芘分子及其阳离子的Laser诱导电子和振动动力学
Laser-Induced Electronic and Vibronic Dynamics in the Pyrene Molecule and its Cation
摘要：
在多环芳烃中，芘由于其独特的紫外吸收和红外发射特性而被广泛用作光学探针。有趣的是，这种分子也是星际介质的丰富成分，在那里它通过其独特的光谱指纹被检测到。在这项工作中，我们提出了一个全面的第一性原理研究的电子和振动响应的芘及其阳离子的超快，相干脉冲共振与他们的光学活性激发在紫外区。通过对分子对称性、电子结构和线性光谱的分析，解释了超短激光场激发系统的瞬态吸收谱和计算的动能谱密度。通过解开的电子和振动动力学的影响，通过\textit{ad hoc}模拟与静止和运动的离子，并在特定情况下，辅助模型系统的帮助下，我们合理化的核运动主要是谐波的中性物种，而强烈的非谐振荡出现在阳离子，由电子相干性驱动。我们的研究结果提供了额外的洞察超快振动动力学的芘和相关化合物，并为未来的研究更复杂的碳共轭分子。
英文摘要：
Among polycyclic aromatic hydrocarbons, pyrene is widely used as an optical probe thanks to peculiar ultraviolet absorption and infrared emission features. Interestingly, this molecule is also an abundant component of the interstellar medium, where it is detected via its unique spectral fingerprints. In this work, we present a comprehensive first-principles study on the electronic and vibrational response of pyrene and its cation to ultrafast, coherent pulses in resonance with their optically active excitations in the ultraviolet region. The analysis of molecular symmetries, electronic structure, and linear optical spectra is used to interpret transient absorption spectra and kinetic energy spectral densities computed for the systems excited by ultrashort laser fields. By disentangling the effects of the electronic and vibrational dynamics via \textit{ad hoc} simulations with stationary and moving ions, and, in specific cases, with the aid of auxiliary model systems, we rationalize that the nuclear motion is mainly harmonic in the neutral species, while strong anharmonic oscillations emerge in the cation, driven by electronic coherence. Our results provide additional insight into the ultrafast vibronic dynamics of pyrene and related compounds and set the stage for future investigations on more complex carbon-conjugated molecules.
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