This investigation focuses on the nonlinear dynamic behaviors in the trans- verse vibration of an axiMly accelerating viscoelastic Timoshenko beam with the external harmonic excitation. The parametric excitation is ca...This investigation focuses on the nonlinear dynamic behaviors in the trans- verse vibration of an axiMly accelerating viscoelastic Timoshenko beam with the external harmonic excitation. The parametric excitation is caused by the harmonic fluctuations of the axial moving speed. An integro-partial-differential equation governing the transverse vibration of the Timoshenko beam is established. Many factors are considered, such as viscoelasticity, the finite axial support rigidity, and the longitudinally varying tension due to the axial acceleration. With the Galerkin truncation method, a set of nonlinear ordinary differential equations are derived by discretizing the governing equation. Based on the numerical solutions, the bifurcation diagrams are presented to study the effect of the external transverse excitation. Moreover, the frequencies of the two excitations are assumed to be multiple. Further, five different tools, including the time history, the Poincaré map, and the sensitivity to initial conditions, are used to identify the motion form of the nonlinear vibration. Numerical results also show the characteristics of the quasiperiodic motion of the translating Timoshenko beam under an incommensurable re- lationship between the dual-frequency excitations.展开更多
We investigate the dynamics of entanglement in the excitation transfer through a model consisting of three interacting molecules coupled to environments. It is shown that the entanglement can be further enhanced if th...We investigate the dynamics of entanglement in the excitation transfer through a model consisting of three interacting molecules coupled to environments. It is shown that the entanglement can be further enhanced if the distance between the molecules is oscillating. Our results demonstrate that the motional effect plays a constructive role on quantum entanglement in the dynamics of excitation transfer. This mechanism might provide a useful guideline for designing artificial systems to battle against decoherence.展开更多
A surface femtosecond two-photon photoemission (2PPE) spectrometer devoted to the study of ultrafast excited electron dynamics and photochemical kinetics on metal and metal oxide surfaces has been constructed. Low e...A surface femtosecond two-photon photoemission (2PPE) spectrometer devoted to the study of ultrafast excited electron dynamics and photochemical kinetics on metal and metal oxide surfaces has been constructed. Low energy photoelectrons are measured using a hemispherical electron energy analyzer with an imaging detector that allows us to detect the energy and the angular distributions of the photoelectrons simultaneously. A Mach-Zehnder interferom- eter was built for the time-resolved 2PPE (TR-2PPE) measurement to study ultrafast surface excited electron dynamics, which was demonstrated on the Cu(111) surface. A scheme for measuring time-dependent 2PPE (TD-2PPE) spectra has also been developed for studies of surface photochemistry. This technique has been applied to a preliminary study on the photochemical kinetics on ethanol/TiO2(110). We have also shown that the ultrafast dynamics of photoinduced surface excited resonances can be investigated in a reliable way by combining the TR-2PPE and TD-2PPE techniques.展开更多
We investigate a kind of noise-induced transition to noisy chaos in dynamical systems. Due to similar phenomenological structures of stable hyperbolic attractors excited by various physical realizations from a given s...We investigate a kind of noise-induced transition to noisy chaos in dynamical systems. Due to similar phenomenological structures of stable hyperbolic attractors excited by various physical realizations from a given stationary random process, a specific Poincar6 map is established for stochastically perturbed quasi-Hamiltonian system. Based on this kind of map, various point sets in the Poincar6's cross-section and dynamical transitions can be analyzed. Results from the customary Duffing oscillator show that, the point sets in the Poincare's global cross-section will be highly compressed in one direction, and extend slowly along the deterministic period-doubling bifurcation trail in another direction when the strength of the harmonic excitation is fixed while the strength of the stochastic excitation is slowly increased. This kind of transition is called the noise-induced point-overspreading route to noisy chaos.展开更多
The relation between the Lyapunov exponent spectrum of a periodically excited non-autonomous dynamical system and the Lyapunov exponent spectrum of the corresponding autonomous system is given and the validity of the ...The relation between the Lyapunov exponent spectrum of a periodically excited non-autonomous dynamical system and the Lyapunov exponent spectrum of the corresponding autonomous system is given and the validity of the relation is verified theoretically and computationally. A direct method for calculating the Lyapunov exponent spectrum of non-autonomous dynamical systems is suggested in this paper, which makes it more convenient to calculate the Lyapunov exponent spectrum of the dynamical system periodically excited. Following the definition of the Lyapunov dimension D-L((A)) of the autonomous system, the definition of the Lyapunov dimension D-L of the non-autonomous dynamical system is also given, and the difference between them is the integer 1, namely, D-L((A)) - D-L = 1. For a quasi-periodically excited dynamical system, similar conclusions are formed.展开更多
