Spatial and thermal signatures of α and β relaxations in glassy and glacial aliphatic ionic liquids
Abstract
The competition between Coulomb and van der Waals interactions brings forth unique dynamic features and broad applications to ionic liquids. Herein, we present a combined calorimetric, X-ray diffraction, incoherent elastic, and quasi-elastic neutron scattering study, over a wide temperature range (180–340 K), of the relaxational dynamics of the liquid, supercooled liquid, crystalline, glassy, and glacial states of two model ionic liquids: tributylmethylammonium (a good glass-former) and butyltrimethylammonium (a good crystal-former) cations and the bis(trifluoromethanesulfonyl)imide anion. In both systems, we observed two distinct relaxation processes. Finally, the Q-dependence of the respective relaxation time shows that the α-process is diffusive, while the β-process is modulated by the structure of the liquids.
- Authors:
-
- Univ. of Illinois at Urbana-Champaign, IL (United States); Univ. of Sao Paulo (Brazil)
- Univ. of Illinois at Urbana-Champaign, IL (United States)
- National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States); Univ. of Maryland, College Park, MD (United States)
- Univ. of Sao Paulo (Brazil)
- Publication Date:
- Research Org.:
- Univ. of Illinois at Urbana-Champaign, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC); FAPESP
- OSTI Identifier:
- 1612077
- Alternate Identifier(s):
- OSTI ID: 1506171
- Grant/Contract Number:
- SC0014084; 2016/24241-5; 2012/13119-3; SC0014804
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 150; Journal Issue: 14; Journal ID: ISSN 0021-9606
- Publisher:
- American Institute of Physics (AIP)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS; Chemistry; Physics; Crystallography; Glass transitions; Neutron scattering; Thermodynamic measurements and instrumentation; X-ray diffraction; Ionic liquid; Van der Waals forces; Diffusion; Differential scanning calorimetry; Neutron spectroscopy
Citation Formats
Lima, Thamires A., Li, Zhixia, Tyagi, Madhusudan, Ribeiro, Mauro C. C., and Z, Y. Spatial and thermal signatures of α and β relaxations in glassy and glacial aliphatic ionic liquids. United States: N. p., 2019.
Web. doi:10.1063/1.5081684.
Lima, Thamires A., Li, Zhixia, Tyagi, Madhusudan, Ribeiro, Mauro C. C., & Z, Y. Spatial and thermal signatures of α and β relaxations in glassy and glacial aliphatic ionic liquids. United States. https://doi.org/10.1063/1.5081684
Lima, Thamires A., Li, Zhixia, Tyagi, Madhusudan, Ribeiro, Mauro C. C., and Z, Y. Wed .
"Spatial and thermal signatures of α and β relaxations in glassy and glacial aliphatic ionic liquids". United States. https://doi.org/10.1063/1.5081684. https://www.osti.gov/servlets/purl/1612077.
@article{osti_1612077,
title = {Spatial and thermal signatures of α and β relaxations in glassy and glacial aliphatic ionic liquids},
author = {Lima, Thamires A. and Li, Zhixia and Tyagi, Madhusudan and Ribeiro, Mauro C. C. and Z, Y.},
abstractNote = {The competition between Coulomb and van der Waals interactions brings forth unique dynamic features and broad applications to ionic liquids. Herein, we present a combined calorimetric, X-ray diffraction, incoherent elastic, and quasi-elastic neutron scattering study, over a wide temperature range (180–340 K), of the relaxational dynamics of the liquid, supercooled liquid, crystalline, glassy, and glacial states of two model ionic liquids: tributylmethylammonium (a good glass-former) and butyltrimethylammonium (a good crystal-former) cations and the bis(trifluoromethanesulfonyl)imide anion. In both systems, we observed two distinct relaxation processes. Finally, the Q-dependence of the respective relaxation time shows that the α-process is diffusive, while the β-process is modulated by the structure of the liquids.},
doi = {10.1063/1.5081684},
journal = {Journal of Chemical Physics},
number = 14,
volume = 150,
place = {United States},
year = {Wed Apr 10 00:00:00 EDT 2019},
month = {Wed Apr 10 00:00:00 EDT 2019}
}
Web of Science
Works referenced in this record:
Classification of secondary relaxation in glass-formers based on dynamic properties
journal, January 2004
- Ngai, K. L.; Paluch, M.
- The Journal of Chemical Physics, Vol. 120, Issue 2
Thermophysical properties of sulfonium- and ammonium-based ionic liquids
journal, November 2014
- Bhattacharjee, Arijit; Luís, Andreia; Santos, João H.
