The time-resolved photoelectron spectrum (TRPES) of RbI molecule is simulated using the time-dependent wave-packet method. Both the normal three-photon ionization process and auto-ionization process are involved in th...The time-resolved photoelectron spectrum (TRPES) of RbI molecule is simulated using the time-dependent wave-packet method. Both the normal three-photon ionization process and auto-ionization process are involved in the simulation. The calculated results show that the change of delay time will influence the shape of the photoelectron spectrum (PES), and the influence is sub- stantially due to the existence of the crossing between excited states and the strong laser field which will change the position of relevant curves.展开更多
Dynamics of the Au + H2 reaction are studied using time-dependent wave packet(TDWP) and quasi-classical trajectory(QCT) methods based on a new potential energy surface [Int. J. Quantum Chem. 118 e25493(2018)]. The dyn...Dynamics of the Au + H2 reaction are studied using time-dependent wave packet(TDWP) and quasi-classical trajectory(QCT) methods based on a new potential energy surface [Int. J. Quantum Chem. 118 e25493(2018)]. The dynamic properties such as reaction probability, integral cross section, differential cross section and the distribution of product are studied at state-to-state level of theory. Furthermore, the present results are compared with the theoretical studies available.The results indicate that the complex-forming reaction mechanism is dominated in the reaction in the low collision energy region and the abstract reaction mechanism plays a dominant role at high collision energies. Different from previous theoretical calculations, the side-ways scattering signals are found in the present work and become more and more apparent with increasing collision energy.展开更多
The dynamics of the double-channel dissociation of the NaCs molecule is investigated by using the time-dependent wave packet （TDWP） method with the ＂split operator-Fourier transform＂ scheme. At a given wavelength ...The dynamics of the double-channel dissociation of the NaCs molecule is investigated by using the time-dependent wave packet （TDWP） method with the ＂split operator-Fourier transform＂ scheme. At a given wavelength and intensity of laser pulse, the population of each state changing with time is obtained. The photo-absorption spectra and kinetic- energy distribution of the dissociation fragments, which exhibit vibration-level structure and dispersion of the wave packet, respectively, are also obtained. The results show that by increasing the laser intensity, one can find not only the band center shift of the photo-absorption spectrum, but also the change of the fragment energy. The appearance of the diffusive band in the photo-absorption spectrum and the multiple peaks in the kinetic-energy spectrum can be attributed to the effects of the predissoeiation limit and the external field.展开更多
The average variational principle was employed in this paper to study the evolution of large-scale and slowly varying Rossby wave packet with basic flow both in barotropic and baroclinic atmospheres. The evolution of ...The average variational principle was employed in this paper to study the evolution of large-scale and slowly varying Rossby wave packet with basic flow both in barotropic and baroclinic atmospheres. The evolution of the structure of Rossby wave packet with both time and space was studied. The results obtained in this paper are similar to the results of by WKBJ method. In addition, the dispersive process of the wave packet was analysed by taking Gaussian type wave packet as an initial disturbance. The valid time scale for application of wave packet theory in the atmosphere was obtained.展开更多
Employing the two-state model and the time-dependent wave packet method, we have investigated the influences of the parameters of the intense femtosecond laser field on the evolution of the wave packet, as well as the...Employing the two-state model and the time-dependent wave packet method, we have investigated the influences of the parameters of the intense femtosecond laser field on the evolution of the wave packet, as well as the population of ground and double-minimum electronic states of the NaRb molecule. For the different laser wavelengths, the evolution of the wave packet of 6{ }^1／Sigma ^ ＋ state with time and internuclear distance is different, and the different laser intensity brings different influences on the population of the electronic states of the NaRb molecule. One can control the evolutions of wave packet and the population in each state by varying the laser parameters appropriately, which will be a benefit for the light manipulation of atomic and molecular processes.展开更多
The time-dependent wave packet method is used to investigate the influence of laser-fields on the vibrational population of molecules. For a two-state system in laser fields, the populations on different vibrational l...The time-dependent wave packet method is used to investigate the influence of laser-fields on the vibrational population of molecules. For a two-state system in laser fields, the populations on different vibrational levels of the upper and lower electronic states are given by wavefunctions obtained by solving the Schrbdinger equation with the split- operator method. The calculation shows that the field parameters, such as intensity, wavelength, duration, and delay time etc. can have different influences on the vibrational population. By varying the laser parameters appropriately one can control the evolution of wave packet and so the vibrational population in each state, which will benefit the light manipulation of atomic and molecular processes.展开更多
