Recently, an effective exciton diffusion length L exceeding 100μm has been reported for organic- inorganic halide perovskites owing to both the high mobility and ultra-long lifetime of the excitons; however, the orig...Recently, an effective exciton diffusion length L exceeding 100μm has been reported for organic- inorganic halide perovskites owing to both the high mobility and ultra-long lifetime of the excitons; however, the origin of ultra-long L is still unclear in nature. In some photoelectric materials, reverse intersystem crossing (RISC) from the triplet to the singlet state can enhance the quantum yield of pho- toluminescence greatly. In this study, our theoretical investigation indicated that the energy difference △E_st between the singlet state and the triplet state of CH_3NH_3Pbl_3 was less than 0.1 eV, which represents one crucial prerequisite for the occurrence of RISC. Meanwhile, the experimental results showed that the photoluminescence lifetime increased with the increasing temperature, a typical feature of RISC. Based on this study, we put forward the hypothesis that the ultra-long lifetime of excitons in organic-inorganic halide perovskite might be caused by the RISC process. This may provide a new insight into the important photophysical properties of such novel photovoltaic materials.展开更多
GaN-based continuous-wave operated blue-violet laser diodes(LDs) with long lifetime are demonstrated, which are grown on a c-plane GaN substrate by metal organic chemical vapor deposition with a 10 × 600 μm^2 ri...GaN-based continuous-wave operated blue-violet laser diodes(LDs) with long lifetime are demonstrated, which are grown on a c-plane GaN substrate by metal organic chemical vapor deposition with a 10 × 600 μm^2 ridge waveguide structure.The electrical and optical characteristics of a blue-violet LD are investigated under direct-current injection at room temperature(25 °C). The stimulated emission wavelength and peak optical power of the LD are around 413 nm and over 600 mW, respectively.In addition, the threshold current density and voltage are as small as 1.46 kA/cm^2 and 4.1 V, respectively. Moreover, the lifetime is longer than 1000 hours under room-temperature continuous-wave operation.展开更多
Ultracold plasma provides a possible route to approach the strongly-coupled regime under laboratory conditions. Normally, the lifetime of ultracold plasma is very limited due to plasma heating and expansion mechanisms...Ultracold plasma provides a possible route to approach the strongly-coupled regime under laboratory conditions. Normally, the lifetime of ultracold plasma is very limited due to plasma heating and expansion mechanisms. We present a new method to generate long lifetime ultracold plasmas consisting mainly of cations and anions. This plasma demonstrates a capability of traversing a DC barrier of up to 5 (or -3) V. The lifetime of this plasma is expected to be more than 250us. Finally, molecular dynamics (MD) simulation is used to explain how anions slow the expansion rate and prolong the lifetime of this plasma.展开更多
Atmospheric lifetimes and traveling distances of 15 PAHs(Ac:acenaphthylene,Ace:acenaphthene,Ph:phenanthrene,MePh3:3-methyl-phenanthrene,MePh9:9-methyl-phenanthrene,MePh1:1-methyl-phenanthrene,MePh2:2-methyl-phenanthre...Atmospheric lifetimes and traveling distances of 15 PAHs(Ac:acenaphthylene,Ace:acenaphthene,Ph:phenanthrene,MePh3:3-methyl-phenanthrene,MePh9:9-methyl-phenanthrene,MePh1:1-methyl-phenanthrene,MePh2:2-methyl-phenanthrene,Ret:retene,B[a]A:benzo[a]anthracene,Chry:chrysene,B[b,j,k]F:benzo[b,j,k]fluoranthene,B[e]P:benzo[e]pyrene,B[a]P:benzo[a]pyrene,Ind:indeno[1,2,3-cd]pyrene,B[g,h,i]P:benzo[g,h,i]perylene)at Whitbourne,UK,were estimated by using the rate constants for reaction with OH,O3,and the first order rate constants of eight