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Effect of adding nanometre-sized heterogeneities on the structural dynamics and the excess wing of a molecular glass former

Journal Article · · Scientific Reports
DOI:https://doi.org/10.1038/srep35034· OSTI ID:1624863
 [1];  [2];  [2];  [2];  [3];  [4];  [4]
  1. Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS) outstation Juelich Centre for Neutron Science (JCNS), Forschungszentrum Juelich GmbH; Louisiana State Univ., Baton Rouge, LA (United States); DOE/OSTI
  2. Univ. of Augsburg (Germany)
  3. Univ. of Tennessee, Knoxville, TN (United States)
  4. Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS) outstation Juelich Centre for Neutron Science (JCNS), Forschungszentrum Juelich GmbH

We present the relaxation dynamics of glass-forming glycerol mixed with 1.1 nm sized polyhedral oligomeric silsesquioxane (POSS) molecules using dielectric spectroscopy (DS) and two different neutron scattering (NS) techniques. Both, the reorientational dynamics as measured by DS and the density fluctuations detected by NS reveal a broadening of the α relaxation when POSS molecules are added. Moreover, we find a significant slowing down of the α-relaxation time. These effects are in accord with the heterogeneity scenario considered for the dynamics of glasses and supercooled liquids. The addition of POSS also affects the excess wing in glycerol arising from a secondary relaxation process, which seems to exhibit a dramatic increase in relative strength compared to the α relaxation.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1624863
Journal Information:
Scientific Reports, Journal Name: Scientific Reports Journal Issue: 1 Vol. 6; ISSN 2045-2322
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

References (56)

Theorie des elektrischen Rückstandes in der Leidener Flasche journal January 1854
A complex plane analysis of α-dispersions in some polymer systems journal January 1966
Die Abhängigkeit der Viscosität von der Temperatur bie unterkühlten Flüssigkeiten journal October 1926
Scaling of broadband dielectric data of glass-forming liquids and plastic crystals journal April 2000
The dielectric response of simple organic glass formers journal April 1999
Heterogeneity at the glass transition: a review journal February 1999
Dielectric spectroscopy of glass-forming materials: α-relaxation and excess wing journal November 2002
Diffusion in confinement as a microscopic relaxation mechanism in glass-forming liquids journal March 2012
Molecular-level mixed matrix membranes comprising Pebax® and POSS for hydrogen purification via preferential CO2 removal journal October 2010
High-frequency dynamics of type B glass formers investigated by broadband dielectric spectroscopy journal January 2011
Probing nanoscale structure and dynamics of amyloidogenic proteins using single-molecule fluorescence journal December 2007
Recent Developments in the Chemistry of Cubic Polyhedral Oligosilsesquioxanes journal April 2010
On the Decoupling of Relaxation Modes in a Molecular Liquid Caused by Isothermal Introduction of 2 nm Structural Inhomogeneities journal December 2011
Supercooled Liquids and Glasses journal January 1996
Heterogeneity at the Glass Transition:  Translational and Rotational Self-Diffusion journal October 1997
Thermomechanical Properties of Poly(methyl methacrylate)s Containing Tethered and Untethered Polyhedral Oligomeric Silsesquioxanes journal November 2004
Dielectric Spectroscopy in the αβ Splitting Region of Glass Transition in Poly(ethyl methacrylate) and Poly(n-butyl methacrylate):  Different Evaluation Methods and Experimental Conditions journal November 1998
Probe dependence of spatially heterogeneous dynamics in supercooled glycerol as revealed by single molecule microscopy journal January 2011
A robust comparison of dynamical scenarios in a glass-forming liquid journal January 2016
Slow dynamics of water molecules in an aqueous solution of lithium chloride probed by neutron spin-echo journal January 2013
Non-symmetrical dielectric relaxation behaviour arising from a simple empirical decay function journal January 1970
Relaxation in glassforming liquids and amorphous solids journal September 2000
Length scale of dynamic heterogeneity in supercooled glycerol near Tg  journal May 2001
Nature and properties of the Johari–Goldstein β-relaxation in the equilibrium liquid state of a class of glass-formers journal July 2001
Viscous Liquids and the Glass Transition. II. Secondary Relaxations in Glasses of Rigid Molecules journal September 1970
Dielectric Relaxation in Glycerine journal October 1950
Dispersion and Absorption in Dielectrics I. Alternating Current Characteristics journal April 1941
A time-of-flight backscattering spectrometer at the Spallation Neutron Source, BASIS journal August 2011
Structural relaxation in viscous glycerol: Coherent neutron scattering journal September 1996
Effects of 2 nm size added heterogeneity on non-exponential dielectric response, and the dynamic heterogeneity view of molecular liquids journal September 2012
Note: Effects of adding a viscosity-increasing 2 nm-size molecule on dielectric relaxation features and the dynamic heterogeneity view journal May 2013
Glassy dynamics journal January 2000
Relaxation processes in supercooled liquids journal March 1992
Fast dynamics of glass-forming glycerol journal October 1995
Broadband dielectric spectroscopy on glass-forming propylene carbonate journal June 1999
Comment on “Merging of theαandβrelaxations in polybutadiene: A neutron spin echo and dielectric study” journal July 1999
Broadband dielectric spectroscopy on benzophenone: α relaxation, β relaxation, and mode coupling theory journal March 2008
Ions in glass-forming glycerol: Close correlation of primary and fast β relaxation journal June 2013
Picosecond Dynamic Heterogeneity, Hopping, and Johari-Goldstein Relaxation in Glass-Forming Liquids journal September 2014
Validity of the Stokes-Einstein Relation in Soft Colloids up to the Glass Transition journal September 2015
Scaling in the relaxation of supercooled liquids journal August 1990
Length Scale of Dynamic Heterogeneities at the Glass Transition Determined by Multidimensional Nuclear Magnetic Resonance journal September 1998
Excess Wing in the Dielectric Loss of Glass Formers: A Johari-Goldstein β Relaxation? journal June 2000
From Strong to Fragile Glass Formers: Secondary Relaxation in Polyalcohols journal February 2002
Origin of the High-Frequency Contributions to the Dielectric Loss in Supercooled Liquids journal June 2002
Nearly Logarithmic Decay of Correlations in Glass-Forming Liquids journal March 2004
Anelastic to Plastic Transition in Metallic Glass-Forming Liquids journal September 2007
Glass Transition and Secondary Relaxations in Molecular Liquids and Crystals journal October 1976
A Topographic View of Supercooled Liquids and Glass Formation journal March 1995
Nonresonant Spectral Hole Burning in the Slow Dielectric Response of Supercooled Liquids journal November 1996
Direct Observation of Dynamical Heterogeneities in Colloidal Hard-Sphere Suspensions journal January 2000
Excess wing in glass-forming glycerol and LiCl-glycerol mixtures detected by neutron scattering journal January 2015
Characteristic length scales of the secondary relaxations in glass-forming glycerol journal March 2016
S PATIALLY H ETEROGENEOUS D YNAMICS IN S UPERCOOLED L IQUIDS journal October 2000
High-frequency asymptotic shape of the primary relaxation in supercooled liquids journal August 1997
Dielectric Spectroscopy at High Frequencies on Glass Forming Liquids journal January 1996

Figures / Tables (7)


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