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Title: Water is not a dynamic polydisperse branched polymer

Abstract

In PNAS, Naserifar and Goddard report that their RexPoN water model under ambient conditions comprises a “dynamic polydisperse branched polymer,” which they speculate explains the existence of the liquid–liquid critical point (LLCP) in the supercooled region. The observable they rely on to support this is the oxygen–oxygen radial distribution function, gOO, from a dated neutron scattering experiment. While it is well known that neutron scattering is almost exclusively sensitive to hydrogen correlations, and gOO is more reliably obtained from X-ray scattering, they make the unsupported statement that “the most reliable gOO curve is neutron where there is no inference from electrons”. Yet, two X-ray gOO curves in figure 1B of ref. 1 are from a joint neutron X-ray analysis (X-ray1) and neutron scattering study (X-ray3). Given the importance that Naserifar and Goddard place on gOO, it is evident that their RexPoN model is in disagreement with the most reliable estimate of X-ray2.

Authors:
ORCiD logo [1];  [2]
  1. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Univ. of California, San Diego, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1561929
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Volume: 116; Journal Issue: 27; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Head-Gordon, Teresa, and Paesani, Francesco. Water is not a dynamic polydisperse branched polymer. United States: N. p., 2019. Web. doi:10.1073/pnas.1902031116.
Head-Gordon, Teresa, & Paesani, Francesco. Water is not a dynamic polydisperse branched polymer. United States. doi:10.1073/pnas.1902031116.
Head-Gordon, Teresa, and Paesani, Francesco. Tue . "Water is not a dynamic polydisperse branched polymer". United States. doi:10.1073/pnas.1902031116.
@article{osti_1561929,
title = {Water is not a dynamic polydisperse branched polymer},
author = {Head-Gordon, Teresa and Paesani, Francesco},
abstractNote = {In PNAS, Naserifar and Goddard report that their RexPoN water model under ambient conditions comprises a “dynamic polydisperse branched polymer,” which they speculate explains the existence of the liquid–liquid critical point (LLCP) in the supercooled region. The observable they rely on to support this is the oxygen–oxygen radial distribution function, gOO, from a dated neutron scattering experiment. While it is well known that neutron scattering is almost exclusively sensitive to hydrogen correlations, and gOO is more reliably obtained from X-ray scattering, they make the unsupported statement that “the most reliable gOO curve is neutron where there is no inference from electrons”. Yet, two X-ray gOO curves in figure 1B of ref. 1 are from a joint neutron X-ray analysis (X-ray1) and neutron scattering study (X-ray3). Given the importance that Naserifar and Goddard place on gOO, it is evident that their RexPoN model is in disagreement with the most reliable estimate of X-ray2.},
doi = {10.1073/pnas.1902031116},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 27,
volume = 116,
place = {United States},
year = {2019},
month = {6}
}

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