We propose a minimal model for spherical proteins with aeolotopic pair interactions to describe the equilibrium phase behavior of lysozyme. The repulsive screened Coulomb interactions between the particles are taken into account assuming that the net charges are smeared out homogeneously over the spherical protein surfaces. We incorporate attractive surface patches, with the interactions between patches on different spheres modeled by an attractive Yukawa potential. The parameters entering the attractive Yukawa potential part are determined using information on the experimentally accessed gas-liquid-like critical point. The Helmholtz free energy of the fluid and solid phases is calculated using second-order thermodynamic perturbation theory. Our predictions for the solubility curve are in fair agreement with experimental data. In addition, we present new experimental data for the gas-liquid coexistence curves at various salt concentrations and compare these with our model calculations. In agreement with earlier findings, we observe that the strength and the range of the attractive potential part only weakly depend on the salt content.

1.
A.
McPherson
,
Crystallization of Biological Macromolecules
, 1st ed. (
Cold Spring Harbor
,
New York
,
1999
).
2.
R.
Cudney
,
S.
Patel
,
K.
Weisgraber
,
Y.
Newhouse
, and
A.
McPherson
,
Acta Crystallogr., Sect. D: Biol. Crystallogr.
50
,
414
(
1994
).
3.
E. J. W.
Verwey
and
J. T. G.
Overbeek
,
Theory of the Stability of Lyophobic Colloids
(
Dover
,
New York
,
2000
).
4.
G.
Pellicane
,
D.
Costa
, and
C.
Caccamo
,
J. Phys.: Condens. Matter
15
,
375
(
2003
).
5.
A.
Tardieu
,
A. L.
Verge
,
M.
Malfois
,
F.
Bonnete
,
S.
Finet
,
M.
Ries-Kautt
, and
L.
Belloni
,
J. Cryst. Growth
196
,
193
(
1999
).
6.
M.
Muschol
and
F.
Rosenberger
,
J. Chem. Phys.
103
,
10424
(
1995
).
7.
P.
Prinsen
and
T.
Odijk
,
J. Chem. Phys.
125
,
074903
(
2006
).
8.
9.
D.
Rosenbaum
and
C. F.
Zukoski
,
J. Cryst. Growth
169
,
752
(
1996
).
10.
M. L.
Broide
,
T. M.
Tominc
, and
M. D.
Saxowsky
,
Phys. Rev. E
53
,
6325
(
1996
).
11.
V. G.
Taratuta
,
A.
Holschbach
,
G. M.
Thurston
,
D.
Blankschtein
, and
G. B.
Benedek
,
J. Chem. Phys.
94
,
2140
(
1990
).
12.
A.
George
and
W. W.
Wilson
,
Acta Crystallogr., Sect. D: Biol. Crystallogr.
50
,
361
(
1994
).
13.
P. R.
ten Wolde
and
D.
Frenkel
,
Science
277
,
1975
(
1997
).
14.
R.
Piazza
,
Curr. Opin. Colloid Interface Sci.
5
,
38
(
2000
).
15.
A.
Lomakin
,
N.
Asherie
, and
G. B.
Benedek
,
Proc. Natl. Acad. Sci. U.S.A.
96
,
9465
(
1999
).
16.
A.
Lomakin
,
N.
Asherie
, and
G. B.
Benedek
,
J. Chem. Phys.
104
,
1646
(
1996
).
17.
N.
Kern
and
D.
Frenkel
,
J. Chem. Phys.
118
,
9882
(
2003
).
18.
H.
Liu
,
S. K.
Kumar
, and
F.
Sciortino
,
J. Chem. Phys.
127
,
084902
(
2007
).
19.
R. P.
Sear
,
J. Chem. Phys.
111
,
4800
(
1999
).
20.
M. S.
Wertheim
,
J. Stat. Phys.
35
,
19
(
1984
).
21.
M. S.
Wertheim
,
J. Stat. Phys.
35
,
35
(
1984
).
22.
P. B.
Warren
,
J. Phys.: Condens. Matter
14
,
7617
(
2002
).
23.
N. M.
Dixit
and
C. F.
Zukoski
,
J. Chem. Phys.
117
,
8540
(
2002
).
24.
N. M.
Dixit
,
A. M.
Kulkarni
, and
C. F.
Zukoski
,
Colloids Surf., A
190
,
47
(
2001
).
25.
R.
Fantoni
,
D.
Gazzillo
,
A.
Giacometti
,
M. A.
Miller
, and
G.
Pastore
,
J. Chem. Phys.
127
,
234507
(
2007
).
26.
V.
Talanquer
,
J. Chem. Phys.
122
,
084704
(
2005
).
