The S_(1) state decay dynamics of 2-hydroxypyridine following UV excitation at a wavelength range of 276.9-250.0 nm is investigated using femtosecond time-resolved photoelectron imaging technique.Based on pump wavelen...The S_(1) state decay dynamics of 2-hydroxypyridine following UV excitation at a wavelength range of 276.9-250.0 nm is investigated using femtosecond time-resolved photoelectron imaging technique.Based on pump wavelength dependence of the decay dynamics,a refined decay picture is proposed.At pump wavelength of 276.9 nm,the S_(1) state is depopulated through intersystem crossing to lower triplet state(s).At 264.0 nm,both intersystem crossing to lower triplet state(s)and internal conversion to the ground state are in operation.At 250.0 nm,internal conversion to the ground state becomes dominated.展开更多
The decay dynamics of N, N-dimethylthioacetamide after excitation to the S3(ππ*) state was studied by using the resonance Raman spectroscopy and complete active space self- consistent field method calculations. T...The decay dynamics of N, N-dimethylthioacetamide after excitation to the S3(ππ*) state was studied by using the resonance Raman spectroscopy and complete active space self- consistent field method calculations. The UV-absorption and vibrational spectra were as- signed. The A-band resonance Raman spectra were obtained in acetonitrile, methanol and water with the laser excitation wavelengths in resonance with the first intense absorption band to probe the Franck-Condon region structural dynamics. The CASSCF calculations were carried out to determine the excitation energies and optimized structures of the lower- lying singlet states and conical intersection point. The A-band structural dynamics and the corresponding decay mechanism were obtained by the analysis of the resonance Raman in- tensity pattern and the CASSCF calculated structural parameters. The major decay channel of S3,FC (ππ*)→S3(ππ*)/S1 (nπ*)→S1(nπ*) is proposed.展开更多
Starting from vorticity equation, the triggering mechanism and amplitude decay of shear waves in the ocean are discussed in this paper. The theoretical analysis indicates that by the action of stripped external force ...Starting from vorticity equation, the triggering mechanism and amplitude decay of shear waves in the ocean are discussed in this paper. The theoretical analysis indicates that by the action of stripped external force (for examples, the sudden setting of stripped wind, moving stripped wind, etc. ), shear waves can be triggered. This is qualitatively consistent with satellite observations. The amplitude decay process of shear waves by the action of side friction is also discussed in the paper. The theoretical model is quantitatively consistent with satellite observations.展开更多
In this work we re-examine a model of the nucleons that involve the weak interaction which was once considered by Heisenberg;that is a neutron may have the structure of a dwarf hydrogen-like atom. We formulate a quant...In this work we re-examine a model of the nucleons that involve the weak interaction which was once considered by Heisenberg;that is a neutron may have the structure of a dwarf hydrogen-like atom. We formulate a quantum dynamics for the Heisenberg model of the neutron associated with interaction that involves the beta decay in terms of a mixed Coulomb-Yukawa potential and the More General Exponential Screened Coulomb Potential (MGESCP), which has been studied and applied to various fields of physics. We show that all the components that form the MGESCP potential can be derived from a general system of linear first order partial differential equations similar to Dirac relativistic equation in quantum mechanics. There are many interesting features that emerge from the MGESCP potential, such as the MGESCP potential can be reduced to the potential that has been proposed to describe the interaction between the quarks for strong force in particle physics, and the energy spectrum of the bound states of the dwarf hydrogen-like atom is continuous with respect to distance. This result leads to an unexpected implication that a proton and an electron may also interact strongly at short distances. We also show that the Yukawa potential when restrained can generate and determine the mathematical structures of fundamental particles associated with the strong and weak fields.展开更多
The excited state structural dynamics of phenyl absorbing S2(A'), S3(A'), and S6(A') states were troseopy and complete active space self-consistent and the UV absorption bands were assigned on azide (PhN3) ...The excited state structural dynamics of phenyl absorbing S2(A'), S3(A'), and S6(A') states were troseopy and complete active space self-consistent and the UV absorption bands were assigned on azide (PhN3) after excitation to the light studied using the resonance Raman specfield calculations. The vibrational spectra the basis of the Fourier transform (FT)- Raman, FT-infrared measurements, the density-functional theory computations and the normal mode analysis. The A-, B-, and C-bands resonance Raman spectra in cyclohex- ane, acetonitrile, and methanol solvents were, respectively, obtained at 273.9, 252.7, 245.9, 228.7, 223.1, and 208.8 nm excitation wavelengths to probe the corresponding structural dynamics of PhN3. The results indicated that the structural dynamics in the S2 (A'), S3(A'), and S6(A') states were significantly different. The crossing points of the potential energy surfaces, S2S1(1) and S2S1(2), were predicted to play a key role in the low-lying excited state decay dynamics, in accordance with Kasha's rule, and NT=N8 dissociation. Two decay channels initiated from the Franck-Condon region of the S2(A') state were predicted: the radiative S2,min→S0 radiative decay and the S2→S1 internal conversion through the crossing points S2S1 (1)/S2S1(2).展开更多
Azadirachta indica A. Juss, Dalbergia, sissoo Roxb., and Melia azedarach L. are little studied species in nutrient return capabilities from leaf litter decomposition to maintenance of the soil fertility despite their ...Azadirachta indica A. Juss, Dalbergia, sissoo Roxb., and Melia azedarach L. are little studied species in nutrient return capabilities from leaf litter decomposition to maintenance of the soil fertility despite their importance in agroforestry practices of Bangladesh. A leaf litter decomposition experiment was conducted using a litterbag teeh7 nique to assess the nutrient reaun efficiency of these species. The de- composition rate of leaf litter was highest for M. azedarach and lowest for D. sissoo. Rainfall and temperature of study sites showed a significant (p〈0.05) positive relationship with the rate of leaf litter decomposition. The highest decay constant was observed for M. azedarach (6.67). Nitrogen and Phosphorus concentration in leaf litter showed a decreased trend sharply at the end of the first month, whereas rapid decrease of Potassium concentration was reported within 10 days. Conversely, higher concentration of nutrient was observed at the later stages of decomposition. All three species showed a similar pattern of nutrient release (K 〉 N 〉 P) during the decomposition process of leaf litter. Among the studied species, D. sissoo was best in terms of N and P return and A. indica was best in terms of K return.展开更多
