Dynamics of Water Molecules and Ions in Concentrated Lithium Chloride Solutions Probed with Ultrafast 2D IR Spectroscopy

Yuan, Rongfeng; Fayer, Michael D.

doi:10.1021/acs.jpcb.9b06038

Title: Dynamics of Water Molecules and Ions in Concentrated Lithium Chloride Solutions Probed with Ultrafast 2D IR Spectroscopy

Journal Article · Sun Aug 11 00:00:00 EDT 2019 · Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry

DOI:https://doi.org/10.1021/acs.jpcb.9b06038· OSTI ID:1782467

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Stanford Univ., CA (United States)

Water and ions dynamics in concentrated LiCl solutions were studied using ultrafast 2D IR spectroscopy with the methylthiocyanate (MeSCN) CN stretch as the vibrational probe. The IR absorption spectrum of MeSCN has two peaks, one peak for water-associated with the nitrogen lone pair of MeSCN (W) and the other peak corresponding to Li+ associated with the lone pair (L). To extract the spectral diffusion (structural dynamics) of W and L species, we developed a method that isolates the peak of interest by subtracting the 2D Gaussian proxies of multiple interfering peaks. Center line slope data (CLS – normalized frequency-frequency correlation function) for 2D bands from the W and L are fit with triexponential functions. The fastest component (1.1~1.6 ps) is assigned to local hydrogen bond length fluctuations. The intermediate timescale (~4.0 ps) corresponds to the hydrogen bond network rearrangement. The slowest component decays in ~40 ps and corresponds to ion pair and ion cluster dynamics. The very similar W and L spectral diffusion indicates that the motions of the water and ions are strongly coupled. Orientational relaxations of the W and L species were extracted using a new method to eliminate the effects of overlapping peaks. The results show that MeSCN bound to water undergoes orientational relaxation significantly faster than MeSCN bound to Li+. The orientational and spectral diffusion results are compared. A Stark coupling model is used to extract the rms average electric field caused by the ion clouds along the CN moiety as a function of concentration.

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Research Organization:: Stanford Univ., CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: FG02-84ER13251

OSTI ID:: 1782467

Alternate ID(s):: OSTI ID: 1782468

Journal Information:: Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry, Vol. 123, Issue 35; Related Information: Dynamics of Water Molecules and Ions in Concentrated Lithium Chloride SolutionsProbed with Ultrafast 2D IR SpectroscopyRongfeng Yuan, and Michael Fayer*Department of ChemistryStanford University, Stanford, CA 94305*phone: 650 723-4446; email: fayer@stanford.edu; ISSN 1520-6106

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 31 works

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Title: Dynamics of Water Molecules and Ions in Concentrated Lithium Chloride Solutions Probed with Ultrafast 2D IR Spectroscopy

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