species of high molecular weight PAHs(i.e.B[a]A,Chry,B[b]F,B[k]F,B[a]P,Ind,B[g,h,i]P and Ret)as a function of humidity,solar intensity and temperature by using Multiple Regression Analysis.The predicted atmospheric lifetime of Ac,Ace,Ph,MePh3,MePh9,MePh2 and MePh1 ranged between 11.42 h-79.12 h in cold period and 1/31 h-14.33 h in warm period respectively.The binary ratios of atmospheric lifetime of B[k]F/B[g,h,i]P,B[k]F/B[g,h,i]P,B[g,h,i]P/Ind and B[k]F/Ind displayed non-significant differences between cold and warm period,indicating that high molecular weight PAHs are difficult to be decomposed by UV light and thus may be conveyed to the rural regions via long range atmospheric transportation(LRAT).The decreased level of the atmospheric lifetime of low molecular weight PAHs in summer can be attributed to an increased level of OH radical content and solar radiation.展开更多
The lifetime of a lunar satellite orbit is constrained by the non-spherical nature of the Moon’s gravity field. The orbital lifetime of lunar orbits depends significantly on the initial conditions of the orbit. Right...The lifetime of a lunar satellite orbit is constrained by the non-spherical nature of the Moon’s gravity field. The orbital lifetime of lunar orbits depends significantly on the initial conditions of the orbit. Right ascension of ascending node (Ω) is one of the important orbital parameter affecting the orbital lifetime. In the present work we have analyzed the effect of Ω on the variation of lifetime with altitude for circular lunar orbits. It is found that at a particular initial altitude, a small increase in the altitude results in substantial increase in the orbital lifetime due to effect of the long periodic terms of Earth’s gravity on eccentricity and this transition altitude is different for different Ω. Further, it is observed that the variation of transition altitude with Ω follows a definite, but different trend for orbits with different inclinations. The transition altitude for polar orbits is found to be higher without the effect of Sun and Earth gravity. Variation of transition altitude with orbital inclination is also analyzed. Lifetimes of high altitude circular lunar orbits are analyzed and it is observed that at high altitudes lifetime decreases with altitude.展开更多
Thermally activated delayedfluorescence(TADF)molecules are regarded as promis-ing materials for realizing high-performance organic light-emitting diodes(OLEDs).The connecting groups between donor(D)and acceptor(A)units...Thermally activated delayedfluorescence(TADF)molecules are regarded as promis-ing materials for realizing high-performance organic light-emitting diodes(OLEDs).The connecting groups between donor(D)and acceptor(A)units in D–A type TADF molecules could affect the charge transfer and luminescence performance of TADF materials in aggregated states.In this work,we design and synthesize four TADF molecules using planar and twisted linkers to connect the aza-azulene donor(D)and triazine acceptor(A).Compared with planar linkers,the twisted ones(Az-NP-T and Az-NN-T)can enhance A–A aggregation interaction between adjacent molecules to balance hole and electron density.As a result,highly efficient and stable deep-red top-emission OLEDs with a high electroluminescence efficiency of 57.3%and an impressive long operational lifetime(LT_(95)∼30,000 h,initial luminance of 1000 cd m^(-2))are obtained.This study provides a new strategy for designing more effi-cient and stable electroluminescent devices through linker aggregation engineering in donor–acceptor molecules.展开更多
