Vibrational dynamics of aqueous hydroxide solutions probed using broadband 2DIR spectroscopy

Mandal, Aritra; Tokmakoff, Andrei

doi:10.1063/1.4935174

Title: Vibrational dynamics of aqueous hydroxide solutions probed using broadband 2DIR spectroscopy

Journal Article · Mon Nov 16 00:00:00 EST 2015 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4935174· OSTI ID:1469646

Mandal, Aritra ^[1]; Tokmakoff, Andrei ^[2]

Univ. of Chicago, IL (United States); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Univ. of Chicago, IL (United States)

We employed ultrafast transient absorption and broadband 2DIR spectroscopy to study the vibrational dynamics of aqueous hydroxide solutions by exciting the O–H stretch vibrations of the strongly hydrogen-bonded hydroxide solvation shell water and probing the continuum absorption of the solvated ion between 1500 and 3800 cm^-1. We observe rapid vibrational relaxation processes on 150–250 fs time scales across the entire probed spectral region as well as slower vibrational dynamics on 1–2 ps time scales. Furthermore, the O–H stretch excitation loses its frequency memory in 180 fs, and vibrational energy exchange between bulk-like water vibrations and hydroxide-associated water vibrations occurs in ~200 fs. The fast dynamics in this system originate in strong nonlinear coupling between intra- and intermolecular vibrations and are explained in terms of non-adiabatic vibrational relaxation. These measurements indicate that the vibrational dynamics of the aqueous hydroxide complex are faster than the time scales reported for long-range transport of protons in aqueous hydroxide solutions.

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Research Organization:: Univ. of Chicago, IL (United States)

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

Grant/Contract Number:: SC0011456; SC0014305

OSTI ID:: 1469646

Alternate ID(s):: OSTI ID: 1226104

Journal Information:: Journal of Chemical Physics, Vol. 143, Issue 19; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 19 works

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