Traditional computing method is inefficient for getting key dynamical parameters of complicated structure.Pseudo Excitation Method(PEM)is an effective method for calculation of random vibration.Due to complicated an...Traditional computing method is inefficient for getting key dynamical parameters of complicated structure.Pseudo Excitation Method(PEM)is an effective method for calculation of random vibration.Due to complicated and coupling random vibration in rocket or shuttle launching,the new staging white noise mathematical model is deduced according to the practical launch environment.This deduced model is applied for PEM to calculate the specific structure of Time of Flight Counter(ToFC).The responses of power spectral density and the relevant dynamic characteristic parameters of ToFC are obtained in terms of the flight acceptance test level.Considering stiffness of fixture structure,the random vibration experiments are conducted in three directions to compare with the revised PEM.The experimental results show the structure can bear the random vibration caused by launch without any damage and key dynamical parameters of ToFC are obtained.The revised PEM is similar with random vibration experiment in dynamical parameters and responses are proved by comparative results.The maximum error is within 9%.The reasons of errors are analyzed to improve reliability of calculation.This research provides an effective method for solutions of computing dynamical characteristic parameters of complicated structure in the process of rocket or shuttle launching.展开更多
We investigate the collective dynamics of network-organized identical excitable nodes. We theoretically analyze the stability of the rest state and propose that there are two different transition paths: the stationar...We investigate the collective dynamics of network-organized identical excitable nodes. We theoretically analyze the stability of the rest state and propose that there are two different transition paths: the stationary path and the oscillatory path. We find that, although the onset of collective dynamics strongly depend on the network topology, the local dynamics and how local nodes interact with each other decide the transition path and the involved bifurcation.展开更多
As one of the biological endogenous pigments,biliverdin(BV)and its dimethyl ester(BVE)have extremely weak uorescence in solution with quantum yield less than 0.01%.However,the situation reverses with the addition of z...As one of the biological endogenous pigments,biliverdin(BV)and its dimethyl ester(BVE)have extremely weak uorescence in solution with quantum yield less than 0.01%.However,the situation reverses with the addition of zinc ions.The strength for uorescence of BVE-Zn^2+ complex is greatly enhanced and uorescence quantum yield can increase to5%.Herein,we studied ultrafast excited state dynamics of BVE-Zn^2+ complex in ethanol,npropanol,and DMSO solutions in order to reveal the mechanism of uorescence quantum yield enhancement.The results show that BVE can form a stable coordination complex with zinc with 1:1 stoichiometry in solution.BVE is structurally and energetically more stable in the complex.Using picosecond time-resolve uorescence and femtosecond transient absorption spectroscopy,we show that smaller non-radiative rate constant of BVE-Zn^2+ complex in DMSO is the key to increasing its uorescence quantum yield and the excited state decay mechanism is also revealed.These results provide valuable information about the uorescence property change after BVE binding to metal ions and may provide a guidance for the study of phytochromes or other uorescence proteins in which BV/BVE acts as chromophores.展开更多
Time-resolved photoionization is a powerful experimental approach to unravel the excited state dynamics in isolated polyatomic molecules. Depending on species of the collected signals, different methods can be perform...Time-resolved photoionization is a powerful experimental approach to unravel the excited state dynamics in isolated polyatomic molecules. Depending on species of the collected signals, different methods can be performed: time-resolved ion yield spectroscopy (TR-IYS) and time-resolved photoelectron imaging (TR-PEI). In this review, the essential concepts linking photoionization measurement with electronic structure are presented, together with several important breakthroughs in experimentally distinguishing the oscillating wavepacket motion between different geometries. We illustrate how femtosecond TR-IYS and TR-PEI are employed to visualize the evolution of a coherent vibrational wavepacket on the excited state surface.展开更多