We investigate the entanglement dynamics of two coupled chromophore pairs embedded in a protein-solvent environment.The non-Markovian and non-perturbative hierarchical expansion technique is used in the solution of th...We investigate the entanglement dynamics of two coupled chromophore pairs embedded in a protein-solvent environment.The non-Markovian and non-perturbative hierarchical expansion technique is used in the solution of the quantum dynamics.The spectral distribution function of the bath is set with the Drude–Lorentz form.It is shown that the evolutions of the entanglement described by the measures of negativity and concurrence are in agreement with each other.They decay to zero in a short time and the sudden death and sudden birth can be observed in the process of the evolutions of the entanglement.展开更多
The decay estimations of the solution to an elliptic equation with dynamical boundary condition is considered.We proved that,for suitable initial datum,the energy of the solution decays "in time" exponential...The decay estimations of the solution to an elliptic equation with dynamical boundary condition is considered.We proved that,for suitable initial datum,the energy of the solution decays "in time" exponentially if p=0,whereas the decay is polynomial order if p>0.展开更多
The structure determination of metal nanoclusters protected by ligands is critical in understanding their physical and chemical properties,yet it remains elusive how the metal core and ligand of metal clusters coopera...The structure determination of metal nanoclusters protected by ligands is critical in understanding their physical and chemical properties,yet it remains elusive how the metal core and ligand of metal clusters cooperatively contribute to the observed performances.Here,with the successful synthesis of Au_(44)TBPA_(22)Cl_(2)cluster(TBPA=4-tert-butylphenylacetylene),the structural isomer of previously reported Au_(44)L_(28)clusters(L denoted as ligand)is filled,thereby providing an opportunity to explore the property evolution rules imparted by different metal core structures or different surface ligands.Time-resolved transient absorption spectroscopy reveals that the difference in the core structure between Au_(44)TBPA_(22)Cl_(2)and Au_(44)L_(28)can bring nearly 360 times variation of excited-state lifetime,while only 3–24 times differences in excited-state lifetimes of the three Au_(44)L_(28)nanoclusters with identical metal core but different ligands are observed,which is due to much stronger impact of the metal core than the surface ligands in the electronic energy bands of the clusters.In addition,the Au_(44)clusters protected by alkyne ligands are shown to be highly effective toward the electrochemical oxidation of ethanol,compared to the Au_(44)clusters capped by thiolates,which is ascribed to smaller charge transfer impedance of the former clusters.We anticipate that the study will enhance the process in controlling the nanomaterial properties by precisely tailoring metal core or surface patterns.展开更多
The decay dynamic of an excited quantum emitter(QE)is one of the most important contents in quantum optics.It has been widely applied in the field of quantum computing and quantum state manipulation.When the electroma...The decay dynamic of an excited quantum emitter(QE)is one of the most important contents in quantum optics.It has been widely applied in the field of quantum computing and quantum state manipulation.When the electromagnetic environment is described by several pseudomodes,the effective Hamiltonian method based on the multi-mode Jaynes-Cummings model provides a clear physical picture and a simple and convenient way to solve the decay dynamics.However,in previous studies,only the resonant modes are taken into account,while the non-resonant contributions are ignored.In this work,we study the applicability and accuracy of the effective Hamiltonian method for the decay dynamics.We consider different coupling strengths between a two-level QE and a gold nanosphere.The results for dynamics by the resolvent operator technique are used as a reference.Numerical results show that the effective Hamiltonian method provides accurate results when the two-level QE is resonant with the plasmon.However,when the detuning is large,the effective Hamiltonian method is not accurate.In addition,the effective Hamiltonian method cannot be applied when there is a bound state between the QE and the plasmon.These results are of great significance to the study of the decay dynamics in micro-nano structures described by quasi-normal modes.展开更多
Luminescent metal halides doped with ns^(2-)metal ions such as 6s^(2-)metal Bi^(3+)have aroused reviving interest owing to their outstanding optical properties;however,the origin of the photoluminescence(PL)remains co...Luminescent metal halides doped with ns^(2-)metal ions such as 6s^(2-)metal Bi^(3+)have aroused reviving interest owing to their outstanding optical properties;however,the origin of the photoluminescence(PL)remains controversial and unclear.Herein,we report a strategy for the controlled synthesis of Bi^(3+)-doped vacancy-ordered double perovskite Cs_(2)SnCl_(6)nanocrystals(NCs)and unravel the triplet excited-state dynamics of Bi^(3+)through temperature-dependent PL and ultrafast femtosecond transient absorption spectroscopies.Owing to the aliovalent Bi^(3+)doping in the spatially confined zero-dimensional(0D)structure of Cs2SnCl6,Bi^(3+)ions experience an enhancive Jahn-Teller distortion in the excited state,which results in intense broadband blue PL originating from the inter-configurational 3P0,1→1S0 transitions of Bi^(3+)at 450 nm,with a large Stokes shift and a quantum yield of 35.2%.Specifically,an unusual thermal-enhanced Jahn-Teller splitting of the excitation band and a remarkable transition of the PL lifetime from ms at 10 K toμs at 300 K were observed,as solid evidence for the isolated Bi^(3+)emission.These findings clarify the controversy about the PL origin in ns^(2-)metal ion-doped lead-free luminescent metal halides,thereby paving the way for exploring their optoelectronic applications.展开更多