Wave packet dynamics of the Li2 molecule are investigated by using the time-dependent quantum wave packet method, and the time-resolved photoelectron spectra of the Li2 molecule are calculated. The time-resolved wave ...Wave packet dynamics of the Li2 molecule are investigated by using the time-dependent quantum wave packet method, and the time-resolved photoelectron spectra of the Li2 molecule are calculated. The time-resolved wave packet theory is used to reasonably interpret the phenomena of the photoelectron spectra for different parameters. Our calculation shows that the loss of the wave packets in the shelf state area of E1∑g＋ plays a prominent role in the process of photoionization with the increase of the delay time. Moreover, the oscillation of the wave packet on the E1∑g＋ curve symbolizes a decreasing process of energy.展开更多
Three-dimensional quantum mechanical calculations for vibrational predissociation of HeI2(B) van der Waals molecules are presented using the time-dependent wave packet technique within the golden rule approxima tion.T...Three-dimensional quantum mechanical calculations for vibrational predissociation of HeI2(B) van der Waals molecules are presented using the time-dependent wave packet technique within the golden rule approxima tion.The total and partial decay widths,lifetimes,rates and their dependence on initial vibrational states were obtained for HeI2 at low initial vibrational excited levels.Our calculations show that the calculated tota decay widths,lifetimes and rates agree well with those extrapolated from experimental data available The predicted total decay widths as a function of initial vibrational states exhibit highly nonlinear behavior.The very short propagation time (less.than 1 ps) required in the golden rule wave packet calculation is determined by the duration time of the final state inter-action between the fragments on the vibrationally deexcited adiabatic potential surface.The final state interaction between the fragments is shown to play an important role in determining the final rotational展开更多
The influence of the ultra-short pulse wavelength on the populations in the three electronic states of CsI molecule is investigated using the time-dependent wave packet method. The calculated results show that the pop...The influence of the ultra-short pulse wavelength on the populations in the three electronic states of CsI molecule is investigated using the time-dependent wave packet method. The calculated results show that the populations in the two excited states approach to the maxima at the wavelengths of 369 nm and 297 nm, respectively. The photodissociation reaction channels of the CsI molecule can be chosen by controlling the pump pulse wavelength.展开更多
The photo-dissociation dynamics of LiF is investigated with newly constructed accurate ab initio potential energy curves （PECs） using the time-dependent quantum wave packet method. The oscillations and decay of the ...The photo-dissociation dynamics of LiF is investigated with newly constructed accurate ab initio potential energy curves （PECs） using the time-dependent quantum wave packet method. The oscillations and decay of the wave packet on the adiabats as a function of time are given, which can be compared with the femtosecond transition-state （FTS） spectroscopy. The photo-absorption spectra and the kinetic-energy distribution of the dissociation fragments, which can exhibit the vibration-level structure and the dispersion of the wave packet, respectively, are also obtained. The investigation shows a blue shift of the band center for the photo-absorption spectrum and multiple peaks in the kinetic-energy spectrum with increasing laser intensity, which can be attributed to external field effects. By analyzing the oscillations of the wave packet evolving on the upper adiabat, an approximate inversion scheme is devised to roughly deduce its shape.展开更多
基金This work was supported by the National Natural Science Foundation of China (Grant Nos.10474060 and 10574083) the Natural Science Foundation of Shandong Province of China (Grant No. Y2003A02).
文摘The time-resolved photoelectron spectrum (TRPES) of RbI molecule is simulated using the time-dependent wave-packet method. Both the normal three-photon ionization process and auto-ionization process are involved in the simulation. The calculated results show that the change of delay time will influence the shape of the photoelectron spectrum (PES), and the influence is sub- stantially due to the existence of the crossing between excited states and the strong laser field which will change the position of relevant curves.
文摘Dynamics of the Au + H2 reaction are studied using time-dependent wave packet(TDWP) and quasi-classical trajectory(QCT) methods based on a new potential energy surface [Int. J. Quantum Chem. 118 e25493(2018)]. The dynamic properties such as reaction probability, integral cross section, differential cross section and the distribution of product are studied at state-to-state level of theory. Furthermore, the present results are compared with the theoretical studies available.The results indicate that the complex-forming reaction mechanism is dominated in the reaction in the low collision energy region and the abstract reaction mechanism plays a dominant role at high collision energies. Different from previous theoretical calculations, the side-ways scattering signals are found in the present work and become more and more apparent with increasing collision energy.
基金Project supported by the National Natural Science Foundation of China(Grant No.11074151)the Doctoral Program Foundation of Institutions of Higher Education of China(Grant No.20123704110002)
文摘The dynamics of the double-channel dissociation of the NaCs molecule is investigated by using the time-dependent wave packet （TDWP） method with the ＂split operator-Fourier transform＂ scheme. At a given wavelength and intensity of laser pulse, the population of each state changing with time is obtained. The photo-absorption spectra and kinetic- energy distribution of the dissociation fragments, which exhibit vibration-level structure and dispersion of the wave packet, respectively, are also obtained. The results show that by increasing the laser intensity, one can find not only the band center shift of the photo-absorption spectrum, but also the change of the fragment energy. The appearance of the diffusive band in the photo-absorption spectrum and the multiple peaks in the kinetic-energy spectrum can be attributed to the effects of the predissoeiation limit and the external field.
