Dissipative systems often exhibit novel and unexpected properties. This is, for instance, the case of simple liquids, which, when subjected to shear and after reaching a steady state, can exhibit a negative entropy production over finite length scales and timescales. This result, among others, is captured by nonequilibrium relations known as fluctuation theorems. Using nonequilibrium molecular dynamics simulations, we examine how, by fine-tuning the properties of the components of a complex fluid, we can steer the nonequilibrium response of the fluid. More specifically, we show how we control the nonequilibrium probability distribution for the shear stress and, in turn, how often states with a negative entropy production can occur. To achieve this, we start by characterizing how the size for the liquid matrix impacts the probability of observing negative entropy states, as well as the timescale over which these can be observed. We then measure how the addition of larger particles to this liquid matrix, i.e., simulating a model colloidal suspension, results in an increase in the occurrence of such states. This suggests how modifications in the composition of the mixture and in the properties of its components lead to an increase in the probability of observing states of negative entropy production and, thus, for the system to run in reverse.

1.
C.
Bustamante
,
J.
Liphardt
, and
F.
Ritort
,
Phys. Today
58
(
7
),
43
(
2005
).
2.
D. J.
Evans
,
E. G. D.
Cohen
, and
G. P.
Morriss
,
Phys. Rev. Lett.
71
,
2401
(
1993
).
3.
D. J.
Evans
and
D. J.
Searles
,
Phys. Rev. E
50
,
1645
(
1994
).
4.
D. J.
Evans
and
D. J.
Searles
,
Adv. Phys.
51
,
1529
(
2002
).
5.
G.
Gallavotti
and
E. G. D.
Cohen
,
J. Stat. Phys.
80
,
931
(
1995
).
6.
G.
Gallavotti
and
E. G. D.
Cohen
,
Phys. Rev. Lett.
74
,
2694
(
1995
).
7.
G.
Gallavotti
,
Phys. Rev. Lett.
77
,
4334
(
1996
).
8.
D.
Ruelle
,
Am. J. Math.
98
,
619
(
1976
).
9.
10.
C.
Jarzynski
,
Phys. Rev. Lett.
78
,
2690
(
1997
).
11.
G. E.
Crooks
,
Phys. Rev. E
60
,
2721
(
1999
).
12.
S.
Ciliberto
and
C.
Laroche
,
J. Phys. IV
08
,
Pr6
(
1998
).
13.
G.
Wang
,
E. M.
Sevick
,
E.
Mittag
,
D. J.
Searles
, and
D. J.
Evans
,
Phys. Rev. Lett.
89
,
050601
(
2002
).
14.
A. N.
Gupta
,
A.
Vincent
,
K.
Neupane
,
H.
Yu
,
F.
Wang
, and
M. T.
Woodside
,
Nat. Phys.
7
,
631
(
2011
).
15.
S.
Ciliberto
,
Phys. Rev. X
7
,
021051
(
2017
).
16.
J. R.
Gomez-Solano
,
A.
Petrosyan
,
S.
Ciliberto
,
R.
Chetrite
, and
K.
Gawedzki
,
Phys. Rev. Lett.
103
,
040601
(
2009
).
17.
V.
Blickle
,
T.
Speck
,
C.
Lutz
,
U.
Seifert
, and
C.
Bechinger
,
Phys. Rev. Lett.
98
,
210601
(
2007
).
18.
P.
Reimann
,
C.
Van den Broeck
,
H.
Linke
,
P.
Hänggi
,
J.
Rubi
, and
A.
Pérez-Madrid
,
Phys. Rev. Lett.
87
,
010602
(
2001
).
19.
J.
Mehl
,
V.
Blickle
,
U.
Seifert
, and
C.
Bechinger
,
Phys. Rev. E
82
,
032401
(
2010
).
20.
J. R.
Gomez-Solano
,
A.
Petrosyan
,
S.
Ciliberto
, and
C.
