| Autor: |
Hellmers, Janine, König, Carolin |
| Předmět: |
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| Zdroj: |
Journal of Chemical Physics; 9/14/2023, Vol. 159 Issue 10, p1-15, 15p |
| Abstrakt: |
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. [ABSTRACT FROM AUTHOR] |
| Databáze: |
Complementary Index |
| Externí odkaz: |
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