Electron-Photon Exchange-Correlation Approximation for QEDFT
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arXiv
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| Main Authors: | , , , , , |
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| Format: | Preprint |
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2024
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| _version_ | 1866929244324495360 |
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| author | Lu, I-Te Ruggenthaler, Michael Tancogne-Dejean, Nicolas Latini, Simone Penz, Markus Rubio, Angel |
| author_facet | Lu, I-Te Ruggenthaler, Michael Tancogne-Dejean, Nicolas Latini, Simone Penz, Markus Rubio, Angel |
| contents | Quantum-electrodynamical density-functional theory (QEDFT) provides a promising avenue for exploring complex light-matter interactions in optical cavities for real materials. Similar to conventional density-functional theory, the Kohn-Sham formulation of QEDFT needs approximations for the generally unknown exchange-correlation functional. In addition to the usual electron-electron exchange-correlation potential, an approximation for the electron-photon exchange-correlation potential is needed. A recent electron-photon exchange functional [C. Schäfer et al., Proc. Natl. Acad. Sci. USA, 118, e2110464118 (2021), https://www.pnas.org/doi/abs/10.1073/pnas.2110464118], derived from the equation of motion of the non-relativistic Pauli-Fierz Hamiltonian, shows robust performance in one-dimensional systems across weak- and strong-coupling regimes. Yet, its performance in reproducing electron densities in higher dimensions remains unexplored. Here we consider this QEDFT functional approximation from one to three-dimensional finite systems and across weak to strong light-matter couplings. The electron-photon exchange approximation provides excellent results in the ultra-strong-coupling regime. However, to ensure accuracy also in the weak-coupling regime across higher dimensions, we introduce a computationally efficient renormalization factor for the electron-photon exchange functional, which accounts for part of the electron-photon correlation contribution. These findings extend the applicability of photon-exchange-based functionals to realistic cavity-matter systems, fostering the field of cavity QED (quantum electrodynamics) materials engineering. |
| format | Preprint |
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arxiv_https___arxiv_org_abs_2402_09794 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Electron-Photon Exchange-Correlation Approximation for QEDFT Lu, I-Te Ruggenthaler, Michael Tancogne-Dejean, Nicolas Latini, Simone Penz, Markus Rubio, Angel Computational Physics Materials Science Atomic and Molecular Clusters Chemical Physics Quantum Physics Quantum-electrodynamical density-functional theory (QEDFT) provides a promising avenue for exploring complex light-matter interactions in optical cavities for real materials. Similar to conventional density-functional theory, the Kohn-Sham formulation of QEDFT needs approximations for the generally unknown exchange-correlation functional. In addition to the usual electron-electron exchange-correlation potential, an approximation for the electron-photon exchange-correlation potential is needed. A recent electron-photon exchange functional [C. Schäfer et al., Proc. Natl. Acad. Sci. USA, 118, e2110464118 (2021), https://www.pnas.org/doi/abs/10.1073/pnas.2110464118], derived from the equation of motion of the non-relativistic Pauli-Fierz Hamiltonian, shows robust performance in one-dimensional systems across weak- and strong-coupling regimes. Yet, its performance in reproducing electron densities in higher dimensions remains unexplored. Here we consider this QEDFT functional approximation from one to three-dimensional finite systems and across weak to strong light-matter couplings. The electron-photon exchange approximation provides excellent results in the ultra-strong-coupling regime. However, to ensure accuracy also in the weak-coupling regime across higher dimensions, we introduce a computationally efficient renormalization factor for the electron-photon exchange functional, which accounts for part of the electron-photon correlation contribution. These findings extend the applicability of photon-exchange-based functionals to realistic cavity-matter systems, fostering the field of cavity QED (quantum electrodynamics) materials engineering. |
| title | Electron-Photon Exchange-Correlation Approximation for QEDFT |
| topic | Computational Physics Materials Science Atomic and Molecular Clusters Chemical Physics Quantum Physics |
| url | https://arxiv.org/abs/2402.09794 |