Abstract
We analyze the short-time dynamics of 'cyclic' and 'branched' water tetramers after an ionization event, with the aid of a scheme that partitions the kinetic energy of a solute plus solvent system into separate solute and solvent (or bath) contributions, using instantaneous internal coordinates and atomic velocities. The analysis supports the partitioning of the tetrameric systems into two subsystems, a 'reactive trimer' and a 'solvent' molecule. The partitioned kinetic energy exhibits two features, a broad peak assigned to the interaction between the two sub-systems and a sharper peak arising from the proton transfer that occurs upon ionization. It is found that the stability of the hydroxyl radical formed upon ionization is sensitive to the configuration of the water molecules around the ionized water at the moment of the ionization event.
| Original language | English |
|---|---|
| Pages (from-to) | 2033-2042 |
| Number of pages | 10 |
| Journal | Physical Chemistry Chemical Physics |
| Volume | 10 |
| Issue number | 15 |
| DOIs | |
| Publication status | Published - 2008 |
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ASJC Scopus subject areas
- Physical and Theoretical Chemistry
- Atomic and Molecular Physics, and Optics
Cite this
Application of a kinetic energy partitioning scheme for ab initio molecular dynamics to reactions associated with ionization in water tetramers. / Furuhama, Ayako; Dupuis, Michel; Hirao, Kimihiko.
In: Physical Chemistry Chemical Physics, Vol. 10, No. 15, 2008, p. 2033-2042.Research output: Contribution to journal › Article
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TY - JOUR
T1 - Application of a kinetic energy partitioning scheme for ab initio molecular dynamics to reactions associated with ionization in water tetramers
AU - Furuhama, Ayako
AU - Dupuis, Michel
AU - Hirao, Kimihiko
PY - 2008
Y1 - 2008
N2 - We analyze the short-time dynamics of 'cyclic' and 'branched' water tetramers after an ionization event, with the aid of a scheme that partitions the kinetic energy of a solute plus solvent system into separate solute and solvent (or bath) contributions, using instantaneous internal coordinates and atomic velocities. The analysis supports the partitioning of the tetrameric systems into two subsystems, a 'reactive trimer' and a 'solvent' molecule. The partitioned kinetic energy exhibits two features, a broad peak assigned to the interaction between the two sub-systems and a sharper peak arising from the proton transfer that occurs upon ionization. It is found that the stability of the hydroxyl radical formed upon ionization is sensitive to the configuration of the water molecules around the ionized water at the moment of the ionization event.
AB - We analyze the short-time dynamics of 'cyclic' and 'branched' water tetramers after an ionization event, with the aid of a scheme that partitions the kinetic energy of a solute plus solvent system into separate solute and solvent (or bath) contributions, using instantaneous internal coordinates and atomic velocities. The analysis supports the partitioning of the tetrameric systems into two subsystems, a 'reactive trimer' and a 'solvent' molecule. The partitioned kinetic energy exhibits two features, a broad peak assigned to the interaction between the two sub-systems and a sharper peak arising from the proton transfer that occurs upon ionization. It is found that the stability of the hydroxyl radical formed upon ionization is sensitive to the configuration of the water molecules around the ionized water at the moment of the ionization event.
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U2 - 10.1039/b713456h
DO - 10.1039/b713456h
M3 - Article
VL - 10
SP - 2033
EP - 2042
JO - Physical Chemistry Chemical Physics
JF - Physical Chemistry Chemical Physics
SN - 1463-9076
IS - 15
ER -