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www.elsevier.com/locate/jcis

Comparison between theoretical values and simulation results of viscosity

for the dissipative particle dynamics method

Akira Satoh

a,

, Tamotsu Majima

b

a

Department of Machine Intelligence and System Engineering, Faculty of System Science and Technology, Akita Prefectural University, 84-4, Ebinokuchi,

Tsuchiya-aza, Honjo 015-0055, Japan

b

Graduate School of Science and Technology, Chiba University, 1-33, Yayoicho, Inage-ku, Chiba 263-8522, Japan

Received 10 October 2003; accepted 13 September 2004

Abstract

In order to investigate the validity of the dissipative particle dynamics method, which is a mesoscopic simulation technique, we have derived

an expression for viscosity from the equation of motion of dissipative particles. In the concrete, we have shown the FokkerPlanck equation

in phase space, and macroscopic conservation equations such as the equation of continuity and the equation of momentum conservation.

The basic equations of the single-particle and pair distribution functions have been derived using the FokkerPlanck equation. The solutions

of these distribution functions have approximately been solved by the perturbation method under the assumption of molecular chaos. The

expressions of the viscosity due to momentum and dissipative forces have been obtained using the approximate solutions of the distribution

functions. Also, we have conducted nonequilibrium dynamics simulations to investigate the inuence of the parameters, which have appeared

in dening the equation of motion in the dissipative particle dynamics method. The theoretical values of the viscosity due to dissipative forces

in the HoogerbruggeKoelman theory are in good agreement with the simulation results obtained by the nonequilibrium dynamics method,

except in the range of small number densities. There are restriction conditions for taking appropriate values of the number density, number

of particles, time interval, shear rate, etc., to obtain physically reasonable results by means of dissipative particle dynamics simulations.

2004 Published by Elsevier Inc.

Keywords: Dissipative particle dynamics method; Mesoscopic approach; Nonequilibrium dynamics method; Transport coefcients; Viscosity

1. Introduction

The hydrodynamic solution for a three-particle system

has to be combined into a simulation method in order to take

into account multibody hydrodynamic interactions among

colloidal particles more precisely. However, it is highly dif-

cult even to solve analytically the ow eld for a three-

particle system [1,2], and, therefore, it seems to be almost

hopeless to obtain an analytical solution for a nonspherical

particle system such as a system composed of rodlike par-

ticles. Thus, we have the choice to take another approach

to develop a more precise simulation method for colloidal

dispersions. If both colloidal particles and solvent mole-

*

Corresponding author. Fax: +81-184-27-2188.

E-mail address: asatoh@akita-pu.ac.jp (A. Satoh).

cules are simulated, we can obtain the particle motion and

the solution of the ow eld simultaneously. However, if

molecules themselves are treated in simulations, we cannot

develop an effective simulation method, since the character-

istic time for the motion of colloidal particles is signicantly

different from that of solvent molecules. In other words, this

kind of molecular-dynamics-like method is unrealistic as a

technique for simulation of a colloidal dispersion from a

simulation time point of view. To circumvent this difculty,

the concept of uid particles seems to be promising. Hooger-

brugge and Koelman [3,4] have developed the dissipative

particle dynamics method in terms of uid particles. In their

theory, a uid is regarded as being composed of such virtual

particles, and the ow eld is solved by simulating these par-

ticles. The uid particles interact with each other, exchange

momentum, and should make random motion like Brownian

0021-9797/$ see front matter 2004 Published by Elsevier Inc.

doi:10.1016/j.jcis.2004.09.050

252 A. Satoh, T. Majima / Journal of Colloid and Interface Science 283 (2005) 251266

particles. From now on, such uid particles are called dissi-

pative particles.

For the simulation of the ow eld for a colloidal dis-

persion, the motion of colloidal particles is dependent on

the interaction between colloidal particles themselves, the

interaction between colloidal particles and dissipative par-

ticles, and the interaction between colloidal particles and

an applied eld such as a magnetic eld. Hence, in this

simulation technique, the solution of pair or three-body hy-

drodynamic interactions need not be combined with it, in

order to simulate colloidal particles. This is in high con-

trast with the ordinary simulation methods such as Stokesian

dynamics methods [511]. Multibody hydrodynamic inter-

actions among colloidal particles are automatically taken

into account from the interactions of colloidal particles with

dissipative ones. This is a signicant feature in the dissi-

pative particle dynamics method compared with ordinary

simulation methods. It is clear from these discussions that

the concept of the dissipative particle dynamics method is

straightforwardly applicable to a colloidal dispersion com-

posed of nonspherical particles, and, therefore, seems to be a

highly promising technique from a simulation point of view.

