-assembly is of profound significance for biomolecules for their biological functions.Atom-precise metal nanoclusters(NCs)offer better opportunities to construct hierarchical superlattices.Nevertheless,achieving hierarchical homochiral assembly of nanocrystals protected by achiral ligands has proven to be a formidable task,with existing examples primarily limited to heterochiral assembly.Here we put forward a hierarchical assembly strategy towards precisely fabricating highly ordered homochiral superstructures.First,clusterin-nanocage type copper-hydride NCs act as synthons,of which entity is featured with a hexagonal close-packed Cu_(9)kernel embedded in a C_(3)-symmetric trigonal-prismatic metallacage,leading to a chiral core-shell primary structure with either P or M conformation.Then four homochiral NCs combined with guests through synergistic noncovalent interactions spontaneously organize into a supramolecular tetrahedral secondary structure within a unit cell.Finally,these nanoscopic supramolecular motifs pack into tertiary hierarchical superlattice of chiral cubic crystalline phase.Additionally,the crystalline material shows excellent robustness,and fascinating blueexcitable near-infrared thermally activated delayed fluorescence behavior.This work not only exhibits that nanocage-type NCs can be smart as proteins to translate chiral primary structure into tertiary chiral hierarchical complexity,but also provides new insights into structure-to-superstructure,enabling bottom-up creation of higher-level hierarchical homochiral superlattice structures.展开更多
基金supported by the National Key Research and Development Program of China(No.2019YFA0705400)the National Natural Science Foundation of China(Nos.21925404,22002128,22104135,62004095,and 22021001)Zhejiang Provincial Natural Science Foundation of China(No.LY23B050003).
文摘Monolayer graphene has attracted enormous attention owing to its unique electronic and optical properties.However,achieving an effective approach without applying electrical bias for manipulating the charge transfer based on graphene is elusive to date.Herein,we realized the manipulation of excitons’transition from emitter to the graphene surface with plasmonic engineering nanostructures and firstly obtained large enhancements for photon emission on the graphene surface.The localized plasmons generated from the plasmonic nanostructures of shell-isolated nanoparticle coupling to ultra-flat Au substrate would dictate a consistent junction geometry while enhancing the optical field and dominating the electron transition pathways,which may cause obvious perturbations for molecular radiation behaviors.Additionally,the three-dimensional finite-difference time-domain and time-dependent density functional theory were also carried out to simulate the distributions of electromagnetic field and energy levels of hybrid nanostructure respectively and the results agreed well with the experimental data.Therefore,this work paves a novel approach for tunning graphene charge/energy transfer processes,which may hold great potential for applications in photonic devices based on graphene.
基金the National Key Technologies R&D Program of China(No.2018YFA900)the National Natural Science Foundation of China(No.51872012)the Fundamental Research Funds for the Central Universities。
文摘Lithium-sulfur batteries are recognized as one of the most promising next-generation high-performance energy storage systems. However, obstacles like the irreversible capacity loss hinder its broad application. Herein,we fabricated an interconnected three-dimensional MoS_(2)-MoN heterostructure(3D-MoS_(2)-MoN) via a facile salttemplate method, overcoming the intrinsic shortcomings such as poor conductivity and compact morphology of traditionally-synthesized transition metal sulfides(TMSs).Furthermore, excellent electrocatalysis ability and hierarchical pore structure effectively accelerate the sluggish lithium polysulfides conversions during cycling. As a result, 3D-MoS_(2)-MoN showed a high initial specific capacity of 1466 mAh·g^(-1)and excellent high-rate capability up to 4℃. A stable cycling performance with a sulfur loading of 2 mg·cm^(-2) was realized with a low decay rate of 0.069% per cycle. This work introduced a rational design route for the appliance of TMSs in the lithiumsulfur batteries.
基金supported by the National Key Research and Development Program of China(2019YFA0705400,2020YFB1505800,2019YFD0901100.and 2021YFA12015021.the National Natural Science Foundation of China(21925404,22021001,22002128,21991151,and 92161118).the Science and Technology Planning Project of Fujian Province(2021Y0104).the State Key Laboratory of Fine Chemicals Dalian University of Technology(KF2002 and the“111”Project(B17027).
文摘The light-matter interaction between plasmonic nanocavity and exciton at the sub-diffraction limit is a central research field in nanophotonics.Here,we demonstrated the vertical distribution of the light-matter interactions at~1 nm spatial resolution by coupling A excitons of MoS2 and gap-mode plasmonic nanocavities.Moreover,we observed the significant photoluminescence(PL)enhancement factor reaching up to 2800 times,which is attributed to the Purcell effect and large local density of states in gap-mode plasmonic nanocavities.Meanwhile,the theoretical calculations are well reproduced and support the experimental results.
基金supported by the National Natural Science Foundation of China(grant nos.22325105,92361301,52261135637,22171164,92161118,91961105,and 21641011)the Natural Science Foundation of Fujian Province(grant no.2022J01298)the Open Project Program of the State Key Laboratory of Photocatalysis on Energy and Environment(grant no.SKLPEE-KF202109).
文摘Hierarchical chiral self-assembly is of profound significance for biomolecules for their biological functions.Atom-precise metal nanoclusters(NCs)offer better opportunities to construct hierarchical superlattices.Nevertheless,achieving hierarchical homochiral assembly of nanocrystals protected by achiral ligands has proven to be a formidable task,with existing examples primarily limited to heterochiral assembly.Here we put forward a hierarchical assembly strategy towards precisely fabricating highly ordered homochiral superstructures.First,clusterin-nanocage type copper-hydride NCs act as synthons,of which entity is featured with a hexagonal close-packed Cu_(9)kernel embedded in a C_(3)-symmetric trigonal-prismatic metallacage,leading to a chiral core-shell primary structure with either P or M conformation.Then four homochiral NCs combined with guests through synergistic noncovalent interactions spontaneously organize into a supramolecular tetrahedral secondary structure within a unit cell.Finally,these nanoscopic supramolecular motifs pack into tertiary hierarchical superlattice of chiral cubic crystalline phase.Additionally,the crystalline material shows excellent robustness,and fascinating blueexcitable near-infrared thermally activated delayed fluorescence behavior.This work not only exhibits that nanocage-type NCs can be smart as proteins to translate chiral primary structure into tertiary chiral hierarchical complexity,but also provides new insights into structure-to-superstructure,enabling bottom-up creation of higher-level hierarchical homochiral superlattice structures.