The isospin fractionations in 124Sn,107Sn+120Sn at 600 MeV/nucleon,and 136Xe,124Xe+208Pb at 1000 MeV/nucleon are investigated by the isospin-dependent quantum molecular dynamics model coupled with the statistical code...The isospin fractionations in 124Sn,107Sn+120Sn at 600 MeV/nucleon,and 136Xe,124Xe+208Pb at 1000 MeV/nucleon are investigated by the isospin-dependent quantum molecular dynamics model coupled with the statistical code GEMINI.The yield ratio as a function of the binding energy difference for light mirror nuclei 3H/3He,7Li/7Be,11B/11C,and 15N/15O is applied to estimate the ratio between neutrons and protons in the gas of the fragmenting system.By comparing the estimated values resulting from the simulations with and without the GEMINI code,it was found that the secondary decay distorts the signal of the isospin fractionation.To minimize the secondary decay effects,the yield ratio of the light mirror nuclei 3H/3He as well as its double ratio between two systems with different isospin asymmetries of the projectiles is recommended as robust isospin observables.展开更多
The beam windows of high-energy beam lines are important,and it is sometimes difficult to design because it is necessary to ensure particle propagation with minimum disturbance and fulfill mechanical requirements at t...The beam windows of high-energy beam lines are important,and it is sometimes difficult to design because it is necessary to ensure particle propagation with minimum disturbance and fulfill mechanical requirements at the same time.The upstream decay pipe window of the long baseline neutrino facility at Fermilab has an extremely large diameter(1.8 m),with a thickness of only 1.5 mm to separate the helium atmosphere in the decay pipe and the nitrogen atmosphere on the other side.Furthermore,the center of this dish-shaped window is expected to be a200-mm-diameter beryllium dish welded to the outside aluminum alloy A6061,and this welded combination must withstand extreme conditions of a 2.4-MW,high-energy proton beam without leakage.These severe conditions make the design of this window an unprecedented challenge.This paper describes the static thermal-structural analyses based on which the structure has been optimized,as well as dynamic analyses for understanding the shockwave effects originating in the beam.After optimization,the maximum von Mises stresses in the window decreased significantly in both normal operation and accident cases,making our design very reasonable.展开更多
One of the practical approaches in identifying structures is the non-linear resonant decay method which identifies a non-linear dynamic system utilizing a model based on linear modal space containing the underlying li...One of the practical approaches in identifying structures is the non-linear resonant decay method which identifies a non-linear dynamic system utilizing a model based on linear modal space containing the underlying linear system and a small number of extra terms that exhibit the non-linear effects.In this paper,the method is illustrated in a simulated system and an experimental structure.The main objective of the non-linear resonant decay method is to identify the non-linear dynamic systems based on the use of a multi-shaker excitation using appropriated excitation which is obtained from the force appropriation approach.The experimental application of the method is indicated to provide suitable estimates of modal parameters for the identification of non-linear models of structures.展开更多
In this paper,a one-dimension particle-in-cell(PIC)code(EDIPIC)is employed to simulate the parallel-plate ion extraction process under an externally applied electrostatic field,focusing on the analysis of the influe n...In this paper,a one-dimension particle-in-cell(PIC)code(EDIPIC)is employed to simulate the parallel-plate ion extraction process under an externally applied electrostatic field,focusing on the analysis of the influe nee of the initial electron temperature on the extracted ion fluxes to the metal plates during the ion extraction process.Compared with previously published results,the plasma oscillations on a timescale of the electron plasma period,and the excitation of the ion acoustic rarefaction waves resulting from the plasma oscillations originating from both the negative and positive electrodes,are studied for the first time.The modeling results show that both the negative and positive extractors can collect ions due to the plasma oscillations and the propagation of the ion acoustic rarefaction waves.With the in crease of the initial electron temperature achieved by keeping other parameters unchanged,on the one hand,both the ion speed and flux to the negative and positive plates increase,which leads to a significant decrease of the ion extraction time,while on the other hand,the ion flux to the positive plate after the formation of a Child-Langmuir sheath is much more sensitive to an increase of the initial electron temperature than that to the negative plate.The PIC simulation results provide a deeper physical understanding of the influence of the initial electron temperature on the characteristics of the entire ion extraction process in a decaying plasma.展开更多
Photo-induced excited-state dynamics within organic materials fundamentally determine their photophysical properties for various applications,and thus understanding the primary excited-state dynamics behavior is of fu...Photo-induced excited-state dynamics within organic materials fundamentally determine their photophysical properties for various applications,and thus understanding the primary excited-state dynamics behavior is of fundamental and practical significance.Until recently,the excited-state dynamics of organic materials towards biophotonics have been rarely studied,although numerous endeavors have been devoted to the design of organic materials for biophotonics.Herein,various spectroscopy technologies including femtosecond transient absorption(fs-TA)spectroscopy clearly reveal a totally different excited state dynamics behavior within Bodipy monomer(2B-BDP dye)and aggregates(2B-BDP NPs),indicating strongly morphology dependent character.2B-BDP dye undergoes an ultrafast conversion from S1 to intramolecular charge transfer(ICT)state for subsequent photoluminescence(PL)and nonradiative(NR)decay,while 2B-BDP NPs show an accelerated excited-state deactivation mainly through S1→S0 NR decay.The potential bioapplications based on the corresponding excited state dynamics behavior are discussed together with experimental results.Interestingly,the accelerated NR decay in 2B-BDP NPs does not yield a stronger photoacoustic(PA)signal than that in 2B-BDP dye,which violates the conventional wisdom that faster NR decay would benefit the photothermal effects for better photoacoustic imaging(PAI).These insightful and fundamental observations of the excited-state dynamics may contribute an alternative approach at the molecular level towards the future design of functional Bodipy-based organic molecules with desirable performances.展开更多
