Cavity molecular dynamics simulations of liquid water under vibrational ultrastrong coupling

Li, Tao E.; Subotnik, Joseph E.; Nitzan, Abraham

doi:10.1073/pnas.2009272117

Cavity molecular dynamics simulations of liquid water under vibrational ultrastrong coupling

Journal Article · Fri Jul 17 00:00:00 EDT 2020 · Proceedings of the National Academy of Sciences of the United States of America

DOI:https://doi.org/10.1073/pnas.2009272117· OSTI ID:1647756

^[1]; Subotnik, Joseph E. ^[2]; ^[3]

Univ. of Pennsylvania, Philadelphia, PA (United States); University fo Pennsylvania, Department of Chemistry
Univ. of Pennsylvania, Philadelphia, PA (United States)
Univ. of Pennsylvania, Philadelphia, PA (United States); Tel Aviv Univ., Ramat Aviv (Israel)

We simulate vibrational strong coupling (VSC) and vibrational ultrastrong coupling (V-USC) for liquid water with classical molecular dynamics simulations. When the cavity modes are resonantly coupled to the O–H stretch mode of liquid water, the infrared spectrum shows asymmetric Rabi splitting. The lower polariton (LP) may be suppressed or enhanced relative to the upper polariton (UP) depending on the frequency of the cavity mode. Furthermore, although the static properties and the translational diffusion of water are not changed under VSC or V-USC, we do find the modification of the orientational autocorrelation function of H₂O molecules especially under V-USC, which could play a role in ground-state chemistry.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of Pennsylvania, Philadelphia, PA (United States)

Sponsoring Organization:: Israel–US Binational Science Foundation; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; Vagelos Institute for Energy Science and Technology

Grant/Contract Number:: AC02-05CH11231; SC0019397

OSTI ID:: 1647756

Alternate ID(s):: OSTI ID: 1648119
OSTI ID: 1656850

Journal Information:: Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Issue: 31 Vol. 117; ISSN 1091-6490; ISSN 0027-8424

Publisher:: National Academy of SciencesCopyright Statement

Country of Publication:: United States

Language:: English

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