Phaseless auxiliary-field quantum Monte Carlo method for cavity-QED matter systems
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arXiv
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| Hauptverfasser: | , , , , |
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| Format: | Preprint |
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2024
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| _version_ | 1866909517643513856 |
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| author | Weber, Lukas Cunha, Leonardo dos Anjos Morales, Miguel A. Rubio, Angel Zhang, Shiwei |
| author_facet | Weber, Lukas Cunha, Leonardo dos Anjos Morales, Miguel A. Rubio, Angel Zhang, Shiwei |
| contents | We present a generalization of the phaseless auxiliary-field quantum Monte Carlo (AFQMC) method to cavity quantum-electrodynamical (QED) matter systems. The method can be formulated in both the Coulomb and the dipole gauge. We verify its accuracy by benchmarking calculations on a set of small molecules against full configuration interaction and state-of-the-art QED coupled cluster (QED-CCSD) calculations. Our results show that (i) gauge invariance can be achieved within correlation-consistent Gaussian basis sets, (ii) the accuracy of QED-CCSD can be enhanced significantly by adding the standard perturbative triples correction without light-matter coupling, and (iii) there is a straightforward way to evaluate the differential expression for the photon occupation number that works in any gauge. The high accuracy and favorable computational scaling of our AFQMC approach will enable a broad range of applications. Besides polaritonic chemistry, the method opens a way to simulate extended QED matter systems. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2410_18838 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Phaseless auxiliary-field quantum Monte Carlo method for cavity-QED matter systems Weber, Lukas Cunha, Leonardo dos Anjos Morales, Miguel A. Rubio, Angel Zhang, Shiwei Chemical Physics We present a generalization of the phaseless auxiliary-field quantum Monte Carlo (AFQMC) method to cavity quantum-electrodynamical (QED) matter systems. The method can be formulated in both the Coulomb and the dipole gauge. We verify its accuracy by benchmarking calculations on a set of small molecules against full configuration interaction and state-of-the-art QED coupled cluster (QED-CCSD) calculations. Our results show that (i) gauge invariance can be achieved within correlation-consistent Gaussian basis sets, (ii) the accuracy of QED-CCSD can be enhanced significantly by adding the standard perturbative triples correction without light-matter coupling, and (iii) there is a straightforward way to evaluate the differential expression for the photon occupation number that works in any gauge. The high accuracy and favorable computational scaling of our AFQMC approach will enable a broad range of applications. Besides polaritonic chemistry, the method opens a way to simulate extended QED matter systems. |
| title | Phaseless auxiliary-field quantum Monte Carlo method for cavity-QED matter systems |
| topic | Chemical Physics |
| url | https://arxiv.org/abs/2410.18838 |