The branching ratios and CP violations of the B →Dπ decays, including both the color-allowed and the color-suppressed modes, are investigated in detail within QCD framework by considering all diagrams that lead to t...The branching ratios and CP violations of the B →Dπ decays, including both the color-allowed and the color-suppressed modes, are investigated in detail within QCD framework by considering all diagrams that lead to three effective currents of two quarks. An intrinsic mass scale as a dynamical gluon mass is introduced to treat the infrared divergence caused by the soft collinear approximation in the endpoint regions, and the Cutkosky rule is adopted to deal with a physical-region singularity of the on mass-shell quark propagators. When the dynamical gluon mass μg is regarded as a universal sca/e, it is extracted to be around μg = 440 MeV from one of the well-measured B →Dπ decay modes. The resulting predictions for all branching ratios are in agreement with the current experimental measurements. As these decays have no penguin contributions, there are no direct CP asymmetries. Due to interference between the Cabibbo-suppressed and the Cabibbo-favored amplitudes, mixing-induced CP violations are predicted in the B →D^±π^±↓ decays to be consistent with the experimental data at 1-σ level. More precise measurements will be helpful to extracting weak angle 2β+γ.展开更多
Based on the latest oceanic surface drifter dataset from the global drifter program during 2000–2019,this study investigated the global variation of relative frequency shift(RFS),near-inertial energy(NIE)and inverse ...Based on the latest oceanic surface drifter dataset from the global drifter program during 2000–2019,this study investigated the global variation of relative frequency shift(RFS),near-inertial energy(NIE)and inverse excess bandwidth(IEB)of near-inertial motions,and analyzed their relations with oceanic mesoscale dynamics,relative vorticity and strain.Compared with previous works,we have some new findings in this study:(1)the RFS was high with negative values in some regions in which we found a significant blue shift of the RFS in the equatorward of 30°N(S)and from 50°N to 60°N in the Pacific,and a red shift in the western boundary currents and their extension regions,the North Atlantic and the Antarctic Circumpolar Current regions;(2)more peak values of the NIE were found in global regions like the South Indian Ocean,the Luzon Strait and some areas of the South Ocean;(3)the global distribution of the IEB were characterized by clear zonal bands and affected by vorticity and wind field;(4)the RFS was elevated as the absolute value of the gradient of vorticity increased,the IEB did not depend on the gradient of vorticity,and the eddy kinetic energy(EKE)weakened with the decrease of the absolute value of RFS;(5)the NIE decreased with increasing absolute value of the relative vorticity and the gradient of vorticity,but it increased with increasing strain and EKE when EKE was larger than 0.0032 m2/s2.展开更多
We propose a method for calculating the nonradiative decay rates for polyatomic molecules including anharmonic effects of the potential energy surface(PES)in the Franck-Condon region.The method combines the n-mode rep...We propose a method for calculating the nonradiative decay rates for polyatomic molecules including anharmonic effects of the potential energy surface(PES)in the Franck-Condon region.The method combines the n-mode repre-sentation method to construct the ab initio PES and the nearly exact time-dependent density matrix renormalization group method(TD-DMRG)to simulate quantum dynamics.In addition,in the framework of TD-DMRG,we further develop an algorithm to calculate the final-state-resolved rate coefficient which is very useful to analyze the contribution from each vibrational mode to the transition process.We use this method to study the internal conversion(IC)process of azulene after taking into account the anharmonicity of the ground state PES.The results show that even for this semi-rigid molecule,the intramode anharmonicity enhances the IC rate significantly,and after considering the two-mode coupling effect,the rate increases even further.The reason is that the anharmonicity enables the C-H vibrations to receive electronic energy while C-H vibrations do not contribute on the harmonic PES as the Huang-Rhys factor is close to 0.展开更多
Unlike regular stabilizations, we construct in the paper a specific feedback control system such that u(t) decays exponentially with the designated decay rate, and that some non-trivial linear functionals of u decay e...Unlike regular stabilizations, we construct in the paper a specific feedback control system such that u(t) decays exponentially with the designated decay rate, and that some non-trivial linear functionals of u decay exactly faster than . The system contains a dynamic compensator with another state v in the feedback loop, and consists of two states u and v. This problem entirely differs from the one with static feedback scheme in which the system consists only of a single state u. To show the essential difference, some specific property of the spectral subspaces associated with our control system is studied.展开更多
基金supported by the National Natural Science Foundation of China(No.21833003)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB17000000)the Key Technology Team of the Chinese Academy of Sciences(GJJSTD20190002)。
文摘The S_(1) state decay dynamics of 2-hydroxypyridine following UV excitation at a wavelength range of 276.9-250.0 nm is investigated using femtosecond time-resolved photoelectron imaging technique.Based on pump wavelength dependence of the decay dynamics,a refined decay picture is proposed.At pump wavelength of 276.9 nm,the S_(1) state is depopulated through intersystem crossing to lower triplet state(s).At 264.0 nm,both intersystem crossing to lower triplet state(s)and internal conversion to the ground state are in operation.At 250.0 nm,internal conversion to the ground state becomes dominated.
