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arXiv · 2305.09911

Impact of high-rank excitations on accuracy of the unitary coupled cluster downfolding formalism

Karol Kowalski·Bo Peng·Nicholas P. Bauman
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Abstract

In this paper, we evaluate the accuracy of the Hermitian form of the downfolding procedure utilizing the double unitary coupled cluster Ansatz (DUCC) on the H6 and H8 benchmark systems. The computational infrastructure employs the occupation-number-representation codes to construct the matrix representation of arbitrary second-quantized operators, enabling the exact representation of exponentials of various operators. The tests utilize external excitations estimated from standard single-reference coupled cluster methods (SR-CC) to demonstrate that higher-rank SR-CC external amplitudes were necessary to describe the energies in the strongly correlated regime adequately. We show that this approach can offset problems of the corresponding SR-CC theories associated with losing the variational character of corresponding energies.

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Karol Kowalski, Bo Peng, Nicholas P. Bauman. 2023-05-17. Impact of high-rank excitations on accuracy of the unitary coupled cluster downfolding formalism. https://arxiv.org/abs/2305.09911

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