The topic of thixotropy has historically received much attention due to its importance in a wide range of complex fluids and their applications. However, a thorough understanding of the phenomenon and how to model it remain outstanding challenges. In this work, we examine two materials that exhibit phenomenology often referred to as thixotropic through the lens of stress-controlled recovery rheology. When subjected to an oscillatory shear stress, the materials, an aqueous surfactant system that structurally forms multilamellar vesicles as well as a frequently studied fumed silica suspension, show a transient increase in the resulting strain amplitude. We use both creep and oscillatory tests in conjunction with recovery rheology to measure the elastic and viscous contributions to flow and deformation and find that the elastic contributions remain constant, even at larger amplitudes where nonlinear responses are induced. We conclude that the observed behavior is, therefore, strictly a viscous phenomenon, in contrast with common modeling efforts that describe both the viscous and elastic behaviors as being transient. We additionally examine how typical use of the dynamic moduli can give a misleading description of the material’s behavior, whereas examination of the energetic contributions provides a description consistent with the recovery measurements.
REFERENCES
1.
2.
Schalek
, E.
, and A.
Szegvari
, “Die langsame Koagulation konzentrierter Eisenoxydsole zu reversiblen Gallerten
,” Kolloid-Z.
33
, 326
–334
(1923
). 3.
Péterfi
, T.
, “Die Abhebung der Befruchtungsmembran bei Seeigeleiern
,” Wilhelm Roux' Arch. Entwicklungsmech. Org.
112
, 660
–695
(1927
). 4.
Freundlich
, H.
, “Ueber thixotropie
,” Kolloid-Z.
46
, 289
–299
(1928
). 5.
Mewis
, J.
, “Thixotropy—A general review
,” J. Nonnewton. Fluid Mech.
6
, 1
–20
(1979
). 6.
Bauer
, W. H.
, and E. A.
Collins
, “Thixotropy and dilatancy
,” in Rheology
(Academic
, 1967
), pp. 423–459. 7.
Barnes
, H. A.
, “Thixotropy—A review
,” J. Nonnewton. Fluid Mech.
70
, 1
–33
(1997
). 8.
Mewis
, J.
, and N. J.
Wagner
, “Thixotropy
,” Adv. Colloid Interface Sci.
147–148
, 214
–227
(2009
). 9.
Larson
, R. G.
, and Y.
Wei
, “A review of thixotropy and its rheological modeling
,” J. Rheol.
63
, 477
–501
(2019
). 10.
Willenbacher
, N.
, “Unusual thixotropic properties of aqueous dispersions of Laponite RD
,” J. Colloid Interface Sci.
182
, 501
–510
(1996
). 11.
Singh
, P. K.
, C. J.
Lee
, K. A.
Patankar
, and S. A.
Rogers
, “Revisiting the basis of transient rheological material functions: Insights from recoverable strain measurements
,” J. Rheol.
65
, 129
–144
(2021
). 12.
Shim
, Y. H.
, J. J.
Griebler
, and S. A.
Rogers
, “A reexamination of the Cox–Merz rule through the lens of recovery rheology
,” J. Rheol.
68
, 381
–396
(2024
). 13.
Scott Blair
, G. W.
, “An extension of Reiner’s ‘Deborah number’ concept to a Wide field of rheological investigations
,” Rheol. Acta
12
, 319
–320
(1973
). 14.
Horner
, J. S.
, M. J.
Armstrong
, N. J.
Wagner
, and A. N.
Beris
, “Measurements of human blood viscoelasticity and thixotropy under steady and transient shear and constitutive modeling thereof
,” J. Rheol.
63
, 799
–813
(2019
). 15.
Apostolidis
, A. J.
, M. J.
Armstrong
, and A. N.
Beris
, “Modeling of human blood rheology in transient shear flows
,” J. Rheol.
59
, 275
–298
(2015
). 16.
Armstrong
, M. J.
, A. N.
Beris
, S. A.
Rogers
, and N. J.
Wagner
, “Dynamic shear rheology and structure kinetics modeling of a thixotropic carbon black suspension
,” Rheol. Acta
56
, 811
–824
(2017
). 17.
Beris
, A. N.
, E.
Stiakakis
, and D.
Vlassopoulos
, “A thermodynamically consistent model for the thixotropic behavior of concentrated star polymer suspensions
,” J. Non-Newtonian Fluid Mech.
152
, 76
–85
(2008
). 18.
de Souza Mendes
, P. R.
, and R. L.
Thompson
, “A critical overview of elasto-viscoplastic thixotropic modeling
,” J. Nonnewton. Fluid Mech.
187–188
, 8
–15
(2012
). 19.
Ewoldt
, R. H.
, and G. H.
McKinley
, “Mapping thixo-elasto-visco-plastic behavior
,” Rheol. Acta
56
, 195
–210
(2017
). 20.
Jamali
, S.
, G. H.
McKinley
, and R. C.
