Inelastic neutron scattering study on boson peaks of imidazolium-based ionic liquids
Abstract
Low energy excitations of 1-alkyl-3-methylimidazolium ionic liquids (ILs) have been investigated by means of neutron spectroscopy. In the spectra of inelastic scattering, a broad excitation peak referred to as a “boson peak” appeared at 1–3 meV in all of the ILs measured. The intensity of the boson peak was enhanced at the Q positions corresponding to the diffraction peaks, reflecting the in-phase vibrational nature of the boson peak. Furthermore the boson peak energy (EBP) was insensitive to the length of the alkyl-chain but changed depending on the radius of the anion. From the correlation among EBP, the anion radius, and the glass transition temperature Tg, we conclude that both EBP and Tg in ILs are predominantly governed by the inter-ionic Coulomb interaction which is less influenced by the alkyl-chain length. Furthermore, we also found that the EBP is proportional to the inverse square root of the molecular weight as observed in molecular glasses.
- Authors:
-
- Univ. of Tokyo, Chiba (Japan)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1214030
- Alternate Identifier(s):
- OSTI ID: 1250296
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Molecular Liquids
- Additional Journal Information:
- Journal Volume: 210; Journal Issue: 1; Journal ID: ISSN 0167-7322
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 74 ATOMIC AND MOLECULAR PHYSICS; ionic liquid; inelastic neutron scattering; boson peak; glass
Citation Formats
Kofu, Maiko, Inamura, Yasuhiro, Podlesnyak, Andrey A., Ehlers, Georg, Yamamuro, Osamu, and Moriya, Yosuke. Inelastic neutron scattering study on boson peaks of imidazolium-based ionic liquids. United States: N. p., 2015.
Web. doi:10.1016/j.molliq.2015.07.021.
Kofu, Maiko, Inamura, Yasuhiro, Podlesnyak, Andrey A., Ehlers, Georg, Yamamuro, Osamu, & Moriya, Yosuke. Inelastic neutron scattering study on boson peaks of imidazolium-based ionic liquids. United States. https://doi.org/10.1016/j.molliq.2015.07.021
Kofu, Maiko, Inamura, Yasuhiro, Podlesnyak, Andrey A., Ehlers, Georg, Yamamuro, Osamu, and Moriya, Yosuke. Sun .
"Inelastic neutron scattering study on boson peaks of imidazolium-based ionic liquids". United States. https://doi.org/10.1016/j.molliq.2015.07.021. https://www.osti.gov/servlets/purl/1214030.
@article{osti_1214030,
title = {Inelastic neutron scattering study on boson peaks of imidazolium-based ionic liquids},
author = {Kofu, Maiko and Inamura, Yasuhiro and Podlesnyak, Andrey A. and Ehlers, Georg and Yamamuro, Osamu and Moriya, Yosuke},
abstractNote = {Low energy excitations of 1-alkyl-3-methylimidazolium ionic liquids (ILs) have been investigated by means of neutron spectroscopy. In the spectra of inelastic scattering, a broad excitation peak referred to as a “boson peak” appeared at 1–3 meV in all of the ILs measured. The intensity of the boson peak was enhanced at the Q positions corresponding to the diffraction peaks, reflecting the in-phase vibrational nature of the boson peak. Furthermore the boson peak energy (EBP) was insensitive to the length of the alkyl-chain but changed depending on the radius of the anion. From the correlation among EBP, the anion radius, and the glass transition temperature Tg, we conclude that both EBP and Tg in ILs are predominantly governed by the inter-ionic Coulomb interaction which is less influenced by the alkyl-chain length. Furthermore, we also found that the EBP is proportional to the inverse square root of the molecular weight as observed in molecular glasses.},
doi = {10.1016/j.molliq.2015.07.021},
journal = {Journal of Molecular Liquids},
number = 1,
volume = 210,
place = {United States},
year = {Sun Jul 26 00:00:00 EDT 2015},
month = {Sun Jul 26 00:00:00 EDT 2015}
}
Web of Science
Works referenced in this record:
Physical Properties of Ionic Liquids: Database and Evaluation
journal, December 2006
- Zhang, Suojiang; Sun, Ning; He, Xuezhong
- Journal of Physical and Chemical Reference Data, Vol. 35, Issue 4, p. 1475-1517
High-frequency vibrational dynamics in glasses
journal, September 2001
- Ruocco, Giancarlo; Sette, Francesco
- Journal of Physics: Condensed Matter, Vol. 13, Issue 41
Universal link between the boson peak and transverse phonons in glass
journal, October 2008
- Shintani, Hiroshi; Tanaka, Hajime
- Nature Materials, Vol. 7, Issue 11
Breakdown of the Debye approximation for the acoustic modes with nanometric wavelengths in glasses
journal, February 2009
- Monaco, G.; Giordano, V. M.
- Proceedings of the National Academy of Sciences, Vol. 106, Issue 10
Equivalence of the Boson Peak in Glasses to the Transverse Acoustic van Hove Singularity in Crystals
journal, May 2011
- Chumakov, A. I.; Monaco, G.; Monaco, A.