As will be shown later, the equation of motion for the dis-

sipative particle dynamics, which has been presented to date

[3,4,1214], is not unique, but has considerable freedom;

for example, the equation of motion has unknown constants

which are parameters representing the strength of conserv-

ative and dissipative forces. However, whether or not the

equation of motion can yield physically reasonable solu-

tions has not been sufciently claried [3,4,15], although

there is uncertainty in the equation of motion for dissipa-

tive particles. Hence, in order to apply the dissipative par-

ticle dynamics method widely to the usual ow problems

and physicsengineering problems of colloidal dispersions,

it is very important to investigate the inuence of such un-

certainty in the equation of motion on the solution of the

ow properties such as the ow eld and transport coef-

cients. This may be accomplished by comparing simulation

results with theoretical solutions concerning transport coef-

cients, which can be derived analytically from the equation

of motion.

The present study, therefore, attempts rst to derive an

analytical expression for viscosity using the equation of mo-

tion, secondly to obtain the numerical data in terms of dis-

sipative particle dynamics simulations, and nally to com-

pare the simulation results with the analytical solutions. In

the concrete, we show the FokkerPlanck equation in phase

space, and macroscopic conservation equations such as the

equation of continuity and the equation of momentum con-

servation. The basic equations of the single-particle and pair

distribution functions are derived using the FokkerPlanck

equation. These equations of the distribution functions are

approximately solved to obtain an expression for the viscos-

ity due to momentumand dissipative forces. Nonequilibrium

dynamics simulations have been conducted under circum-

stances of simple shear ow. Finally, these simulation results

are compared with the theoretical solutions to investigate the

inuence of the model parameters, which have appeared in

denitions of the equation of motion, number density, num-

ber of particles, time interval, etc., on this transport coef-

cient and also the internal structure of a dissipative particle

system. The present study may stimulate the development of

a new equation of motion for the dissipative particle dynam-

ics, which gives rise to more physically reasonable simula-

tion results.

2. Dynamics of dissipative particles

2.1. Kinetic equation of dissipative particles

The equation of motion for dissipative particles has to

obey some physical constraints in order for the solution

obtained by the dissipative particle dynamics method to

agree with that obtained by the NavierStokes equation. The

conservation of the total momentum of a system and the

Galilean invariance have to be satised by the equation of

motion as a minimum request [3,4,12,13].

We concentrate our attention on particle i and consider

the forces acting on this particle. The following three kinds

of forces may be physically reasonable as forces acting on

particle i: a repulsive conservative force F

C

ij

exerted by the

other particles, a dissipative force F

D

ij

providing a viscous

drag to the system, and a random or stochastic force F

R

ij

in-

ducing the thermal motion of particles. With these forces, the

equation of motion of particle i can be written as [1214]

(1) m

dv

i

dt

=

j (=i)

F

C

ij

+

j (=i)

F

D

ij

+

j (=i)

F

R

ij

,

in which m is the mass of particle i, v

i

is the velocity, and,

concerning the subscripts, for example, F

C

ij

is the force act-

ing on particle i from particle j.

Now we have to embody specic forms of the above-

mentioned forces. It may be reasonable to assume that the

conservative force F

C

ij

depends only on the relative position

r

ij

(= r

i

r

j

), and not on the particle velocities. An ex-

plicit expression for this force will be shown later. Since the

Galilean invariance has to be satised, the dissipative force

F

D

ij

and the random force F

R

ij

should not be dependent on

the position r

i

and velocity v

i

themselves, but should be

functions of the relative position r

ij

and relative velocity v

ij

(= v

i

v

j

), if necessarily. Additionally, it may be reason-

able to assume that the randomforce F

R

ij

does not depend on

the relative velocity but the relative position r

ij

alone. Fur-

thermore, we have to take into account the isotropy of the

particle motion and the decrease in the magnitude of forces

with particleparticle separation. The following expressions

for F

D

ij

and F

R

ij

satisfy these physical requirements [1214],

(2) F

D

ij

= w

D

(r

ij

)(e

ij

v

ij

)e

ij

,

(3) F

R

ij

=w

R

(r

ij

)e

ij

ij

,

A. Satoh, T. Majima / Journal of Colloid and Interface Science 283 (2005) 251266 253

in which r

ij

= |r

ij

|, and e

ij

is the unit vector denoting the

direction of particle i from particle j, expressed as e

ij

=

r

ij

/r

ij

. Also

ij

is a random variable inducing the random

motion of particles and has to satisfy the following stochastic

properties:

_

ij

(t )

_

= 0,

(4)

_

ij

(t )

i

j

(t

)

_

= (

ii

jj

+

ij

ji

)(t t

).

This variable satises the characteristic of the symmetry

ij

=

ji

, which ensures that the total momentum of the

system is conserved. The w

D

(r

ij

) and w

R

(r

ij

) are weight

functions to reproduce the decrease in forces with particle

particle separation, and and are constants specifying the

magnitude of forces. These constants can be related to the

system temperature and friction coefcient, which will be

shown later. It is seen from the expression for F

D

ij

that this

force acts in such a way as to relax the relative motion of

particles i and j. On the other hand, F

R

ij

acts as if inducing

the thermal motion of particles, but this force satises the

actionreaction formula, so that the conservation of the total

momentum of the system is ensured.

The substitution of Eqs. (2) and (3) into Eq. (1) leads to

the following equation:

m

dv

i

dt

=

j (=i)

F

C

ij

(r

ij

)

j (=i)

w

D

(r

ij

)(e

ij

v

ij

)e

ij

(5) +

j (=i)

w

R

(r

ij

)e

ij

ij

.

If this equation is integrated with respect to time over a small

time interval fromt to t +t , then the nite difference equa-

tions governing the particle motion in simulations can be

obtained as

(6) r

i

= v

i

t ,

(7)

v

i

=

1

m

_

j (=i)

F

C

ij

(r

ij

)

j (=i)

w

D

(r

ij

)(e

ij

v

ij

)e

ij

_

t

+

1

m

j (=i)

w

R

(r

ij

)e

ij

W

ij

,

in which

(8) W

ij

=

t +t

_

t

ij

d.

This W

ij

has to satisfy the following stochastic properties,

which arise from Eq. (4):

W

ij

= 0,

(9) W

ij

W

i

j

=(

ii

jj

+

ij

ji

)t .

If a new stochastic variable

ij

is introduced from the deni-

tion W

ij

=

ij

as

(10)

1

m

j (=i)

w

R

(r

ij

)e

ij

ij

t ,

in which

ij

has to satisfy the following stochastic proper-

ties:

(11)

ij

= 0,

ij

j

=(

ii

jj

+

ij

ji

).

It is seen fromEq. (11) that the stochastic variable

ij

is sam-

pled froma uniformor normal distribution with zero average

value and unit variance [3,4,1214].

The equation of motion in Eq. (5) satises the conserva-

tion law of the total momentum of the system, but not the

energy conservation law. The equation of motion has to be

modied to satisfy the conservation of the system energy

[16,17].

The coefcients and and the weight functions

w

D

(r

ij

) and w

R

(r

ij

) cannot be determined independently,

because there are some relationships among these quanti-

ties. The derivation of these relationships will be shown in

the next section.

2.2. FokkerPlanck equation

We use the notation r

i

for the position vector of particle i

and v

i

for the velocity vector. Also, for simplicity of expres-

sion, the vector v

N

is used for describing the velocity vectors

of all the particles (that is, v

N

represents v

1

, v

2

, v

3

, . . .), and

similarly r

N

is for the position vectors of all the particles

(that is, r

N

represents r

1

, r

2

, r

3

, . . .). If the probability that

a particle position and velocity are found within the range

from (r

N

, v

N

) to (r

N

+ r

N

, v

N

+ v

N

) is denoted by

W(r

N

, v

N

, t ) dr

N

dv

N

, then the probability density function

W(r

N

, v

N

, t ) satises the following stochastic formula, i.e.,

the ChapmanKolmogorov equation,

W(r

N

, v

N

, t ) =

_ _

W(r

N

r

N

, v

N

v

N

, t t )

(12)