Armstrong
, “Microstructural rearrangements and their rheological implications in a model thixotropic elastoviscoplastic fluid
,” Phys. Rev. Lett.
118
, 048003
(2017
). 21.
Wei
, Y.
, M. J.
Solomon
, and R. G.
Larson
, “A multimode structural kinetics constitutive equation for the transient rheology of thixotropic elasto-viscoplastic fluids
,” J. Rheol.
62
, 321
–342
(2018
). 22.
Sharma
, S.
, V.
Shankar
, and Y. M.
Joshi
, “Viscoelasticity and rheological hysteresis
,” J. Rheol.
67
, 139
–155
(2023
). 23.
Dinkgreve
, M.
, M. M.
Denn
, and D.
Bonn
, “‘Everything flows?’: Elastic effects on startup flows of yield-stress fluids
,” Rheol. Acta
56
, 189
–194
(2017
). 24.
Coussot
, P.
, and S. A.
Rogers
, “Oldroyd’s model and the foundation of modern rheology of yield stress fluids
,” J. Nonnewton. Fluid Mech.
295
, 104604
(2021
). 25.
26.
Casson
, N.
, “Flow equation for pigment-oil suspensions of the printing ink-type
,” in Rheology of Disperse Systems
(Pergamon
, Oxford, 1959
), pp. 84
–104
.27.
Herschel
, W. H.
, and R.
Bulkley
, “Konsistenzmessungen von Gummi-Benzollösungen
,” Kolloid-Z.
39
, 291
–300
(1926
). 28.
Saramito
, P.
, “A new constitutive equation for elastoviscoplastic fluid flows
,” J. Nonnewton. Fluid Mech.
145
, 1
–14
(2007
). 29.
Dinkgreve
, M.
, J.
Paredes
, M. M.
Denn
, and D.
Bonn
, “On different ways of measuring ‘the’ yield stress
,” J. Nonnewton. Fluid Mech.
238
, 233
–241
(2016
). 30.
Barnes
, H. A.
, and K.
Walters
, “The yield stress myth?
,” Rheol. Acta
24
, 323
–326
(1985
). 31.
Barnes
, H. A.
, “The ‘yield stress myth?’ paper—21 years on
,” Appl. Rheol.
17
, 43110-1
–43110-5
(2007
). 32.
Bonn
, D.
, M. M.
Denn
, L.
Berthier
, T.
Divoux
, and S.
Manneville
, “Yield stress materials in soft condensed matter
,” Rev. Mod. Phys.
89
, 1
–44
(2017
). 33.
Hartnett
, J. P.
, and R. Y. Z.
Hu
, “Technical note: The yield stress—An engineering reality
,” J. Rheol.
33
, 671
–679
(1989
). 34.
Barnes
, H. A.
, “The yield stress—A review or ‘παντα ρει’—everything flows?
,” J. Nonnewton. Fluid Mech.
81
, 133
–178
(1999
). 35.
Donley
, G. J.
, P. K.
Singh
, A.
Shetty
, and S. A.
Rogers
, “Elucidating the G″ overshoot in soft materials with a yield transition via a time-resolved experimental strain decomposition
,” Proc. Natl. Acad. Sci. U.S.A.
117
, 21945
–21952
(2020
). 36.
Kamani
, K.
, G. J.
Donley
, and S. A.
Rogers
, “Unification of the rheological physics of yield stress fluids
,” Phys. Rev. Lett.
126
, 218002
(2021
). 37.
Choi
, J.
, M.
Armstrong
, and S. A.
Rogers
, “The role of elasticity in thixotropy: Transient elastic stress during stepwise reduction in shear rate
,” Phys. Fluids
33
, 033112
(2021
). 38.
Hough
, L. A.
, D.
Bendejacq
, and T. J.
Fütterer
, “Characterization of multilamellar vesicles for cleansing applications
,” Cosmet. Toilet.
123
, 59
–66
(2008
).39.
Dullaert
, K.
, and J.
Mewis
, “A model system for thixotropy studies
,” Rheol. Acta
45
, 23
–32
(2005
). 40.
Dullaert
, K.
, and J.
Mewis
, “A structural kinetics model for thixotropy
,” J. Nonnewton. Fluid Mech.
139
, 21
–30
(2006
). 41.
Dullaert
, K.
, and J.
Mewis
, “Thixotropy: Build-up and breakdown curves during flow
,” J. Rheol.
49
, 1213
–1230
(2005
). 42.
Armstrong
, M. J.
, A. N.
Beris
, S. A.
Rogers
, and N. J.
Wagner
, “Dynamic shear rheology of a thixotropic suspension: Comparison of an improved structure-based model with large amplitude oscillatory shear experiments
,” J. Rheol.
60
, 433
–450
(2016
). 43.
Colombo
, G.
, S.
Kim
, T.
Schweizer
, B.
Schroyen
, C.
Clasen
, J.
Mewis
, and J.