Doping foreign atom(s)in metal nanoclusters is an effective strategy to engineer the properties and functionalities of metal nanoclusters.However,until now,to dope Pd atom into Ag nanoclusters remains a huge challenge...Doping foreign atom(s)in metal nanoclusters is an effective strategy to engineer the properties and functionalities of metal nanoclusters.However,until now,to dope Pd atom into Ag nanoclusters remains a huge challenge.Here we develop a one-step rapid method to synthesize the Pd-doped Ag nanocluster with high yield.The prepared Pd1Ag28 nanocluster was characterized by mass spectroscopy,X-ray photoelectron spectroscopy,X-ray crystallography,fluorescence spectroscopy,ultraviolet-visible absorption spectroscopy and transient absorption spectroscopy.The nanocluster exhibits a perfect face-centered cubic(FCC)kernel structure with a tetrahedron-like shell.Of note,Pd1Ag28 nanocluster had an unexpectedly long excited-state lifetime of 3.3 microseconds,which is the longest excited-state lifetime for Ag-based nanoclusters S0 far.Meanwhile,the excellent near-infrared luminescence indicated the nanocluster has the potential in fluorescent bio-imaging.Besides,it was revealed that Pd1Ag28 nanocluster could be transformed into Au1Ag28 nanocluster via ion exchange reaction of AuPPhzCl with Pd1Ag28 nanocluster.This work provides an efficient synthetic protocol of alloy nanoclusters and wil contribute to study the effect of foreign atom on the properties of metal nanoclusters.展开更多
小型棒控压水堆舍弃了可溶硼,并高度依赖控制棒与可燃毒物棒控制堆芯的反应性。为研究控制棒对堆芯关键性能的影响,本文以核动力破冰船用KLT-40模型为对象,以轴向功率偏移、堆芯寿期、燃料利用率与径向功率峰因子为指标,开展长寿期小型...小型棒控压水堆舍弃了可溶硼,并高度依赖控制棒与可燃毒物棒控制堆芯的反应性。为研究控制棒对堆芯关键性能的影响,本文以核动力破冰船用KLT-40模型为对象,以轴向功率偏移、堆芯寿期、燃料利用率与径向功率峰因子为指标,开展长寿期小型棒控压水堆控制棒布置与动作策略设计分析。首先,基于OpenMC程序开发带棒燃耗程序;其次,比较堆芯带控制棒与无控制棒运行时的堆芯寿期等指标;最后,分析不同动作策略对轴向功率偏移等指标的影响。结果表明:控制棒将堆芯寿期从590 EFPDs(等效满功率天,Effective full power days)延长至650~698 EFPDs;低价值棒组优先动作策略使轴向功率偏移程度由−0.69与+0.80分别下降至−0.29与+0.52。因此,要准确计算长寿期压水堆寿期必须采用带控制棒燃耗计算策略,并且通过合理的动作策略能够有效减小控制棒带来的轴向功率偏移。展开更多
As predicted by classical macroscopic theory, the lifetime for nanoscale gas bub-bles is extremely short. However, stable gas nanobubbles have been experimen-tally observed in recent years. In this report, we theoreti...As predicted by classical macroscopic theory, the lifetime for nanoscale gas bub-bles is extremely short. However, stable gas nanobubbles have been experimen-tally observed in recent years. In this report, we theoretically show that, if the inner density of gas bubbles is sufficiently high, the lifetime of nanobubbles can increase by at least 4 orders of magnitude, and even approaches the timescale for experi-mental observations.展开更多
Herein,we design and synthesize a series of oligomers[Ir(ppy)2(dabpy)-ODPA]n(D1-n)by copolymerization of[Ir(ppy)2(dabpy)][PF6](D2)with 4,4′-Oxydiphthalic anhydride(ODPA),to resolve the problem of simultaneous improve...Herein,we design and synthesize a series of oligomers[Ir(ppy)2(dabpy)-ODPA]n(D1-n)by copolymerization of[Ir(ppy)2(dabpy)][PF6](D2)with 4,4′-Oxydiphthalic anhydride(ODPA),to resolve the problem of simultaneous improvement of sta-bility and activity of classical iridium complex for photocatalytic water-splitting.Fourier-transform infrared spectroscopy,X-ray photoelectron spectroscopy,solid-state nuclear magnetic resonance,and gel permeation chromatography results indicate that the degree of polymerization(n)of D1-n could be tuned by the syn-thesis method.The best photocatalytic performance is reached by D1-n with n at of 2 and/or 3(D1-2/3),which exhibits a photocatalytic lifetime up to 676 h and a photocatalytic hydrogen evolution of 162055.1 Compared with classicalμmol⋅g-1.iridium complex D2,the photocatalytic lifetime of D1-2/3 is about 38 times longer and the photocatalytic activity is 1.3 times higher.Further increase of n leads to a decrease in both photocatalytic lifetime and activity.According to the spectro-scopic characterizations,photoelectrochemical experiments,and density functional theory calculation,the significantly enhanced photocatalytic performance of