The Integral- and Intermediate-Screened Coupled-Cluster Method

TL;DR

The paper introduces the integral- and intermediate-screened coupled-cluster (IISCC) method, which significantly reduces computational scaling while maintaining accuracy, enabling large-scale quantum chemical calculations.

Contribution

It presents a novel IISCC approach that rigorously screens integrals and intermediates, achieving linear scaling for all CC hierarchy levels without range-dependent parameters.

Findings

Achieves linear scaling for large systems

Maintains accuracy with adjustable error control

Suitable for large molecular systems and charge-separated systems

Abstract

We present the formulation and implementation of the integral- and intermediate-screened coupled-cluster method (ISSCC). The IISCC method gives a simple and rigorous integral and intermediate screening (IIS) of the coupled-cluster method and will significantly reduces the scaling for all orders of the CC hierarchy exactly like seen for the integral-screened configuration-interaction method (ISCI). The rigorous IIS in the IISCC gives a robust and adjustable error control which should allow for the possibility of converging the energy without any loss of accuracy while retaining low or linear scaling at the same time. The derivation of the IISCC is performed in a similar fashion as in the ISCI where we show that the tensor contractions for the nested commutators are separable up to an overall sign and that this separability can lead to a rigorous IIS. In the nested commutators the integrals are screened in the first tensor contraction and the intermediates are screened in all successive tensor contractions. The rigorous IIS will lead to linear scaling for all nested commutators for large systems in a similar way as seen for the ISCI. The reduced scaling can in this way be obtained without any range dependent parameter for the interaction, unlike other low scaling methods and is therefore also suitable for charge separated systems. It is expected that the IISCC, just like the ISCI, can use dramatically larger orbital spaces combined with large CC expansions as compared with traditional CC methods. Due to the size extensive nature of the CC method the IISCC should not only be applicable to few electron systems but also to large molecular system unlike the ISCI. The IISCC can here either be used as a stand alone method or combined with other linear scaling approaches like the fragmentation method or other methods which introduces a range dependent interaction screening.