Quantum embedding for molecules using auxiliary particles – the ghost Gutzwiller Ansatz

Mejuto-Zaera, Carlos

doi:10.1039/d4fd00053f

Faraday Discuss.

2024

DOI: 10.1039/d4fd00053f

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Quantum embedding for molecules using auxiliary particles – the ghost Gutzwiller Ansatz

Carlos Mejuto-Zaera

Abstract: Strong/static electronic correlation mediates the emergence of remarkable phases of matter, and underlies the exceptional reactivity properties in transition metal-based catalysts. Modeling strongly correlated molecules and solids calls for multi-reference...

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2024

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Fragment quantum embedding using the Householder transformation: A multi-state extension based on ensembles

Cernatic,

Fromager,

Yalouz

2024

The Journal of Chemical Physics

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In recent studies by Yalouz et al. [J. Chem. Phys. 157, 214112 (2022)] and Sekaran et al. [Phys. Rev. B 104, 035121 (2021) and Computation 10, 45 (2022)], density matrix embedding theory (DMET) has been reformulated through the use of the Householder transformation as a novel tool to embed a fragment within extended systems. The transformation was applied to a reference non-interacting one-electron reduced density matrix to construct fragments’ bath orbitals, which are crucial for subsequent ground state calculations. In the present work, we expand upon these previous developments and extend the utilization of the Householder transformation to the description of multiple electronic states, including ground and excited states. Based on an ensemble noninteracting density matrix, we demonstrate the feasibility of achieving exact fragment embedding through successive Householder transformations, resulting in a larger set of bath orbitals. We analytically prove that the number of additional bath orbitals scales directly with the number of fractionally occupied natural orbitals in the reference ensemble density matrix. A connection with the regular DMET bath construction is also made. Then, we illustrate the use of this ensemble embedding tool in single-shot DMET calculations to describe both ground and first excited states in a Hubbard lattice model and an ab initio hydrogen system. Finally, we discuss avenues for enhancing ensemble embedding through self-consistency and explore potential future directions.

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Fragment quantum embedding using the Householder transformation: A multi-state extension based on ensembles

Cernatic,

Fromager,

Yalouz

2024

The Journal of Chemical Physics

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Quantum embedding for molecules using auxiliary particles – the ghost Gutzwiller Ansatz

Abstract: Strong/static electronic correlation mediates the emergence of remarkable phases of matter, and underlies the exceptional reactivity properties in transition metal-based catalysts. Modeling strongly correlated molecules and solids calls for multi-reference...

Cited by 1 publication

References 96 publications

Fragment quantum embedding using the Householder transformation: A multi-state extension based on ensembles

Fragment quantum embedding using the Householder transformation: A multi-state extension based on ensembles

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