Raman(resonance Raman,FT-Raman),IR and UV-visible spectroscopy and quantum chemistry calculations were used to investigate the photodissociation dynamics of furfural in S2 state.The resonance Raman(RR)spectra indicate...Raman(resonance Raman,FT-Raman),IR and UV-visible spectroscopy and quantum chemistry calculations were used to investigate the photodissociation dynamics of furfural in S2 state.The resonance Raman(RR)spectra indicate that the photorelaxation dynamics for the S0→S2 excited state is predominantly along nine motions:C=O stretchν5(1667 cm-1),ring C=C antisymmetric stretchν6(1570 cm-1),ring C=C symmetric stretchν7(1472 cm-1),C2-O6-C5 symmetric stretch/C1-H8 rock in planeν8(1389 cm-1),C3-C4 stretch/C1-H8 rock in planeν9(1370 cm-1),C5-O6 stretch in planeν12(1154 cm-1),ring breathν13(1077 cm-1),C3-C4 stretchν14(1020 cm-1),C3-C2-O6 symmetric stretchν16(928 cm-1).Stable structures of S0,S1,S2,T1 and T2 states with Cs point group were optimized at CASSCF method in Franck-Condon region there are S2/S1 conical intersection was found by state average method and RR spectra.展开更多
Two-photon absorption in systems with parity permits access to states that cannot be directly prepared by one-photon absorption. Here we investigate ultrafast internal conversion (IC) dynamics of furan by using this...Two-photon absorption in systems with parity permits access to states that cannot be directly prepared by one-photon absorption. Here we investigate ultrafast internal conversion (IC) dynamics of furan by using this strategy in combination with femtosecond time-resolved photoelectron imaging. The dark Rydberg S1 and bright valence S2 states are simultaneously excited by two photons of 405 nm, and then ionized by two photons of 800nm. The IC from S2 to S1 is clearly observed and extracted from the time dependence of the higher photoelectron kinetic energy (PKE) component. More importantly, the internal conversions to hot So from directly-prepared S1 and secondarily-populated S1 are unambiguously identified by the time-dependence of the lower PKE component. The average lifetime of the S2 and S1 states is measured to be 29 fs. The internal conversions of S2 to S1, S1 to hot So occur on estimated timescales of 15.4 fs and 38 fs, respectively.展开更多
A computer software named VDAS (Vehicle Dynamic Analysis Simulation) is presented.Based on the mathematical modelling for a military vehicle as a 3-D dynamic system, the softwarecreates random excitation resulting fro...A computer software named VDAS (Vehicle Dynamic Analysis Simulation) is presented.Based on the mathematical modelling for a military vehicle as a 3-D dynamic system, the softwarecreates random excitation resulting from double side road-surface roughness by statisticalsimulation, and solves for the time series of the system response from the system state equations,and gives out the results in probability statistics as well as performance evaluations.展开更多
Liquid storage tanks are essential structures that are often located in residential and industrial areas; thus an assessment of their seismic performance is an important engineering issue. In this paper, the seismic r...Liquid storage tanks are essential structures that are often located in residential and industrial areas; thus an assessment of their seismic performance is an important engineering issue. In this paper, the seismic response ofunanchored steel liquid storage tanks is investigated using the endurance time (ET) dynamic analysis procedure and compared to responses obtained for anchored tanks under actual ground motions and intensifying ET records. In most cases, the results from ground motions are properly obtained with negligible differences using ET records. It is observed that uplifting of the tank base, which is closely related to the tank aspect ratio, has the greatest significance in the responses of the tank and can be predicted with reasonable accuracy by using currently available ET records.展开更多
A new and innovative base isolation device is introduced in this paper based on extensive research carried out by the authors and their co-workers. A prototype of the device was built and experimentally tested on the ...A new and innovative base isolation device is introduced in this paper based on extensive research carried out by the authors and their co-workers. A prototype of the device was built and experimentally tested on the shaking table. The new base isolation device consists of two disks, one vertical cylinder with an upper enlargement sustained by three horizontal cantilevers, and at least three inclined shape memory alloy (SMA) bars. The role of the SMA bars is to limit the relative motion between the base and the superstructure, to dissipate energy by their super-elastic constitutive law and to guarantee the re-centring of the device. To verify the expected performance, a prototype was built and tested under sinusoidal waves of displacement of increasing frequency with different amplitudes. It is shown that the main feature of the proposed base isolation device is that for cyclic loading, the super-elastic behavior of the alloy results in wide load-displacement loops, where a large amount of energy is dissipated.展开更多
