分类: 光学 >> 量子光学 提交时间: 2023-02-19
摘要: Nonadiabatic dynamics around an avoid 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 spectroscopy different from the case of avoid crossing. The coherence built up when the system crosses the avoid 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 time-resolved spectrum allow capturing the snapshot dynamics with sub-femtosecond resolution.
分类: 光学 >> 量子光学 提交时间: 2023-02-19
摘要: High harmonic generation (HHG) from crystals in strong laser fields has been understood by the band theory of solid, which is based on the periodic boundary condition (PBC) of translational invariant. For systems having PBC of rotational invariant, in principles an analogous Bloch theorem can be developed and applied. Taking a ring-type cluster of cyclo[18]carbon as a representative, we theoretically suggest a quasi-band model and study its HHG by solving time-dependent Liouville-von Neumann equation. Under the irradiation of circularly polarized laser, explicit selection rules for left-handed and right-handed harmonics are observed, while in linearly polarized laser field, cyclo[18]carbon exhibits solid-like HHG originated from intra-band oscillations and inter-band transitions, which in turn is promising to optically detect the symmetry and geometry of controversial structures. In a sense, this work presents a connection linking the high harmonics of gases and solids.