(r

N

r

N

, v

N

v

N

; r

N

, v

N

) d(r

N

) d(v

N

),

in which (r

N

r

N

, v

N

v

N

; r

N

, v

N

) is the transi-

tion probability for the state (r

N

r

N

, v

N

v

N

) trans-

ferring to another state (r

N

, v

N

) during a time interval t

and this does not depend on the time point t . If the veloc-

ity v

N

does not change appreciably during the small time

interval t , then can be written as

(r

N

r

N

, v

N

v

N

; r

N

, v

N

)

(13)

=(r

N

r

N

, v

N

v

N

; v

N

)(r

N

v

N

t ),

in which is the transition probability and is independent

of r

N

. The substitution of Eq. (13) into Eq. (12) leads to

the following different form of the ChapmanKolmogorov

equation:

W(r

N

+v

N

t , v

N

, t +t )

=

_ _

W(r

N

, v

N

v

N

, t )

(14) (r

N

, v

N

v

N

; v

N

) d(v

N

).

254 A. Satoh, T. Majima / Journal of Colloid and Interface Science 283 (2005) 251266

The FokkerPlanck equation in phase space (or the Chan-

drasekhar equation) can be derived by reforming Eq. (14) in

terms of Taylor series expansions with the nite difference

equations (6) and (7). Since the detailed derivation proce-

dure is shown in Ref. [18], we here show the nal result:

W

t

+

i

v

i

W

r

i

+

j

(i=j)

F

C

ij

m

W

v

i

=

j

(i=j)

e

ij

v

i

_

1

m

w

D

(r

ij

)(e

ij

v

ij

)W

_

+

1

2

j

(i=j)

1

m

2

2

w

2

R

(r

ij

)

(15) e

ij

v

i

_

e

ij

v

i

e

ij

v

j

_

W.

2.3. Final expression of equation of motion and its

nondimensional form

If a system composed of dissipative particles is in equi-

librium, then the equilibrium distribution W

eq

becomes the

canonical distribution for an ensemble which is specied by

a given particle number N, volume V , and temperature T .

With the notation U for the potential energy, W

eq

is written

as

(16) W

eq

=

1

Z

exp

_

1

kT

_

N

i=1

m

v

2

i

2

+U

__

,

in which Z is the partition function, and U is related to the

conservative force F

C

ij

by

(17) F

C

ij

=

U

r

ij

.

The equilibrium distribution W

eq

has to satisfy the Fokker

Planck equation in phase space in Eq. (15). Since the left-

hand side in Eq. (15) vanishes for the substitution of W

eq

,

the right-hand side also has to become zero. This is accom-

plished by the requirements

(18) w

D

(r

ij

) =w

2

R

(r

ij

),

2

= 2 kT,

in which k is Boltzmanns constant. The second equation is

the uctuationdissipation theorem for the dissipative parti-

cle dynamics.

We nowhave to determine the explicit expressions for the

conservative force F

C

ij

(r

ij

) and the weight function w

R

(r

ij

).

F

C

ij

(r

ij

) is a repulsive force preventing unphysical exces-

sive overlaps between particles, and w

R

(r

ij

) has to be set

so that interparticle forces decrease with increasing particle

particle separations. These requirements are satised by the

expressions

(19) F

C

ij

=w

R

(r

ij

)e

ij

,

(20) w

R

(r

ij

) =

_

1

r

ij

r

c

for r

ij

r

c

,

0 for r

ij

>r

c

,

in which is a constant representing the magnitude of the re-

pulsive forces. By substituting these equations into Eqs. (6)

and (7) with considering Eq. (10), the nal expression for

the equation of motion of the dissipative particle dynamics

can be written as

(21) r

i

= v

i

t ,

(22)

v

i

=

m

j (=i)

w

R

(r

ij

)e

ij

t

j (=i)

w

2

R

(r

ij

)(e

ij

v

ij

)e

ij

t

+

(2 kT )

1/2

m

j (=i)

w

R

(r

ij

)e

ij

ij

t ,

in which the expression for w

R

(r

ij

) has already been shown

in Eq. (20). The stochastic variable

ij

has to obey the sto-

chastic properties shown in Eq. (11) and is sampled from a

uniform or normal distribution with zero average and unit

variance, as already pointed out. The dissipative particle dy-

namics method uses Eqs. (21) and (22) to simulate the mo-

tion of dissipative particles.

