Go Green: Selected Configuration Interaction as a More Sustainable Alternative for High Accuracy

Abstract

Recently, a new distributed implementation of the full configuration interaction (FCI) method has been reported [Gao et al. J. Chem Theory Comput. 2024, 20, 1185]. Thanks to a hybrid parallelization scheme, the authors were able to compute the exact energy of propane (\ce{C3H8}) in the minimal basis STO-3G. This formidable task involves handling an active space of 26 electrons in 23 orbitals or a Hilbert space of \SI{1.3d12} determinants. This is, by far, the largest FCI calculation reported to date. Here, we illustrate how, from a general point of view, selected configuration interaction (SCI) can achieve microhartree accuracy at a fraction of the computational and memory cost, via a sparse exploration of the FCI space. The present SCI calculations are performed with the \textit{Configuration Interaction using a Perturbative Selection made Iteratively} (CIPSI) algorithm, as implemented in a determinant-driven way in the \textsc{quantum package} software. The present study reinforces the common wisdom that among the exponentially large number of determinants in the FCI space, only a tiny fraction of them significantly contribute to the energy. More importantly, it demonstrates the feasibility of achieving comparable accuracy using more reasonable and sustainable computational resources, hence reducing the ever-growing carbon footprint of computational chemistry.