基金This work was supported by the National Natu- ral Science Foundation of China (No.21033002 and No.21202032) and the National Basic Research Pro- gram of China (No.2013CB834604).
文摘The decay dynamics of N, N-dimethylthioacetamide after excitation to the S3(ππ*) state was studied by using the resonance Raman spectroscopy and complete active space self- consistent field method calculations. The UV-absorption and vibrational spectra were as- signed. The A-band resonance Raman spectra were obtained in acetonitrile, methanol and water with the laser excitation wavelengths in resonance with the first intense absorption band to probe the Franck-Condon region structural dynamics. The CASSCF calculations were carried out to determine the excitation energies and optimized structures of the lower- lying singlet states and conical intersection point. The A-band structural dynamics and the corresponding decay mechanism were obtained by the analysis of the resonance Raman in- tensity pattern and the CASSCF calculated structural parameters. The major decay channel of S3,FC (ππ*)→S3(ππ*)/S1 (nπ*)→S1(nπ*) is proposed.
文摘Starting from vorticity equation, the triggering mechanism and amplitude decay of shear waves in the ocean are discussed in this paper. The theoretical analysis indicates that by the action of stripped external force (for examples, the sudden setting of stripped wind, moving stripped wind, etc. ), shear waves can be triggered. This is qualitatively consistent with satellite observations. The amplitude decay process of shear waves by the action of side friction is also discussed in the paper. The theoretical model is quantitatively consistent with satellite observations.
文摘In this work we re-examine a model of the nucleons that involve the weak interaction which was once considered by Heisenberg;that is a neutron may have the structure of a dwarf hydrogen-like atom. We formulate a quantum dynamics for the Heisenberg model of the neutron associated with interaction that involves the beta decay in terms of a mixed Coulomb-Yukawa potential and the More General Exponential Screened Coulomb Potential (MGESCP), which has been studied and applied to various fields of physics. We show that all the components that form the MGESCP potential can be derived from a general system of linear first order partial differential equations similar to Dirac relativistic equation in quantum mechanics. There are many interesting features that emerge from the MGESCP potential, such as the MGESCP potential can be reduced to the potential that has been proposed to describe the interaction between the quarks for strong force in particle physics, and the energy spectrum of the bound states of the dwarf hydrogen-like atom is continuous with respect to distance. This result leads to an unexpected implication that a proton and an electron may also interact strongly at short distances. We also show that the Yukawa potential when restrained can generate and determine the mathematical structures of fundamental particles associated with the strong and weak fields.
基金This work is supported by the National Natural Science Foundation of China (No.21473163, No.21033002, No.21202032) and the National Basic Research Program of China (No.2013CB834604).
文摘The excited state structural dynamics of phenyl absorbing S2(A'), S3(A'), and S6(A') states were troseopy and complete active space self-consistent and the UV absorption bands were assigned on azide (PhN3) after excitation to the light studied using the resonance Raman specfield calculations. The vibrational spectra the basis of the Fourier transform (FT)- Raman, FT-infrared measurements, the density-functional theory computations and the normal mode analysis. The A-, B-, and C-bands resonance Raman spectra in cyclohex- ane, acetonitrile, and methanol solvents were, respectively, obtained at 273.9, 252.7, 245.9, 228.7, 223.1, and 208.8 nm excitation wavelengths to probe the corresponding structural dynamics of PhN3. The results indicated that the structural dynamics in the S2 (A'), S3(A'), and S6(A') states were significantly different. The crossing points of the potential energy surfaces, S2S1(1) and S2S1(2), were predicted to play a key role in the low-lying excited state decay dynamics, in accordance with Kasha's rule, and NT=N8 dissociation. Two decay channels initiated from the Franck-Condon region of the S2(A') state were predicted: the radiative S2,min→S0 radiative decay and the S2→S1 internal conversion through the crossing points S2S1 (1)/S2S1(2).
基金supported by Bangladesh Academy of Science and University Grants Commissions of Bangladesh
文摘Azadirachta indica A. Juss, Dalbergia, sissoo Roxb., and Melia azedarach L. are little studied species in nutrient return capabilities from leaf litter decomposition to maintenance of the soil fertility despite their importance in agroforestry practices of Bangladesh. A leaf litter decomposition experiment was conducted using a litterbag teeh7 nique to assess the nutrient reaun efficiency of these species. The de- composition rate of leaf litter was highest for M. azedarach and lowest for D. sissoo. Rainfall and temperature of study sites showed a significant (p〈0.05) positive relationship with the rate of leaf litter decomposition. The highest decay constant was observed for M. azedarach (6.67). Nitrogen and Phosphorus concentration in leaf litter showed a decreased trend sharply at the end of the first month, whereas rapid decrease of Potassium concentration was reported within 10 days. Conversely, higher concentration of nutrient was observed at the later stages of decomposition. All three species showed a similar pattern of nutrient release (K 〉 N 〉 P) during the decomposition process of leaf litter. Among the studied species, D. sissoo was best in terms of N and P return and A. indica was best in terms of K return.
