4.7 Article

Decoupling charge transport from the structural dynamics in room temperature ionic liquids

Journal

JOURNAL OF CHEMICAL PHYSICS
Volume 135, Issue 11, Pages -

Publisher

AMER INST PHYSICS
DOI: 10.1063/1.3638269

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Funding

  1. National Science Foundation (NSF) [DMR-1059562]
  2. Division of Materials Sciences and Engineering, (U.S.) Department of Energy (DOE) Office of Basic Energy Sciences
  3. ORNL [LOIS 5843]
  4. Russian Federation for Basic Research (RFBR) [09-02-01297a]

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Light scattering and dielectric spectroscopy measurements were performed on the room temperature ionic liquid (RTIL) [C4mim][NTf2] in a broad temperature and frequency range. Ionic conductivity was used to estimate self-diffusion of ions, while light scattering was used to study structural relaxation. We demonstrate that the ionic diffusion decouples from the structural relaxation process as the temperature of the sample decreases toward T-g. The strength of the decoupling appears to be significantly lower than that expected for a supercooled liquid of similar fragility. The structural relaxation process in the RTIL follows well the high-temperature mode coupling theory (MCT) scenario. Using the MCT analysis we estimated the dynamic crossover temperature in [C4mim][NTf2] to be T-c similar to 225 +/- 5 K. However, our analysis reveals no sign of the dynamic crossover in the ionic diffusion process. (C) 2011 American Institute of Physics. [doi:10.1063/1.3638269]

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