Colloidal glasses are out-of-equilibrium in nature. When such materials are quenched from a shear-melted state into a quiescent one, their structure freezes due to entropic caging of the constituents. However, thermal fluctuations allow slow structural evolution, a process known as aging, in favor of minimizing free energy. Here, we examine the rheological signatures of aging, in a model system of nearly hard sphere colloidal glass. Subtle changes in the linear viscoelastic properties are detected with the age of the colloidal glass where viscous modulus shows a decrease with aging whereas the elastic modulus remains unaffected. This is associated with the slowing-down of long-time out-of-cage dynamics as the glass ages. On the contrary, nonlinear rheological measurements such as start-up shear flow, stress relaxation, and creep experiments show a strong dependence on sample age. Moreover, creep and stress relaxation experiments show ample evidence of avalanche type processes that occur during aging of colloidal glasses. Finally, comparison of creep and start-up shear flow measurements indicate that the latter is more energy efficient in inducing flow in colloidal glasses irrespective of aging dynamics.

1.
R.
Zargar
,
B.
Nienhuis
,
P.
Schall
, and
D.
Bonn
, “
Direct measurement of the free energy of aging hard sphere colloidal glasses
,”
Phys. Rev. Lett.
110
,
258301
(
2013
).
2.
Y. M.
Joshi
and
G.
Petekidis
, “
Yield stress fluids and ageing
,”
Rheol. Acta
57
,
521
549
(
2018
).
3.
Y. M.
Joshi
, “
Dynamics of colloidal glasses and gels
,”
Annu. Rev. Chem. Biomol. Eng.
5
,
181
202
(
2014
).
4.
L. C. E.
Struik
,
Physical Aging in Amorphous Polymers and Other Materials
(
Elsevier
,
1978
).
5.
G. B.
McKenna
,
T.
Narita
, and
F.
Lequeux
, “
Soft colloidal matter: A phenomenological comparison of the aging and mechanical responses with those of molecular glasses
,”
J. Rheol.
53
,
489
516
(
2009
).
6.
P. A.
O’Connell
and
G. B.
McKenna
, “
Large deformation response of polycarbonate: Time-temperature, time-aging time, and time-strain superposition
,”
Polym. Eng. Sci.
37
,
1485
1495
(
1997
).
7.
C. A.
Angell
,
K. L.
Ngai
,
G. B.
McKenna
,
P. F.
McMillan
, and
S. W.
Martin
, “
Relaxation in glass forming liquids and amorphous solids
,”
J. Appl. Phys.
88
,
3113
3157
(
2000
).
8.
R.
Angelini
,
E.
Zaccarelli
,
F.
De Melo Marques
,
M.
Sztucki
,
A.
Fluerasu
,
G.
Ruocco
, and
B.
Ruzicka
, “
Glass-glass transition during aging of a colloidal clay
,”
Nat. Commun.
5
,
4049
(
2014
).
9.
N.
Koumakis
,
A. B.
Schofield
, and
G.
Petekidis
, “
Effects of shear induced crystallization on the rheology and ageing of hard sphere glasses
,”
Soft Matter
4
,
2008
2018
(
2008
).
10.
M.
Bellour
,
A.
Knaebel
,
J. L.
Harden
,
F.
Lequeux
, and
J.-P.
Munch
, “
Aging processes and scale dependence in soft glassy colloidal suspensions
,”
Phys. Rev. E
67
,
031405
(
2003
).
11.
M.
Kaushal
and
Y. M.
Joshi
, “
Linear viscoelasticity of soft glassy materials
,”
Soft Matter
10
,
1891
1894
(
2014
).
12.
L. C.
Johnson
,
E.
Moghimi
,
G.
Petekidis
, and
R. N.
Zia
, “
Influence of structure on the linear response rheology of colloidal gels
,”
J. Rheol.
63
,
583
608
(
2019
).
13.
N.
Koumakis
and
G.
Petekidis
, “
Two step yielding in attractive colloids: Transition from gels to attractive glasses
,”
Soft Matter
7
,
2456
2470
(
2011
).
14.
A.
Fluerasu
,
A.
Moussaïd
,
A.
Madsen
, and
A.
Schofield
, “
Slow dynamics and aging in colloidal gels studied by x-ray photon correlation spectroscopy
,”
Phys. Rev. E
76
,
010401
(
2007
).
15.
N.
Koumakis
,
E.
Moghimi
,
R.
