The inception and harnessing of excitons are paramount for the electroluminescence performance of organic light-emitting devices(OLEDs).Through-space charge transfer(TSCT)via intramolecular interaction has proved to b...The inception and harnessing of excitons are paramount for the electroluminescence performance of organic light-emitting devices(OLEDs).Through-space charge transfer(TSCT)via intramolecular interaction has proved to be one of the most potent techniques employed to achieve 100% internal quantum efficiency.However,molecular strategies utilized to comprehensively enhance the electroluminescent performance of TSCT emitters regarding improving the photoluminescence quantum yield(PLQY)and elevating the light out-coupling efficiency remain arduous.To surmount this challenge,we deliberately designed and synthesized a proof-of-concept TSCT emitter called CzO-TRZ by incorporating an extra carbazole donor into spiroheterocyclic architecture.The introduction of rigid spiral fragments can immensely boost the horizontal orientation dipole ratio and establish an extra through-bond charge transfer(TBCT)radiative decay channel.As a result,a very high PLQY of 98.7%,fast kRISCof 2.2×10^(5)s^(-1)and high k_(r)^(s) of 2.2×10^(7)s^(-1),and an ultrahigh horizontal dipolar ratio of 90%were concurrently achieved for Cz O-TRZ blended films.Furthermore,corresponding thermally activated delayed fluorescence(TADF)-and TADF-sensitized fluorescence(TSF)-OLEDs based on CzO-TRZ demonstrated external quantum efficiencies(EQEs)of 33.4% and 30.3%,respectively,highlighting its versatile applications as both an emitter and sensitized host.展开更多
We study the connection between the central limit theorem and law of large numbers for exchangeable sequences, and provide a counterexample to the Gnedenko-Raikov theorem for such sequences.
P2-type layered Na_(0.67)MnO_(2)has been considered to be a promising candidate cathode material for sodium ion batteries.Nevertheless,the undesired phase transitions during operation and the large Na^(+)radius induce...P2-type layered Na_(0.67)MnO_(2)has been considered to be a promising candidate cathode material for sodium ion batteries.Nevertheless,the undesired phase transitions during operation and the large Na^(+)radius induced sluggish ion diffusion remain the stumbling blocks to realize its high performance.Herein,we propose a Zn/Mg co-doping strategy,which is proved to have bifunctional effects.First,relative to the pristine P2-Na_(0.67)MnO_(2)and the single-ion(Zn/Mg)doped samples,the Zn/Mg dual-doped P2-Na_(0.67)MnO_(2)demonstrates a lower Mn^(3+)/Mn^(4+)ratio and a higher lattice O content,which facilitate the structural stability of the cathode material.More intriguingly,the Zn/Mg co-doping gives rise to enlarged interplanar spacing,which provides spacious ion diffusion channels for fast Na^(+)intercalation/extraction.As a result,the Zn/Mg dual-doped sample exhibits a high Na^(+)diffusion coefficient and a solid-solution reaction during charge/discharge,with a cell volume change determined to be only 0.55%.Taking advantages of the above favorable features,the Zn/Mg dual-doped P2-Na_(0.67)MnO_(2)demonstrates a high rate performance with 67.2 mAh·g^(-1)delivered at 10 C and a decent cycling stability with a capacity retention of 93.8%achieved at 1 C after 100 cycles.This work introduces the Zn/Mg co-doping strategy to simultaneously improve the cycling stability and rate capability of P2-Na_(0.67)MnO_(2),which may offer a promising avenue for further performance enhancement of the layered Na-ion batteries cathode materials.展开更多
This paper deals with the conditional quantile estimation based on left-truncated and right-censored data.Assuming that the observations with multivariate covariates form a stationary α-mixing sequence,the authors de...This paper deals with the conditional quantile estimation based on left-truncated and right-censored data.Assuming that the observations with multivariate covariates form a stationary α-mixing sequence,the authors derive the strong convergence with rate,strong representation as well as asymptotic normality of the conditional quantile estimator.Also,a Berry-Esseen-type bound for the estimator is established.In addition,the finite sample behavior of the estimator is investigated via simulations.展开更多