Lastly, we showan example of the nondimensionalization

method used for actual simulations. To nondimensionalize

each quantity, the following representative values are used:

(kT/m)

1/2

for velocities, r

c

for distances, r

c

(m/kT )

1/2

for

time, (1/r

3

c

) for number densities, etc. With these represen-

tative values, Eqs. (21) and (22) can be nondimensionalized

as

(23) r

i

= v

i

t

,

(24)

v

i

=

j (=i)

w

R

(r

ij

)e

ij

t

j (=i)

w

2

R

(r

ij

)(e

ij

v

ij

)e

ij

t

+(2

)

1/2

j (=i)

w

R

(r

ij

)e

ij

ij

,

in which

(25) w

R

(r

ij

) =

_

1 r

ij

for r

ij

1,

0 for r

ij

>1,

(26)

=

r

c

kT

,

=

r

c

(mkT )

1/2

.

In these equations, the quantities with superscript

*

are di-

mensionless. Equations (23) and (24) clearly show that one

can start a dissipative particle dynamics simulation if appro-

priate values of the nondimensional parameters

and

sity n

0

(=r

3

c

N/V , V is the system volume), and the particle

number N are properly specied. Results obtained by the

A. Satoh, T. Majima / Journal of Colloid and Interface Science 283 (2005) 251266 255

simulations should not depend on the nondimensional para-

meters which have been introduced in embodying the equa-

tion of motion; one has to be, therefore, careful in setting

appropriate values for these values in conducting dissipa-

tive particle dynamics simulations. For example, since time

is nondimensionalized by the representative value based on

the mean velocity v ( (kT/m)

1/2

) and the radius r

c

, the

magnitude of the dimensionless time interval t

may have

to be taken sufciently smaller than unity [19].

3. Transport equations

In the present section, the dissipative particle dynamics

method, the equation of continuity, and the momentumequa-

tion of the uid are derived using the equation of motion of

the dissipative particle dynamics.

If an arbitrary physical quantity A(r

N

, v

N

) is not de-

pendent on time explicitly, the time average A can be

expressed, using the probability density function W which

satises Eq. (15), as

(27) A =

_ _

AW(r

N

, v

N

, t ) dr

N

dv

N

,

in which

(28)

_ _

W(r

N

, v

N

, t ) dr

N

dv

N

= 1.

Hence, the time variation of A can be expressed, from

Eq. (15), as

t

A =

_ _

A

W

t

dr

N

dv

N

=

_ _

A

_

i

v

i

W

r

i

j

(i=j)

F

C

ij

m

W

v

i

+

j

(i=j)

e

ij

v

i

_

1

m

w

D

(r

ij

)(e

ij

v

ij

)W

_

+

1

2

j

(i=j)

1

m

2

2

w

2

R

(r

ij

)

(29)

e

ij

v

i

_

e

ij

v

i

e

ij

v

j

_

W

_

dr

N

dv

N

.

By applying integration by parts, this equation is written as

t

A =

_

i

v

i

A

r

i

j

(i=j)

F

C

ij

m

A

v

i

j

(i=j)

m

w

D

(r

ij

)(e

ij

v

ij

)e

ij

A

v

i

+

1

2

j

(i=j)

1

m

2

2

w

2

R

(r

ij

)

_

e

ij

v

i

_

(30)

_

e

ij

v

i

e

ij

v

j

_

A

_

.

Next we derive the equation of continuity and the momen-

tum equation of the uid using Eq. (30). If A is dened by

the equation

(31) A=

N

i=1

m(r r

i

),

then the average A, which is evaluated from Eq. (27), is

equal to a local density (r). That is,

(32) A =

_

N

i=1

m(r r

i

)

_

=(r).

If A is taken as

(33) A =

N

i=1

mv

i

(r r

i

),

then the average A is now

(34) A =(r)u(r),

in which u(r) is a macroscopic uid velocity at position r.

The substitution of Eq. (31) into Eq. (30) leads to the fol-

lowing expression:

(35)

t

+

r

(u) = 0.

This is no other than the equation of continuity.