基金by the National Natural Science Foundation of China under Grant No 61078065,and the K.C.Wong Magna Foundation in Ningbo University。
文摘We investigate the entanglement dynamics of two coupled chromophore pairs embedded in a protein-solvent environment.The non-Markovian and non-perturbative hierarchical expansion technique is used in the solution of the quantum dynamics.The spectral distribution function of the bath is set with the Drude–Lorentz form.It is shown that the evolutions of the entanglement described by the measures of negativity and concurrence are in agreement with each other.They decay to zero in a short time and the sudden death and sudden birth can be observed in the process of the evolutions of the entanglement.
基金Supported by the National Natural Science Foundation of China(10671182)Supported by the Natural Science Foundation of Henan Province(0611053300+1 种基金200510463024)Supported by the Young Skeleton Teacher Project of the Higher School of Henan Province
文摘The decay estimations of the solution to an elliptic equation with dynamical boundary condition is considered.We proved that,for suitable initial datum,the energy of the solution decays "in time" exponentially if p=0,whereas the decay is polynomial order if p>0.
基金We acknowledge financial support from the National Natural Science Foundation of China(Nos.22125202,22273095,and 22101128)Programs for high-level entrepreneurial and innovative talents introduction of Jiangsu Province,the Fundamental Research Funds for the Central Universities,Chinese Academy of Sciences(No.YSBR-007)China Postdoctoral Science Foundation(No.2022M721551).
文摘The structure determination of metal nanoclusters protected by ligands is critical in understanding their physical and chemical properties,yet it remains elusive how the metal core and ligand of metal clusters cooperatively contribute to the observed performances.Here,with the successful synthesis of Au_(44)TBPA_(22)Cl_(2)cluster(TBPA=4-tert-butylphenylacetylene),the structural isomer of previously reported Au_(44)L_(28)clusters(L denoted as ligand)is filled,thereby providing an opportunity to explore the property evolution rules imparted by different metal core structures or different surface ligands.Time-resolved transient absorption spectroscopy reveals that the difference in the core structure between Au_(44)TBPA_(22)Cl_(2)and Au_(44)L_(28)can bring nearly 360 times variation of excited-state lifetime,while only 3–24 times differences in excited-state lifetimes of the three Au_(44)L_(28)nanoclusters with identical metal core but different ligands are observed,which is due to much stronger impact of the metal core than the surface ligands in the electronic energy bands of the clusters.In addition,the Au_(44)clusters protected by alkyne ligands are shown to be highly effective toward the electrochemical oxidation of ethanol,compared to the Au_(44)clusters capped by thiolates,which is ascribed to smaller charge transfer impedance of the former clusters.We anticipate that the study will enhance the process in controlling the nanomaterial properties by precisely tailoring metal core or surface patterns.
基金Project supported by the National Natural Science Foundation of China(11964010,11564013 and 11464014)the Natural Science Foundation of Hunan Province(2020JJ4495)+1 种基金the Scientific Research Fund of Hunan Provincial Education Department(22A0377 and 21A0333)the Jishou University Innovation Foundation for Postgraduate(Jdy20038)。
文摘The decay dynamic of an excited quantum emitter(QE)is one of the most important contents in quantum optics.It has been widely applied in the field of quantum computing and quantum state manipulation.When the electromagnetic environment is described by several pseudomodes,the effective Hamiltonian method based on the multi-mode Jaynes-Cummings model provides a clear physical picture and a simple and convenient way to solve the decay dynamics.However,in previous studies,only the resonant modes are taken into account,while the non-resonant contributions are ignored.In this work,we study the applicability and accuracy of the effective Hamiltonian method for the decay dynamics.We consider different coupling strengths between a two-level QE and a gold nanosphere.The results for dynamics by the resolvent operator technique are used as a reference.Numerical results show that the effective Hamiltonian method provides accurate results when the two-level QE is resonant with the plasmon.However,when the detuning is large,the effective Hamiltonian method is not accurate.In addition,the effective Hamiltonian method cannot be applied when there is a bound state between the QE and the plasmon.These results are of great significance to the study of the decay dynamics in micro-nano structures described by quasi-normal modes.
基金supported by the National Natural Science Foundation of China(NSFC,Nos.12074379,U1805252,21875250,12074380,11904365,and 12004384)the Chinese Academy of Sciences/State Administration of Foreign Experts Affairs(CAS/SAFEA)International Partnership Program for Creative Research Teams.