D1-2/3 originates from the oligomeric structure.The oligomer chain of D1-2/3 with suit-able length acts as a large steric hindrance to reduce the undesired photoinduced decomposition and prolong its lifetime.The possible coupling of adjacent Ir com-plexes in D1-2/3 lowers the energy gap and increases the utilization of visible light,which overcomes the adverse effect of large steric hindrance andfinally improve the activity.This workfirst provides a simple strategy for constructing oligomeric Ir photosensitizers to simultaneously achieve long lifetime and high activity,it will lay the foundation for the design of highly efficient photosensitizers in the future.展开更多
基金The financial supports of the National Natural Science Foundation of China (grant nos. 21373042, 21677029 and 51402036)the Fundamental Research Funds for the Central Universities (grant no. DUT15YQ109)
文摘Recently, an effective exciton diffusion length L exceeding 100μm has been reported for organic- inorganic halide perovskites owing to both the high mobility and ultra-long lifetime of the excitons; however, the origin of ultra-long L is still unclear in nature. In some photoelectric materials, reverse intersystem crossing (RISC) from the triplet to the singlet state can enhance the quantum yield of pho- toluminescence greatly. In this study, our theoretical investigation indicated that the energy difference △E_st between the singlet state and the triplet state of CH_3NH_3Pbl_3 was less than 0.1 eV, which represents one crucial prerequisite for the occurrence of RISC. Meanwhile, the experimental results showed that the photoluminescence lifetime increased with the increasing temperature, a typical feature of RISC. Based on this study, we put forward the hypothesis that the ultra-long lifetime of excitons in organic-inorganic halide perovskite might be caused by the RISC process. This may provide a new insight into the important photophysical properties of such novel photovoltaic materials.
基金supported by the National Key R&D Program of China (Nos. 2016YFB0401801, 2016YFB0400803)the Science Challenge Project (No. TZ2016003)+1 种基金the National Natural Science Foundation of China (Nos. 61674138, 61674139, 61604145, 61574135, 61574134, 61474142, 61474110)the Beijing Municipal Science and Technology Project (No. Z161100002116037)
文摘GaN-based continuous-wave operated blue-violet laser diodes(LDs) with long lifetime are demonstrated, which are grown on a c-plane GaN substrate by metal organic chemical vapor deposition with a 10 × 600 μm^2 ridge waveguide structure.The electrical and optical characteristics of a blue-violet LD are investigated under direct-current injection at room temperature(25 °C). The stimulated emission wavelength and peak optical power of the LD are around 413 nm and over 600 mW, respectively.In addition, the threshold current density and voltage are as small as 1.46 kA/cm^2 and 4.1 V, respectively. Moreover, the lifetime is longer than 1000 hours under room-temperature continuous-wave operation.
基金supported by National Natural Science Foundation of China(No.21043010)the Research Foundation of the Key Laboratory of Chemical Lasers of Dalian Institute of Chemical Physics(No.KLCL-2011-N4)
文摘Ultracold plasma provides a possible route to approach the strongly-coupled regime under laboratory conditions. Normally, the lifetime of ultracold plasma is very limited due to plasma heating and expansion mechanisms. We present a new method to generate long lifetime ultracold plasmas consisting mainly of cations and anions. This plasma demonstrates a capability of traversing a DC barrier of up to 5 (or -3) V. The lifetime of this plasma is expected to be more than 250us. Finally, molecular dynamics (MD) simulation is used to explain how anions slow the expansion rate and prolong the lifetime of this plasma.