The joints connecting vertical and horizontal elements are the "weak link" in structural systems assembled from wood panels. If they are too weak, local failures may occur, resulting in performance that is significa...The joints connecting vertical and horizontal elements are the "weak link" in structural systems assembled from wood panels. If they are too weak, local failures may occur, resulting in performance that is significantly below expectations. If they are too resistant, the joints may be unable to dissipate energy during vibrations, thus possibly initiating a fast progressive failure. This paper re-processes and re-elaborates the results of shaking table tests previously carried out by the author and other co-workers. The goal is to assess the feasibility of a joint which is able to dissipate energy during vibration, without degrading the connection performance.展开更多
The A-band resonance Raman spectra of thiourea were obtained in water and acetonitrile solution. B3LYP/6-311++G(3df,3pd) and RCIS/6-311++G(3df,3pd) calculations were done to elucidate the ultraviolet electroni...The A-band resonance Raman spectra of thiourea were obtained in water and acetonitrile solution. B3LYP/6-311++G(3df,3pd) and RCIS/6-311++G(3df,3pd) calculations were done to elucidate the ultraviolet electronic transitions, the distorted geometry structure and the saddle point of thiourea in 21A excited state, respectively. The resonance Raman spectra were assigned. The absorption spectrum and resonance Raman intensities were modeled using Heller's time-dependent wavepacket approach to resonance Raman scattering. The results indicate that largest change in the displacement takes place with the C--S stretch mode u6 (|△|=0.95) and noticeable changes appear in the H5N3H6+H8N4H7 wag v5 (|△|=0.19), NCN symmetric stretch^-C--S stretch+N3H6+H8N4 wag v4 (|△|=0.18), while the moderate intensities of 2-15 and 4-15 are mostly due to the large excited state frequency changes of v15, but not due to its significant change in the normal mode displacement. The mechanism of the appearance of even overtones of the S-CN2 out of plane deformation is explored. The results indicate that a Franck-Condon region saddle point is the driving force for the quadric phonon mechanism within the standard A-term of resonance Raman scattering, which leads to the pyramidalization of the carbon center and the geometry distortion of thiourea molecule in 21A excited state.展开更多
The β-carotene(β-Car) aggregate was prepared by self-assembly in cetyltrimethylammoniuln bromide (CTAB) micelle. The ground state absorption measurement showed that the aggregate has J-type characteristics and r...The β-carotene(β-Car) aggregate was prepared by self-assembly in cetyltrimethylammoniuln bromide (CTAB) micelle. The ground state absorption measurement showed that the aggregate has J-type characteristics and resonance Raman spectra gave the intrinsic explanation of molecular interaction in aggregate. Upon excitation at the optical allowed S2 state of aggregate, direct generation of triplet state via singlet fission(SF)mechanism was observed. Excitation dynamics was elucidated by fs-transient absorption spectroscopy and ns-flash photolysis, respectively. The triplet state life time of aggregate was found to be independent of the ambient oxygen molecules.展开更多
Upon anthracene-sensitizing, triplet excitation dynamics of β-carotene(β-Car) were studied in nhexane, in methanol, and in acetonitrile, respectively, by ns flash photolysis spectroscopy. In n-hexane,only the blea...Upon anthracene-sensitizing, triplet excitation dynamics of β-carotene(β-Car) were studied in nhexane, in methanol, and in acetonitrile, respectively, by ns flash photolysis spectroscopy. In n-hexane,only the bleaching of the ground state absorption(GSB) and the excitation triplet(^3Car*) absorption were observed, and there were no cationic species detected. In both methanol and acetonitrile, similar excitation dynamics were observed, i.e.,^3Car* having a similar lifetime to that in n-hexane, and the immediate generation of the cation dehydrodimer(^#[Car]2^+) upon excitation following transformation into the radical cation Car*^+, since Car*^+ has much longer lifetime in acetonitrile than in methanol. The results prove that both solvent and carotenoid structure determine the triplet excitation mechanism.展开更多
The photochemical reaction of potassium ferrocyanide(K_(4)Fe(CN)_(6))exhibits excitation wavelength dependence and non-Kasha rule behavior.In this study,the excited-state dynamics of K_(4)Fe(CN)_(6) were studied by tr...The photochemical reaction of potassium ferrocyanide(K_(4)Fe(CN)_(6))exhibits excitation wavelength dependence and non-Kasha rule behavior.In this study,the excited-state dynamics of K_(4)Fe(CN)_(6) were studied by transient absorption spectroscopy.Excited state electron detachment(ESED)and photoaquation reactions were clarified by comparing the results of 260,320,340,and 350 nm excitations.ESED is the path to generate a hydrated electron(e^(−)_(aq)).ESED energy barrier varies with the excited state,and it occurs even at the first singlet excited state(^(1)T_(1g)).The ^(1)T_(1g) state shows∼0.2 ps lifetime and converts into triplet[Fe(CN)_(6)]4−by intersystem crossing.Subsequently,3Fe(CN)_(5)]^(3-)appears after one CN−ligand is ejected.In sequence,H2O attacksFe(CN)_(5)]^(3-)to generate[Fe(CN)_(5)H_(2)O]^(3−)with a time constant of approximately 20 ps.The ^(1)T_(1g) state and e−aq exhibit strong reducing power.The addition of uridine 5′-monophosphate(UMP)to the K_(4)Fe(CN)_(6) solution decrease the yield of e−aq and reduce the lifetimes of the e−aq and ^(1)T_(1g) state.The obtained reaction rate constant of ^(1)T_(1g) state and UMP is 1.7×10^(14)(mol/L)^(−1)·s^(−1),and the e−aq attachment to UMP is∼8×10^(9)(mol/L)^(−1)·s^(−1).Our results indicate that the reductive damage of K_(4)Fe(CN)_(6) solution to nucleic acids under ultraviolet irradiation cannot be neglected.展开更多