- Physical Review Letters, Vol. 106, Issue 22
The Boson peak of model glass systems and its relation to atomic structure
journal, May 2012
- Derlet, P. M.; Maaß, R.; Löffler, J. F.
- The European Physical Journal B, Vol. 85, Issue 5
Inelastic neutron scattering study of low-energy excitations in vapor-deposited glassy propylene
journal, February 1997
- Yamamuro, Osamu; Tsukushi, Itaru; Matsuo, Takasuke
- The Journal of Chemical Physics, Vol. 106, Issue 8
Boson peaks in hydrogen-bonded molecular glasses
journal, January 2002
- Yamamuro, Osamu; Takeda, Kiyoshi; Tsukushi, Itaru
- Physica B: Condensed Matter, Vol. 311, Issue 1-2
Neutron Scattering Study of the Low-Frequency Vibrations in Vitreous Silica
journal, December 1984
- Buchenau, U.; Nücker, N.; Dianoux, A. J.
- Physical Review Letters, Vol. 53, Issue 24
Low-frequency modes in vitreous silica
journal, October 1986
- Buchenau, U.; Prager, M.; Nücker, N.
- Physical Review B, Vol. 34, Issue 8
Glass-Specific Behavior in the Damping of Acousticlike Vibrations
journal, January 2006
- Rufflé, B.; Guimbretière, G.; Courtens, E.
- Physical Review Letters, Vol. 96, Issue 4
Floppy Modes in Crystalline and Amorphous Silicates
journal, February 1997
- Dove, Martin T.; Harris, Mark J.; Hannon, Alex C.
- Physical Review Letters, Vol. 78, Issue 6
Comment on “Glass-Specific Behavior in the Damping of Acousticlike Vibrations”
journal, February 2007
- Ruocco, G.; Matic, A.; Scopigno, T.
- Physical Review Letters, Vol. 98, Issue 7
Low-frequency Raman spectra and fragility of imidazolium ionic liquids
journal, July 2010
- Ribeiro, Mauro C. C.
- The Journal of Chemical Physics, Vol. 133, Issue 2
Intermolecular vibrations and fast relaxations in supercooled ionic liquids
journal, June 2011
- Ribeiro, Mauro C. C.
- The Journal of Chemical Physics, Vol. 134, Issue 24
Pressure and temperature effects on intermolecular vibrational dynamics of ionic liquids
journal, March 2013
- Penna, Tatiana C.; Faria, Luiz F. O.; Matos, Jivaldo R.
- The Journal of Chemical Physics, Vol. 138, Issue 10
Heat capacity and glass transition of an ionic liquid 1-butyl-3-methylimidazolium chloride
journal, June 2006
- Yamamuro, Osamu; Minamimoto, Yoko; Inamura, Yasuhiro
- Chemical Physics Letters, Vol. 423, Issue 4-6
Glass Transitions and Low-Frequency Dynamics of Room-Temperature Ionic Liquids
conference, January 2006
- Yamamuro, O.
- FLOW DYNAMICS: The Second International Conference on Flow Dynamics, AIP Conference Proceedings
Hierarchical structure and dynamics of an ionic liquid 1-octyl-3-methylimidazolium chloride
journal, August 2011
- Yamamuro, Osamu; Yamada, Takeshi; Kofu, Maiko
- The Journal of Chemical Physics, Vol. 135, Issue 5
Heterogeneous Slow Dynamics of Imidazolium-Based Ionic Liquids Studied by Neutron Spin Echo
journal, February 2013
- Kofu, Maiko; Nagao, Michihiro; Ueki, Takeshi
- The Journal of Physical Chemistry B, Vol. 117, Issue 9
Construction of the TOF-type cold-neutron spectrometer, AGNES
journal, August 1995
- Kajitani, T.; Shibata, K.; Ikeda, S.
- Physica B: Condensed Matter, Vol. 213-214
The new cold neutron chopper spectrometer at the Spallation Neutron Source: Design and performance
journal, August 2011
- Ehlers, G.; Podlesnyak, A. A.; Niedziela, J. L.
- Review of Scientific Instruments, Vol. 82, Issue 8
Cluster size determination in amorphous structures using the Boson peak
journal, June 1990
- Pócsik, I.; Koós, M.
- Solid State Communications, Vol. 74, Issue 12
Log-normal spectrum of low-energy vibrational excitations in glasses
journal, February 1991
- Malinovsky, V. K.; Novikov, V. N.; Sokolov, A. P.
- Physics Letters A, Vol. 153, Issue 1
Pressure and density dependence of the boson peak in polymers
journal, October 2008
- Hong, L.; Begen, B.; Kisliuk, A.
- Physical Review B, Vol. 78, Issue 13
Composition Dependence of the Boson Peak and Universality in Lithium Borate Binary Glasses: Inelastic Neutron and Raman Scattering Studies
journal, March 2010
- Matsuda, Yu; Kawashima, Mitsuru; Moriya, Yosuke
- Journal of the Physical Society of Japan, Vol. 79, Issue 3
Novel existence of collective propagating mode and strongly localized mode in vitreous silica
journal, March 1999
- Arai, M.; Inamura, Y.; Otomo, T.