Besseling
,
W. C. K.
Poon
,
J. F.
Brady
, and
G.
Petekidis
, “
Tuning colloidal gels by shear
,”
Soft Matter
11
,
4640
4648
(
2015
).
16.
E.
Moghimi
,
A. R.
Jacob
,
N.
Koumakis
, and
G.
Petekidis
, “
Colloidal gels tuned by oscillatory shear
,”
Soft Matter
13
,
2371
2383
(
2017
).
17.
W.
van Megen
,
T. C.
Mortensen
,
S. R.
Williams
, and
J.
Müller
, “
Measurement of the self-intermediate scattering function of suspensions of hard spherical particles near the glass transition
,”
Phys. Rev. E
58
,
6073
6085
(
1998
).
18.
V. A.
Martinez
,
G.
Bryant
, and
W.
van Megen
, “
Slow dynamics and aging of a colloidal hard sphere glass
,”
Phys. Rev. Lett.
101
,
135702
(
2008
).
19.
V. A.
Martinez
,
G.
Bryant
, and
W.
van Megen
, “
Aging dynamics of colloidal hard sphere glasses
,”
J. Chem. Phys.
133
,
114906
(
2010
).
20.
G.
Brambilla
,
D.
El Masri
,
M.
Pierno
,
L.
Berthier
,
L.
Cipelletti
,
G.
Petekidis
, and
A. B.
Schofield
, “
Probing the equilibrium dynamics of colloidal hard spheres above the mode-coupling glass transition
,”
Phys. Rev. Lett.
102
,
085703
(
2009
).
21.
D. E.
Masri
,
G.
Brambilla
,
M.
Pierno
,
G.
Petekidis
,
A. B.
Schofield
,
L.
Berthier
, and
L.
Cipelletti
, “
Dynamic light scattering measurements in the activated regime of dense colloidal hard spheres
,”
J. Stat. Mech.: Theory Exp.
2009
,
P07015
.
22.
N. B.
Simeonova
and
W. K.
Kegel
, “
Gravity-induced aging in glasses of colloidal hard spheres
,”
Phys. Rev. Lett.
93
,
035701
(
2004
).
23.
R. E.
Courtland
and
E. R.
Weeks
, “
Direct visualization of ageing in colloidal glasses
,”
J. Phys.: Condens. Matter
15
,
S359
(
2003
).
24.
S.
Golde
,
T.
Palberg
, and
H. J.
Schöpe
, “
Correlation between dynamical and structural heterogeneities in colloidal hard-sphere suspensions
,”
Nat. Phys.
12
,
712
(
2016
).
25.
W.
Kob
,
F.
Sciortino
, and
P.
Tartaglia
, “
Aging as dynamics in configuration space
,”
Europhys. Lett.
49
,
590
(
2000
).
26.
W.
Kob
,
J. L.
Barrat
,
F.
Sciortino
, and
P.
Tartaglia
, “
Aging in a simple glass former
,”
J. Phys.: Condens. Matter
12
,
6385
(
2000
).
27.
M.
Utz
,
P. G.
Debenedetti
, and
F. H.
Stillinger
, “
Atomistic simulation of aging and rejuvenation in glasses
,”
Phys. Rev. Lett.
84
,
1471
1474
(
2000
).
28.
L.
Ramos
and
L.
Cipelletti
, “
Ultraslow dynamics and stress relaxation in the aging of a soft glassy system
,”
Phys. Rev. Lett.
87
,
245503
(
2001
).
29.
L.
Ramos
and
L.
Cipelletti
, “
Intrinsic aging and effective viscosity in the slow dynamics of a soft glass with tunable elasticity
,”
Phys. Rev. Lett.
94
,
158301
(
2005
).
30.
S.
Mazoyer
,
L.
Cipelletti
, and
L.
Ramos
, “
Origin of the slow dynamics and the aging of a soft glass
,”
Phys. Rev. Lett.
97
,
238301
(
2006
).
31.
O.
Lieleg
,
J.
Kayser
,
G.
Brambilla
,
L.
Cipelletti
, and
A. R.
Bausch
, “
Slow dynamics and internal stress relaxation in bundled cytoskeletal networks
,”
Nat. Mater.
10
,
236
(
2011
).
32.
N.
Koumakis
,
M.
Laurati
,
A. R.
Jacob
,
K. J.
Mutch
,
A.
Abdellali
,
A. B.
Schofield
,
S. U.
Egelhaaf
,
J. F.
Brady
, and
G.
