Journal
CHEMICAL PHYSICS LETTERS
Volume 516, Issue 4-6, Pages 115-124Publisher
ELSEVIER SCIENCE BV
DOI: 10.1016/j.cplett.2011.08.027
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Funding
- NDSEG
- NSF-GRFP
- NSF Science and Technology Center of Advanced Materials for Purification of Water with Systems (Water CAMPWS) [CTS-0120978]
- Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division of the US Department of Energy [DE-AC02-05CH11231]
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Recent molecular simulations of liquid interfaces yield surface sum-frequency vibrational spectra that can be highly sensitive to the seemingly-arbitrary choice of molecular center in the calculation method. We show that the ambiguity arises because widely-used approaches, focusing exclusively on electric-dipole contributions from the surface, neglect coordinate-dependent quadrupole-order contributions of comparable magnitude from the bulk. The correct calculation includes both surface and bulk responses. With a judicious choice of molecular center, however, it may be possible to minimize the bulk contribution, allowing the surface-only calculation to produce a reasonably accurate spectrum. We use water as an example to elucidate the problem. (C) 2011 Elsevier B.V. All rights reserved.
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