We employed high-pressure Brillouin scattering to study the pressure dependencies of acoustic modes of glycerol up to 14 GPa at 300 K. We observed longitudinal acoustic velocities and transverse acoustic velocities for the first time from 5 to 14 GPa. The results allow the determination of a complete set of elastic properties and an accurate determination of the pressure–volume (P–V) equation of state (EOS). EOS parameters, K0 = 14.9 ± 1.8 GPa and K′0 = 5.6 ± 0.5, were determined from fits to the data from ambient pressure to 14 GPa. Direct volume measurements of the P–V EOS are consistent with those determined by Brillouin scattering. A deviation from a Cauchy-like relationship for elastic properties was observed, and the pressure dependencies of the photoelastic constants and relaxation times were documented from 5 to 14 GPa. These results have broad implications for glass-forming liquids, viscoelastic theory, and mode coupling theory.
REFERENCES
1.
R.
Christoph
, B.
Schmidt
, U.
Steinberner
, W.
Dilla
, and R.
Karinen
, “Glycerol
,” Ullmann’s Encyclopedia of Industrial Chemistry
(Wiley
, 2006
).2.
A.
Mortensen
et al, “Re-evaluation of glycerol (E 422) as a food additive
,” EFSA J.
15
, e04720
(2017
).3.
R. D.
Hudgens
, R. D.
Hercamp
, J.
Francis
, D. A.
Nyman
, and Y.
Bartoli
, “An evaluation of glycerin (glycerol) as a heavy duty engine antifreeze/coolant base
,” SAE Trans.
116
, 834
–849
(2007
).4.
S.
Kojima
, “Low-frequency Raman investigation of the liquid-glass transition in glycerol
,” Phys. Rev. B
47
, 2924
–2927
(1993
).5.
S.
Klotz
, K.
Takemura
, Th.
Strässle
, and T.
Hansen
, “Freezing of glycerol–water mixtures under pressure
,” J. Phys.: Condens. Matter
24
, 325103
(2012
).6.
K.
Rolle
, H.-J.
Butt
, and J.
Fytas
, “Flash Brillouin scattering: A confocal technique for measuring glass transitions at high scan rates
,” ACS Photonics
8
(2
), 531
–539
(2021
).7.
S.
Pawlus
, M.
Paluch
, J.
Ziolo
, and C. M.
Roland
, “On the pressure dependence of the fragility of glycerol
,” J. Phys.: Condens. Matter
21
, 332101
(2009
).8.
C. A.
Angell
, “Formation of glasses from liquids and biopolymers
,” Science
267
, 1924
–1935
(1995
).9.
M.
Ahart
, F.
Jiang
, M.
Mikami
, I.-S.
Park
, and S.
Kojima
, “Microscopic Brillouin scattering study of relaxation phenomena in low weight alcohols of methanol and ethanol
,” Jpn. J. Appl. Phys.
38
, 3058
–3061
(1999
).10.
W.
Gotze
and L.
Sjogren
, “The glass transition singularity
,” Z. Phys. B: Condens. Matter
65
, 415
–427
(1987
).11.
W.
Gotze
and L.
Sjogren
, “Relaxation processes in supercooled liquids
,” Rep. Prog. Phys.
55
, 241
–376
(1992
).12.
D. M.
Paolucci
and K. A.
Nelson
, “Impulsive stimulated thermal scattering study of structural relaxation in supercooled glycerol
,” J. Chem. Phys.
112
(15
), 6725
–6732
(2000
).13.
M. -S.
Jeong
, J.-H.
Ko
, Y. H.
Ko
, and K. J.
Kim
, “High-pressure acoustic properties of glycerol studied by Brillouin spectroscopy
,” Physica B
478
, 27
–30
(2015
).14.
G.
Fytas
, G.
Meier
, and T.
Dorfmueller
, “Rayleigh-Brillouin spectra of [poly(phenylmethyl)] siloxane under high pressures
,” Macromolecules
18
, 993
–996
(1985
).15.
F.
Scarponi
, L.
Comez
, D.
Fioretto
, and L.
Palmieri
, “Brillouin light scattering from transverse and longitudinal acoustic wave in glycerol
,” Phys. Rev. B
70
, 054203
(2004
).16.
A. G.
Lyapin
, E. L.
Gromnitskaya
, I. V.
Danilov
, and V. V.
Brazhkin
, “Elastic properties of the hydrogen-bonded liquid and glassy glycerol under high pressure
,” RSC Adv.
7
, 33278
–33284
(2017
).17.
E. L.
Gromnitskaya
, I. V.
Danilov
, A. G.
Lyapin
, and V. V.
