A class of networked control systems is investigated whose communication network is shared with other applications. The design objective for such a system setting is not only the optimization of the control performanc...A class of networked control systems is investigated whose communication network is shared with other applications. The design objective for such a system setting is not only the optimization of the control performance but also the efficient utilization of the communication resources. We observe that at a large time scale the data packet delay in the communication network is roughly varying piecewise constant, which is typically true for data networks like the Internet. Based on this observation, a dynamic data packing scheme is proposed within the recently developed packet-based control framework for networked control systems. As expected this proposed approach achieves a fine balance between the control performance and the communication utilization: the similar control performance can be obtained at dramatically reduced cost of the communication resources. Simulations illustrate the effectiveness of the proposed approach.展开更多
Revealing the molecular packing,intermolecular interactions,and aggregation behaviors in the nanocrystalline bulk heterojunction(BHJ)domains undertake the tasks for future materials design for efficient solar cells,es...Revealing the molecular packing,intermolecular interactions,and aggregation behaviors in the nanocrystalline bulk heterojunction(BHJ)domains undertake the tasks for future materials design for efficient solar cells,especially in understanding the structure–property relationship of isomeric non-fullerene acceptors(NFAs).Theoretical calculations reveal that 2ClIC-βδ,withβ-andδ-chlorine-substituted terminal groups,achieves a relatively higher dipole moment for enhanced intermolecular interactions.More importantly,when comparing the single-crystal X-ray diffraction patterns of three isomeric NFAs,BTIC-BO4Cl-βδ,BTIC-BO4Cl-βγ,and BTIC-BO4Cl,the synergistic effect of chlorine atoms at theβ-andδ-positions endows BTIC-BO4Cl-βδbetter molecular planarity with a dihedral angle of 1.14°.In turn,this creates the shortestπ∙∙∙πdistance(3.28Å)and smallest binding energies(−51.66 kcal mol^(−1))of the three NFAs,resulting in the tightest three-dimensional network packing structure with a framework of L_(x)=14.0Åand L_(y)=13.6Å.Such a structure has multiple intermolecular interactions for better charge transfer.However,the chlorine atomat theγ-position in the other two isomers contributes to non-intermolecular interactions with subordinate packing arrangements.Subsequently,the red-shifted UV-absorption and higher electron mobility observed in neat films of BTIC-BO4Cl-βδagree well with its more ordered crystallinity.This leads to a more suitable fiber-like phase separation in the corresponding active blend,ultimately improving the device performance with superior charge transport.As a result,the highest power conversion efficiency of 17.04%with a current density of 26.07 mA cm^(−2)was obtained with the BTIC-BO4Cl-βδ-based device.The carrier dynamics test and grazing incidence wide-angle X-ray scattering measurement indicate that the packing arrangement of molecules in the nanocrystalline BHJ domains is consistent with their crystallinity.This work investigates the structure–property differences in three acceptors and emphasizes the effect of isomeric chlorine substitution,which suggests that changes in the crystal packing arrangement,especially the size of the framework,have a considerable influence on charge carrier transport and ultimately are reflected on the device efficiency elevation.展开更多
Understanding the molecular packing arrangement and aggregation behaviors of organic semiconductor materials is crucial in comprehending their unique properties,particularly in complex structures required for solution...Understanding the molecular packing arrangement and aggregation behaviors of organic semiconductor materials is crucial in comprehending their unique properties,particularly in complex structures required for solution processing in organic photovoltaics.However,there has been limited focus on studying the diverse self-assembly behaviors induced by varying molecular skeletons.To address this issue,we designed and synthesized i-9R4Cl,i-7R4Cl,and 7R4Cl with nine-and seven-membered ring backbones,respectively.The single crystal structures revealed a standard H-type aggregate in i-9R4Cl,which is rare fully face-to-face packing in nonfullerene acceptors.Conversely,i-7R4Cl exhibited a typical J-type aggregate,while 7R4Cl demonstrated a synergistic H/J-type aggregate as conventional Y-series acceptors.Moreover,it reveals a unique three-dimensional(3D)network packing structure dominated by H-aggregation in i-9R4Cl,a linear packing structure in i-7R4Cl,and an elliptical 3D network packing structure in 7R4Cl.The grazing incidence wide-angle X-ray scattering tests confirmed that the packing arrangement in crystal structures was preserved in the film state.Despite i-9R4Cl’s favorable properties in stacking,it achieved a lower power conversion efficiency(PCE)of 1.97%compared to the other two acceptors,which should be attributed to poor exciton separation and carrier recombination induced by the morphology of aggregation regulation.Surprisingly,the electron paramagnetic resonance indicates that i-9R4Cl possesses radical properties,and when introduced as the third component in the PBDB-TF:BTIC-C9-4Cl based devices,it led to an enhancement in PCE from 18.42%to 19.08%,making it one of the highest efficiencies based on the BTIC-C9-4Cl system.It underscores how even subtle changes in molecular structure can significantly impact material properties.Our work aims to control the aggregation states of molecules,transitioning from standard H-type to J-type and to synergistic H/J-type aggregates,subsequently investigating the corresponding relationship between aggregation states,material properties,and devices performance.This is critical for designing new acceptor materials to overcome the bottlenecks in efficiency.展开更多
基金supported by the National Natural Science Foundation of China(Grant Nos.6142230761174061&61304048)+4 种基金the Scientific Research Starting Foundation for the Returned Overseas Chinese Scholars,Ministry of Education of Chinathe National Hi-Tech Research and Development Program of China("863"Project)(Grant No.2014AA06A503)the Youth Innovation Promotion Association,Chinese Academy of Sciences,in part by the Youth Top-Notch Talent Support Programthe 1000-Talent Youth ProgramZhejiang 1000-Talent Program
文摘A class of networked control systems is investigated whose communication network is shared with other applications. The design objective for such a system setting is not only the optimization of the control performance but also the efficient utilization of the communication resources. We observe that at a large time scale the data packet delay in the communication network is roughly varying piecewise constant, which is typically true for data networks like the Internet. Based on this observation, a dynamic data packing scheme is proposed within the recently developed packet-based control framework for networked control systems. As expected this proposed approach achieves a fine balance between the control performance and the communication utilization: the similar control performance can be obtained at dramatically reduced cost of the communication resources. Simulations illustrate the effectiveness of the proposed approach.
