D-π hybridization is a key structural feature that may significantly affect the intrinsic electronic properties of metallopolymers.Herein,we present the electrosynthesis and memristive properties of metallopolymers u...D-π hybridization is a key structural feature that may significantly affect the intrinsic electronic properties of metallopolymers.Herein,we present the electrosynthesis and memristive properties of metallopolymers using the distinct d-π hybridization monomers R_(1) and R_(2).R_(1)(Ru^(Ⅱ)-(tpz)Cl_(2))features tetradentate ligands(tpz,6,6'-di(1H-pyrazol-1-yl)-2,2'-bipyridine)enforcing quasi-octahedral geometry;R_(2)(Ru^(Ⅱ)-(bpp)_(2))incorporates tridentate ligands(bpp,2,6-di(1H-pyrazol-1-yl)pyridine)inducing pronounced geometric distortion.The planar ligand(tpz)in R_(1) facilitates ordered molecular assembly through high conformational rigidity and extensive π-π stacking,resulting in increased molecular densities and enhanced morphological uniformity compared to R_(2) metallopolymers.Due to pyrazole’s weaker π-acceptance and strongerσ-donation compared to pyridine,R_(1) exhibits a 119 nm red-shift in metal-to-ligand charge transfer(MLCT)band and a 30 mV anodic shift in Ru^(+2/+3)redox potential relative to R_(2).Coupled with a reduced HOMO-LUMO gap,the uniform and ordered structure leads to a lower conductance decay constant in R_(1).Additionally,R_(2) metallopolymers exhibit superior memristive performance(characterized by lower switching voltage and higher switching ratio)via redox-induced aromatic transitions in axial ligands enhancing electronic delocalization.This work compares two metallopolymers with different ligand geometries,revealing how this difference leads to distinct charge transport and memristive behaviors.展开更多
The advancement of flexible memristors has significantly promoted the development of wearable electronic for emerging neuromorphic computing applications.Inspired by in-memory computing architecture of human brain,fle...The advancement of flexible memristors has significantly promoted the development of wearable electronic for emerging neuromorphic computing applications.Inspired by in-memory computing architecture of human brain,flexible memristors exhibit great application potential in emulating artificial synapses for highefficiency and low power consumption neuromorphic computing.This paper provides comprehensive overview of flexible memristors from perspectives of development history,material system,device structure,mechanical deformation method,device performance analysis,stress simulation during deformation,and neuromorphic computing applications.The recent advances in flexible electronics are summarized,including single device,device array and integration.The challenges and future perspectives of flexible memristor for neuromorphic computing are discussed deeply,paving the way for constructing wearable smart electronics and applications in large-scale neuromorphic computing and high-order intelligent robotics.展开更多
文摘D-π hybridization is a key structural feature that may significantly affect the intrinsic electronic properties of metallopolymers.Herein,we present the electrosynthesis and memristive properties of metallopolymers using the distinct d-π hybridization monomers R_(1) and R_(2).R_(1)(Ru^(Ⅱ)-(tpz)Cl_(2))features tetradentate ligands(tpz,6,6'-di(1H-pyrazol-1-yl)-2,2'-bipyridine)enforcing quasi-octahedral geometry;R_(2)(Ru^(Ⅱ)-(bpp)_(2))incorporates tridentate ligands(bpp,2,6-di(1H-pyrazol-1-yl)pyridine)inducing pronounced geometric distortion.The planar ligand(tpz)in R_(1) facilitates ordered molecular assembly through high conformational rigidity and extensive π-π stacking,resulting in increased molecular densities and enhanced morphological uniformity compared to R_(2) metallopolymers.Due to pyrazole’s weaker π-acceptance and strongerσ-donation compared to pyridine,R_(1) exhibits a 119 nm red-shift in metal-to-ligand charge transfer(MLCT)band and a 30 mV anodic shift in Ru^(+2/+3)redox potential relative to R_(2).Coupled with a reduced HOMO-LUMO gap,the uniform and ordered structure leads to a lower conductance decay constant in R_(1).Additionally,R_(2) metallopolymers exhibit superior memristive performance(characterized by lower switching voltage and higher switching ratio)via redox-induced aromatic transitions in axial ligands enhancing electronic delocalization.This work compares two metallopolymers with different ligand geometries,revealing how this difference leads to distinct charge transport and memristive behaviors.
基金supported by the NSFC(12474071)Natural Science Foundation of Shandong Province(ZR2024YQ051)+5 种基金Open Research Fund of State Key Laboratory of Materials for Integrated Circuits(SKLJC-K2024-12)the Shanghai Sailing Program(23YF1402200,23YF1402400)Natural Science Foundation of Jiangsu Province(BK20240424)Taishan Scholar Foundation of Shandong Province(tsqn202408006)Young Talent of Lifting engineering for Science and Technology in Shandong,China(SDAST2024QTB002)the Qilu Young Scholar Program of Shandong University.
文摘The advancement of flexible memristors has significantly promoted the development of wearable electronic for emerging neuromorphic computing applications.Inspired by in-memory computing architecture of human brain,flexible memristors exhibit great application potential in emulating artificial synapses for highefficiency and low power consumption neuromorphic computing.This paper provides comprehensive overview of flexible memristors from perspectives of development history,material system,device structure,mechanical deformation method,device performance analysis,stress simulation during deformation,and neuromorphic computing applications.The recent advances in flexible electronics are summarized,including single device,device array and integration.The challenges and future perspectives of flexible memristor for neuromorphic computing are discussed deeply,paving the way for constructing wearable smart electronics and applications in large-scale neuromorphic computing and high-order intelligent robotics.