Maes
,
J. Stat. Mech.: Theory Exp.
2011
,
P01008
.
21.
M.
Baiesi
,
S.
Ciliberto
,
G.
Falasco
, and
C.
Yolcu
,
Phys. Rev. E
94
,
022144
(
2016
).
22.
C.
Yolcu
,
A.
Bérut
,
G.
Falasco
,
A.
Petrosyan
,
S.
Ciliberto
, and
M.
Baiesi
,
J. Stat. Phys.
167
,
29
(
2017
).
23.
S.
Toyabe
,
T.
Sagawa
,
M.
Ueda
,
E.
Muneyuki
, and
M.
Sano
,
Nat. Phys.
6
,
988
(
2010
).
24.
A.
Bérut
,
A.
Arakelyan
,
A.
Petrosyan
,
S.
Ciliberto
,
R.
Dillenschneider
, and
E.
Lutz
,
Nature
483
,
187
(
2012
).
25.
26.
J. M. R.
Parrondo
,
J. M.
Horowitz
, and
T.
Sagawa
,
Nat. Phys.
11
,
131
(
2015
).
27.
D.
Collin
,
F.
Ritort
,
C.
Jarzynski
,
S. B.
Smith
,
I.
Tinoco
, and
C.
Bustamante
,
Nature
437
,
231
(
2005
).
28.
P.
Gaspard
,
J. Chem. Phys.
120
,
8898
(
2004
).
29.
K.
Hayashi
,
H.
Ueno
,
R.
Iino
, and
H.
Noji
,
Phys. Rev. Lett.
104
,
218103
(
2010
).
30.
D.
Lacoste
,
A.
Lau
, and
K.
Mallick
,
Phys. Rev. E
78
,
011915
(
2008
).
31.
P.
Maragakis
,
M.
Spichty
, and
M.
Karplus
,
J. Phys. Chem. B
112
,
6168
(
2008
).
32.
E. A.
Calzetta
,
Eur. Phys. J. B
68
,
601
(
2009
).
33.
P.
Ranjith
,
D.
Lacoste
,
K.
Mallick
, and
J.-F.
Joanny
,
Biophys. J.
96
,
2146
(
2009
).
34.
E.
Gerritsma
and
P.
Gaspard
,
Biophys. Rev.
05
,
163
(
2010
).
35.
S.
Nakamura
,
Y.
Yamauchi
,
M.
Hashisaka
,
K.
Chida
,
K.
Kobayashi
,
T.
Ono
,
R.
Leturcq
,
K.
Ensslin
,
K.
Saito
,
Y.
Utsumi
 et al.,
Phys. Rev. Lett.
104
,
080602
(
2010
).
36.
T.
Chou
,
K.
Mallick
, and
R. K. P.
Zia
,
Rep. Prog. Phys.
74
,
116601
(
2011
).
37.
G.
Verley
,
K.
Mallick
, and
D.
Lacoste
,
EPL (Europhys. Lett.)
93
,
10002
(
2011
).
38.
S.
Toyabe
,
T.
Watanabe-Nakayama
,
T.
Okamoto
,
S.
Kudo
, and
E.
Muneyuki
,
Proc. Natl. Acad. Sci. U. S. A.
108
,
17951
(
2011
).
39.
A.
Faggionato
and
D.
Di Pietro
,
J. Stat. Phys.
143
,
11
(
2011
).
40.
O.-P.
Saira
,
Y.
Yoon
,
T.
Tanttu
,
M.
Möttönen
,
D.
Averin
, and
J. P.
Pekola
,
Phys. Rev. Lett.
109
,
180601
(
2012
).
41.
S.
Joubaud
,
D.
Lohse
, and
D.
Van Der Meer
,
Phys. Rev. Lett.
108
,
210604
(
2012
).
42.
T.
Sagawa
and
M.
Ueda
,
Phys. Rev. Lett.
109
,
180602
(
2012
).
43.
J.
Gieseler
,
R.