文摘Atmospheric lifetimes and traveling distances of 15 PAHs(Ac:acenaphthylene,Ace:acenaphthene,Ph:phenanthrene,MePh3:3-methyl-phenanthrene,MePh9:9-methyl-phenanthrene,MePh1:1-methyl-phenanthrene,MePh2:2-methyl-phenanthrene,Ret:retene,B[a]A:benzo[a]anthracene,Chry:chrysene,B[b,j,k]F:benzo[b,j,k]fluoranthene,B[e]P:benzo[e]pyrene,B[a]P:benzo[a]pyrene,Ind:indeno[1,2,3-cd]pyrene,B[g,h,i]P:benzo[g,h,i]perylene)at Whitbourne,UK,were estimated by using the rate constants for reaction with OH,O3,and the first order rate constants of eight species of high molecular weight PAHs(i.e.B[a]A,Chry,B[b]F,B[k]F,B[a]P,Ind,B[g,h,i]P and Ret)as a function of humidity,solar intensity and temperature by using Multiple Regression Analysis.The predicted atmospheric lifetime of Ac,Ace,Ph,MePh3,MePh9,MePh2 and MePh1 ranged between 11.42 h-79.12 h in cold period and 1/31 h-14.33 h in warm period respectively.The binary ratios of atmospheric lifetime of B[k]F/B[g,h,i]P,B[k]F/B[g,h,i]P,B[g,h,i]P/Ind and B[k]F/Ind displayed non-significant differences between cold and warm period,indicating that high molecular weight PAHs are difficult to be decomposed by UV light and thus may be conveyed to the rural regions via long range atmospheric transportation(LRAT).The decreased level of the atmospheric lifetime of low molecular weight PAHs in summer can be attributed to an increased level of OH radical content and solar radiation.
文摘The lifetime of a lunar satellite orbit is constrained by the non-spherical nature of the Moon’s gravity field. The orbital lifetime of lunar orbits depends significantly on the initial conditions of the orbit. Right ascension of ascending node (Ω) is one of the important orbital parameter affecting the orbital lifetime. In the present work we have analyzed the effect of Ω on the variation of lifetime with altitude for circular lunar orbits. It is found that at a particular initial altitude, a small increase in the altitude results in substantial increase in the orbital lifetime due to effect of the long periodic terms of Earth’s gravity on eccentricity and this transition altitude is different for different Ω. Further, it is observed that the variation of transition altitude with Ω follows a definite, but different trend for orbits with different inclinations. The transition altitude for polar orbits is found to be higher without the effect of Sun and Earth gravity. Variation of transition altitude with orbital inclination is also analyzed. Lifetimes of high altitude circular lunar orbits are analyzed and it is observed that at high altitudes lifetime decreases with altitude.
基金National Key R&D Program of China,Grant/Award Number:2022YFE0109000National Natural Science Foundation of China,Grant/Award Number:21975152+1 种基金China Postdoctoral Science Foundation,Grant/Award Number:2022M722028Deutsche Forschungsgemeinschaft,Grant/Award Number:3DMM2O−EXC−2082/1−390761711。
文摘Thermally activated delayedfluorescence(TADF)molecules are regarded as promis-ing materials for realizing high-performance organic light-emitting diodes(OLEDs).The connecting groups between donor(D)and acceptor(A)units in D–A type TADF molecules could affect the charge transfer and luminescence performance of TADF materials in aggregated states.In this work,we design and synthesize four TADF molecules using planar and twisted linkers to connect the aza-azulene donor(D)and triazine acceptor(A).Compared with planar linkers,the twisted ones(Az-NP-T and Az-NN-T)can enhance A–A aggregation interaction between adjacent molecules to balance hole and electron density.As a result,highly efficient and stable deep-red top-emission OLEDs with a high electroluminescence efficiency of 57.3%and an impressive long operational lifetime(LT_(95)∼30,000 h,initial luminance of 1000 cd m^(-2))are obtained.This study provides a new strategy for designing more effi-cient and stable electroluminescent devices through linker aggregation engineering in donor–acceptor molecules.
基金We acknowledge the National Natural Science Foundation of China(No.21601178).
文摘Doping foreign atom(s)in metal nanoclusters is an effective strategy to engineer the properties and functionalities of metal nanoclusters.However,until now,to dope Pd atom into Ag nanoclusters remains a huge challenge.Here we develop a one-step rapid method to synthesize the Pd-doped Ag nanocluster with high yield.The prepared Pd1Ag28 nanocluster was characterized by mass spectroscopy,X-ray photoelectron spectroscopy,X-ray crystallography,fluorescence spectroscopy,ultraviolet-visible absorption spectroscopy and transient absorption spectroscopy.The nanocluster exhibits a perfect face-centered cubic(FCC)kernel structure with a tetrahedron-like shell.Of note,Pd1Ag28 nanocluster had an unexpectedly long excited-state lifetime of 3.3 microseconds,which is the longest excited-state lifetime for Ag-based nanoclusters S0 far.Meanwhile,the excellent near-infrared luminescence indicated the nanocluster has the potential in fluorescent bio-imaging.Besides,it was revealed that Pd1Ag28 nanocluster could be transformed into Au1Ag28 nanocluster via ion exchange reaction of AuPPhzCl with Pd1Ag28 nanocluster.This work provides an efficient synthetic protocol of alloy nanoclusters and wil contribute to study the effect of foreign atom on the properties of metal nanoclusters.
