Conical Intersection versus Avoided Crossing: Geometric Phase Effect in Molecular High-Order Harmonics

a Institute of Ultrafast Optical Physics, MIIT Key Laboratory of Semiconductor Microstructure and Quantum Sensing, Department of Applied Physics, Nanjing University of Science and Technology, Nanjing 210094, China.
b State Key Laboratory of Precision Spectroscopy, East China Normal University, Shanghai 200062, China.
c Center for Theoretical Physics and School of Science, Hainan University, Haikou 570228, China.
d Collaborative Innovation Center of Extreme Optics, Shanxi University, Taiyuan, Shanxi 030006, China.
e Himalayan Institute for Advanced Study, Unit of Gopinath Seva Foundation, MIG 38, Avas Vikas, Rishikesh, Uttarakhand 249201, India.

a Institute of Ultrafast Optical Physics, MIIT Key Laboratory of Semiconductor Microstructure and Quantum Sensing, Department of Applied Physics, Nanjing University of Science and Technology, Nanjing 210094, China.
b State Key Laboratory of Precision Spectroscopy, East China Normal University, Shanghai 200062, China.
c Center for Theoretical Physics and School of Science, Hainan University, Haikou 570228, China.
d Collaborative Innovation Center of Extreme Optics, Shanxi University, Taiyuan, Shanxi 030006, China.
e Himalayan Institute for Advanced Study, Unit of Gopinath Seva Foundation, MIG 38, Avas Vikas, Rishikesh, Uttarakhand 249201, India.

摘要: 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.

Abstract: 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.

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