- Physica B: Condensed Matter, Vol. 263-264
Dispersive excitation in different forms of SiO2
journal, November 2001
- Nakamura, Mitsutaka; Arai, Masatoshi; Otomo, Toshiya
- Journal of Non-Crystalline Solids, Vol. 293-295
On the wave vector dependence of the Boson peak in silicate glasses and crystals
journal, March 1999
- Harris, M. J.; Bennington, S. M.; Dove, M. T.
- Physica B: Condensed Matter, Vol. 263-264
Floppy modes and the Boson peak in crystalline and amorphous silicates: an inelastic neutron scattering study
journal, June 2000
- Harris, M. J.; Dove, M. T.; Parker, J. M.
- Mineralogical Magazine, Vol. 64, Issue 3
A Convenient Method to Estimate Ion Size for Electrolyte Materials Design
journal, January 2002
- Ue, Makoto; Murakami, Akinori; Nakamura, Shinichiro
- Journal of The Electrochemical Society, Vol. 149, Issue 10
How Ionic Are Room-Temperature Ionic Liquids? An Indicator of the Physicochemical Properties
journal, October 2006
- Tokuda, Hiroyuki; Tsuzuki, Seiji; Susan, Md. Abu Bin Hasan
- The Journal of Physical Chemistry B, Vol. 110, Issue 39
Influence of Structural Variation in Room-Temperature Ionic Liquids on the Selectivity and Efficiency of Competitive Alkali Metal Salt Extraction by a Crown Ether
journal, August 2001
- Chun, Sangki; Dzyuba, Sergei V.; Bartsch, Richard A.
- Analytical Chemistry, Vol. 73, Issue 15
Thermal and Structural Studies of Imidazolium-Based Ionic Liquids with and without Liquid-Crystalline Phases: The Origin of Nanostructure
journal, April 2015
- Nemoto, Fumiya; Kofu, Maiko; Yamamuro, Osamu
- The Journal of Physical Chemistry B, Vol. 119, Issue 15
Thermodynamic properties of 1-alkyl-3-methylimidazolium bromide ionic liquids
journal, January 2007
- Paulechka, Y. U.; Kabo, G. J.; Blokhin, A. V.
- The Journal of Chemical Thermodynamics, Vol. 39, Issue 1
Thermodynamic Properties of 1-Butyl-3-methylimidazolium Hexafluorophosphate in the Condensed State
journal, May 2004
- Kabo, Gennady J.; Blokhin, Andrey V.; Paulechka, Yauheni U.
- Journal of Chemical & Engineering Data, Vol. 49, Issue 3
Physicochemical Properties, Structure, and Conformations of 1-Butyl-3-methylimidazolium Bis(trifluoromethanesulfonyl)imide [C 4 mim]NTf 2 Ionic Liquid
journal, April 2008
- Blokhin, Andrey V.; Paulechka, Yauheni U.; Strechan, Aliaksei A.
- The Journal of Physical Chemistry B, Vol. 112, Issue 14
Thermodynamic properties and polymorphism of 1-alkyl-3-methylimidazolium bis(triflamides)
journal, June 2007
- Paulechka, Y. U.; Blokhin, A. V.; Kabo, G. J.
- The Journal of Chemical Thermodynamics, Vol. 39, Issue 6
Relaxation and phonons in viscous and glassy orthoterphenyl by neutron scattering
journal, September 1993
- Wuttke, J.; Kiebel, M.; Bartsch, E.
- Zeitschrift f�r Physik B Condensed Matter, Vol. 91, Issue 3
Vibrational behaviour of amorphous and crystalline ethylbenzene
journal, August 1995
- Frick, B.; Williams, J.; Treviño, S.
- Physica B: Condensed Matter, Vol. 213-214
Low Energy Excitations in Simple Molecular Glasses
journal, January 1997
- Yamamuro, Osamu; Tsukushi, Itaru; Matsuo, Takasuke
- Progress of Theoretical Physics Supplement, Vol. 126
Works referencing / citing this record:
Boson peak, elasticity, and glass transition temperature in polymer glasses: Effects of the rigidity of chain bending
journal, December 2019
- Tomoshige, Naoya; Mizuno, Hideyuki; Mori, Tatsuya
- Scientific Reports, Vol. 9, Issue 1
Mechanical heterogeneity in ionic liquids
journal, May 2018
- Veldhorst, Arno A.; Ribeiro, Mauro C. C.
- The Journal of Chemical Physics, Vol. 148, Issue 19
Low-frequency Raman spectra of a glass-forming ionic liquid at low temperature and high pressure
journal, April 2019
- Lima, Thamires A.; Ribeiro, Mauro C. C.
- The Journal of Chemical Physics, Vol. 150, Issue 16
Fast Parallel Algorithms for Short-Range Molecular Dynamics
journal, March 1995
- Plimpton, Steve
- Journal of Computational Physics, Vol. 117, Issue 1
Boson peak, elasticity, and glass transition temperature in polymer glasses: Effects of the rigidity of chain bending
journal, December 2019
- Tomoshige, Naoya; Mizuno, Hideyuki; Mori, Tatsuya
- Scientific Reports, Vol. 9, Issue 1