Wang, Yanting and Hodas, Nathan O. and Jung, Yousung and Marcus, R. A. (2011) Microscopic structure and dynamics of air/water interface by computer simulations-comparison with sum-frequency generation experiments. Physical Chemistry Chemical Physics, 13 (12). pp. 5388-5393. ISSN 1463-9076 http://resolver.caltech.edu/CaltechAUTHORS:20110330-082835207
- Published Version
See Usage Policy.
Use this Persistent URL to link to this item: http://resolver.caltech.edu/CaltechAUTHORS:20110330-082835207
The air/water interface was simulated and the mode amplitudes and their ratios of the effective nonlinear sum-frequency generation (SFG) susceptibilities (A_(eff)'s) were calculated for the ssp, ppp, and sps polarization combinations and compared with experiments. By designating “surface-sensitive” free OH bonds on the water surface, many aspects of the SFG measurements were calculated and compared with those inferred from experiment. We calculate an average tilt angle close to the SFG observed value of 35, an average surface density of free OH bonds close to the experimental value of about 2.8 × 10^(18) m^(−2), computed ratios of A_(eff)'s that are very similar to those from the SFG experiment, and their absolute values that are in reasonable agreement with experiment. A one-parameter model was used to calculate these properties. The method utilizes results available from independent IR and Raman experiments to obtain some of the needed quantities, rather than calculating them ab initio. The present results provide microscopic information on water structure useful to applications such as in our recent theory of on-water heterogeneous catalysis.
|Additional Information:||© 2011 the Owner Societies. Received 2nd December 2010, Accepted 9th February 2011. It is a pleasure to dedicate this article to the master of surface phenomena, friend and colleague, John Albery, on the occasion of his 75th birthday. The various authors received their support from different sources and they are pleased to acknowledge this support. The One Hundred Talents Program of the Chinese Academy of Sciences, the Senior Visiting Scholar Program of the Chinese Academy of Sciences, the General Program of the National Natural Science Foundation of China (No. 10974208), WCU program (R31-2008-000-10055-0) through the National Research Foundation of Korea, the Biological Imaging Center of the Beckman Institute at California Institute of Technology, and also by the National Science Foundation, the Office of Naval Research, and the Army Research Office.|
|Usage Policy:||No commercial reproduction, distribution, display or performance rights in this work are provided.|
|Deposited By:||Tony Diaz|
|Deposited On:||30 Mar 2011 20:59|
|Last Modified:||26 Dec 2012 13:07|
Repository Staff Only: item control page