- Fluid Phase Equilibria, Vol. 381
Quasielastic neutron scattering characterization of the relaxation processes in a room temperature ionic liquid
journal, October 2003
- Triolo, Alessandro; Russina, Olga; Arrighi, Valeria
- The Journal of Chemical Physics, Vol. 119, Issue 16
DAVE: A Comprehensive Software Suite for the Reduction, Visualization, and Analysis of Low Energy Neutron Spectroscopic Data
journal, November 2009
- Azuah, Richard Tumanjong; Kneller, Larry R.; Qiu, Yiming
- Journal of Research of the National Institute of Standards and Technology, Vol. 114, Issue 6
Localized molecular motions of β-relaxation and its energy landscape
journal, September 2002
- Johari, G. P.
- Journal of Non-Crystalline Solids, Vol. 307-310
Dielectric Relaxation and Solvation Dynamics in a Room-Temperature Ionic Liquid: Temperature Dependence
journal, September 2013
- Shim, Youngseon; Kim, Hyung J.
- The Journal of Physical Chemistry B, Vol. 117, Issue 39
Odd–Even Glass Transition Temperatures in Network-Forming Ionic Glass Homologue
journal, January 2014
- Yang, Ke; Tyagi, Madhusudan; Moore, Jeffrey S.
- Journal of the American Chemical Society, Vol. 136, Issue 4
Atomic Dynamics in Simple Liquid: de Gennes Narrowing Revisited
journal, March 2018
- Wu, Bin; Iwashita, Takuya; Egami, Takeshi
- Physical Review Letters, Vol. 120, Issue 13
Applications of ionic liquids in the chemical industry
journal, January 2008
- Plechkova, Natalia V.; Seddon, Kenneth R.
- Chem. Soc. Rev., Vol. 37, Issue 1
Origin of the excess wing and slow relaxation of glass formers: A unified picture of local orientational fluctuations
journal, February 2004
- Tanaka, Hajime
- Physical Review E, Vol. 69, Issue 2
Structural rearrangements governing Johari-Goldstein relaxations in metallic glasses
journal, November 2017
- Yu, Hai-Bin; Richert, Ranko; Samwer, Konrad
- Science Advances, Vol. 3, Issue 11
Non-symmetrical dielectric relaxation behaviour arising from a simple empirical decay function
journal, January 1970
- Williams, Graham; Watts, David C.
- Transactions of the Faraday Society, Vol. 66
Properties of ionic liquid solvents for catalysis
journal, May 2004
- Wilkes, J.
- Journal of Molecular Catalysis A: Chemical, Vol. 214, Issue 1
A universal origin for secondary relaxations in supercooled liquids and structural glasses
journal, November 2009
- Stevenson, Jacob D.; Wolynes, Peter G.
- Nature Physics, Vol. 6, Issue 1
Glassy dynamics
journal, January 2000
- Lunkenheimer, P.; Schneider, U.; Brand, R.
- Contemporary Physics, Vol. 41, Issue 1
Cation Dynamics in the Pyridinium Based Ionic Liquid 1- N -Butylpyridinium Bis((trifluoromethyl)sulfonyl) As Seen by Quasielastic Neutron Scattering
journal, October 2012
- Embs, Jan P.; Burankova, Tatsiana; Reichert, Elena
- The Journal of Physical Chemistry B, Vol. 116, Issue 44
The high-flux backscattering spectrometer at the NIST Center for Neutron Research
journal, May 2003
- Meyer, A.; Dimeo, R. M.; Gehring, P. M.
- Review of Scientific Instruments, Vol. 74, Issue 5
Applications of ionic liquids in electrochemical sensors
journal, January 2008
- Wei, Di; Ivaska, Ari
- Analytica Chimica Acta, Vol. 607, Issue 2
Further considerations of non symmetrical dielectric relaxation behaviour arising from a simple empirical decay function
journal, January 1971
- Williams, G.; Watts, D. C.; Dev, S. B.
- Transactions of the Faraday Society, Vol. 67
Vibrational Spectroscopy of Ionic Liquids
journal, January 2017
- Paschoal, Vitor H.; Faria, Luiz F. O.; Ribeiro, Mauro C. C.
- Chemical Reviews, Vol. 117, Issue 10
Relation between some secondary relaxations and the α relaxations in glass-forming materials according to the coupling model
journal, October 1998
- Ngai, K. L.
- The Journal of Chemical Physics, Vol. 109, Issue 16
Supercooled liquids and the glass transition
journal, March 2001
- Debenedetti, Pablo G.; Stillinger, Frank H.
- Nature, Vol. 410, Issue 6825
Magnetic Surfactant Ionic Liquids and Polymers With Tetrahaloferrate (III) Anions as Antimicrobial Agents With Low Cytotoxicity
journal, January 2018
- de la Fuente-Nunez, Cesar; Brown, Paul; Torres, Marcelo D. T.
- Colloid and Interface Science Communications, Vol. 22
Liquid dynamics and inelastic scattering of neutrons
journal, January 1959
- De Gennes, P. G.