文摘Luminescent metal halides doped with ns^(2-)metal ions such as 6s^(2-)metal Bi^(3+)have aroused reviving interest owing to their outstanding optical properties;however,the origin of the photoluminescence(PL)remains controversial and unclear.Herein,we report a strategy for the controlled synthesis of Bi^(3+)-doped vacancy-ordered double perovskite Cs_(2)SnCl_(6)nanocrystals(NCs)and unravel the triplet excited-state dynamics of Bi^(3+)through temperature-dependent PL and ultrafast femtosecond transient absorption spectroscopies.Owing to the aliovalent Bi^(3+)doping in the spatially confined zero-dimensional(0D)structure of Cs2SnCl6,Bi^(3+)ions experience an enhancive Jahn-Teller distortion in the excited state,which results in intense broadband blue PL originating from the inter-configurational 3P0,1→1S0 transitions of Bi^(3+)at 450 nm,with a large Stokes shift and a quantum yield of 35.2%.Specifically,an unusual thermal-enhanced Jahn-Teller splitting of the excitation band and a remarkable transition of the PL lifetime from ms at 10 K toμs at 300 K were observed,as solid evidence for the isolated Bi^(3+)emission.These findings clarify the controversy about the PL origin in ns^(2-)metal ion-doped lead-free luminescent metal halides,thereby paving the way for exploring their optoelectronic applications.
基金the Natural Science Foundation of China under(Nos.U2032137 and U1832182)the Natural Science Foundation of Guangdong Province,China(No.18zxxt65)Fundamental Research Funds for the Central Universities(No.19lgpy306).
文摘The isospin fractionations in 124Sn,107Sn+120Sn at 600 MeV/nucleon,and 136Xe,124Xe+208Pb at 1000 MeV/nucleon are investigated by the isospin-dependent quantum molecular dynamics model coupled with the statistical code GEMINI.The yield ratio as a function of the binding energy difference for light mirror nuclei 3H/3He,7Li/7Be,11B/11C,and 15N/15O is applied to estimate the ratio between neutrons and protons in the gas of the fragmenting system.By comparing the estimated values resulting from the simulations with and without the GEMINI code,it was found that the secondary decay distorts the signal of the isospin fractionation.To minimize the secondary decay effects,the yield ratio of the light mirror nuclei 3H/3He as well as its double ratio between two systems with different isospin asymmetries of the projectiles is recommended as robust isospin observables.
基金supported by the National Key Research and Development Program of China(No.2017YFE0106100)。
文摘The beam windows of high-energy beam lines are important,and it is sometimes difficult to design because it is necessary to ensure particle propagation with minimum disturbance and fulfill mechanical requirements at the same time.The upstream decay pipe window of the long baseline neutrino facility at Fermilab has an extremely large diameter(1.8 m),with a thickness of only 1.5 mm to separate the helium atmosphere in the decay pipe and the nitrogen atmosphere on the other side.Furthermore,the center of this dish-shaped window is expected to be a200-mm-diameter beryllium dish welded to the outside aluminum alloy A6061,and this welded combination must withstand extreme conditions of a 2.4-MW,high-energy proton beam without leakage.These severe conditions make the design of this window an unprecedented challenge.This paper describes the static thermal-structural analyses based on which the structure has been optimized,as well as dynamic analyses for understanding the shockwave effects originating in the beam.After optimization,the maximum von Mises stresses in the window decreased significantly in both normal operation and accident cases,making our design very reasonable.
文摘One of the practical approaches in identifying structures is the non-linear resonant decay method which identifies a non-linear dynamic system utilizing a model based on linear modal space containing the underlying linear system and a small number of extra terms that exhibit the non-linear effects.In this paper,the method is illustrated in a simulated system and an experimental structure.The main objective of the non-linear resonant decay method is to identify the non-linear dynamic systems based on the use of a multi-shaker excitation using appropriated excitation which is obtained from the force appropriation approach.The experimental application of the method is indicated to provide suitable estimates of modal parameters for the identification of non-linear models of structures.
文摘In this paper,a one-dimension particle-in-cell(PIC)code(EDIPIC)is employed to simulate the parallel-plate ion extraction process under an externally applied electrostatic field,focusing on the analysis of the influe nee of the initial electron temperature on the extracted ion fluxes to the metal plates during the ion extraction process.Compared with previously published results,the plasma oscillations on a timescale of the electron plasma period,and the excitation of the ion acoustic rarefaction waves resulting from the plasma oscillations originating from both the negative and positive electrodes,are studied for the first time.The modeling results show that both the negative and positive extractors can collect ions due to the plasma oscillations and the propagation of the ion acoustic rarefaction waves.With the in crease of the initial electron temperature achieved by keeping other parameters unchanged,on the one hand,both the ion speed and flux to the negative and positive plates increase,which leads to a significant decrease of the ion extraction time,while on the other hand,the ion flux to the positive plate after the formation of a Child-Langmuir sheath is much more sensitive to an increase of the initial electron temperature than that to the negative plate.The PIC simulation results provide a deeper physical understanding of the influence of the initial electron temperature on the characteristics of the entire ion extraction process in a decaying plasma.
