Estimating vibrational and thermodynamic properties of adsorbates with uncertainty using data driven surrogates
Estimating vibrational and thermodynamic properties of adsorbates with uncertainty using data driven surrogates
复制标题
使用数据驱动的替代物估计具有不确定性的吸附物的振动和热力学特性
DOI：
10.1002/aic.16838
复制
发表时间：
2019
期刊：
影响因子：
3.7
通讯作者：
S. Rangarajan
中科院分区：
文献类型：
--
作者：
Huijie Tian;Christopher Rzepa;Ronak Upadhyay;S. Rangarajan
在这项工作中，我们提出了一种策略，以开发数据驱动的局部替代模型的从头计算势能函数描述吸附在多相催化材料上的相互作用。结果表明，这些基于正交多项式展开式的多变量替代模型可以用来计算简谐振动频率和吸附态的熵。此外，我们证明了我们的代理模型中的误差可以被估计和传播以计算计算性质中的不确定性。我们给出了我们的方法的概念验证插图，以计算乙烯在硫化钼(MoS_2)一维边缘上的振动频率，(B)铂(111)的二维表面，和(C)HZSM-5沸石的三维微孔，乙烷在铂(111)上的吸附熵，以及所有情况下的相关不确定度。
In this work, we propose a strategy to develop data driven local surrogate models of ab initio potential energy functions describing the interaction of adsorbates on heterogeneous catalytic materials. We show that these multivariable surrogate models, based on orthogonal polynomial expansion and trained on sampled ab‐initio energies/forces, can be used to compute harmonic vibrational frequencies and the entropy of adsorbates. Further, we show that the errors in our surrogate model can be estimated and propagated to calculate the uncertainty in the computed properties. We show proof‐of‐concept illustrations of our method to calculate the vibrational frequencies of ethene on 1D edges of molybdenum sulfide (MoS2), (b) 2D surfaces of Pt(111), and (c) 3D micropores of a HZSM‐5 zeolite; the entropy of ethane adsorbed on Pt(111); and the associated uncertainties in all the cases.