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The Journal of Chemical Physics
Article . 2023 . Peer-reviewed
License: CC BY
Data sources: Crossref
https://dx.doi.org/10.15488/17...
Article . 2023
License: CC BY
Data sources: Datacite
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Vibrational embedding theory

Authors: Janine Hellmers; Carolin König;

Vibrational embedding theory

Abstract

We suggest a consistent framework for the embedding of reduced-space correlated vibrational wave functions in a potential of the remaining modes and generalize this concept to arbitrary many subspaces. We present an implementation of this framework for vibrational coupled-cluster theory and response treatments. For C=O stretches of small molecules, we show that the embedded treatment accelerates convergence for enlarging subsets. For the water dimer and trimer as well as a water wire in bacteriorhodopsin, we investigate different partitioning schemes for the embedding approach: In the local partitioning of the vibrations, the modes dominated by motions in the same spatial region are correlated, whereas in the energy-based partitioning, modes of similar fundamental frequencies are correlated. In most cases, we obtain better agreement with superset reference results for the local partitioning than for energy-based partitioning. This work represents an important step toward multi-level methodologies in vibrational-structure theory required for its application to sizable (bio-)molecular systems.

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Keywords

Self consistent field methods, Dewey Decimal Classification::500 | Naturwissenschaften::540 | Chemie, Coupled-cluster methods, Potential energy surfaces, Vibrational spectra, Quantum chemical calculations, Configuration interaction, Dewey Decimal Classification::500 | Naturwissenschaften::530 | Physik, Multiscale methods, Linear response, Quantum chemistry computer programs

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selected citations
These citations are derived from selected sources.
This is an alternative to the "Influence" indicator, which also reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).
BIP!Citations provided by BIP!
popularity
This indicator reflects the "current" impact/attention (the "hype") of an article in the research community at large, based on the underlying citation network.
BIP!Popularity provided by BIP!
influence
This indicator reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).
BIP!Influence provided by BIP!
impulse
This indicator reflects the initial momentum of an article directly after its publication, based on the underlying citation network.
BIP!Impulse provided by BIP!
6
Top 10%
Average
Top 10%
hybrid