Next the substitution of Eq. (33) into Eq. (30) leads to the

following equation:

t

(u) =

_

i

mv

i

r

i

_

v

i

(r r

i

)

_

+

j

(i=j)

F

C

ij

v

i

_

v

i

(r r

i

)

_

j

(i=j)

w

D

(r

ij

)(e

ij

v

ij

)

_

e

ij

v

i

_

v

i

(r r

i

)

_

_

+

1

2

j

(i=j)

1

m

2

w

2

R

(r

ij

)

_

e

ij

v

i

_

(36) e

ij

_

v

i

_

v

i

(r r

i

)

_

v

j

_

v

j

(r r

j

)

_

_

_

.

Thus, by taking into account Eq. (2), and conducting a simi-

lar reformation, Eq. (36) can be simplied as

256 A. Satoh, T. Majima / Journal of Colloid and Interface Science 283 (2005) 251266

t

(u) =

_

r

_

i

mv

i

v

i

(r r

i

)

_

(37) +

j

(i=j)

_

F

C

ij

+F

D

ij

_

(r r

i

)

_

.

By taking account of the relation F

D

ij

=F

D

ij

e

ij

, the following

equation can be obtained:

j

(i=j)

F

D

ij

(r r

i

)

=

1

2

j

(i=j)

_

F

D

ij

(r r

i

) +F

D

ji

(r r

j

)

_

(38) =

1

2

j

(i=j)

F

D

ij

e

ij

_

(r r

i

) (r r

j

)

_

.

If the following relationship concerning the Dirac delta func-

tion is taken into account,

(r r

j

) =(r r

i

+r

ij

)

(39)

=(r r

i

) +

r

_

e

ij

r

ij

_

0

(r r

i

+

e

ij

) d

_

,

then Eq. (38) can be reformed further as

j

(i=j)

F

D

ij

(r r

i

)

(40)

=

1

2

j

(i=j)

r

_

F

D

ij

e

ij

e

ij

r

ij

_

0

(r r

i

+

e

ij

) d

_

.

By conducting a similar reformation concerning F

C

ij

, Eq. (37)

can nally be written as

(41)

t

(u) =

r

(uu) +

r

(

K

+

U

),

in which

K

=

_

i

m(v

i

u)(v

i

u)(r r

i

)

_

,

(42)

U

=

1

2

_

j

(i=j)

_

F

C

ij

+F

D

ij

_

e

ij

e

ij

r

ij

_

0

(r r

i

+e

ij

) d

_

.

If the equation of continuity in Eq. (35) is taken into consid-

eration, Eq. (41) reduces to the momentum equation of the

uid,

(43)

_

u

t

+u

u

r

_

=

r

(

K

+

U

),

in which

K

and

U

are stress tensors due to the particle

momentum and the forces acting between particles, respec-

tively. It has now been shown that the equation of motion of

the dissipative particle dynamics gives rise to the momen-

tum equation of the uid. The virial equation of state can be

derived by evaluating directly

K

and

U

in Eq. (42).

4. Expressions for transport coefcients

4.1. Distribution functions

The local number density n(r, t ) at position r at time t

can be expressed using W(r

N

, v

N

, t ) as [18]

n(r, t ) =

_

N

i=1

(r r

i

)

_

=

_

_

i

(r r

i

)W(r

N

, v

N

, t ) dr

N

dv

N

=N

_

_

W(r, r

2

, . . . , r

N

, v

N

, t )

(44) dr

2

. . . dr

N

dv

N

.

Similarly, the pair correlation function g(r, r

, t ) can be writ-

ten as [18]

g(r, r

, t )

=

1

n

2

0

_

_ N

i

N

j

(i=j)

(r r

i

)(r

r

j

)

W(r

N

, v

N

, t ) dr

N

dv

N

=

N(N 1)

n

2

0

(45)

_

_

W(r, r

, r

3

, . . . , r

N

, v

N

, t ) dr

3

. . . dr

N

dv

N

,

in which n

0

is the mean number density, given by n

0

=

N/V , as dened before.

If the distribution function f (r, v, t ) is dened as [14]

(46) f (r, v, t ) =

_

N

i=1

(r r

i

)(v v

i

)

_

,

f (r, v, t ) can be written, using W(r

N

, v

N

, t ), as

(47)

f (r, v, t ) =N

_

_

W(r, r

2

, . . . , r

N

, v, v

2

, . . . , v

N

, t )

dr

2

. . . dr

N

dv

2

. . . dv

N

.

