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A hybrid stochastic configuration interaction-coupled cluster approach for multireference systems.

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The development of multireference coupled cluster (MRCC) techniques has remained an open area of study in electronic structure theory for decades due to the inherent complexity of expressing a multiconfigurational wavefunction in the fundamentally single-reference coupled cluster framework. The recently developed multireference-coupled cluster Monte Carlo (mrCCMC) technique uses the formal simplicity of the Monte Carlo approach to Hilbert space quantum chemistry to avoid some of the complexities of conventional MRCC, but there is room for improvement in terms of accuracy and, particularly, computational cost. In this paper, we explore the potential of incorporating ideas from conventional MRCC-namely, the treatment of the strongly correlated space in a configuration interaction formalism-to the mrCCMC framework, leading to a series of methods with increasing relaxation of the reference space in the presence of external amplitudes. These techniques offer new balances of stability and cost against accuracy, as well as a means to better explore and better understand the structure of solutions to the mrCCMC equations.



51 Physical Sciences, 34 Chemical Sciences, 5102 Atomic, Molecular and Optical Physics, 3406 Physical Chemistry

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J Chem Phys

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AIP Publishing
Royal Society (UF160398)
The Cambridge Commonwealth, European & International Trust
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