论文标题
部分可观测时空混沌系统的无模型预测
Polyaromatic Hydrocarbons with an Imperfect Aromatic System as Catalysts of Interstellar H$_{2}$ Formation
论文作者
论文摘要
储层计算是预测湍流的有力工具,其简单的架构具有处理大型系统的计算效率。然而,其实现通常需要完整的状态向量测量和系统非线性知识。我们使用非线性投影函数将系统测量扩展到高维空间,然后将其输入到储层中以获得预测。我们展示了这种储层计算网络在时空混沌系统上的应用,该系统模拟了湍流的若干特征。我们表明,使用径向基函数作为非线性投影器,即使只有部分观测并且不知道控制方程,也能稳健地捕捉复杂的系统非线性。最后,我们表明,当测量稀疏、不完整且带有噪声,甚至控制方程变得不准确时,我们的网络仍然可以产生相当准确的预测,从而为实际湍流系统的无模型预测铺平了道路。
Although H$_{2}$ is the simplest and the most abundant molecule in the Universe, its formation in the interstellar medium, especially in the photodissociation regions is far from being fully understood. According to suggestions, the formation of H$_{2}$ is catalyzed by polyaromatic hydrocarbons (PAHs) on the surface of interstellar grains. In the present study, we have investigated the catalytic effect of small PAHs with an imperfect aromatic system. Quantum chemical computations were performed for the H-atom-abstraction and H-atom-addition reactions of benzene, cyclopentadiene, cycloheptatriene, indene, and 1H-phenalene. Heights of reaction barriers and tunneling reaction rate constants were computed with density functional theory using the MPWB1K functional. For each molecule, the reaction path and the \warn{rate constants} were determined at 50 K using ring-polymer instanton theory, and the temperature dependence of the \warn{rate constants} was investigated for cyclopentadiene and cycloheptatriene. The computational results reveal that defects in the aromatic system compared to benzene can increase the rate of the catalytic H$_{2}$ formation at 50 K.