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  Wavefunction Embedding for Molecular Polaritons

Pavošević, F., & Rubio, A. (2022). Wavefunction Embedding for Molecular Polaritons.

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2204.01777.pdf (Preprint), 3MB
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2204.01777.pdf
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File downloaded from arXiv at 2022-04-06
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2022
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https://arxiv.org/abs/2204.01777 (Preprint)
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 Creators:
Pavošević, F.1, Author
Rubio, A.2, 3, 4, Author              
Affiliations:
1Center for Computational Quantum Physics, Flatiron Institute, ou_persistent22              
2Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_2266715              
3Center for Free-Electron Laser Science, ou_persistent22              
4Nano-Bio Spectroscopy Group and European Theoretical Spectroscopy Facility (ETSF), Universidad del País Vasco (UPV/EHU), ou_persistent22              

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Free keywords: Physics, Chemical Physics, physics.chem-ph
 Abstract: Polaritonic chemistry relies on the strong light-matter interaction phenomena for altering the chemical reaction rates inside optical cavities. To explain and to understand these processes, the development of reliable theoretical models is essential. While computationally efficient quantum electrodynamics self-consistent field (QED-SCF) methods, such as quantum electrodynamics density functional theory (QEDFT) needs accurate functionals, quantum electrodynamics coupled cluster (QED-CC) methods provide a systematic increase in accuracy but at much greater cost. To overcome this computational bottleneck, herein we introduce and develop the QED-CC-in-QED-SCF projection-based embedding method that inherits all the favorable properties from the two worlds, computational efficiency and accuracy. The performance of the embedding method is assessed by studying some prototypical but relevant reactions, such as methyl transfer reaction, proton transfer reaction, as well as protonation reaction in a complex environment. The results obtained with the new embedding method are in excellent agreement with more expensive QED-CC results. The analysis performed on these reactions indicate that the strong light-matter interaction is very local in nature and that only a small region should be treated at the QED-CC level for capturing important effects due to cavity. This work sets the stage for future developments of polaritonic quantum chemistry methods and it will serve as a guideline for development of other polaritonic embedding models.

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Language(s): eng - English
 Dates: 2022-04-04
 Publication Status: Published online
 Pages: 9
 Publishing info: -
 Table of Contents: -
 Rev. Type: No review
 Identifiers: arXiv: 2204.01777
 Degree: -

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