On the Range of Water Structure Models Compatible with X-ray and Neutron Diffraction Data
2009 (English)In: Journal of Physical Chemistry B, ISSN 1520-6106, E-ISSN 1520-5207, Vol. 113, no 18, 6246-6255 p.Article in journal (Refereed) Published
We use the reverse Monte Carlo (RMC) method to critically evaluate the structural information content of diffraction data on bulk water by ﬁtting simultaneously or separately to X-ray and neutron data; the O-H and H-H, but not the O-O, pair-correlation functions (PCFs) are well-described by the neutron data alone. Enforcing at the same time different H-bonding constraints, we generate four topologically different structure models of liquid water, including a simple mixture model, that all equally well reproduce the diffraction data. Although earlier work [Leetmaa, M.; et al. J. Chem. Phys. 2008, 129, 084502] has focused on tetrahedrality in the H-bond network in liquid water, we show here that, even for the O-O-O three-body correlation, tetrahedrality is not strictly deﬁned by the data. We analyze how well two popular MD models (TIP4P-pol2 and SPC/E) reproduce the neutron data in q-space and ﬁnd differences in important aspects from the experiment. From the RMC ﬁts, we obtain pair-correlation functions (PCFs) that are in optimal agreement with the diffraction data but still show a surprisingly strong variability both in position and height of the ﬁrst intermolecular (H-bonding) O-H peak. We conclude that, although diffraction data impose important constraints on the range of possible water structures, additional data are needed to narrow the range of possible structure models.
Place, publisher, year, edition, pages
2009. Vol. 113, no 18, 6246-6255 p.
IdentifiersURN: urn:nbn:se:su:diva-31446DOI: 10.1021/jp9007619ISI: 000265687500010OAI: oai:DiVA.org:su-31446DiVA: diva2:277034