TY - JOUR
T1 - Free Energy Decomposition Analysis Based on the Fragment Molecular Orbital Method
AU - Fedorov, Dmitri G.
AU - Nakamura, Taiji
N1 - Funding Information:
The financial support by JSPS KAKENHI (Grant 19H02682) is gratefully acknowledged.
Publisher Copyright:
© 2022 American Chemical Society
PY - 2022/2/17
Y1 - 2022/2/17
N2 - A decomposition of the free energy is developed in the many-body expansion framework of the fragment molecular orbital (FMO) method combined with umbrella sampling molecular dynamics (MD). In FMO/MD simulations, performed with density-functional tight-binding and periodic boundary conditions, all atoms are treated quantum mechanically. The free energy is computed and decomposed for a series of SN2 Menshutkin reactions in water. The barrier lowering by the solvent is attributed to the competition between the solvent polarization and the solute-solvent interactions including charge transfer.
AB - A decomposition of the free energy is developed in the many-body expansion framework of the fragment molecular orbital (FMO) method combined with umbrella sampling molecular dynamics (MD). In FMO/MD simulations, performed with density-functional tight-binding and periodic boundary conditions, all atoms are treated quantum mechanically. The free energy is computed and decomposed for a series of SN2 Menshutkin reactions in water. The barrier lowering by the solvent is attributed to the competition between the solvent polarization and the solute-solvent interactions including charge transfer.
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U2 - 10.1021/acs.jpclett.2c00040
DO - 10.1021/acs.jpclett.2c00040
M3 - Article
C2 - 35142207
AN - SCOPUS:85124794938
SN - 1948-7185
VL - 13
SP - 1596
EP - 1601
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
IS - 6
ER -