基金supported by the National Natural Science Foundation of China(61805118,21674048)the Natural Science Foundation of Jiangsu Province of China(BK20171020)Open Research Fund of Key Laboratory for Organic Electronics and Information Displays。
文摘Photo-induced excited-state dynamics within organic materials fundamentally determine their photophysical properties for various applications,and thus understanding the primary excited-state dynamics behavior is of fundamental and practical significance.Until recently,the excited-state dynamics of organic materials towards biophotonics have been rarely studied,although numerous endeavors have been devoted to the design of organic materials for biophotonics.Herein,various spectroscopy technologies including femtosecond transient absorption(fs-TA)spectroscopy clearly reveal a totally different excited state dynamics behavior within Bodipy monomer(2B-BDP dye)and aggregates(2B-BDP NPs),indicating strongly morphology dependent character.2B-BDP dye undergoes an ultrafast conversion from S1 to intramolecular charge transfer(ICT)state for subsequent photoluminescence(PL)and nonradiative(NR)decay,while 2B-BDP NPs show an accelerated excited-state deactivation mainly through S1→S0 NR decay.The potential bioapplications based on the corresponding excited state dynamics behavior are discussed together with experimental results.Interestingly,the accelerated NR decay in 2B-BDP NPs does not yield a stronger photoacoustic(PA)signal than that in 2B-BDP dye,which violates the conventional wisdom that faster NR decay would benefit the photothermal effects for better photoacoustic imaging(PAI).These insightful and fundamental observations of the excited-state dynamics may contribute an alternative approach at the molecular level towards the future design of functional Bodipy-based organic molecules with desirable performances.
基金supported by National Natural Science Foundation of China (NSFC) under Grant Nos.10475105,10491306,and 10675039the Knowledge Innovation Program (PKIP) of the Chinese Academy of Sciences
文摘The branching ratios and CP violations of the B →Dπ decays, including both the color-allowed and the color-suppressed modes, are investigated in detail within QCD framework by considering all diagrams that lead to three effective currents of two quarks. An intrinsic mass scale as a dynamical gluon mass is introduced to treat the infrared divergence caused by the soft collinear approximation in the endpoint regions, and the Cutkosky rule is adopted to deal with a physical-region singularity of the on mass-shell quark propagators. When the dynamical gluon mass μg is regarded as a universal sca/e, it is extracted to be around μg = 440 MeV from one of the well-measured B →Dπ decay modes. The resulting predictions for all branching ratios are in agreement with the current experimental measurements. As these decays have no penguin contributions, there are no direct CP asymmetries. Due to interference between the Cabibbo-suppressed and the Cabibbo-favored amplitudes, mixing-induced CP violations are predicted in the B →D^±π^±↓ decays to be consistent with the experimental data at 1-σ level. More precise measurements will be helpful to extracting weak angle 2β+γ.
基金The Global Change and Air-Sea Interaction Project under contract No.GASI-IPOVAI-01-03the National Key Research and Development Program under contract Nos 2016YFC1401403 and 2018YFC0309800+2 种基金the National Natural Science Foundation of China under contract Nos 41576009 and 41576006the Strategic Priority Research Program of the CAS under contract No.XDA13030302the Chinese Academy of Sciences Frontier Basic Research Project under contract No.QYJC201910
文摘Based on the latest oceanic surface drifter dataset from the global drifter program during 2000–2019,this study investigated the global variation of relative frequency shift(RFS),near-inertial energy(NIE)and inverse excess bandwidth(IEB)of near-inertial motions,and analyzed their relations with oceanic mesoscale dynamics,relative vorticity and strain.Compared with previous works,we have some new findings in this study:(1)the RFS was high with negative values in some regions in which we found a significant blue shift of the RFS in the equatorward of 30°N(S)and from 50°N to 60°N in the Pacific,and a red shift in the western boundary currents and their extension regions,the North Atlantic and the Antarctic Circumpolar Current regions;(2)more peak values of the NIE were found in global regions like the South Indian Ocean,the Luzon Strait and some areas of the South Ocean;(3)the global distribution of the IEB were characterized by clear zonal bands and affected by vorticity and wind field;(4)the RFS was elevated as the absolute value of the gradient of vorticity increased,the IEB did not depend on the gradient of vorticity,and the eddy kinetic energy(EKE)weakened with the decrease of the absolute value of RFS;(5)the NIE decreased with increasing absolute value of the relative vorticity and the gradient of vorticity,but it increased with increasing strain and EKE when EKE was larger than 0.0032 m2/s2.
基金supported by the National Natural Science Foundation of China through the Project "Science Center for Luminescence from Molecular Aggregates(SCELMA)" (No.21788102)the Ministry of Science and Technology of China through the National Key R&D Plan (No.2017YFA0204501)supported by the National Natural Science Foundation of China (No.22003029)
文摘We propose a method for calculating the nonradiative decay rates for polyatomic molecules including anharmonic effects of the potential energy surface(PES)in the Franck-Condon region.The method combines the n-mode repre-sentation method to construct the ab initio PES and the nearly exact time-dependent density matrix renormalization group method(TD-DMRG)to simulate quantum dynamics.In addition,in the framework of TD-DMRG,we further develop an algorithm to calculate the final-state-resolved rate coefficient which is very useful to analyze the contribution from each vibrational mode to the transition process.We use this method to study the internal conversion(IC)process of azulene after taking into account the anharmonicity of the ground state PES.The results show that even for this semi-rigid molecule,the intramode anharmonicity enhances the IC rate significantly,and after considering the two-mode coupling effect,the rate increases even further.The reason is that the anharmonicity enables the C-H vibrations to receive electronic energy while C-H vibrations do not contribute on the harmonic PES as the Huang-Rhys factor is close to 0.
文摘Unlike regular stabilizations, we construct in the paper a specific feedback control system such that u(t) decays exponentially with the designated decay rate, and that some non-trivial linear functionals of u decay exactly faster than . The system contains a dynamic compensator with another state v in the feedback loop, and consists of two states u and v. This problem entirely differs from the one with static feedback scheme in which the system consists only of a single state u. To show the essential difference, some specific property of the spectral subspaces associated with our control system is studied.