Brazhkin
, “Elastic properties of liquid and glassy propane-based alcohols under high pressure: The increasing role of hydrogen bonds in a homologous family
,” Phys. Chem. Chem. Phys.
21
, 2665
–2672
(2019
).18.
M.
Ahart
, D.
Aihaiti
, R. J.
Hemley
, and S.
Kojima
, “Pressure dependence of the Boson peak of glassy glycerol
,” J. Phys. Chem. B
121
, 6667
–6672
(2017
).19.
R. A.
Forman
, G. J.
Piermarini
, J. D.
Barnett
, and S.
Block
, “Pressure measurement made by the utilization of ruby sharp-line luminescence
,” Science
176
, 284
–285
(1972
).20.
C. H.
Whitfield
, E. M.
Brody
, and W. A.
Bassett
, “Elastic moduli of NaCl by Brillouin scattering at high pressure in a diamond anvil cell
,” Rev. Sci. Instrum.
47
, 942
–947
(1976
).21.
L. W.
Bosart
and A. O.
Snoddy
, “New glycerol tables
,” Ind. Eng. Chem.
19
, 506
–510
(1927
).22.
P.
Vinet
, J. R.
Smith
, J.
Ferrante
, and J. H.
Rose
, “Temperature effects on the universal equation of state of solids
,” Phys. Rev. B
35
, 1945
–1953
(1987
).23.
F.
Birch
, “Finite elastic strain of cubic crystals
,” Phys. Rev.
71
, 809
–824
(1947
).24.
L.
Comez
, D.
Fioretto
, F.
Scarponi
, and G.
Monaco
, “Density fluctuations in the intermediate glass-former glycerol: A Brillouin light scattering study
,” J. Chem. Phys.
119
, 6032
–6043
(2003
).25.
H.
Khelladi
, F.
Plantier
, J. L.
Daridon
, and H.
Djelouah
, “Measurements under high pressure of ultrasonic velocity in glycerol
,” J. Acoust. Soc. Am.
123
(5
), 3928
(2008
).26.
A. P. V.
Egas
, N. M. C.
Talavera-Prieto
, A. G. M.
Ferreira
, J. B.
Santos
, M. J.
Santos
, Z. L.
Almeida
, and I. M.
Fonseca
, “Speed of sound and derived thermodynamic properties of glycerol
,” J. Chem. Thermodyn.
156
, 106367
(2021
).27.
L. J.
Root
and B. J.
Berne
, “Effect of pressure on hydrogen bonding in glycerol: A molecular dynamics investigation
,” J. Chem. Phys.
107
, 4350
–4357
(1997
).28.
R.
Chelli
, P.
Procacci
, G.
Cardini
, R. G. D.
Della Valle
, and S.
Califano
, “Glycerol condensed phases. Part I. A molecular dynamics study
,” Phys. Chem. Chem. Phys.
1
, 871
–877
(1999
).29.
S. R.
Atalla
, A. A.
El-Sharkawy
, and F. A.
Gasser
, “Measurement of thermal properties of liquids with an AC heated-wire technique
,” Int. J. Thermophys.
2
, 155
–162
(1981
).30.
P.
Voudouris
, N.
Gomopoulos
, A.
Le Grand
, N.
Hadjichristidis
, G.
Floudas
, M. D.
Ediger
, and G.
Fytas
, “Does Brillouin light scattering probe the primary glass transition process at temperatures well above glass transition?
,” J. Chem. Phys.
132
, 074906
(2010
).31.
C. J.
Montrose
, V. A.
Solovyev
, and T. A.
Litovitz
, “Brillouin scattering and relaxation in liquids
,” J. Acoust. Soc. Am.
43
, 117
–130
(1968
).32.
N. J.
Tao
, G.
Li
, and H. Z.
Cummins
, “Brillouin-scattering study of the liquid-glass transition in CaKNO3: Mode-coupling analysis
,” Phys. Rev. B
45
, 686
–696
(1992
).33.
W. F.
Oliver
, C. A.
Herbst
, S. M.
Lindsay
, and G. H.
Wolf
, “High-pressure viscoelastic properties and equation of state of liquids derived from Brillouin data
,” Phys. Rev. Lett.
67
, 2795
–2798
(1991
).34.
Y.
Takagi
, M.
Ahart
, T.
Yano
, and S.
Kojima
, “The liquid–glass transition in n-propanol: The pressure dependence of the Brillouin spectra
,” J. Phys.: Condens. Matter
9
, 6995
–7002
(1997
).35.
L.
Loubeyre
, M.
Ahart
, S. A.
Gramsch
, and R. J.
