Ultrafast vibrational dynamics of a trigonal planar anionic probe in ionic liquids (ILs): A two-dimensional infrared (2DIR) spectroscopic investigation

Guchhait, Biswajit; Tibbetts, Clara A.; Tracy, Kathryn M.; Luther, Bradley M.; Krummel, Amber T.

doi:10.1063/1.5141751

Title: Ultrafast vibrational dynamics of a trigonal planar anionic probe in ionic liquids (ILs): A two-dimensional infrared (2DIR) spectroscopic investigation

Journal Article · Wed Apr 22 00:00:00 EDT 2020 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.5141751· OSTI ID:1802839

Guchhait, Biswajit ^[1]; Tibbetts, Clara A. ^[2]; Tracy, Kathryn M. ^[2]; Luther, Bradley M. ^[2];

^[2]

Colorado State Univ., Fort Collins, CO (United States); Shiv Nadar Univ., Dadri (India)
Colorado State Univ., Fort Collins, CO (United States)

A major impediment limiting the widespread application of ionic liquids (ILs) is their high shear viscosity. Incorporation of a tricyanomethanide (TCM^-) anion in ILs leads to low shear viscosity and improvement of several characteristics suitable for large scale applications. However, properties including interactions of TCM^- with the local environment and dynamics of TCM^- have not been thoroughly investigated. Herein, we have studied the ultrafast dynamics of TCM^- in several imidazolium ILs using linear IR and two-dimensional infrared spectroscopy techniques. The spectral diffusion dynamics of the CN stretching modes of TCM^- in all ILs exhibit a nonexponential behavior with a short time component of ~2 ps and a long time component spanning ~9 ps to 14 ps. The TCM^- vibrational probe reports a significantly faster relaxation of ILs compared to those observed previously using linear vibrational probes, such as thiocyanate and selenocyanate. Our results indicate a rapid relaxation of the local ion-cage structure embedding the vibrational probe in the ILs. The faster relaxation suggests that the lifetime of the local ion-cage structure decreases in the presence of TCM^- in the ILs. Linear IR spectroscopic results show that the hydrogen-bonding interaction between TCM^- and imidazolium cations in ILs is much weaker. Shorter ion-cage lifetimes together with weaker hydrogen-bonding interactions account for the low shear viscosity of TCM^- based ILs compared to commonly used ILs. In addition, this work demonstrates that TCM^- can be used as a potential vibrational reporter to study the structure and dynamics of ILs and other molecular systems.

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Research Organization:: Colorado State Univ., Fort Collins, CO (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: SC0016137

OSTI ID:: 1802839

Alternate ID(s):: OSTI ID: 1615691; OSTI ID: 2311837

Journal Information:: Journal of Chemical Physics, Vol. 152, Issue 16; ISSN 0021-9606

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

Country of Publication:: United States

Language:: English

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Cited by: 5 works

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Title: Ultrafast vibrational dynamics of a trigonal planar anionic probe in ionic liquids (ILs): A two-dimensional infrared (2DIR) spectroscopic investigation

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