Physics

Cluster (spacecraft)

Mathematics

Truncation (statistics)

Statistical physics

Mathematical optimization

Wave function

Machine learning

Hamiltonian (control theory)

Mathematical analysis

Coupled cluster

Amplitude

Programming language

Solver

Molecule

Computer science

Quantum mechanics

Applied mathematics

System of linear equations

The Journal of Physical Chemistry Letters

Solving the coupled-cluster (CC) equations is a cost-prohibitive process that exhibits poor scaling with system size. These equations are solved by determining the set of amplitudes (t) that minimize the system energy with respect to the coupled-cluster equations at the selected level of truncation. Here, a novel approach to predict the converged coupled-cluster singles and doubles (CCSD) amplitudes, thus the coupled-cluster wave function, is explored by using machine learning and electronic structure properties inherent to the MP2 level. Features are collected from quantum chemical data, such as orbital energies, one-electron Hamiltonian, Coulomb, and exchange terms. The data-driven CCSD (DDCCSD) is not an alchemical method because the actual iterative coupled-cluster equations are solved. However, accurate energetics can also be obtained by bypassing solving the CC equations entirely. Our preliminary data show that it is possible to achieve remarkable speedups in solving the CCSD equations, especially when the correct physics are encoded and used for training of machine learning models.

Data-Driven Acceleration of the Coupled-Cluster Singles and Doubles Iterative Solver