Petekidis
, “
Start-up shear of concentrated colloidal hard spheres: Stresses, dynamics, and structure
,”
J. Rheol.
60
,
603
623
(
2016
).
33.
P.
Ballesta
and
G.
Petekidis
, “
Creep and aging of hard-sphere glasses under constant stress
,”
Phys. Rev. E
93
,
042613
(
2016
).
34.
M.
Siebenbürger
,
M.
Ballauff
, and
T.
Voigtmann
, “
Creep in colloidal glasses
,”
Phys. Rev. Lett.
108
,
255701
(
2012
).
35.
Y. M.
Joshi
, “
A model for aging under deformation field, residual stresses and strains in soft glassy materials
,”
Soft Matter
11
,
3198
3214
(
2015
).
36.
A. R.
Jacob
,
A. S.
Poulos
,
S.
Kim
,
J.
Vermant
, and
G.
Petekidis
, “
Convective cage release in model colloidal glasses
,”
Phys. Rev. Lett.
115
,
218301
(
2015
).
37.
E.
Moghimi
,
J.
Vermant
, and
G.
Petekidis
, “
Orthogonal superposition rheometry of model colloidal glasses with short-ranged attractions
,”
J. Rheol.
63
,
533
546
(
2019
).
38.
N.
Koumakis
,
J. F.
Brady
, and
G.
Petekidis
, “
Complex oscillatory yielding of model hard-sphere glasses
,”
Phys. Rev. Lett.
110
,
178301
(
2013
).
39.
P.
Ballesta
,
R.
Besseling
,
L.
Isa
,
G.
Petekidis
, and
W. C. K.
Poon
, “
Slip and flow of hard-sphere colloidal glasses
,”
Phys. Rev. Lett.
101
,
258301
(
2008
).
40.
P.
Ballesta
,
G.
Petekidis
,
L.
Isa
,
W. C. K.
Poon
, and
R.
Besseling
, “
Wall slip and flow of concentrated hard-sphere colloidal suspensions
,”
J. Rheol.
56
,
1005
1037
(
2012
).
41.
P.
Ballesta
,
N.
Koumakis
,
R.
Besseling
,
W. C.
Poon
, and
G.
Petekidis
, “
Slip of gels in colloid–polymer mixtures under shear
,”
Soft Matter
9
,
3237
3245
(
2013
).
42.
R.
Besseling
,
L.
Isa
,
P.
Ballesta
,
G.
Petekidis
,
M. E.
Cates
, and
W. C. K.
Poon
, “
Shear banding and flow-concentration coupling in colloidal glasses
,”
Phys. Rev. Lett.
105
,
268301
(
2010
).
43.
N.
Koumakis
,
A.
Pamvouxoglou
,
A.
Poulos
, and
G.
Petekidis
, “
Direct comparison of the rheology of model hard and soft particle glasses
,”
Soft Matter
8
,
4271
4284
(
2012
).
44.
N. J.
Wagner
and
J. F.
Brady
, “
Shear thickening in colloidal dispersions
,”
Phys. Today
62
(
10
),
27
32
(
2009
).
45.
J.
Mewis
and
N. J.
Wagner
,
Colloidal Suspension Rheology
(
Cambridge Series in Chemical Engineering
,
2012
).
46.
E. H.
Purnomo
,
D.
van den Ende
,
J.
Mellema
, and
F.
Mugele
, “
Rheological properties of aging thermosensitive suspensions
,”
Phys. Rev. E
76
,
021404
(
2007
).
47.
N.
Koumakis
,
M.
Laurati
,
S. U.
Egelhaaf
,
J. F.
Brady
, and
G.
Petekidis
, “
Yielding of hard-sphere glasses during start-up shear
,”
Phys. Rev. Lett.
108
,
098303
(
2012
).
48.
G.
Petekidis
,
A.
Moussaid
, and
P. N.
Pusey
, “
Rearrangements in hard-sphere glasses under oscillatory shear strain
,”
Phys. Rev. E
66
,
051402
(
2002
).
49.
J. M.
Brader
,
M.
Siebenbürger
,
M.
Ballauff
,
K.
Reinheimer
,
M.
Wilhelm
,
S. J.
Frey
,
F.
Weysser
, and
M.
Fuchs
, “
Nonlinear response of dense colloidal suspensions under oscillatory shear: Mode-coupling theory and Fourier transform rheology experiments
,”
Phys. Rev. E
82
,
061401
(
2010
).