- Physica, Vol. 25, Issue 7-12
Neutron Scattering from Liquid Argon
journal, January 1965
- Dasannacharya, B. A.; Rao, K. R.
- Physical Review, Vol. 137, Issue 2A
Onset of Cooperative Dynamics in an Equilibrium Glass-Forming Metallic Liquid
journal, February 2016
- Jaiswal, Abhishek; O’Keeffe, Stephanie; Mills, Rebecca
- The Journal of Physical Chemistry B, Vol. 120, Issue 6
The β-relaxation in metallic glasses
journal, June 2014
- Yu, Hai Bin; Wang, Wei Hua; Bai, Hai Yang
- National Science Review, Vol. 1, Issue 3
Comparing two tetraalkylammonium ionic liquids. II. Phase transitions
journal, June 2016
- Lima, Thamires A.; Paschoal, Vitor H.; Faria, Luiz F. O.
- The Journal of Chemical Physics, Vol. 144, Issue 22
Liquid dynamics and inelastic scattering of neutrons
journal, January 1959
- Degennes, P.
- Antiviral Research, Vol. 25, Issue 7-12
Application of Ionic Liquids to Energy Storage and Conversion Materials and Devices
journal, January 2017
- Watanabe, Masayoshi; Thomas, Morgan L.; Zhang, Shiguo
- Chemical Reviews, Vol. 117, Issue 10
Comparing two tetraalkylammonium ionic liquids. I. Liquid phase structure
journal, June 2016
- Lima, Thamires A.; Paschoal, Vitor H.; Faria, Luiz F. O.
- The Journal of Chemical Physics, Vol. 144, Issue 22
Properties of Ionic Liquid Solvents for Catalysis
journal, January 2005
- Wilkes, John S.
- ChemInform, Vol. 36, Issue 1
Quasielastic neutron scattering studies on glass-forming ionic liquids with imidazolium cations
journal, December 2015
- Kofu, Maiko; Tyagi, Madhusudan; Inamura, Yasuhiro
- The Journal of Chemical Physics, Vol. 143, Issue 23
Dynamics of Imidazolium Ionic Liquids from a Combined Dielectric Relaxation and Optical Kerr Effect Study: Evidence for Mesoscopic Aggregation
journal, August 2009
- Turton, David A.; Hunger, Johannes; Stoppa, Alexander
- Journal of the American Chemical Society, Vol. 131, Issue 31
Viscous Liquids and the Glass Transition. II. Secondary Relaxations in Glasses of Rigid Molecules
journal, September 1970
- Johari, Gyan P.; Goldstein, Martin
- The Journal of Chemical Physics, Vol. 53, Issue 6
Structural origins of Johari-Goldstein relaxation in a metallic glass
journal, February 2014
- Liu, Y. H.; Fujita, T.; Aji, D. P. B.
- Nature Communications, Vol. 5, Issue 1
The Dielectric Response of Room-Temperature Ionic Liquids: Effect of Cation Variation †
journal, May 2007
- Weingärtner, Hermann; Sasisanker, Padmanabhan; Daguenet, Corinne
- The Journal of Physical Chemistry B, Vol. 111, Issue 18
Dielectric Response of Imidazolium-Based Room-Temperature Ionic Liquids
journal, June 2006
- Daguenet, Corinne; Dyson, Paul J.; Krossing, Ingo
- The Journal of Physical Chemistry B, Vol. 110, Issue 25
Collective Ion Diffusion and Localized Single Particle Dynamics in Pyridinium-Based Ionic Liquids
journal, November 2014
- Burankova, Tatsiana; Hempelmann, Rolf; Wildes, Andrew
- The Journal of Physical Chemistry B, Vol. 118, Issue 49
Nanostructural Organization in Ionic Liquids
journal, February 2006
- Canongia Lopes, José N. A.; Pádua, Agílio A. H.
- The Journal of Physical Chemistry B, Vol. 110, Issue 7
Structure and Nanostructure in Ionic Liquids
journal, June 2015
- Hayes, Robert; Warr, Gregory G.; Atkin, Rob
- Chemical Reviews, Vol. 115, Issue 13
Formation of Glasses from Liquids and Biopolymers
journal, March 1995
- Angell, C. A.
- Science, Vol. 267, Issue 5206
A universal origin for secondary relaxations in supercooled liquids and structural glasses
text, January 2009
- Stevenson, Jacob D.; Wolynes, Peter G.
- arXiv
The High-Flux Backscattering Spectrometer at the NIST Center for Neutron Research
text, January 2002
- Meyer, A.; Dimeo, R. M.; Gehring, P. M.
- arXiv
Works referencing / citing this record:
Molecular simulation study of the glass transition in a soft primitive model for ionic liquids
journal, October 2019
- Rodríguez-Rivas, A.; Romero-Enrique, J. M.; Rull, L. F.
- Molecular Physics, Vol. 117, Issue 23-24