基金Project supported by the State Key Program of National Natural Science Foundation of China(No.11232009)the National Natural Science Foundation of China(Nos.11372171 and 11422214)
文摘This investigation focuses on the nonlinear dynamic behaviors in the trans- verse vibration of an axiMly accelerating viscoelastic Timoshenko beam with the external harmonic excitation. The parametric excitation is caused by the harmonic fluctuations of the axial moving speed. An integro-partial-differential equation governing the transverse vibration of the Timoshenko beam is established. Many factors are considered, such as viscoelasticity, the finite axial support rigidity, and the longitudinally varying tension due to the axial acceleration. With the Galerkin truncation method, a set of nonlinear ordinary differential equations are derived by discretizing the governing equation. Based on the numerical solutions, the bifurcation diagrams are presented to study the effect of the external transverse excitation. Moreover, the frequencies of the two excitations are assumed to be multiple. Further, five different tools, including the time history, the Poincaré map, and the sensitivity to initial conditions, are used to identify the motion form of the nonlinear vibration. Numerical results also show the characteristics of the quasiperiodic motion of the translating Timoshenko beam under an incommensurable re- lationship between the dual-frequency excitations.
基金Supported by the National Natural Science Foundation of China under Grant Nos 11374085,61073048 and 11274010the Specialized Research Fund for the Doctoral Program of Higher Education under Grant No 20113401110002+3 种基金the 211 Project of Anhui Universitythe Anhui Provincial Natural Science Foundation under Grant No 1408085MA20the Personnel Department of Anhui Provincethe 136 Foundation of Hefei Normal University under Grant No 2014136KJB04
文摘We investigate the dynamics of entanglement in the excitation transfer through a model consisting of three interacting molecules coupled to environments. It is shown that the entanglement can be further enhanced if the distance between the molecules is oscillating. Our results demonstrate that the motional effect plays a constructive role on quantum entanglement in the dynamics of excitation transfer. This mechanism might provide a useful guideline for designing artificial systems to battle against decoherence.
文摘A surface femtosecond two-photon photoemission (2PPE) spectrometer devoted to the study of ultrafast excited electron dynamics and photochemical kinetics on metal and metal oxide surfaces has been constructed. Low energy photoelectrons are measured using a hemispherical electron energy analyzer with an imaging detector that allows us to detect the energy and the angular distributions of the photoelectrons simultaneously. A Mach-Zehnder interferom- eter was built for the time-resolved 2PPE (TR-2PPE) measurement to study ultrafast surface excited electron dynamics, which was demonstrated on the Cu(111) surface. A scheme for measuring time-dependent 2PPE (TD-2PPE) spectra has also been developed for studies of surface photochemistry. This technique has been applied to a preliminary study on the photochemical kinetics on ethanol/TiO2(110). We have also shown that the ultrafast dynamics of photoinduced surface excited resonances can be investigated in a reliable way by combining the TR-2PPE and TD-2PPE techniques.
基金supported by the National Natural Science Foundation of China (11172260 and 11072213)the Fundamental Research Fund for the Central University of China (2011QNA4001)
文摘We investigate a kind of noise-induced transition to noisy chaos in dynamical systems. Due to similar phenomenological structures of stable hyperbolic attractors excited by various physical realizations from a given stationary random process, a specific Poincar6 map is established for stochastically perturbed quasi-Hamiltonian system. Based on this kind of map, various point sets in the Poincar6's cross-section and dynamical transitions can be analyzed. Results from the customary Duffing oscillator show that, the point sets in the Poincare's global cross-section will be highly compressed in one direction, and extend slowly along the deterministic period-doubling bifurcation trail in another direction when the strength of the harmonic excitation is fixed while the strength of the stochastic excitation is slowly increased. This kind of transition is called the noise-induced point-overspreading route to noisy chaos.