27.
J.
Chang
,
A. M.
Lenhoff
, and
S. I.
Sandler
,
J. Chem. Phys.
120
,
3003
(
2004
).
28.
E.
Bianchi
,
J.
Largo
,
P.
Tartaglia
,
E.
Zaccarelli
, and
F.
Sciortino
,
Phys. Rev. Lett.
97
,
168301
(
2006
).
29.
A. J.
Archer
and
N. B.
Wilding
,
Phys. Rev. E
76
,
031501
(
2007
).
30.
A. J.
Archer
,
D.
Pini
,
R.
Evans
, and
L.
Reatto
,
J. Chem. Phys.
126
,
014104
(
2007
).
31.
R. P.
Sear
and
W. M.
Gelbart
,
J. Chem. Phys.
110
,
4582
(
1999
).
32.
A.
Stradner
,
H.
Sedgwick
,
F.
Cardinaux
,
W. C. K.
Poon
,
S. U.
Egelhaaf
, and
P.
Schurtenberger
,
Nature (London)
432
,
492
(
2004
).
33.
E.
Allahyarov
,
H.
Löwen
,
J. P.
Hansen
, and
A. A.
Louis
,
Phys. Rev. E
67
,
051404
(
2003
).
34.
J.
Chang
,
A. M.
Lenhoff
, and
S. I.
Sandler
,
J. Phys. Chem. B
109
,
19507
(
2005
).
35.
M.
Carpineti
and
R.
Piazza
,
Phys. Chem. Chem. Phys.
6
,
1506
(
2004
).
36.
R. A.
Curtis
,
C.
Steinbrecher
,
M.
Heinemann
,
H. W.
Blanch
, and
J. M.
Prausnitz
,
Biophys. Chem.
98
,
249
(
2002
).
37.
M. G.
Noro
and
D.
Frenkel
,
J. Chem. Phys.
113
,
2941
(
2000
).
38.
F.
Cardinaux
,
T.
Gibaud
,
A.
Stradner
, and
P.
Schurtenberger
,
Phys. Rev. Lett.
99
,
118301
(
2007
).
39.
A.
Stradner
,
F.
Cardinaux
, and
P.
Schurtenberger
,
J. Phys. Chem. B
110
,
21222
(
2006
).
40.
F.
Cardinaux
,
A.
Stradner
,
P.
Schurtenberger
,
F.
Sciortino
, and
E.
Zaccarelli
,
Europhys. Lett.
77
,
48004
(
2007
).
41.
C.
Tanford
and
R.
Roxby
,
Biochemistry
11
,
2192
(
1972
).
42.
J. A.
Thomson
,
P.
Schurtenberger
,
G. M.
Thurston
, and
G. B.
Benedek
,
Proc. Natl. Acad. Sci. U.S.A.
84
,
7079
(
1987
).
43.
D. C.
Phillips
,
Proc. Natl. Acad. Sci. U.S.A.
57
,
483
(
1967
).
44.
L.
Belloni
,
J. Chem. Phys.
85
,
519
(
1986
).
45.
P.
Prinsen
and
T.
Odijk
,
J. Chem. Phys.
127
,
115102
(
2007
).
46.
E.
Allahyarov
,
H.
Löwen
,
A. A.
Louis
, and
J. P.
Hansen
,
Europhys. Lett.
57
,
731
(
2002
).
47.
D. E.
Kuehner
,
C.
Heyer
,
C.
Ramsch
,
U. M.
Fornefeld
,
H. W.
Blanch
, and
J. M.
Prausnitz
,
Biophys. J.
73
,
3211
(
1997
).
48.
W. C. K.
Poon
,
S. U.
Egelhaaf
,
P. A.
Beales
,
A.
Salonen
, and
L.
Sawyer
,
J. Phys.: Condens. Matter
12
,
L569
(
2000
).
49.
J. A.
Barker
and
D.
Henderson
,
Rev. Mod. Phys.
48
,
587
(
1976
).
50.
J. A.
Barker
and
D.
Henderson
,
J. Chem. Phys.
47
,
2856
(
1967
).
51.
N. F.
Carnahan
and
K. E.
Starling
,
J. Chem. Phys.
51
,
635
(
1969
).
52.
L. K.
Steinrauf
,
Acta Crystallogr.
12
,
77
(
1959
).
53.
S.
Zhou
,
J. Chem. Phys.
127
,
084512
(
2007
).
54.
C.
Rascón
,
L.
Mederos
, and
G.
Navascués
,
Phys. Rev. E
54
,
1261
(
1996
).
55.
C.
Rascón
,
L.
Mederos
, and
G.