Quidant
,
C.
Dellago
, and
L.
Novotny
,
Nat. Nanotechnol.
9
,
358
(
2014
).
44.
P.
Pietzonka
,
E.
Zimmermann
, and
U.
Seifert
,
EPL (Europhys. Lett.)
107
,
20002
(
2014
).
45.
S.
Toyabe
and
M.
Sano
,
J. Phys. Soc. Jpn.
84
,
102001
(
2015
).
46.
T. M.
Hoang
,
R.
Pan
,
J.
Ahn
,
J.
Bang
,
H.
Quan
, and
T.
Li
,
Phys. Rev. Lett.
120
,
080602
(
2018
).
47.
A. F.
Demirörs
,
M. T.
Akan
,
E.
Poloni
, and
A. R.
Studart
,
Soft Matter
14
,
4741
(
2018
).
48.
Y.
Luo
,
D. A.
Beller
,
G.
Boniello
,
F.
Serra
, and
K. J.
Stebe
,
Nat. Commun.
9
,
1
(
2018
).
49.
S.
Palagi
and
P.
Fischer
,
Nat. Rev. Mater.
3
,
113
(
2018
).
50.
J.
Palacci
,
S.
Sacanna
,
A. P.
Steinberg
,
D. J.
Pine
, and
P. M.
Chaikin
,
Science
339
,
936
(
2013
).
51.
J. D.
Weeks
,
D.
Chandler
, and
H. C.
Andersen
,
J. Chem. Phys.
54
,
5237
(
1971
).
52.
J.
Delhommelle
and
J.
Petravic
,
J. Chem. Phys.
123
,
074707
(
2005
).
53.
M. P.
Allen
and
D. J.
Tildesley
,
Computer Simulation of Liquids
(
Clarendon
,
Oxford
,
1987
).
54.
D.
Evans
and
G.
Morriss
,
Nonequilibrium Statistical Mechanics of Liquids
(
Cambridge University Press
,
Cambridge
,
2008
).
55.
W. G.
Hoover
,
D. J.
Evans
,
R. B.
Hickman
,
A. J. C.
Ladd
,
W. T.
Ashurst
, and
B.
Moran
,
Phys. Rev. A
22
,
1690
(
1980
).
56.
R.
Van Zon
and
E.
Cohen
,
Phys. Rev. Lett.
91
,
110601
(
2003
).
57.
J.
Kurchan
,
J. Phys. A: Math. Gen.
31
,
3719
(
1998
).
58.
59.
J. L.
Lebowitz
and
H.
Spohn
,
J. Stat. Phys.
95
,
333
(
1999
).
60.
C.
Giardina
,
J.
Kurchan
, and
L.
Peliti
,
Phys. Rev. Lett.
96
,
120603
(
2006
).
61.
J.
Delhommelle
and
D. J.
Evans
,
J. Chem. Phys.
115
,
43
(
2001
).
62.
J.
Delhommelle
,
J.
Petravic
, and
D. J.
Evans
,
Phys. Rev. E
68
,
031201
(
2003
).
63.
C.
Desgranges
and
J.
Delhommelle
,
Phys. Rev. B
78
,
184202
(
2008
).
64.
C.
Desgranges
and
J.
Delhommelle
,
J. Chem. Phys.
149
,
111101
(
2018
).
65.
C.
Desgranges
and
J.
Delhommelle
,
J. Chem. Phys.
153
,
054502
(
2020
).
66.
A. W.
Lees
and
S. F.
Edwards
,
J. Phys. C: Solid State Phys.
5
,
1921
(
1972
).
67.
J.
Towns
,
T.
Cockerill
,
M.
Dahan
,
I.
Foster
,
K.
Gaither
,
A.
Grimshaw
,
V.
Hazlewood
,
S.
Lathrop
,
D.
Lifka
,
G. D.
Peterson
etal.,
Comput. Sci. Eng.
16
,
62
(
2014
).
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