TY - JOUR
T1 - Anisotropy of the Proton Momentum Distribution in Water
AU - Kapil, Venkat
AU - Cuzzocrea, Alice
AU - Ceriotti, Michele
N1 - Funding Information:
M.C. and V.K. acknowledge financial support by the Swiss National Science Foundation (project ID 200021-159896) and computational time from CSCS under the project IDs s466, s553, and s618. A.C. was supported by a MARVEL INSPIRE Potentials Master’s Fellowship. MARVEL is a National Center of Competence in Research funded by the Swiss National Science Foundation. This work was also supported by EPFL through the use of the facilities of its Scientific IT and Application Support Center. We would like to thank C. Andreani, R. Senesi, and G. Romanelli for insightful discussion and for sharing unpublished experimental results.
Publisher Copyright:
© 2018 American Chemical Society.
PY - 2018/6/7
Y1 - 2018/6/7
N2 - One of the many peculiar properties of water is the pronounced deviation of the proton momentum distribution from Maxwell-Boltzmann behavior. This deviation from the classical limit is a manifestation of the quantum mechanical nature of protons. Its extent, which can be probed directly by deep inelastic neutron scattering experiments, gives important insight on the potential of mean force felt by H atoms. The determination of the full distribution of particle momenta, however, is a real tour de force for both experiments and theory, which has led to unresolved discrepancies between the two. In this study, we present comprehensive, fully converged momentum distributions for water at several thermodynamic state points, focusing on the components that cannot be described in terms of a scalar contribution to the quantum kinetic energy, and providing a benchmark that can serve as a reference for future simulations and experiments. In doing so, we also introduce a number of technical developments that simplify and accelerate greatly the calculation of momentum distributions by means of atomistic simulations.
AB - One of the many peculiar properties of water is the pronounced deviation of the proton momentum distribution from Maxwell-Boltzmann behavior. This deviation from the classical limit is a manifestation of the quantum mechanical nature of protons. Its extent, which can be probed directly by deep inelastic neutron scattering experiments, gives important insight on the potential of mean force felt by H atoms. The determination of the full distribution of particle momenta, however, is a real tour de force for both experiments and theory, which has led to unresolved discrepancies between the two. In this study, we present comprehensive, fully converged momentum distributions for water at several thermodynamic state points, focusing on the components that cannot be described in terms of a scalar contribution to the quantum kinetic energy, and providing a benchmark that can serve as a reference for future simulations and experiments. In doing so, we also introduce a number of technical developments that simplify and accelerate greatly the calculation of momentum distributions by means of atomistic simulations.
UR - http://www.scopus.com/inward/record.url?scp=85046806450&partnerID=8YFLogxK
U2 - 10.1021/acs.jpcb.8b03896
DO - 10.1021/acs.jpcb.8b03896
M3 - Article
C2 - 29733649
AN - SCOPUS:85046806450
SN - 1520-6106
VL - 122
SP - 6048
EP - 6054
JO - The Journal of physical chemistry B
JF - The Journal of physical chemistry B
IS - 22
ER -