MLatom 3: A Platform for Machine Learning-Enhanced Computational Chemistry Simulations and Workflows.

Machine learning (ML) is increasingly becoming a common tool in computational chemistry. At the same time, the rapid development of ML methods requires a flexible software framework for designing custom workflows. MLatom 3 is a program package designed to leverage the power of ML to enhance typical computational chemistry simulations and to create complex workflows. This open-source package provides plenty of choice to the users who can run simulations with the command-line options, input files, or with scripts using MLatom as a Python package, both on their computers and on the online XACS cloud computing service at XACScloud.com. Computational chemists can calculate energies and thermochemical properties, optimize geometries, run molecular and quantum dynamics, and simulate (ro)vibrational, one-photon UV/vis absorption, and two-photon absorption spectra with ML, quantum mechanical, and combined models. The users can choose from an extensive library of methods containing pretrained ML models and quantum mechanical approximations such as AIQM1 approaching coupled-cluster accuracy. The developers can build their own models using various ML algorithms. The great flexibility of MLatom is largely due to the extensive use of the interfaces to many state-of-the-art software packages and libraries.

Benchmark of general-purpose machine learning-based quantum mechanical method AIQM1 on reaction barrier heights.

Artificial intelligence-enhanced quantum mechanical method 1 (AIQM1) is a general-purpose method that was shown to achieve high accuracy for many applications with a speed close to its baseline semiempirical quantum mechanical (SQM) method ODM2*. Here, we evaluate the hitherto unknown performance of out-of-the-box AIQM1 without any refitting for reaction barrier heights on eight datasets, including a total of ∼24 thousand reactions. This evaluation shows that AIQM1's accuracy strongly depends on the type of transition state and ranges from excellent for rotation barriers to poor for, e.g., pericyclic reactions. AIQM1 clearly outperforms its baseline ODM2* method and, even more so, a popular universal potential, ANI-1ccx. Overall, however, AIQM1 accuracy largely remains similar to SQM methods (and B3LYP/6-31G* for most reaction types) suggesting that it is desirable to focus on improving AIQM1 performance for barrier heights in the future. We also show that the built-in uncertainty quantification helps in identifying confident predictions. The accuracy of confident AIQM1 predictions is approaching the level of popular density functional theory methods for most reaction types. Encouragingly, AIQM1 is rather robust for transition state optimizations, even for the type of reactions it struggles with the most. Single-point calculations with high-level methods on AIQM1-optimized geometries can be used to significantly improve barrier heights, which cannot be said for its baseline ODM2* method.