By comparing Eq. (47) with Eq. (44), it is seen that there is

a relationship between f (r, v, t ) and n(r, t ):

(48) n(r, t ) =

_

f (r, v, t ) dv.

A. Satoh, T. Majima / Journal of Colloid and Interface Science 283 (2005) 251266 257

Similarly,

(49) n(r, t )u(r, t ) =

_

N

i

v

i

(r r

i

)

_

=

_

vf (r, v, t ) dv.

Next, if we dene the pair distribution f

(2)

(r, r

, v, v

, t )

by the equation [14]

f

(2)

(r, r

, v, v

, t )

=

_

N

i=1

N

j=1

(i=j)

(r r

i

)(r

r

j

)(v v

i

)(v

v

j

)

_

=N(N 1)

(50)

_

_

W(r, r

, r

3

, . . . , r

N

, v, v

, v

3

, . . . , v

N

, t )

dr

3

. . . dr

N

dv

3

. . . dv

N

,

then the pair distribution can be related to the pair correlation

function g(r, r

, t ) as

(51) n

2

0

g(r, r

, t ) =

_ _

f

(2)

(r, r

, v, v

, t ) dv dv

.

It is clear from Eq. (30) that the average of an arbi-

trary quantity A(r

N

, v

N

) can be evaluated using f (r, v, t )

and f

(2)

(r, r

, v, v

W(r

N

, v

N

, t ). Hence, we here rst show the basic equations

for f and f

(2)

, and then solve the equations analytically to

obtain the approximate solutions.

If we set A =

i

(r r

i

)(v v

i

) in Eq. (30), and re-

formthe equation with the formulae of vector operations, the

following equation can be obtained:

t

f (r, v, t ) +v

r

f (r, v, t )

=

m

_ _

w

D

(R)

R

:

v

_

(v v

)f

(2)

(r, r +R, v, v

, t )

_

dRdv

+

2

2m

2

_ _

w

2

R

(R)

R

R

(52) :

2

vv

f

(2)

(r, r +R, v, v

, t ) dRdv

.

It has been assumed in deriving this equation that there are

no conservative forces. In Eq. (25),

R is the unit vector,

denoted by

R = R/|R|. It is seen from Eq. (52) that the

pair distribution function f

(2)

(r, r

, v, v

, t ) is necessary for

obtaining the solution of f (r, v, t ), and, similarly, the multi-

body distribution functions more than the pair distribution is

required to get the solution of f

(2)

. This clearly shows that

Eq. (52) is not closed, but a hierarchy equation. To close the

equation for f , the following assumption of molecular chaos

is introduced [14]:

(53) f

(2)

(r, r

, v, v

, t ) f (r, v, t )f (r

, v

, t ).

This assumption theoretically enables us to solve the equa-

tion of the distribution function. The substitution of Eq. (53)

into Eq. (52) leads to the following equation:

t

f (r, v, t ) +v

r

f (r, v, t )

=

m

_ _

w

D

(R)f (r +R, v

, t )

R

R

:

v

_

(v v

)f (r, v, t )

_

dRdv

+

2

2m

2

_ _

w

2

R

(R)f (r +R, v

, t )

R

(54) :

2

vv

f (r, v, t ) dRdv

.

The validity of solutions which are obtained from Eq. (54)

is strongly dependent on the physical reasonability of the

assumption of molecular chaos.

The nondimensional formof Eq. (54) may be more under-

standable to be solved analytically. According to the nondi-

mensionalization method, which has been shown in Sec-

tion 2.3, Eq. (54) is nondimensionalized as

(r

, v

, t

) +v

(r

, v

, t

)

=

0

_ _

w

D

(R

)f

(r

+R

, v

, t

R

:

v

_

(v

v

)f

(r

, v

, t

)

_

dR

dv

+

0

_ _

w

D

(R

)f

(r

+R

, v

, t

R

(55) :

2

v

(r

, v

, t

) dR

dv

,

in which the distribution function f has been nondimension-

alized as f

= (1/n

0

)(kT/m)

3/2

f . If we set = 1/

0

and assume to be much smaller than unity, the perturba-

tion method is applicable. Hence, f

perturbation parameter , as

f

(r

, v

, t

) =f

0

(r

, v

, t

) +f

1

(r

, v

, t

)

(56) +

2

f

2

(r

, v

, t

) + .