基金the National Natural Science Foundation of China(No.19772027)the Science Foundation of Shanghai Municipal Commission of Education(99A01)the Science Foundation of Shanghai Municipal Commission of Science and Technology(No.98JC14032)
文摘The relation between the Lyapunov exponent spectrum of a periodically excited non-autonomous dynamical system and the Lyapunov exponent spectrum of the corresponding autonomous system is given and the validity of the relation is verified theoretically and computationally. A direct method for calculating the Lyapunov exponent spectrum of non-autonomous dynamical systems is suggested in this paper, which makes it more convenient to calculate the Lyapunov exponent spectrum of the dynamical system periodically excited. Following the definition of the Lyapunov dimension D-L((A)) of the autonomous system, the definition of the Lyapunov dimension D-L of the non-autonomous dynamical system is also given, and the difference between them is the integer 1, namely, D-L((A)) - D-L = 1. For a quasi-periodically excited dynamical system, similar conclusions are formed.
基金Supported by National Natural Science Foundation of China(Grant No.51105025)International Science & Technology Cooperation Program of China(Grant No.2013DFB70110)
文摘Traditional computing method is inefficient for getting key dynamical parameters of complicated structure.Pseudo Excitation Method(PEM)is an effective method for calculation of random vibration.Due to complicated and coupling random vibration in rocket or shuttle launching,the new staging white noise mathematical model is deduced according to the practical launch environment.This deduced model is applied for PEM to calculate the specific structure of Time of Flight Counter(ToFC).The responses of power spectral density and the relevant dynamic characteristic parameters of ToFC are obtained in terms of the flight acceptance test level.Considering stiffness of fixture structure,the random vibration experiments are conducted in three directions to compare with the revised PEM.The experimental results show the structure can bear the random vibration caused by launch without any damage and key dynamical parameters of ToFC are obtained.The revised PEM is similar with random vibration experiment in dynamical parameters and responses are proved by comparative results.The maximum error is within 9%.The reasons of errors are analyzed to improve reliability of calculation.This research provides an effective method for solutions of computing dynamical characteristic parameters of complicated structure in the process of rocket or shuttle launching.
基金Supported by the National Natural Science Foundation of China under Grant No 71301012
文摘We investigate the collective dynamics of network-organized identical excitable nodes. We theoretically analyze the stability of the rest state and propose that there are two different transition paths: the stationary path and the oscillatory path. We find that, although the onset of collective dynamics strongly depend on the network topology, the local dynamics and how local nodes interact with each other decide the transition path and the involved bifurcation.
基金the National Nature Science Foundation of China(No.11674101,No.21873030 and No.91850202)。
文摘As one of the biological endogenous pigments,biliverdin(BV)and its dimethyl ester(BVE)have extremely weak uorescence in solution with quantum yield less than 0.01%.However,the situation reverses with the addition of zinc ions.The strength for uorescence of BVE-Zn^2+ complex is greatly enhanced and uorescence quantum yield can increase to5%.Herein,we studied ultrafast excited state dynamics of BVE-Zn^2+ complex in ethanol,npropanol,and DMSO solutions in order to reveal the mechanism of uorescence quantum yield enhancement.The results show that BVE can form a stable coordination complex with zinc with 1:1 stoichiometry in solution.BVE is structurally and energetically more stable in the complex.Using picosecond time-resolve uorescence and femtosecond transient absorption spectroscopy,we show that smaller non-radiative rate constant of BVE-Zn^2+ complex in DMSO is the key to increasing its uorescence quantum yield and the excited state decay mechanism is also revealed.These results provide valuable information about the uorescence property change after BVE binding to metal ions and may provide a guidance for the study of phytochromes or other uorescence proteins in which BV/BVE acts as chromophores.
基金supported by the National Natural Science Foundation of China (No.21327804, No.21773299, No.91121006, No.21573279, No.11574351, No.11774385, No.11674355, No.21503270, and No.21303255)
文摘Time-resolved photoionization is a powerful experimental approach to unravel the excited state dynamics in isolated polyatomic molecules. Depending on species of the collected signals, different methods can be performed: time-resolved ion yield spectroscopy (TR-IYS) and time-resolved photoelectron imaging (TR-PEI). In this review, the essential concepts linking photoionization measurement with electronic structure are presented, together with several important breakthroughs in experimentally distinguishing the oscillating wavepacket motion between different geometries. We illustrate how femtosecond TR-IYS and TR-PEI are employed to visualize the evolution of a coherent vibrational wavepacket on the excited state surface.
基金This work was supported in parts by National Natural Science Foundation of China(No.21673208)Zhejiang Provincial Natural Science Foundation of China(No.LY16B070009).
