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arXiv · 2207.08627

A low-cost four-component relativistic equation of motion coupled cluster method based on frozen natural spinors: Theory, Implementation and Benchmark

Kshitijkumar Surjuse·Somesh Chamoli·Malaya K. Nayak·Achintya Kumar Dutta
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Abstract

We present the theory and the implementation of a low-cost four-component relativistic equation of motion coupled cluster method for ionized states based on frozen natural spinors. A single threshold (natural spinor occupancy) can control the accuracy of the calculated ionization potential values. Frozen natural spinors can significantly reduce the computational cost for valence and core-ionization energies with systematically controllable accuracy. The convergence of the ionization potential values with respect to the natural spinor occupancy threshold becomes slower with the increase in basis set dimension. However, the use of a natural spinor threshold of 10-5 and 10-6 gives excellent agreement with experimental results for valence and core ionization energies, respectively.

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Kshitijkumar Surjuse, Somesh Chamoli, Malaya K. Nayak, Achintya Kumar Dutta. 2022-07-18. A low-cost four-component relativistic equation of motion coupled cluster method based on frozen natural spinors: Theory, Implementation and Benchmark. https://doi.org/10.1063/5.0125868

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