The Impact of Pulse Shaping on Coherent Dynamics near a Conical Intersection

Abstract

Utilizing lasers to probe microscopic physical processes is a crucial tool in contemporary physics research, where the influence of laser properties on excitation processes is a focal point for scientists. In this study, we investigated the impact of laser pulses on the quantum yield of electronic wave packets near conical intersections (CIs). To do so, we employed the time non-local quantum master equation to calculate the time-evolution dynamics of wave packets on excited-state potential energy surfaces (PESs) and projected them onto effective reaction coordinates. The waveform of laser pulses was manipulated by varying the relative amplitude, pulse duration, and center wavelengths of Gaussian profiles. Our calculations revealed that the shape of laser pulses has a discernible impact on the dynamic evolution of electrons in excited states. Furthermore, our research indicated that different pulse profiles exhibit a maximum variation of 6.88% in the quantum yields of electronic wave packets near CIs. Our calculations demonstrate the influence of laser pulse waveform on excitation processes, providing a feasible method for exploring the coherent control of wave packets at conical intersections characterized by strong nonadiabatic coupling.

Keywords

• laser pulse waveform
• quantum open system
• nonadiabatic dynamics
• conical intersection