Second quantization of many-body dispersion interactions for chemical and biological systems
Abstract The many-body dispersion (MBD) framework is a successful approach for modeling the long-range electronic correlation energy and optical response of systems with thousands of atoms. Inspired by field theory, here we develop a second-quantized MBD formalism (SQ-MBD) that recasts a system of a...
| Main Authors: | , , |
|---|---|
| Format: | Article |
| Language: | English |
| Published: |
Nature Portfolio
2023-12-01
|
| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-023-43785-z |
| _version_ | 1797388235751555072 |
|---|---|
| author | Matteo Gori Philip Kurian Alexandre Tkatchenko |
| author_facet | Matteo Gori Philip Kurian Alexandre Tkatchenko |
| author_sort | Matteo Gori |
| collection | DOAJ |
| description | Abstract The many-body dispersion (MBD) framework is a successful approach for modeling the long-range electronic correlation energy and optical response of systems with thousands of atoms. Inspired by field theory, here we develop a second-quantized MBD formalism (SQ-MBD) that recasts a system of atomic quantum Drude oscillators in a Fock-space representation. SQ-MBD provides: (i) tools for projecting observables (interaction energy, transition multipoles, polarizability tensors) on coarse-grained representations of the atomistic system ranging from single atoms to large structural motifs, (ii) a quantum-information framework to analyze correlations and (non)separability among fragments in a given molecular complex, and (iii) a path toward the applicability of the MBD framework to molecular complexes with even larger number of atoms. The SQ-MBD approach offers conceptual insights into quantum fluctuations in molecular systems and enables direct coupling of collective plasmon-like MBD degrees of freedom with arbitrary environments, providing a tractable computational framework to treat dispersion interactions and polarization response in intricate systems. |
| first_indexed | 2024-03-08T22:37:52Z |
| format | Article |
| id | doaj.art-e40bf3f83922478591a727a46cacfada |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-03-08T22:37:52Z |
| publishDate | 2023-12-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-e40bf3f83922478591a727a46cacfada2023-12-17T12:23:36ZengNature PortfolioNature Communications2041-17232023-12-0114111110.1038/s41467-023-43785-zSecond quantization of many-body dispersion interactions for chemical and biological systemsMatteo Gori0Philip Kurian1Alexandre Tkatchenko2Department of Physics and Materials Science, University of LuxembourgQuantum Biology Laboratory, Howard UniversityDepartment of Physics and Materials Science, University of LuxembourgAbstract The many-body dispersion (MBD) framework is a successful approach for modeling the long-range electronic correlation energy and optical response of systems with thousands of atoms. Inspired by field theory, here we develop a second-quantized MBD formalism (SQ-MBD) that recasts a system of atomic quantum Drude oscillators in a Fock-space representation. SQ-MBD provides: (i) tools for projecting observables (interaction energy, transition multipoles, polarizability tensors) on coarse-grained representations of the atomistic system ranging from single atoms to large structural motifs, (ii) a quantum-information framework to analyze correlations and (non)separability among fragments in a given molecular complex, and (iii) a path toward the applicability of the MBD framework to molecular complexes with even larger number of atoms. The SQ-MBD approach offers conceptual insights into quantum fluctuations in molecular systems and enables direct coupling of collective plasmon-like MBD degrees of freedom with arbitrary environments, providing a tractable computational framework to treat dispersion interactions and polarization response in intricate systems.https://doi.org/10.1038/s41467-023-43785-z |
| spellingShingle | Matteo Gori Philip Kurian Alexandre Tkatchenko Second quantization of many-body dispersion interactions for chemical and biological systems Nature Communications |
| title | Second quantization of many-body dispersion interactions for chemical and biological systems |
| title_full | Second quantization of many-body dispersion interactions for chemical and biological systems |
| title_fullStr | Second quantization of many-body dispersion interactions for chemical and biological systems |
| title_full_unstemmed | Second quantization of many-body dispersion interactions for chemical and biological systems |
| title_short | Second quantization of many-body dispersion interactions for chemical and biological systems |
| title_sort | second quantization of many body dispersion interactions for chemical and biological systems |
| url | https://doi.org/10.1038/s41467-023-43785-z |
| work_keys_str_mv | AT matteogori secondquantizationofmanybodydispersioninteractionsforchemicalandbiologicalsystems AT philipkurian secondquantizationofmanybodydispersioninteractionsforchemicalandbiologicalsystems AT alexandretkatchenko secondquantizationofmanybodydispersioninteractionsforchemicalandbiologicalsystems |