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Title: Dynamics in a Room-Temperature Ionic Liquid from the Cation Perspective: 2D IR Vibrational Echo Spectroscopy

Abstract

The dynamics of the room-temperature ionic liquid (RTIL) 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (BmimNTf2) were investigated with two-dimensional infrared (2D IR) vibrational echo spectroscopy and polarization selective pump–probe (PSPP) experiments. The CN stretch frequency of a modified Bmim+ cation (2-SeCN-Bmim+), in which a SeCN moiety was substituted onto the C-2 position of the imidazolium ring, was used as a vibrational probe. A major result of the 2D IR experiments is the observation of a long time scale structural spectral diffusion component of 600 ps in addition to short and intermediate time scales similar to those measured for selenocyanate anion (SeCN–) dissolved in BmimNTf2. In contrast to 2-SeCN-Bmim+, SeCN– samples its inhomogeneous line width nearly an order of magnitude faster than the complete structural randomization time of neat BmimNTf2 liquid (870 ± 20 ps) measured with optical heterodyne-detected optical Kerr effect (OHD-OKE) experiments. The orientational correlation function obtained from PSPP experiments on 2-SeCN-Bmim+ exhibits two periods of restricted angular diffusion (wobbling-in-a-cone) followed by complete orientational randomization on a time scale of 900 ± 20 ps, significantly slower than observed for SeCN– but identical within experimental error to the complete structural randomization time of BmimNTf2. In conclusion, the experiments indicate that 2-SeCN-Bmim+ is sensitive tomore » local motions of the ionic region that influence the spectral diffusion and reorientation of small, anionic, and neutral molecules as well as significantly slower, longer-range fluctuations that are responsible for complete randomization of the liquid structure.« less

Authors:
 [1];  [1]; ORCiD logo [1];  [1]; ORCiD logo [1]
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  1. Stanford Univ., CA (United States)
Publication Date:
Research Org.:
Stanford Univ., CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
OSTI Identifier:
1797769
Grant/Contract Number:  
FG02-84ER13251
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 139; Journal Issue: 6; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; 14 SOLAR ENERGY; Liquids; Diffusion; Solvents; Cations; Probes

Citation Formats

Yamada, Steven A., Bailey, Heather E., Tamimi, Amr, Li, Chunya, and Fayer, Michael D. Dynamics in a Room-Temperature Ionic Liquid from the Cation Perspective: 2D IR Vibrational Echo Spectroscopy. United States: N. p., 2017. Web. doi:10.1021/jacs.6b12011.
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Yamada, Steven A., Bailey, Heather E., Tamimi, Amr, Li, Chunya, & Fayer, Michael D. Dynamics in a Room-Temperature Ionic Liquid from the Cation Perspective: 2D IR Vibrational Echo Spectroscopy. United States. https://doi.org/10.1021/jacs.6b12011
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Yamada, Steven A., Bailey, Heather E., Tamimi, Amr, Li, Chunya, and Fayer, Michael D. Wed . "Dynamics in a Room-Temperature Ionic Liquid from the Cation Perspective: 2D IR Vibrational Echo Spectroscopy". United States. https://doi.org/10.1021/jacs.6b12011. https://www.osti.gov/servlets/purl/1797769.
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@article{osti_1797769,
title = {Dynamics in a Room-Temperature Ionic Liquid from the Cation Perspective: 2D IR Vibrational Echo Spectroscopy},
author = {Yamada, Steven A. and Bailey, Heather E. and Tamimi, Amr and Li, Chunya and Fayer, Michael D.},
abstractNote = {The dynamics of the room-temperature ionic liquid (RTIL) 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (BmimNTf2) were investigated with two-dimensional infrared (2D IR) vibrational echo spectroscopy and polarization selective pump–probe (PSPP) experiments. The CN stretch frequency of a modified Bmim+ cation (2-SeCN-Bmim+), in which a SeCN moiety was substituted onto the C-2 position of the imidazolium ring, was used as a vibrational probe. A major result of the 2D IR experiments is the observation of a long time scale structural spectral diffusion component of 600 ps in addition to short and intermediate time scales similar to those measured for selenocyanate anion (SeCN–) dissolved in BmimNTf2. In contrast to 2-SeCN-Bmim+, SeCN– samples its inhomogeneous line width nearly an order of magnitude faster than the complete structural randomization time of neat BmimNTf2 liquid (870 ± 20 ps) measured with optical heterodyne-detected optical Kerr effect (OHD-OKE) experiments. The orientational correlation function obtained from PSPP experiments on 2-SeCN-Bmim+ exhibits two periods of restricted angular diffusion (wobbling-in-a-cone) followed by complete orientational randomization on a time scale of 900 ± 20 ps, significantly slower than observed for SeCN– but identical within experimental error to the complete structural randomization time of BmimNTf2. In conclusion, the experiments indicate that 2-SeCN-Bmim+ is sensitive to local motions of the ionic region that influence the spectral diffusion and reorientation of small, anionic, and neutral molecules as well as significantly slower, longer-range fluctuations that are responsible for complete randomization of the liquid structure.},
doi = {10.1021/jacs.6b12011},
journal = {Journal of the American Chemical Society},
number = 6,
volume = 139,
place = {United States},
year = {Wed Jan 18 00:00:00 EST 2017},
month = {Wed Jan 18 00:00:00 EST 2017}
}
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https://doi.org/10.1021/jacs.6b12011
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