Salomon Grégoire, Tarrat Nathalie, Schön J Christian, Rapacioli Mathias
ISAE-SUPAERO, 10 Avenue Édouard-Belin BP 54032, 31055 Toulouse CEDEX 4, France.
CEMES, Université de Toulouse, CNRS, 29 Rue Jeanne Marvig, 31055 Toulouse, France.
Molecules. 2023 Jul 31;28(15):5778. doi: 10.3390/molecules28155778.
The transformation pathways between low-energy naphthalene isomers are studied by investigating the topology of the energy landscape of this astrophysically relevant molecule. The threshold algorithm is used to identify the minima basins of the isomers on the potential energy surface of the system and to evaluate the probability flows between them. The transition pathways between the different basins and the associated probabilities were investigated for several lid energies up to 11 eV, this value being close to the highest photon energy in the interstellar medium (13.6 eV). More than a hundred isomers were identified and a set of 23 minima was selected among them, on the basis of their energy and probability of occurrence. The return probabilities of these 23 minima and the transition probabilities between them were computed for several lid energies up to 11 eV. The first connection appeared at 3.5 eV while all minima were found to be connected at 9.5 eV. The local density of state was also sampled inside their respective basins. This work gives insight into both energy and entropic barriers separating the different basins, which also provides information about the transition regions of the energy landscape.
通过研究这种与天体物理学相关分子的能量景观拓扑结构,对低能萘异构体之间的转化途径进行了研究。阈值算法用于识别系统势能面上异构体的极小值盆地,并评估它们之间的概率流。针对高达11 eV的几种激发能量,研究了不同盆地之间的过渡途径及相关概率,该值接近星际介质中的最高光子能量(13.6 eV)。识别出了一百多种异构体,并根据它们的能量和出现概率从中选择了一组23个极小值。针对高达11 eV的几种激发能量,计算了这23个极小值的返回概率以及它们之间的跃迁概率。第一个连接出现在3.5 eV处,而在9.5 eV时发现所有极小值都是相连的。还在它们各自的盆地内对局部态密度进行了采样。这项工作深入了解了分隔不同盆地的能量和熵垒,这也提供了有关能量景观过渡区域的信息。