The interplay between short-range attractions and long-range repulsions (SALR) characterizes the so-called liquids with competing interactions, which are known to exhibit a variety of equilibrium and non-equilibrium phases. The theoretical description of the phenomenology associated with glassy or gel states in these systems has to take into account both the presence of thermodynamic instabilities (such as those defining the spinodal line and the so called λ line) and the limited capability to describe genuine non-equilibrium processes from first principles. Here, we report the first application of the non-equilibrium self-consistent generalized Langevin equation theory to the description of the dynamical arrest processes that occur in SALR systems after being instantaneously quenched into a state point in the regions of thermodynamic instability. The physical scenario predicted by this theory reveals an amazing interplay between the thermodynamically driven instabilities, favoring equilibrium macro- and micro-phase separation, and the kinetic arrest mechanisms, favoring non-equilibrium amorphous solidification of the liquid into an unexpected variety of glass and gel states.

1.
P. E.
Ramírez-González
and
M.
Medina-Noyola
,
Phys. Rev. E
82
,
061503
(
2010
).
2.
P. E.
Ramírez-González
and
M.
Medina-Noyola
,
Phys. Rev. E
82
,
061504
(
2010
).
3.
L. E.
Sánchez-Díaz
,
P. E.
Ramírez-González
, and
M.
Medina-Noyola
,
Phys. Rev. E
87
,
052306
(
2013
).
4.
Y.
Liu
and
Y.
Xi
,
Curr. Opin. Colloid Interface Sci.
39
,
123
(
2019
).
5.
Y.
Liu
,
L.
Porcar
,
J.
Chen
,
W.-R.
Chen
,
P.
Falus
,
A.
Faraone
,
E.
Fratini
,
K.
Hong
, and
P.
Baglioni
,
J. Phys. Chem. B
115
,
7238
7247
(
2011
).
6.
Y.
Zhuang
and
P.
Charbonneau
,
J. Phys. Chem. B
120
,
6178
(
2016
).
7.
J.
Ruiz-Franco
and
E.
Zaccarelli
,
Annu. Rev. Condens. Matter Phys.
12
,
51
(
2021
).
8.
J. D.
van der Waals
,
On the Continuity of the Gaseous and Liquid States
, Studies in Statistical Mechanics XIV, edited by
J. S.
Rowlinson
(
North-Holland
,
1988
).
10.
E. J. W.
Verwey
and
J. T. G.
Overbeek
,
Theory of the Stability of Lyophobic Colloids
(
Elsevier
,
Amsterdam
,
1948
).
B.
Derjaguin
10
,
333
(
1939
);
B.
Derjaguin
and
L.
Landau
Acta Physicochim. URSS
B. Derjaguin and L. Landau, ibid.
14
,
633
(
1941
).
12.
S.
Asakura
and
F.
Oosawa
,
J. Polym. Sci.
33
,
183
(
1958
).
13.
R. P.
Sear
and
W. M.
Gelbart
,
J. Chem. Phys.
110
,
4582
(
1999
).
14.
D.
Pini
,
G.
Jialin
,
A.
Parola
, and
L.
Reatto
,
Chem. Phys. Lett.
327
,
209
(
2000
).
15.
A.
Imperio
and
L.
Reatto
,
J. Phys.: Condens. Matter
16
,
S3769
(
2004
).
16.
Y.
Liu
,
W.-R.
Chen
, and
S.-H.
Chen
,
J. Chem. Phys.
122
,
044507
(
2005
).
17.
A. J.
Archer
,
D.
Pini
,
R.
Evans
, and
L.
Reatto
,
J. Chem. Phys.
126
,
014104
(
2007
).
18.
A. J.
Archer
,
C.
Ionescu
,
D.
Pini
, and
L.
Reatto
,
J. Phys.: Condens. Matter
20
,
415106
(
2008
).
19.
A. J.
Archer
,
Phys. Rev. E
78
,
031402
(
2008
).
20.
B.
Chacko
,
C.
Chalmers
, and
A. J.
Archer
,
J. Chem. Phys.
143
,
244904
(
2015
).
21.
J.
Schmalian
and
P. G.
Wolynes
,
Phys. Rev. Lett.
85
,
836
(
2000
).
22.
M.
