Using principal component analysis for neural network high-dimensional potential energy surface

被引:13
作者
Casier, Bastien [1 ]
Carniato, Stephane [1 ]
Miteva, Tsveta [1 ]
Capron, Nathalie [1 ]
Sisourat, Nicolas [1 ]
机构
[1] Sorbonne Univ, CNRS, UMR 7614, Lab Chim Phys Matiere & Rayonnement, F-75005 Paris, France
关键词
INITIO MOLECULAR-DYNAMICS; KETO-ENOL-TAUTOMERISM;
D O I
10.1063/5.0009264
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Potential energy surfaces (PESs) play a central role in our understanding of chemical reactions. Despite the impressive development of efficient electronic structure methods and codes, such computations still remain a difficult task for the majority of relevant systems. In this context, artificial neural networks (NNs) are promising candidates to construct the PES for a wide range of systems. However, the choice of suitable molecular descriptors remains a bottleneck for these algorithms. In this work, we show that a principal component analysis (PCA) is a powerful tool to prepare an optimal set of descriptors and to build an efficient NN: this protocol leads to a substantial improvement of the NNs in learning and predicting a PES. Furthermore, the PCA provides a means to reduce the size of the input space (i.e., number of descriptors) without losing accuracy. As an example, we applied this novel approach to the computation of the high-dimensional PES describing the keto-enol tautomerism reaction occurring in the acetone molecule.
引用
收藏
页数:9
相关论文
共 38 条
[1]  
[Anonymous], 1961, Adaptive Control Processes: a Guided Tour, DOI DOI 10.1515/9781400874668
[2]  
[Anonymous], SAMORZAD TERYTORIALN
[3]  
[Anonymous], 2011, Neural Networks and Learning Machines
[4]   Principal component analysis and long time protein dynamics [J].
Balsera, MA ;
Wriggers, W ;
Oono, Y ;
Schulten, K .
JOURNAL OF PHYSICAL CHEMISTRY, 1996, 100 (07) :2567-2572
[5]   Generalized neural-network representation of high-dimensional potential-energy surfaces [J].
Behler, Joerg ;
Parrinello, Michele .
PHYSICAL REVIEW LETTERS, 2007, 98 (14)
[6]   Perspective: Machine learning potentials for atomistic simulations [J].
Behler, Joerg .
JOURNAL OF CHEMICAL PHYSICS, 2016, 145 (17)
[7]   Neural network potential-energy surfaces in chemistry: a tool for large-scale simulations [J].
Behler, Joerg .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2011, 13 (40) :17930-17955
[8]   Coordinate reduction for exploring chemical reaction paths [J].
Birkholz, Adam B. ;
Schlegel, H. Bernhard .
THEORETICAL CHEMISTRY ACCOUNTS, 2012, 131 (03) :1-8
[9]   PROJECTOR AUGMENTED-WAVE METHOD [J].
BLOCHL, PE .
PHYSICAL REVIEW B, 1994, 50 (24) :17953-17979
[10]   Probing keto-enol tautomerism using photoelectron spectroscopy [J].
Capron, Nathalie ;
Casier, Bastien ;
Sisourat, Nicolas ;
Piancastelli, Maria Novella ;
Simon, Marc ;
Carniato, Stephane .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2015, 17 (30) :19991-19996