50.
M.
Ballauff
,
J. M.
Brader
,
S. U.
Egelhaaf
,
M.
Fuchs
,
J.
Horbach
,
N.
Koumakis
,
M.
Krüger
,
M.
Laurati
,
K. J.
Mutch
,
G.
Petekidis
,
M.
Siebenbürger
,
T.
Voigtmann
, and
J.
Zausch
, “
Residual stresses in glasses
,”
Phys. Rev. Lett.
110
,
215701
(
2013
).
51.
E.
Moghimi
,
A. R.
Jacob
, and
G.
Petekidis
, “
Residual stresses in colloidal gels
,”
Soft Matter
13
,
7824
7833
(
2017
).
52.
T.
Sentjabrskaja
,
P.
Chaudhuri
,
M.
Hermes
,
W.
Poon
,
J.
Horbach
,
S.
Egelhaaf
, and
M.
Laurati
, “
Creep and flow of glasses: Strain response linked to the spatial distribution of dynamical heterogeneities
,”
Sci. Rep.
5
,
1884
(
2015
).
53.
C.
Baravian
,
G.
Benbelkacem
, and
F.
Caton
, “
Unsteady rheometry: Can we characterize weak gels with a controlled stress rheometer?
,”
Rheol. Acta
46
,
577
581
(
2007
).
54.
J.
Sprakel
,
S. B.
Lindström
,
T. E.
Kodger
, and
D. A.
Weitz
, “
Stress enhancement in the delayed yielding of colloidal gels
,”
Phys. Rev. Lett.
106
,
248303
(
2011
).
55.
T.
Sentjabrskaja
,
J.
Hendricks
,
A. R.
Jacob
,
G.
Petekidis
,
S. U.
Egelhaaf
, and
M.
Laurati
, “
Binary colloidal glasses under transient stress-and strain-controlled shear
,”
J. Rheol.
62
,
149
159
(
2018
).
56.
G.
Petekidis
,
D.
Vlassopoulos
, and
P. N.
Pusey
, “
Yielding and flow of sheared colloidal glasses
,”
J. Phys.: Condens. Matter
16
,
S3955
(
2004
).
57.
K. N.
Pham
,
G.
Petekidis
,
D.
Vlassopoulos
,
S. U.
Egelhaaf
,
W. C. K.
Poon
, and
P. N.
Pusey
, “
Yielding behavior of repulsion- and attraction-dominated colloidal glasses
,”
J. Rheol.
52
,
649
676
(
2008
).
58.
C. E.
Maloney
and
A.
Lemaître
, “
Amorphous systems in athermal, quasistatic shear
,”
Phys. Rev. E
74
,
016118
(
2006
).
59.
N. P.
Bailey
,
J.
Schiøtz
,
A.
Lemaître
, and
K. W.
Jacobsen
, “
Avalanche size scaling in sheared three-dimensional amorphous solid
,”
Phys. Rev. Lett.
98
,
095501
(
2007
).
60.
A.
Lemaître
and
C.
Caroli
, “
Rate-dependent avalanche size in athermally sheared amorphous solids
,”
Phys. Rev. Lett.
103
,
065501
(
2009
).
61.
J. L.
Barrat
and
A.
Lemaître
, “
Heterogeneities in amorphous systems under shear
,” in
Dynamical Heterogeneities in Glasses, Colloids and Granular Media
(
Oxford Science Publications
,
2011
).
62.
V.
Chikkadi
, “
Spatial correlations and deformation modes in sheared colloidal glasses
,” Ph.D. thesis,
Institute of Physics, University of Amsterdam
,
2011
.
63.
J.
Weiss
and
D.
Marsan
, “
Three-dimensional mapping of dislocation avalanches: Clustering and space/time coupling
,”
Science
299
,
89
92
(
2003
).
64.
P.
Coussot
,
Q. D.
Nguyen
,
H. T.
Huynh
, and
D.
Bonn
, “
Avalanche behavior in yield stress fluids
,”
Phys. Rev. Lett.
88
,
175501
(
2002
).
65.
E.
Sanz
,
C.
Valeriani
,
E.
Zaccarelli
,
W. C. K.
Poon
,
M. E.
Cates
, and
P. N.
Pusey
, “
Avalanches mediate crystallization in a hard-sphere glass
,”
Proc. Natl. Acad. Sci. U. S. A.
111
,
75
80
(
2014
).
You do not currently have access to this content.