Tarzia
and
A.
Coniglio
,
Phys. Rev. Lett.
96
,
075702
(
2006
).
23.
M.
Tarzia
and
A.
Coniglio
,
Phys. Rev. E
75
,
011410
(
2007
).
24.
Y.
Zhuang
,
K.
Zhang
, and
P.
Charbonneau
,
Phys. Rev. Lett.
116
,
098301
(
2016
).
25.
A.
de Candia
,
E.
DelGado
,
A.
Fierro
,
N.
Sator
,
M.
Tarzia
, and
A.
Coniglio
,
Phys. Rev. E
74
,
010403(R)
(
2006
).
26.
A.
Imperio
and
L.
Reatto
,
J. Chem. Phys.
124
,
164712
(
2006
).
27.
A. J.
Archer
and
N. B.
Wilding
,
Phys. Rev. E
76
,
031501
(
2007
).
28.
P. D.
Godfrin
,
N. E.
Valadez-Pérez
,
R.
Castañeda-Priego
,
N. J.
Wagner
, and
Y.
Liu
,
Soft Matter
10
,
5061
(
2014
).
29.
J.
Groenewold
and
W. K.
Kegel
,
J. Phys. Chem. B
105
,
11702
(
2001
).
30.
J.
Groenewold
and
W. K.
Kegel
,
J. Phys.: Condens. Matter
16
,
S4877
(
2004
).
31.
J.
Wu
,
Y.
Liu
,
W.-R.
Chen
,
J.
Cao
, and
S.-H.
Chen
,
Phys. Rev. E
70
,
050401
(
2004
).
32.
A.
Coniglio
,
L.
De Arcangelis
,
E.
Del Gado
,
A.
Fierro
, and
N.
Sator
,
J. Phys.: Condens. Matter
16
,
S4831
(
2004
).
33.
F.
Sciortino
,
S.
Mossa
,
E.
Zaccarelli
, and
P.
Tartaglia
,
Phys. Rev. Lett.
93
,
055701
(
2004
).
34.
S.
Mossa
,
F.
Sciortino
,
P.
Tartaglia
, and
E.
Zaccarelli
,
Langmuir
20
,
10756
(
2004
).
35.
F.
Sciortino
,
P.
Tartaglia
, and
E.
Zaccarelli
,
J. Phys. Chem. B
109
,
21942
(
2005
).
36.
P.
Charbonneau
and
D. R.
Reichman
,
Phys. Rev. E
75
,
050401(R)
(
2007
).
37.
J. A.
Bollinger
and
T. M.
Truskett
,
J. Chem. Phys.
145
,
064902
(
2016
).
38.
B. A.
Lindquist
,
S.
Dutta
,
R. B.
Jadrich
,
D. J.
Milliron
, and
T. M.
Truskett
,
Soft Matter
13
,
1335
(
2017
).
39.
H.
Sedgwick
,
S. U.
Egelhaaf
, and
W. C. K.
Poon
,
J. Phys.: Condens. Matter
16
,
S4913
(
2004
).
40.
A.
Stradner
,
H.
Sedgwick
,
F.
Cardinaux
,
W. C. K.
Poon
,
S. U.
Egelhaaf
, and
P.
Schurtenberger
,
Nature
432
,
492
(
2004
).
41.
F.
Bordi
,
C.
Cametti
,
M.
Diociaiuti
, and
S.
Sennato
,
Phys. Rev. E
71
,
050401(R)
(
2005
).
42.
A. I.
Campbell
,
V. J.
Anderson
,
J. S.
van Duijneveldt
, and
P.
Bartlett
,
Phys. Rev. Lett.
94
,
208301
(
2005
).
43.
C. J.
Dibble
,
M.
Kogan
, and
M. J.
Solomon
,
Phys. Rev. E
74
,
041403
(
2006
).
44.
C. L.
Klix
,
C. P.
Royall
, and
H.
Tanaka
,
Phys. Rev. Lett.
104
,
165702
(
2010
).
45.
M.
Mézard
and
G.
Parisi
,
Phys. Rev. Lett.
82
,
747
(
1999
).
46.
M.
Grousson
,
V.
Krakoviack
,
G.
Tarjus
, and
P.