Hemley
, “Density dependence of dynamical heterogeneity in fluid methanol
,” J. Chem. Phys.
138
, 174507
(2013
).36.
S. N.
Tkachev
, M.
Ahart
, V. N.
Novikov
, and S.
Kojima
, “Pressure dependence of Poisson’s ratio of glassy Baltic amber studied by Brillouin scattering spectroscopy
,” Jpn. J. Appl. Phys.
60
, SDDA04
(2021
).37.
L.
Landau
and E.
Lifshitz
, Electrodynamics of Continuous Media
(Pergamon
, New York
, 1968
).38.
M.
Born
and K.
Huang
, Dynamical Theory of Crystal Lattices
(Clarendon Press
, Oxford
, 1956
).39.
D.
Fioretto
, S.
Corezzi
, S.
Caponi
, F.
Scarponi
, G.
Monaco
, A.
Fontana
, and L.
Palmieri
, “Cauchy relation in relaxing liquids
,” J. Chem. Phys.
128
, 214502
(2008
).40.
R.
Zwangzig
and R. D.
Mountain
, “High-frequency elastic moduli of simple fluids
,” J. Chem. Phys.
43
, 4464
–4471
(1965
).41.
H.
Yamura
, M.
Matsukawa
, T.
Otani
, and N.
Ohtori
, “Brillouin scattering study on the elastic properties of epoxy adhesive layer
,” Jpn. J. Appl. Phys.
38
, 3175
–3178
(1999
).42.
J. K.
Kruger
, J.
Baller
, T.
Britz
, A.
le Coutre
, R.
Peter
, R.
Bactavatchalou
, and J.
Schreiber
, “Cauchy-like relation between elastic constants in amorphous materials
,” Phys. Rev. B
66
, 012206
(2002
).43.
L. L.
Stevens
, D. M.
Dattelbaum
, M.
Ahart
, and R. J.
Hemley
, “High-pressure elastic properties of a fluorinated copolymer: Poly(chlorotrifluoroethylene-co-vinylidene fluoride) (Kel-F 800)
,” J. Appl. Phys.
112
(2
), 023523
(2012
).44.
L. L.
Stevens
, E. B.
Orler
, D. M.
Dattelbaum
, M.
Ahart
, and R. J.
Hemley
, “Brillouin-scattering determination of the acoustic properties and their pressure dependence for three polymeric elastomers
,” J. Chem. Phys.
127
(10
), 104906
(2007
).45.
V. N.
Novikov
, Y.
Ding
, and A. P.
Sokolov
, “Correlation of fragility of supercooled liquids with elastic properties of glasses
,” Phys. Rev. E
71
, 061501
(2005
).46.
C.-S.
Zha
, R. J.
Hemley
, S. A.
Gramsch
, H.-K.
Mao
, and W. A.
Bassett
, “Optical study of H2O ice to 120 GPa: Dielectric function, molecular polarizability, and equation of state
,” J. Chem. Phys.
126
, 074506
(2007
).47.
Y.
Gu
, Y.
Zhou
, H.
Tang
, E. W.
Rothe
, and G. P.
Reck
, “Pressure dependence of vibrational Raman scattering of narrow-band, 248-nm, laser light by H2, N2, O2, CO2, CH4, C2H6, and C3H8 as high as 97 bar
,” Appl. Phys.: Lasers Opt.
71
, 865
–871
(2000
).48.
M.
Ahart
, J. L.
Yarger
, K. M.
Lantzky
, S.
Nakano
, H.-K.
Mao
, and R. J.
Hemley
, “High-pressure Brillouin scattering of amorphous BeH2
,” J. Chem. Phys.
124
, 014502
(2006
).49.
M.
Ahart
and R. J.
Hemley
, “Sound velocity and equation of state of ballistic gelatin by Brillouin scattering
,” Materials
16
, 1279
(2023
).50.
S.
Corezzi
, S.
Caponi
, F.
Rossi
, and D.
Fioretto
, “Stress-induced modification of the boson peak scaling behavior
,” J. Phys. Chem. B
117
, 14477
–14485
(2013
).51.
S.
Kojima
, “Mixed-alkali effect in borate glasses: Thermal, elastic, and vibrational properties
,” Solids
1
, 16
–30
(2020
).52.
M.
Maczka
, J.
Hanuza
, J.
Baran
, A.
Hushur
, and S.
Kojima
, “Heat capacity, Raman, and Brillouin scattering studies of M2O–MgO–WO3–P2O5 glasses (M = K, Rb)
,” J. Chem. Phys.
125
, 244503
(2006
).© 2023 Author(s). Published under an exclusive license by AIP Publishing.
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