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Momentum distribution, vibrational dynamics, and the potential of mean force in ice

2011; American Physical Society; Volume: 83; Issue: 22 Linguagem: Inglês

10.1103/physrevb.83.220302

1550-235X

Lin Lin, Joseph A. Morrone, Roberto Car, Michele Parrinello,

Advanced Chemical Physics Studies

By analyzing the momentum distribution obtained from path integral and phonon calculations we find that the protons in hexagonal ice experience an anisotropic quasiharmonic effective potential with three distinct principal frequencies that reflect molecular orientation. Due to the importance of anisotropy, anharmonic features of the environment cannot be extracted from existing experimental distributions that involve the spherical average. The full directional distribution is required, and we give a theoretical prediction for this quantity that could be verified in future experiments. Within the quasiharmonic context, anharmonicity in the ground-state dynamics of the proton is substantial and has quantal origin, a finding that impacts the interpretation of several spectroscopies.