Viot
,
Phys. Rev. E
66
,
026126
(
2002
).
47.
P. L.
Geissler
and
D. R.
Reichman
,
Phys. Rev. E
69
,
021501
(
2004
).
48.
W.
Götze
, in
Liquids, Freezing and Glass Transition
, edited by
J. P.
Hansen
,
D.
Levesque
, and
J.
Zinn-Justin
(
North-Holland
,
Amsterdam
,
1991
).
49.
W.
Götze
and
L.
Sjögren
,
Rep. Prog. Phys.
55
,
241
(
1992
).
50.
L.
Berthier
and
G.
Biroli
,
Rev. Mod. Phys.
83
,
587
(
2011
).
51.
L.
Yeomans-Reyna
and
M.
Medina-Noyola
,
Phys. Rev. E
64
,
066114
(
2001
).
52.
L.
Yeomans-Reyna
,
H.
Acuña-Campa
,
F.
Guevara-Rodríguez
, and
M.
Medina-Noyola
,
Phys. Rev. E
67
,
021108
(
2003
).
53.
R.
Juárez-Maldonado
 et al,
Phys. Rev. E
76
,
062502
(
2007
).
54.
M. A.
Chávez-Rojo
and
M.
Medina-Noyola
,
Physica A
366
,
55
(
2006
).
55.
M. A.
Chávez-Rojo
and
M.
Medina-Noyola
,
Phys. Rev. E
72
,
031107
(
2005
);
M. A.
Chávez-Rojo
and
M.
Medina-Noyola
Phys. Rev. E
76, 039902 (2007).
56.
L.
Yeomans-Reyna
,
M. A.
Chávez-Rojo
,
P. E.
Ramírez-González
,
R.
Juárez-Maldonado
,
M.
Chávez-Páez
, and
M.
Medina-Noyola
,
Phys. Rev. E
76
,
041504
(
2007
).
57.
R.
Juárez-Maldonado
and
M.
Medina-Noyola
,
Phys. Rev. E
77
,
051503
(
2008
).
58.
L. E.
Sánchez-Díaz
,
A.
Vizcarra-Rendón
, and
R.
Juárez-Maldonado
,
Phys. Rev. Lett.
103
,
035701
(
2009
).
59.
L. F.
Elizondo-Aguilera
and
Th.
Voigtmann
,
Phys. Rev. E
100
,
042601
(
2019
).
60.
P. E.
Ramírez-González
and
M.
Medina-Noyola
,
J. Phys.: Condens. Matter
21
,
504103
(
2009
).
61.
62.
63.
L.
Onsager
and
S.
Machlup
,
Phys. Rev.
91
,
1505
(
1953
).
64.
S.
Machlup
and
L.
Onsager
,
Phys. Rev.
91
,
1512
(
1953
).
65.
R.
Peredo-Ortiz
,
M.
Medina-Noyola
,
T.
Voigtmann
, and
L. F.
Elizondo-Aguilera
,
J. Chem. Phys.
156
,
244506
(
2022
).
66.
G.
Pérez-Ángel
,
L. E.
Sánchez-Díaz
,
P. E.
Ramírez-González
,
R.
Juárez-Maldonado
,
A.
Vizcarra-Rendón
, and
M.
Medina-Noyola
,
Phys. Rev. E
83
,
060501(R)
(
2011
).
67.
P.
Mendoza-Méndez
,
E.
Lázaro-Lázaro
,
L. E.
Sánchez-Díaz
,
P. E.
Ramírez-González
,
G.
Pérez-Ángel
, and
M.
Medina-Noyola
,
Phys. Rev. E
96
,
022608
(
2017
).
68.
J. M.
Olais-Govea
,
L.
López-Flores
, and
M.
Medina-Noyola
,
J. Chem. Phys.
143
,
174505
(
2015
).
69.
J. M.
Olais-Govea
,
L.
López-Flores
, and
M.
Medina-Noyola
,
Phys. Rev. E
98
,
040601(R)
(
2018
).
70.
J. M.
Olais-Govea
,
L.
López-Flores
,
J. B.
Zepeda-López
, and
M.
Medina-Noyola
,
Sci. Rep.
9
,
16445
(
2019
).
71.
J. B.
Zepeda-López
and
M.
