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.
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http://www.ncbi.nlm.nih.gov/pmc/articles/PMC10716193 | PMC |
http://dx.doi.org/10.1038/s41467-023-43785-z | DOI Listing |
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