Nonadiabatic dynamics around an avoided crossing or a conical intersection play a crucial role in the photoinduced processes of most polyatomic molecules.The present work shows that the topological phase in conical in...Nonadiabatic dynamics around an avoided crossing or a conical intersection play a crucial role in the photoinduced processes of most polyatomic molecules.The present work shows that the topological phase in conical intersection makes the behavior of pump-probe high-order harmonic signals different from the case of avoided crossing.The coherence built up when the system crosses the avoided crossing will lead to the oscillatory behavior of the spectrum,while the geometric phase erodes these oscillations in the case of conical intersection.Additionally,the dynamical blueshift and the splitting of the time-resolved spectrum allow capturing the snapshot dynamics with the sub-femtosecond resolution.展开更多
基金supported by the National Key Research and Development Program of China (Grant No.2022YFA1604301)the National Natural Science Foundation of China (Grant Nos.12074124 and 11974185)+1 种基金Zijiang Endowed Young Scholar Fund,East China Normal University,and Overseas Expertise Introduction Project for Discipline Innovation (B12024)support by the start-up funding from East China Normal University.
文摘Nonadiabatic dynamics around an avoided crossing or a conical intersection play a crucial role in the photoinduced processes of most polyatomic molecules.The present work shows that the topological phase in conical intersection makes the behavior of pump-probe high-order harmonic signals different from the case of avoided crossing.The coherence built up when the system crosses the avoided crossing will lead to the oscillatory behavior of the spectrum,while the geometric phase erodes these oscillations in the case of conical intersection.Additionally,the dynamical blueshift and the splitting of the time-resolved spectrum allow capturing the snapshot dynamics with the sub-femtosecond resolution.