基金supported by the National Natural Science Foundation of China(U21A20331,51773212,81903743,52003088)the Distinguished Young Scholars(21925506)the Ningbo Key Scientific and Technological Project(2022Z124,2022Z119)。
文摘The inception and harnessing of excitons are paramount for the electroluminescence performance of organic light-emitting devices(OLEDs).Through-space charge transfer(TSCT)via intramolecular interaction has proved to be one of the most potent techniques employed to achieve 100% internal quantum efficiency.However,molecular strategies utilized to comprehensively enhance the electroluminescent performance of TSCT emitters regarding improving the photoluminescence quantum yield(PLQY)and elevating the light out-coupling efficiency remain arduous.To surmount this challenge,we deliberately designed and synthesized a proof-of-concept TSCT emitter called CzO-TRZ by incorporating an extra carbazole donor into spiroheterocyclic architecture.The introduction of rigid spiral fragments can immensely boost the horizontal orientation dipole ratio and establish an extra through-bond charge transfer(TBCT)radiative decay channel.As a result,a very high PLQY of 98.7%,fast kRISCof 2.2×10^(5)s^(-1)and high k_(r)^(s) of 2.2×10^(7)s^(-1),and an ultrahigh horizontal dipolar ratio of 90%were concurrently achieved for Cz O-TRZ blended films.Furthermore,corresponding thermally activated delayed fluorescence(TADF)-and TADF-sensitized fluorescence(TSF)-OLEDs based on CzO-TRZ demonstrated external quantum efficiencies(EQEs)of 33.4% and 30.3%,respectively,highlighting its versatile applications as both an emitter and sensitized host.
文摘We study the connection between the central limit theorem and law of large numbers for exchangeable sequences, and provide a counterexample to the Gnedenko-Raikov theorem for such sequences.
基金The authors are grateful to the financial supports from the National Natural Science Foundation of China(NSFC)(Nos.91834301,91534102,and 21808046)Anhui Provincial Science and Technology Department Foundation(No.201903a05020021).
文摘P2-type layered Na_(0.67)MnO_(2)has been considered to be a promising candidate cathode material for sodium ion batteries.Nevertheless,the undesired phase transitions during operation and the large Na^(+)radius induced sluggish ion diffusion remain the stumbling blocks to realize its high performance.Herein,we propose a Zn/Mg co-doping strategy,which is proved to have bifunctional effects.First,relative to the pristine P2-Na_(0.67)MnO_(2)and the single-ion(Zn/Mg)doped samples,the Zn/Mg dual-doped P2-Na_(0.67)MnO_(2)demonstrates a lower Mn^(3+)/Mn^(4+)ratio and a higher lattice O content,which facilitate the structural stability of the cathode material.More intriguingly,the Zn/Mg co-doping gives rise to enlarged interplanar spacing,which provides spacious ion diffusion channels for fast Na^(+)intercalation/extraction.As a result,the Zn/Mg dual-doped sample exhibits a high Na^(+)diffusion coefficient and a solid-solution reaction during charge/discharge,with a cell volume change determined to be only 0.55%.Taking advantages of the above favorable features,the Zn/Mg dual-doped P2-Na_(0.67)MnO_(2)demonstrates a high rate performance with 67.2 mAh·g^(-1)delivered at 10 C and a decent cycling stability with a capacity retention of 93.8%achieved at 1 C after 100 cycles.This work introduces the Zn/Mg co-doping strategy to simultaneously improve the cycling stability and rate capability of P2-Na_(0.67)MnO_(2),which may offer a promising avenue for further performance enhancement of the layered Na-ion batteries cathode materials.
基金supported by the National Natural Science Foundation of China(No.11271286)the Specialized Research Fund for the Doctor Program of Higher Education of China(No.20120072110007)a grant from the Natural Sciences and Engineering Research Council of Canada
文摘This paper deals with the conditional quantile estimation based on left-truncated and right-censored data.Assuming that the observations with multivariate covariates form a stationary α-mixing sequence,the authors derive the strong convergence with rate,strong representation as well as asymptotic normality of the conditional quantile estimator.Also,a Berry-Esseen-type bound for the estimator is established.In addition,the finite sample behavior of the estimator is investigated via simulations.