Medina-Noyola
,
J. Chem. Phys.
154
,
174901
(
2021
).
72.
L. E.
Sánchez-Díaz
,
E.
Lázaro-Lázaro
,
J. M.
Olais-Govea
, and
M.
Medina-Noyola
,
J. Chem. Phys.
140
,
234501
(
2014
).
73.
T.
Voigtmann
,
Europhys. Lett.
96
,
36006
(
2011
).
74.
E.
Lázaro-Lázaro
 et al,
Phys. Rev. E
99
,
042603
(
2019
).
75.
P. E.
Ramírez-González
,
L. E.
Sánchez-Díaz
,
M.
Medina-Noyola
, and
Y.
Wang
,
J. Chem. Phys.
145
,
191101
(
2016
).
76.
L. F.
Elizondo-Aguilera
,
P. F.
Zubieta-Rico
,
H.
Ruíz Estrada
, and
O.
Alarcón-Waess
,
Phys. Rev. E
90
,
052301
(
2014
).
77.
E. C.
Cortés-Morales
,
L. F.
Elizondo-Aguilera
, and
M.
Medina-Noyola
,
J. Phys. Chem. B
120
,
7975
(
2016
).
78.
R.
Peredo-Ortiz
,
P. F.
Zubieta Rico
,
E. C.
Cortés-Morales
,
G. G.
Pérez-Ángel
,
T.
Voigtmann
,
M.
Medina-Noyola
, and
L. F.
Elizondo-Aguilera
,
J. Phys.: Condens. Matter
34
,
084003
(
2022
).
79.
L. F.
Elizondo-Aguilera
,
E. C.
Cortés-Morales
,
P. F.
Zubieta Rico
,
M.
Medina-Noyola
,
R.
Castañeda-Priego
,
T.
Voigtmann
, and
G.
Pérez-Ángel
,
Soft Matter
16
,
170
(
2020
).
80.

The short-time self-diffusion coefficient D0 is related by Einstein’s relation, D0 = kBT/ζ0, with ζ0 being the corresponding short-time friction coefficient [determined by its Stokes expression81 in colloidal liquids or by the kinetic (or “Doppler”82) friction coefficient in the case of molecular liquids83].

81.
L. D.
Landau
and
E. M.
Lifshitz
,
Fluid Mechanics
(
Pergamon
,
New York
,
1959
).
82.
G. E.
Uhlenbeck
and
L. S.
Ornstein
,
Phys. Rev.
36
,
823
(
1930
).
83.
L.
López-Flores
,
P.
Mendoza-Méndez
,
L. E.
Sánchez-Díaz
,
L. L.
Yeomans-Reyna
,
A.
Vizcarra-Rendón
,
G.
Pérez-Ángel
,
M.
Chávez-Páez
, and
M.
Medina-Noyola
,
Europhys. Lett.
99
,
46001
(
2012
).
84.
D. A.
McQuarrie
.
Statistical Mechanics
(
Harper and Row
,
1973
).
86.
J. K.
Percus
and
G. J.
Yevick
,
Phys. Rev.
110
,
1
(
1957
).
87.
L.
Verlet
and
J.-J.
Weis
,
Phys. Rev. A
5
,
939
(
1972
).
88.
89.
F. de J.
Guevara-Rodríguez
and
M.
Medina-Noyola
,
Phys. Rev. E
68
,
011405
(
2003
).
90.
P. E.
Ramírez-González
,
L.
López-Flores
,
H.
Acuña-Campa
, and
M.
Medina-Noyola
,
Phys. Rev. Lett.
107
,
155701
(
2011
).
91.
L.
López-Flores
,
H.
Ruíz-Estrada
,
M.
Chávez-Páez
, and
M.
Medina-Noyola
,
Phys. Rev. E.
88
,
042301
(
2013
).
92.
H. M.
Lindsay
and
P. M.
Chaikin
,
J. Chem. Phys.
76
,
3774
(
1982
).
93.
E. B.
Sirota
,
H. D.
Ou-Yang
,
S. K.
Sinha
,
P. M.
Chaikin
,
J. D.
Axe
, and
Y.
Fujii
,
Phys. Rev. Lett.
62
,
1524
1527
(
1989
).
You do not currently have access to this content.