TY - JOUR
T1 - Vibrational spectrum at a water surface
T2 - A hybrid quantum mechanics/molecular mechanics molecular dynamics approach
AU - Ishiyama, Tatsuya
AU - Takahashi, Hideaki
AU - Morita, Akihiro
PY - 2012/3/28
Y1 - 2012/3/28
N2 - A hybrid quantum mechanics/molecular mechanics (QM/MM) molecular dynamics (MD) simulation is applied to the calculation of surface orientational structure and vibrational spectrum (second-order nonlinear susceptibility) at the vapor/water interface for the first time. The surface orientational structure of the QM water molecules is consistent with the previous MD studies, and the calculated susceptibility reproduces the experimentally reported one, supporting the previous results using the classical force field MD simulation. The present QM/MM MD simulation also demonstrates that the positive sign of the imaginary part of the second-order nonlinear susceptibility at the lower hydrogen bonding OH frequency region originates not from individual molecular orientational structure, but from cooperative electronic structure through the hydrogen bonding network.
AB - A hybrid quantum mechanics/molecular mechanics (QM/MM) molecular dynamics (MD) simulation is applied to the calculation of surface orientational structure and vibrational spectrum (second-order nonlinear susceptibility) at the vapor/water interface for the first time. The surface orientational structure of the QM water molecules is consistent with the previous MD studies, and the calculated susceptibility reproduces the experimentally reported one, supporting the previous results using the classical force field MD simulation. The present QM/MM MD simulation also demonstrates that the positive sign of the imaginary part of the second-order nonlinear susceptibility at the lower hydrogen bonding OH frequency region originates not from individual molecular orientational structure, but from cooperative electronic structure through the hydrogen bonding network.
UR - http://www.scopus.com/inward/record.url?scp=84858166092&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=84858166092&partnerID=8YFLogxK
U2 - 10.1088/0953-8984/24/12/124107
DO - 10.1088/0953-8984/24/12/124107
M3 - Article
C2 - 22395143
AN - SCOPUS:84858166092
VL - 24
JO - Journal of Physics Condensed Matter
JF - Journal of Physics Condensed Matter
SN - 0953-8984
IS - 12
M1 - 124107
ER -