文摘Raman(resonance Raman,FT-Raman),IR and UV-visible spectroscopy and quantum chemistry calculations were used to investigate the photodissociation dynamics of furfural in S2 state.The resonance Raman(RR)spectra indicate that the photorelaxation dynamics for the S0→S2 excited state is predominantly along nine motions:C=O stretchν5(1667 cm-1),ring C=C antisymmetric stretchν6(1570 cm-1),ring C=C symmetric stretchν7(1472 cm-1),C2-O6-C5 symmetric stretch/C1-H8 rock in planeν8(1389 cm-1),C3-C4 stretch/C1-H8 rock in planeν9(1370 cm-1),C5-O6 stretch in planeν12(1154 cm-1),ring breathν13(1077 cm-1),C3-C4 stretchν14(1020 cm-1),C3-C2-O6 symmetric stretchν16(928 cm-1).Stable structures of S0,S1,S2,T1 and T2 states with Cs point group were optimized at CASSCF method in Franck-Condon region there are S2/S1 conical intersection was found by state average method and RR spectra.
基金Supported by the National Natural Science Foundation of China under Grant Nos 21303255,21273274 and 91121006
文摘Two-photon absorption in systems with parity permits access to states that cannot be directly prepared by one-photon absorption. Here we investigate ultrafast internal conversion (IC) dynamics of furan by using this strategy in combination with femtosecond time-resolved photoelectron imaging. The dark Rydberg S1 and bright valence S2 states are simultaneously excited by two photons of 405 nm, and then ionized by two photons of 800nm. The IC from S2 to S1 is clearly observed and extracted from the time dependence of the higher photoelectron kinetic energy (PKE) component. More importantly, the internal conversions to hot So from directly-prepared S1 and secondarily-populated S1 are unambiguously identified by the time-dependence of the lower PKE component. The average lifetime of the S2 and S1 states is measured to be 29 fs. The internal conversions of S2 to S1, S1 to hot So occur on estimated timescales of 15.4 fs and 38 fs, respectively.
文摘A computer software named VDAS (Vehicle Dynamic Analysis Simulation) is presented.Based on the mathematical modelling for a military vehicle as a 3-D dynamic system, the softwarecreates random excitation resulting from double side road-surface roughness by statisticalsimulation, and solves for the time series of the system response from the system state equations,and gives out the results in probability statistics as well as performance evaluations.
文摘Liquid storage tanks are essential structures that are often located in residential and industrial areas; thus an assessment of their seismic performance is an important engineering issue. In this paper, the seismic response ofunanchored steel liquid storage tanks is investigated using the endurance time (ET) dynamic analysis procedure and compared to responses obtained for anchored tanks under actual ground motions and intensifying ET records. In most cases, the results from ground motions are properly obtained with negligible differences using ET records. It is observed that uplifting of the tank base, which is closely related to the tank aspect ratio, has the greatest significance in the responses of the tank and can be predicted with reasonable accuracy by using currently available ET records.
基金Supported by: Italian National Research Council (CNR) Under Grant No CU07.00016.ST/97
文摘A new and innovative base isolation device is introduced in this paper based on extensive research carried out by the authors and their co-workers. A prototype of the device was built and experimentally tested on the shaking table. The new base isolation device consists of two disks, one vertical cylinder with an upper enlargement sustained by three horizontal cantilevers, and at least three inclined shape memory alloy (SMA) bars. The role of the SMA bars is to limit the relative motion between the base and the superstructure, to dissipate energy by their super-elastic constitutive law and to guarantee the re-centring of the device. To verify the expected performance, a prototype was built and tested under sinusoidal waves of displacement of increasing frequency with different amplitudes. It is shown that the main feature of the proposed base isolation device is that for cyclic loading, the super-elastic behavior of the alloy results in wide load-displacement loops, where a large amount of energy is dissipated.
基金Italian National Research Council (CNR) Unde Grant No. CU07.00016 ST/97
文摘The joints connecting vertical and horizontal elements are the "weak link" in structural systems assembled from wood panels. If they are too weak, local failures may occur, resulting in performance that is significantly below expectations. If they are too resistant, the joints may be unable to dissipate energy during vibrations, thus possibly initiating a fast progressive failure. This paper re-processes and re-elaborates the results of shaking table tests previously carried out by the author and other co-workers. The goal is to assess the feasibility of a joint which is able to dissipate energy during vibration, without degrading the connection performance.
基金This work was supported by the National Natural Science Foundation of China (No.21033002 and No.20803066) and the National Basic Research Program of China (No.2007CB815203).