基金supported by the National Natural Science Foundation of China(grant nos.21733005,21975115)Guangdong Provincial Key Laboratory of Catalysis(grant no.2020B121201002)+2 种基金Guangdong Innovative and Entrepreneurial Research Team Program(grant no.2016ZT06G587)Shenzhen Fundamental Research Program(grant nos.JCYJ20210324120010028,JCYJ20200109140801751)Shenzhen Sci-Tech Fund(grant no.KYTDPT20181011104007).
文摘Revealing the molecular packing,intermolecular interactions,and aggregation behaviors in the nanocrystalline bulk heterojunction(BHJ)domains undertake the tasks for future materials design for efficient solar cells,especially in understanding the structure–property relationship of isomeric non-fullerene acceptors(NFAs).Theoretical calculations reveal that 2ClIC-βδ,withβ-andδ-chlorine-substituted terminal groups,achieves a relatively higher dipole moment for enhanced intermolecular interactions.More importantly,when comparing the single-crystal X-ray diffraction patterns of three isomeric NFAs,BTIC-BO4Cl-βδ,BTIC-BO4Cl-βγ,and BTIC-BO4Cl,the synergistic effect of chlorine atoms at theβ-andδ-positions endows BTIC-BO4Cl-βδbetter molecular planarity with a dihedral angle of 1.14°.In turn,this creates the shortestπ∙∙∙πdistance(3.28Å)and smallest binding energies(−51.66 kcal mol^(−1))of the three NFAs,resulting in the tightest three-dimensional network packing structure with a framework of L_(x)=14.0Åand L_(y)=13.6Å.Such a structure has multiple intermolecular interactions for better charge transfer.However,the chlorine atomat theγ-position in the other two isomers contributes to non-intermolecular interactions with subordinate packing arrangements.Subsequently,the red-shifted UV-absorption and higher electron mobility observed in neat films of BTIC-BO4Cl-βδagree well with its more ordered crystallinity.This leads to a more suitable fiber-like phase separation in the corresponding active blend,ultimately improving the device performance with superior charge transport.As a result,the highest power conversion efficiency of 17.04%with a current density of 26.07 mA cm^(−2)was obtained with the BTIC-BO4Cl-βδ-based device.The carrier dynamics test and grazing incidence wide-angle X-ray scattering measurement indicate that the packing arrangement of molecules in the nanocrystalline BHJ domains is consistent with their crystallinity.This work investigates the structure–property differences in three acceptors and emphasizes the effect of isomeric chlorine substitution,which suggests that changes in the crystal packing arrangement,especially the size of the framework,have a considerable influence on charge carrier transport and ultimately are reflected on the device efficiency elevation.
基金supported by the National Natural Science Foundation of China(grant nos.22225504,22305112,and 22305114)Guangdong Provincial Key Laboratory of Catalysis(grant no.2020B121201002)+2 种基金Shenzhen Fundamental Research Program(grant no.JCYJ20210324120010028)China Postdoctoral Science Foundation(grant no.2022M721466)High level of special funds(grant no.G03050K002).
文摘Understanding the molecular packing arrangement and aggregation behaviors of organic semiconductor materials is crucial in comprehending their unique properties,particularly in complex structures required for solution processing in organic photovoltaics.However,there has been limited focus on studying the diverse self-assembly behaviors induced by varying molecular skeletons.To address this issue,we designed and synthesized i-9R4Cl,i-7R4Cl,and 7R4Cl with nine-and seven-membered ring backbones,respectively.The single crystal structures revealed a standard H-type aggregate in i-9R4Cl,which is rare fully face-to-face packing in nonfullerene acceptors.Conversely,i-7R4Cl exhibited a typical J-type aggregate,while 7R4Cl demonstrated a synergistic H/J-type aggregate as conventional Y-series acceptors.Moreover,it reveals a unique three-dimensional(3D)network packing structure dominated by H-aggregation in i-9R4Cl,a linear packing structure in i-7R4Cl,and an elliptical 3D network packing structure in 7R4Cl.The grazing incidence wide-angle X-ray scattering tests confirmed that the packing arrangement in crystal structures was preserved in the film state.Despite i-9R4Cl’s favorable properties in stacking,it achieved a lower power conversion efficiency(PCE)of 1.97%compared to the other two acceptors,which should be attributed to poor exciton separation and carrier recombination induced by the morphology of aggregation regulation.Surprisingly,the electron paramagnetic resonance indicates that i-9R4Cl possesses radical properties,and when introduced as the third component in the PBDB-TF:BTIC-C9-4Cl based devices,it led to an enhancement in PCE from 18.42%to 19.08%,making it one of the highest efficiencies based on the BTIC-C9-4Cl system.It underscores how even subtle changes in molecular structure can significantly impact material properties.Our work aims to control the aggregation states of molecules,transitioning from standard H-type to J-type and to synergistic H/J-type aggregates,subsequently investigating the corresponding relationship between aggregation states,material properties,and devices performance.This is critical for designing new acceptor materials to overcome the bottlenecks in efficiency.