Navascués
,
Phys. Rev. E
53
,
5698
(
1996
).
56.
J. M.
Kincaid
and
J. J.
Weis
,
Mol. Phys.
34
,
931
(
1977
).
57.
W. W.
Wood
,
J. Chem. Phys.
20
,
1334
(
1952
).
58.
D.
Frenkel
and
A. J. C.
Ladd
,
J. Chem. Phys.
81
,
3188
(
1984
).
59.
G.
Nägele
,
The Physics of Colloidal Soft Matter
,
Lectures Notes
Vol.
14
(
Institute of Fundamental Technological Research/Polish Academy of Sciences
,
Warsaw, Poland
,
2004
).
60.
L.
Verlet
and
J. -J.
Weis
,
Phys. Rev. A
5
,
939
(
1972
).
61.
M. S.
Wertheim
,
Phys. Rev. Lett.
10
,
321
(
1963
).
62.
G. J.
Throop
and
R. J.
Bearman
,
J. Chem. Phys.
42
,
2408
(
1965
).
63.
M. H. J.
Hagen
and
D.
Frenkel
,
J. Chem. Phys.
101
,
4093
(
1994
).
64.
T. W.
Cochran
and
Y. C.
Chiew
,
J. Chem. Phys.
121
,
1480
(
2004
).
65.
B.
Rotenberg
,
J.
Dzubiella
,
J. -P.
Hansen
, and
A. A.
Louis
,
Mol. Phys.
102
,
1
(
2004
).
66.
M.
Dijkstra
,
J. M.
Brader
, and
R.
Evans
,
J. Phys.: Condens. Matter
11
,
10079
(
1999
).
67.
A. P.
Gast
,
C. K.
Hall
, and
W. B.
Russel
,
J. Colloid Interface Sci.
96
,
251
(
1983
).
68.
W. H.
Press
,
S. A.
Teukolsky
,
W. T.
Vetterling
, and
B. P.
Flannery
,
Numerical Recipes in C
, 2nd ed. (
Cambridge University Press
,
New York
,
1992
).
69.
T.
Gibaud
, Ph.D. thesis,
University of Fribourg
,
2008
.
70.
G.
Foffi
and
F.
Sciortino
,
J. Phys. Chem. B
111
,
9702
(
2007
).
71.
P. M.
Chaikin
and
T. C.
Lubensky
,
Principles of Condensed Matter Physics
(
Cambridge University Press
,
New York
,
1992
).
72.
D.
Fu
,
Y.
Li
, and
J.
Wu
,
Phys. Rev. E
68
,
011403
(
2003
).
73.
To our knowledge, the influence of short-ranged repulsion on the metastability of an attractive and repulsive hard-sphere Yukawa potential system has not been investigated. Therefore, we discuss the effect of the range of attraction on the (global) phase diagram by means of the existing literature on purely attractive hard-sphere Yukawa potentials (Ref. 63).
74.
J.
Israelachvili
and
R.
Pashley
,
Nature (London)
300
,
341
(
1982
).
75.
P. R.
ten Wolde
,
J. Phys.: Condens. Matter
14
,
9445
(
2002
).
76.
D.
Horinek
,
A.
Serr
,
M.
Geisler
,
T.
Pirzer
,
U.
Slotta
,
S. Q.
Lud
,
J. A.
Garrido
,
T.
Scheibel
,
T.
Hugel
, and
R. R.
Netz
,
Proc. Natl. Acad. Sci. U.S.A.
105
,
2842
(
2008
).
77.
D. M.
Huang
and
D.
Chandler
,
Proc. Natl. Acad. Sci. U.S.A.
97
,
8324
(
2000
).
78.
A. W.
Wilber
,
J. P. K.
Doye
,
A. A.
Louis
,
E. G.
Noya
,
M. A.
Miller
, and
P.
Wong
,
J. Chem. Phys.
127
,
085106
(
2007
).
79.
J. P. K.
Doye
,
A. A.
Louis
,
I. -C.
Lin
,
L. R.
Allen
,
E. G.
Noya
,
A. W.
Wilber
,
H. C.
Kok
, and
R.
Lyus
,
Phys. Chem. Chem. Phys.
9
,
2197
(
2007
).
80.
J. J.
McManus
,
A.
Lomakin
,
O.
Ogun
,
A.
Pande
,
M.
Basan
,
J.
Pande
, and
G. B.
Benedek
,
Proc. Natl. Acad. Sci. U.S.A.
104
,
16856
(
2007
).
81.
H.
Ruiz-Estrada
,
M.
Medina-Noyola
, and
G.
Nägele
,
Physica A
168
,
919
(
1990
).
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