In recent years, ozone and its isotopologues have been a topic of interest in many fields of research, due to its importance in atmospheric chemistry and its anomalous isotopic enrichment—or the so-called “mass-independent fractionation.” In the field of potential energy surface (PES) creation, debate over the existence of a potential barrier just under the dissociation threshold (referred to as a “potential reef”) has plagued research for some years. Recently, Dawes and co-workers [Dawes, Lolur, Li, Jiang, and Guo (DLLJG) J. Chem. Phys. 139, 201103 (2013)] created a highly accurate global PES, for which the reef is found to be replaced with a (monotonic) “plateau.” Subsequent dynamical calculations on this “DLLJG” PES have shown improved agreement with experiment, particularly the vibrational spectrum. However, it is well known that reaction dynamics is also highly influenced by the rovibrational states, especially in cases like ozone that assume a Lindemann-type mechanism. Accordingly, we present the first significant step toward a complete characterization of the rovibrational spectrum for various isotopologues of ozone, computed using the DLLJG PES together with the ScalIT suite of parallel codes. Additionally, artificial neural networks are used in an innovative fashion—not to construct the PES function per se but rather to greatly speed up its evaluation.

中文翻译：

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利用人工神经网络，精确到J = 10的臭氧同位素分子的旋转振动能

近年来，由于臭氧及其同位素在大气化学中的重要性及其异常同位素富集（即所谓的“质量无关的分离”），在许多研究领域中都引起了人们的关注。在势能面（PES）的创造领域，关于在离解阈值以下存在潜在势垒（称为“潜礁”）的争论一直困扰着研究。最近，Dawes及其同事[Dawes，Lolur，Li，Jiang和Guo（DLLJG）J. Chem。物理 139，201103（2013）]创建了一个高度准确的全球PES，该珊瑚礁被发现用（单调）“高原”代替。随后在该“ DLLJG” PES上进行的动力学计算表明与实验的一致性得到了改善，尤其是振动谱。然而，众所周知，反应动力学也受旋转振动状态的极大影响，特别是在像臭氧那​​样具有Lindemann型机理的情况下。因此，我们展示了朝着完整表征各种臭氧同位素的旋转振动谱迈出的重要的第一步，这是使用DLLJG PES与ScalIT并行代码套件一起计算的。此外，人工神经网络以创新方式使用-本身并不是在构建PES功能 而是大大加快了评估速度。