研究目的
To demonstrate how the carrier envelope phase (CEP) in near single-cycle pulses can control molecular photoexcitation through the Stark effect, using oriented H2CSO (sulfine) as a model system.
研究成果
The CEP in near single-cycle pulses can effectively control molecular photoexcitation via the Stark effect, modulating excitation energies and population transfer. This provides a foundation for dynamically tailoring potential energy surfaces and controlling chemical reactivity in oriented molecules with permanent dipole moments.
研究不足
The study is computational and relies on theoretical models; experimental validation is not provided. The method assumes oriented molecules and specific pulse parameters, which may not be fully achievable in practice. Multiphoton excitation and photoionization are not dominant but could affect results at higher intensities.
1：Experimental Design and Method Selection:
The study uses computational simulations to model photoexcitation and dynamics. The XFAIMS (eXternal Field Ab Initio Multiple Spawning) method is employed to account for light-matter interaction, Stark shifts, and nonadiabatic dynamics, along with Born-Oppenheimer molecular dynamics for ground-state dynamics.
2：Sample Selection and Data Sources:
The molecule H2CSO (sulfine) is chosen due to its symmetry properties, with simulations based on ab initio calculations (SA2-CASSCF(4/3)/6-31G(d) level).
3：List of Experimental Equipment and Materials:
No physical equipment is used; the work is computational, involving software for quantum dynamics simulations.
4：Experimental Procedures and Operational Workflow:
Simulations involve applying near single-cycle pulses with varying CEP and polarization to oriented sulfine molecules, tracking S1 population and subsequent dynamics through conical intersections to photoproducts.
5：Data Analysis Methods:
Analysis includes computing S1 population as a function of CEP and polarization, and yields of photoproducts like oxathiirane and H2S, with results interpreted using Stark effect principles.
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