文摘The A-band resonance Raman spectra of thiourea were obtained in water and acetonitrile solution. B3LYP/6-311++G(3df,3pd) and RCIS/6-311++G(3df,3pd) calculations were done to elucidate the ultraviolet electronic transitions, the distorted geometry structure and the saddle point of thiourea in 21A excited state, respectively. The resonance Raman spectra were assigned. The absorption spectrum and resonance Raman intensities were modeled using Heller's time-dependent wavepacket approach to resonance Raman scattering. The results indicate that largest change in the displacement takes place with the C--S stretch mode u6 (|△|=0.95) and noticeable changes appear in the H5N3H6+H8N4H7 wag v5 (|△|=0.19), NCN symmetric stretch^-C--S stretch+N3H6+H8N4 wag v4 (|△|=0.18), while the moderate intensities of 2-15 and 4-15 are mostly due to the large excited state frequency changes of v15, but not due to its significant change in the normal mode displacement. The mechanism of the appearance of even overtones of the S-CN2 out of plane deformation is explored. The results indicate that a Franck-Condon region saddle point is the driving force for the quadric phonon mechanism within the standard A-term of resonance Raman scattering, which leads to the pyramidalization of the carbon center and the geometry distortion of thiourea molecule in 21A excited state.
基金Supported by the National Natural Science Foundation of China(Nos.21673289, 21273282, 21673288).
文摘The β-carotene(β-Car) aggregate was prepared by self-assembly in cetyltrimethylammoniuln bromide (CTAB) micelle. The ground state absorption measurement showed that the aggregate has J-type characteristics and resonance Raman spectra gave the intrinsic explanation of molecular interaction in aggregate. Upon excitation at the optical allowed S2 state of aggregate, direct generation of triplet state via singlet fission(SF)mechanism was observed. Excitation dynamics was elucidated by fs-transient absorption spectroscopy and ns-flash photolysis, respectively. The triplet state life time of aggregate was found to be independent of the ambient oxygen molecules.
基金supported by the Natural Science Foundation of China (Nos. 21273282 and 21173265)the International Cooperation Project between China and Russia (NSFC-RFBR No. 21411130185)the Fundamental Research Funds for the Central Universities, and the Research Funds of Renmin University of China (No. 16XNH060)
文摘Upon anthracene-sensitizing, triplet excitation dynamics of β-carotene(β-Car) were studied in nhexane, in methanol, and in acetonitrile, respectively, by ns flash photolysis spectroscopy. In n-hexane,only the bleaching of the ground state absorption(GSB) and the excitation triplet(^3Car*) absorption were observed, and there were no cationic species detected. In both methanol and acetonitrile, similar excitation dynamics were observed, i.e.,^3Car* having a similar lifetime to that in n-hexane, and the immediate generation of the cation dehydrodimer(^#[Car]2^+) upon excitation following transformation into the radical cation Car*^+, since Car*^+ has much longer lifetime in acetonitrile than in methanol. The results prove that both solvent and carotenoid structure determine the triplet excitation mechanism.
基金supported by the National Natural Science Foundation of China(No.21873100 and No.21773226)the Open Fund of the State Key Laboratory of Molecular Reaction Dynamics in Dalian Institute of Chemical Physics,Chinese Academy of Sciences。
文摘The photochemical reaction of potassium ferrocyanide(K_(4)Fe(CN)_(6))exhibits excitation wavelength dependence and non-Kasha rule behavior.In this study,the excited-state dynamics of K_(4)Fe(CN)_(6) were studied by transient absorption spectroscopy.Excited state electron detachment(ESED)and photoaquation reactions were clarified by comparing the results of 260,320,340,and 350 nm excitations.ESED is the path to generate a hydrated electron(e^(−)_(aq)).ESED energy barrier varies with the excited state,and it occurs even at the first singlet excited state(^(1)T_(1g)).The ^(1)T_(1g) state shows∼0.2 ps lifetime and converts into triplet[Fe(CN)_(6)]4−by intersystem crossing.Subsequently,3Fe(CN)_(5)]^(3-)appears after one CN−ligand is ejected.In sequence,H2O attacksFe(CN)_(5)]^(3-)to generate[Fe(CN)_(5)H_(2)O]^(3−)with a time constant of approximately 20 ps.The ^(1)T_(1g) state and e−aq exhibit strong reducing power.The addition of uridine 5′-monophosphate(UMP)to the K_(4)Fe(CN)_(6) solution decrease the yield of e−aq and reduce the lifetimes of the e−aq and ^(1)T_(1g) state.The obtained reaction rate constant of ^(1)T_(1g) state and UMP is 1.7×10^(14)(mol/L)^(−1)·s^(−1),and the e−aq attachment to UMP is∼8×10^(9)(mol/L)^(−1)·s^(−1).Our results indicate that the reductive damage of K_(4)Fe(CN)_(6) solution to nucleic acids under ultraviolet irradiation cannot be neglected.