文摘小型棒控压水堆舍弃了可溶硼,并高度依赖控制棒与可燃毒物棒控制堆芯的反应性。为研究控制棒对堆芯关键性能的影响,本文以核动力破冰船用KLT-40模型为对象,以轴向功率偏移、堆芯寿期、燃料利用率与径向功率峰因子为指标,开展长寿期小型棒控压水堆控制棒布置与动作策略设计分析。首先,基于OpenMC程序开发带棒燃耗程序;其次,比较堆芯带控制棒与无控制棒运行时的堆芯寿期等指标;最后,分析不同动作策略对轴向功率偏移等指标的影响。结果表明:控制棒将堆芯寿期从590 EFPDs(等效满功率天,Effective full power days)延长至650~698 EFPDs;低价值棒组优先动作策略使轴向功率偏移程度由−0.69与+0.80分别下降至−0.29与+0.52。因此,要准确计算长寿期压水堆寿期必须采用带控制棒燃耗计算策略,并且通过合理的动作策略能够有效减小控制棒带来的轴向功率偏移。
基金the National Natural Science Foundation of China (Grant Nos. 10474109 and 10674146)
文摘As predicted by classical macroscopic theory, the lifetime for nanoscale gas bub-bles is extremely short. However, stable gas nanobubbles have been experimen-tally observed in recent years. In this report, we theoretically show that, if the inner density of gas bubbles is sufficiently high, the lifetime of nanobubbles can increase by at least 4 orders of magnitude, and even approaches the timescale for experi-mental observations.
基金National Natural Science Foundation of China,Grant/Award Number:51803208the Youth Innovation Promotion Association CAS,Grant/Award Number:E2202005。
文摘Herein,we design and synthesize a series of oligomers[Ir(ppy)2(dabpy)-ODPA]n(D1-n)by copolymerization of[Ir(ppy)2(dabpy)][PF6](D2)with 4,4′-Oxydiphthalic anhydride(ODPA),to resolve the problem of simultaneous improvement of sta-bility and activity of classical iridium complex for photocatalytic water-splitting.Fourier-transform infrared spectroscopy,X-ray photoelectron spectroscopy,solid-state nuclear magnetic resonance,and gel permeation chromatography results indicate that the degree of polymerization(n)of D1-n could be tuned by the syn-thesis method.The best photocatalytic performance is reached by D1-n with n at of 2 and/or 3(D1-2/3),which exhibits a photocatalytic lifetime up to 676 h and a photocatalytic hydrogen evolution of 162055.1 Compared with classicalμmol⋅g-1.iridium complex D2,the photocatalytic lifetime of D1-2/3 is about 38 times longer and the photocatalytic activity is 1.3 times higher.Further increase of n leads to a decrease in both photocatalytic lifetime and activity.According to the spectro-scopic characterizations,photoelectrochemical experiments,and density functional theory calculation,the significantly enhanced photocatalytic performance of D1-2/3 originates from the oligomeric structure.The oligomer chain of D1-2/3 with suit-able length acts as a large steric hindrance to reduce the undesired photoinduced decomposition and prolong its lifetime.The possible coupling of adjacent Ir com-plexes in D1-2/3 lowers the energy gap and increases the utilization of visible light,which overcomes the adverse effect of large steric hindrance andfinally improve the activity.This workfirst provides a simple strategy for constructing oligomeric Ir photosensitizers to simultaneously achieve long lifetime and high activity,it will lay the foundation for the design of highly efficient photosensitizers in the future.