Vermant
, “Superposition rheology and anisotropy in rheological properties of sheared colloidal gels
,” J. Rheol.
61
, 1035
–1048
(2017
). 44.
Wei
, Y.
, M. J.
Solomon
, and R. G.
Larson
, “Time-dependent shear rate inhomogeneities and shear bands in a thixotropic yield-stress fluid under transient shear
,” Soft Matter
15
, 7956
–7967
(2019
). 45.
Choi
, J.
, and S. A.
Rogers
, “Optimal conditions for pre-shearing thixotropic or aging soft materials
,” Rheol. Acta
59
, 921
–934
(2020
). 46.
Wei
, Y.
, M. J.
Solomon
, and R. G.
Larson
, “Quantitative nonlinear thixotropic model with stretched exponential response in transient shear flows
,” J. Rheol.
60
, 1301
–1315
(2016
). 47.
Schofield
, R. K.
, and G. W.
Scott Blair
, “The relationship between viscosity, elasticity and plastic strength of soft materials as illustrated by some mechanical properties of flour doughs, I
,” Proc. R. Soc. London, Ser. A
138
, 707
–718
(1932
).48.
Wesissenberg
, K.
, “A continuum theory of rheological phenomena
,” Nature
159
, 310
–311
(1947
). 49.
Reiner
, M.
, “Rheology
,” in Elasticity and Plasticity/Elastizität und Plastizität
(Springer
, Berlin
, 1958
), pp. 434
–550
. 50.
Di Dio
, B. F.
, F.
Khabaz
, R. T.
Bonnecaze
, and M.
Cloitre
, “Transient dynamics of soft particle glasses in startup shear flow. Part II: Memory and aging
,” J. Rheol.
66
, 717
–730
(2022
). 51.
Green
, H.
, and R.
Weltmann
, “Analysis of thixotropy of pigment-vehicle suspensions—Basic principles of the hysteresis loop
,” Ind. Eng. Chem. Anal. Ed.
15
, 201
–206
(1943
). 52.
Divoux
, T.
, V.
Grenard
, and S.
Manneville
, “Rheological hysteresis in soft glassy materials
,” Phys. Rev. Lett.
110
, 018304
(2013
). 53.
Coussot
, P.
, Q. D.
Nguyen
, H. T.
Huynh
, and D.
Bonn
, “Avalanche behavior in yield stress fluids
,” Phys. Rev. Lett.
88
, 175501
(2002
). 54.
Landrum
, B. J.
, W. B.
Russel
, and R. N.
Zia
, “Delayed yield in colloidal gels: Creep, flow, and re-entrant solid regimes
,” J. Rheol.
60
, 783
–807
(2016
). 55.
Sentjabrskaja
, T.
, P.
Chaudhuri
, M.
Hermes
, W. C. K.
Poon
, J.
Horbach
, S. U.
Egelhaaf
, and M.
Laurati
, “Creep and flow of glasses: Strain response linked to the spatial distribution of dynamical heterogeneities
,” Sci. Rep.
5
, 11884
(2015
). 56.
Rogers
, S. A.
, “Understanding the yielding behavior of graphene oxide colloids via experimental strain decomposition
,” Phys. Fluids
35
, 63117
(2023
). 57.
Moldenaers
, P.
, and J.
Mewis
, “Transient behavior of liquid crystalline solutions of poly(benzylglutamate)
,” J. Rheol.
30
, 567
–584
(1986
). 58.
de Souza Mendes
, P. R.
, “Modeling the thixotropic behavior of structured fluids
,” J. Nonnewton. Fluid Mech.
164
, 66
–75
(2009
). 59.
de Souza Mendes
, P. R.
, and R. L.
Thompson
, “A unified approach to model elasto-viscoplastic thixotropic yield-stress materials and apparent yield-stress fluids
,” Rheol. Acta
52
, 673
–694
(2013
). 60.
de Souza Mendes
, P. R.
, B.
Abedi
, and R. L.
Thompson
, “Constructing a thixotropy model from rheological experiments
,” J. Nonnewton. Fluid Mech.
261
, 1
–8
(2018
). 61.
Larson
, R. G.
, “Constitutive equations for thixotropic fluids
,” J. Rheol.
59
, 595
–611
(2015
). 62.
Lee
, J. C.-W.
, Y.-T.
Hong
, K. M.
Weigandt
, E. G.
Kelley
, H.
Kong
, and S. A.
Rogers
, “Strain shifts under stress-controlled oscillatory shearing in theoretical, experimental, and structural perspectives: Application to probing zero-shear viscosity
,” J. Rheol.
63
, 863
–881
(2019
). 63.
Hassager
, O.
, “Stress-controlled oscillatory flow initiated at time zero: A linear viscoelastic analysis
,” J. Rheol.
64
, 545
–550
(2020
). 64.
Tschoegl
, N. W.
, The Phenomenological Theory of Linear Viscoelastic Behavior
(Springer
, Berlin
, 1989
). You do not currently have access to this content.
