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
Centrifuge is a promising tool for underwater explosion(UNDEX) research as both Mach and Froude similitudes could be satisfied with hyper-gravity in models, which would result in similarities in both shock wave and bu...Centrifuge is a promising tool for underwater explosion(UNDEX) research as both Mach and Froude similitudes could be satisfied with hyper-gravity in models, which would result in similarities in both shock wave and bubble oscillation. Scaling laws for UNDEX in centrifuge have been proposed based on dimensional analysis. Two dimensionless numbers, i.e.,π_3 and π_4, are used to characterize shock wave and bubble oscillation, respectively. To validate scaling laws, 17 UNDEX tests are designed by varying accelerations or explosive weights and positions in centrifuge. The tests are classified into different groups to validate scaling laws as well as calibrate coefficients in empirical formulae for both shock wave and bubble oscillation. The results show that changes of gravity acceleration or hydrodynamic pressure almost has no influence on shock wave peak pressure and time constant as long as π3 is constant. The dimensionless bubble period and maximum radius agreed with each other when π4 is constant. Based on the research, an example is exhibited to suggest method for the computation of initial loading conditions for a submerged obstacle subjected to UNDEX.展开更多
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.
基金supported by the State Key Program of National Natural Science Foundation of China(Grant No.51339006)
文摘Centrifuge is a promising tool for underwater explosion(UNDEX) research as both Mach and Froude similitudes could be satisfied with hyper-gravity in models, which would result in similarities in both shock wave and bubble oscillation. Scaling laws for UNDEX in centrifuge have been proposed based on dimensional analysis. Two dimensionless numbers, i.e.,π_3 and π_4, are used to characterize shock wave and bubble oscillation, respectively. To validate scaling laws, 17 UNDEX tests are designed by varying accelerations or explosive weights and positions in centrifuge. The tests are classified into different groups to validate scaling laws as well as calibrate coefficients in empirical formulae for both shock wave and bubble oscillation. The results show that changes of gravity acceleration or hydrodynamic pressure almost has no influence on shock wave peak pressure and time constant as long as π3 is constant. The dimensionless bubble period and maximum radius agreed with each other when π4 is constant. Based on the research, an example is exhibited to suggest method for the computation of initial loading conditions for a submerged obstacle subjected to UNDEX.
