Second quantization of many-body dispersion interactions for chemical and biological systems.

Chemistry (all); Biochemistry, Genetics and Molecular Biology (all); Physics and Astronomy (all); General Physics and Astronomy; General Biochemistry, Genetics and Molecular Biology; General Chemistry; Multidisciplinary

Abstract :

[en] 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.

Disciplines :

Physics

Author, co-author :

GORI, Matteo ; University of Luxembourg > Faculty of Science, Technology and Medicine (FSTM) > Department of Physics and Materials Science (DPHYMS) ; Quantum Biology Laboratory, Howard University, Washington, DC, 20060, USA. matteo.gori@uni.lu

Kurian, Philip ; Quantum Biology Laboratory, Howard University, Washington, DC, 20060, USA. pkurian@howard.edu

TKATCHENKO, Alexandre ; University of Luxembourg > Faculty of Science, Technology and Medicine (FSTM) > Department of Physics and Materials Science (DPHYMS)

External co-authors :

yes

Language :

English

Title :

Second quantization of many-body dispersion interactions for chemical and biological systems.

Publication date :

12 December 2023

Journal title :

Nature Communications

eISSN :

2041-1723

Publisher :

Nature Research, England

Volume :

Issue :

Pages :

8218

Peer reviewed :

Peer Reviewed verified by ORBi

Additional URL :

https://www.nature.com/articles/s41467-023-43785-z.pdf

Funders :

Fonds National de la Recherche Luxembourg
European Research Council

Funding text :

M.G. and A.T. acknowledge support from the European Research Council (ERC Advanced Grant “FITMOL”) and Fonds National de la Recherche Luxembourg (FNR CORE grant BroadApp C20/MS/14769845). M.G. would like to thank Mario Galante, Marco Pezzutto, and Martin Stöhr for their helpful suggestions. P.K. acknowledges support from the Alfred P. Sloan Foundation (Matter-to-Life program), the U.S. National Science Foundation (Quantum Leap Challenge Institutes and Research Coordination Network programs), the Whole Genome Science Foundation, and the U.S.–Italy Fulbright Commission. The authors would also like to acknowledge discussions at the Institute for Pure and Applied Mathematics, and valuable insights from Georgia Dunston, Marco Pettini, and Giuseppe Vitiello.M.G. and A.T. acknowledge support from the European Research Council (ERC Advanced Grant “FITMOL”) and Fonds National de la Recherche Luxembourg (FNR CORE grant BroadApp C20/MS/14769845). M.G. would like to thank Mario Galante, Marco Pezzutto, and Martin Stöhr for their helpful suggestions. P.K. acknowledges support from the Alfred P. Sloan Foundation (Matter-to-Life program), the U.S. National Science Foundation (Quantum Leap Challenge Institutes and Research Coordination Network programs), the Whole Genome Science Foundation, and the U.S.–Italy Fulbright Commission. The authors would also like to acknowledge discussions at the Institute for Pure and Applied Mathematics, and valuable insights from Georgia Dunston, Marco Pettini, and Giuseppe Vitiello.

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