标题： 绿色行动：选择性配置相互作用作为高精度更可持续的替代方法 显示英文标题

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

摘要： 最近，一种全组态相互作用（FCI）方法的新分布式实现已被报道 [Gao 等，J. Chem Theory Comput. 2024, 20, 1185]。由于采用了一种混合并行化方案，作者能够计算丙烷（\ce{C3H8}）在最小基组 STO-3G 中的精确能量。这项艰巨的任务涉及处理26个电子在23个轨道中的活性空间，或是一个包含\SI{1.3d12}个行列式的希尔伯特空间。这是迄今为止报告的最大FCI计算。在这里，我们从一般观点出发，说明选定组态相互作用（SCI）如何通过FCI空间的稀疏探索，在计算和内存成本的一小部分下实现微哈特里精度。目前的SCI计算是使用\textit{使用逐次摄动选择的组态相互作用}（CIPSI）算法进行的，该算法在\textsc{量子包}软件中以行列式驱动的方式实现。本研究加强了普遍共识，即在FCI空间中数量庞大的行列式中，只有极小一部分对能量有显著贡献。更重要的是，它证明了使用更合理和可持续的计算资源达到相当精度的可行性，从而减少计算化学不断增长的碳足迹。 显示英文摘要

摘要： 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.