文摘The average variational principle was employed in this paper to study the evolution of large-scale and slowly varying Rossby wave packet with basic flow both in barotropic and baroclinic atmospheres. The evolution of the structure of Rossby wave packet with both time and space was studied. The results obtained in this paper are similar to the results of by WKBJ method. In addition, the dispersive process of the wave packet was analysed by taking Gaussian type wave packet as an initial disturbance. The valid time scale for application of wave packet theory in the atmosphere was obtained.
基金supported by the National Natural Science Foundation of China (Grant Nos. 10674114 and 10604045)
文摘Employing the two-state model and the time-dependent wave packet method, we have investigated the influences of the parameters of the intense femtosecond laser field on the evolution of the wave packet, as well as the population of ground and double-minimum electronic states of the NaRb molecule. For the different laser wavelengths, the evolution of the wave packet of 6{ }^1／Sigma ^ ＋ state with time and internuclear distance is different, and the different laser intensity brings different influences on the population of the electronic states of the NaRb molecule. One can control the evolutions of wave packet and the population in each state by varying the laser parameters appropriately, which will be a benefit for the light manipulation of atomic and molecular processes.
基金Project supported by the Natural Science Foundation of Shandong Province of China (Grant No. Y2006A23)the National Basic Research Program of China (Grant No. 2006CB806000)the Open Fund of the State Key Laboratory of High Field Laser Physics (Shanghai Institute of Optics and Fine Mechanics)
文摘The time-dependent wave packet method is used to investigate the influence of laser-fields on the vibrational population of molecules. For a two-state system in laser fields, the populations on different vibrational levels of the upper and lower electronic states are given by wavefunctions obtained by solving the Schrbdinger equation with the split- operator method. The calculation shows that the field parameters, such as intensity, wavelength, duration, and delay time etc. can have different influences on the vibrational population. By varying the laser parameters appropriately one can control the evolution of wave packet and so the vibrational population in each state, which will benefit the light manipulation of atomic and molecular processes.
基金Project supported by the National Natural Science Foundation of China (Grant Nos. 60977063 and 10574039)the Foundation for Key Program of Ministry of Education China (Grant No. 206084)+1 种基金the Innovation Scientists and Technicians Troop Construction Projects of Henan Province,China (Grant No. 084100510011)the Innovation Talents of Institution of Higher Education of Henan Province,China (Grant No. 2006KYCX002)
文摘Wave packet dynamics of the Li2 molecule are investigated by using the time-dependent quantum wave packet method, and the time-resolved photoelectron spectra of the Li2 molecule are calculated. The time-resolved wave packet theory is used to reasonably interpret the phenomena of the photoelectron spectra for different parameters. Our calculation shows that the loss of the wave packets in the shelf state area of E1∑g＋ plays a prominent role in the process of photoionization with the increase of the delay time. Moreover, the oscillation of the wave packet on the E1∑g＋ curve symbolizes a decreasing process of energy.
文摘Three-dimensional quantum mechanical calculations for vibrational predissociation of HeI2(B) van der Waals molecules are presented using the time-dependent wave packet technique within the golden rule approxima tion.The total and partial decay widths,lifetimes,rates and their dependence on initial vibrational states were obtained for HeI2 at low initial vibrational excited levels.Our calculations show that the calculated tota decay widths,lifetimes and rates agree well with those extrapolated from experimental data available The predicted total decay widths as a function of initial vibrational states exhibit highly nonlinear behavior.The very short propagation time (less.than 1 ps) required in the golden rule wave packet calculation is determined by the duration time of the final state inter-action between the fragments on the vibrationally deexcited adiabatic potential surface.The final state interaction between the fragments is shown to play an important role in determining the final rotational
基金Project supported by the National Natural Science Foundation of China (Grant Nos. 10674114 and 10604045)
文摘The influence of the ultra-short pulse wavelength on the populations in the three electronic states of CsI molecule is investigated using the time-dependent wave packet method. The calculated results show that the populations in the two excited states approach to the maxima at the wavelengths of 369 nm and 297 nm, respectively. The photodissociation reaction channels of the CsI molecule can be chosen by controlling the pump pulse wavelength.
基金the International Cooperation Program for Excellent Lectures of 2008 by Shandong Provincial Education Department,Chinathe National Natural Science Foundation of China(Grant No.11074151)Fundao para a Ciência e a Tecnologia,Portugal
文摘The photo-dissociation dynamics of LiF is investigated with newly constructed accurate ab initio potential energy curves （PECs） using the time-dependent quantum wave packet method. The oscillations and decay of the wave packet on the adiabats as a function of time are given, which can be compared with the femtosecond transition-state （FTS） spectroscopy. The photo-absorption spectra and the kinetic-energy distribution of the dissociation fragments, which can exhibit the vibration-level structure and the dispersion of the wave packet, respectively, are also obtained. The investigation shows a blue shift of the band center for the photo-absorption spectrum and multiple peaks in the kinetic-energy spectrum with increasing laser intensity, which can be attributed to external field effects. By analyzing the oscillations of the wave packet evolving on the upper adiabat, an approximate inversion scheme is devised to roughly deduce its shape.