By substituting this equation into Eq. (55) and neglecting the

higher-order terms, we can obtain the following expression:

_

t

0

+v

0

_

+

2

_

t

1

+v

1

_

=

_ _

w

D

(R

)

_

f

0

(r

+R

, v

, t

)

+f

1

(r

+R

, v

, t

)

_

R

:

v

_

(v

v

)

_

f

0

(r

, v

, t

)

+f

1

(r

, v

, t

)

__

dR

dv

+

_ _

w

D

(R

)

_

f

0

(r

+R

, v

, t

)

+f

1

(r

+R

, v

, t

)

_

R

258 A. Satoh, T. Majima / Journal of Colloid and Interface Science 283 (2005) 251266

(57)

:

2

v

_

f

0

(r

, v

, t

) +f

1

(r

, v

, t

)

_

dR

dv

.

The equation for the zeroth order of can be written, from

this equation, as

_ _

w

D

(R

)f

0

(r

+R

, v

, t

R

:

v

_

(v

v

)f

0

(r

, v

, t

)

_

dR

dv

+

_ _

w

D

(R

)f

0

(r

+R

, v

, t

R

(58) :

2

v

0

(r

, v

, t

) dR

dv

= 0.

Similarly, the equation for the rst order of can be ex-

pressed as

0

+v

0

=

_ _

w

D

(R

)

_

f

0

(r

+R

, v

, t

R

:

_

v

(v

v

)f

1

(r

, v

, t

)

_

+f

1

(r

+R

, v

, t

R

:

v

_

(v

v

)f

0

(r

, v

, t

)

_

_

dR

dv

+

_ _

w

D

(R

)

_

f

0

(r

+R

, v

, t

R

:

2

v

1

(r

, v

, t

)

+f

1

(r

+R

, v

, t

R

(59) :

2

v

0

(r

, v

, t

)

_

dR

dv

.

Equation (58) can straightforwardly be solved as

(60) f

0

(r

, v

, t

) =n

_

1

2

_

3/2

exp

_

1

2

(v

)

2

_

.

By reforming Eq. (59) with the formulae of vector opera-

tions, the following equation is obtained:

0

+v

0

=

_

n

(r

+R

, t

)w

D

(R

R

(61) :

_

v

_

(v

)f

1

(r

, v

, t

)

_

+

2

v

1

(r

, v

, t

)

_

dR

.

If it is assumed that n

(r

+R

, t

) (=n/n

0

) is independent

of the position and is constant, and the integration is carried

out using the polar axis coordinates of

R, then Eq. (61) can

be simplied as

0

+v

0

=

[w]

3

_

v

_

(v

)f

1

(r

, v

, t

)

_

(62) +

v

1

(r

, v

, t

)

_

,

in which [w] is dened as

(63) [w] =

1

_

0

w

D

dR

=

1

_

0

w

D

4R

2

dR

.

The left-hand side of Eq. (62) can nally be reformed, by

taking account of Eq. (60), as

0

+v

0

(64) =

1

2

f

0

U

:

_

r

+

_

r

_

t

_

,

in which the notation U

, dened by U

= (v

), has

been used. Also, the superscript t means a transposed ten-

sor. Now we have prepared for solving Eq. (62) to get the

solution of f

1

.

As the rst trial to nd the solution of f

1

, we substitute

f

0

U

into f

1

in Eq. (62) to get the following expression

for the right-hand side of Eq. (62):

(65)

1

3

[w]

_

2U

0

+2If

0

_

.

As the second trail, we substitute f

0

U

2

I

into f

1

in

Eq. (62) to get the following equation for the right-hand side

of Eq. (62):

(66)

1

3

[w]

_

2U

2

f

0

I +6f

0

I

_

.

As the third trial, we substitute f

0

I

into f

1

in Eq. (62) to

obtain zero for the right-hand side of Eq. (62). Finally, if the

expression for f

1

is assumed to be

(67) U

0

1

3

U

2

f

0

I,

then the right-hand side of Eq. (62) becomes the following

expression:

(68)

2

3

[w]

_

U

0

1

3

U

2

f

0

I

_

.

After all, from these considerations, the solution of Eq. (62)

can straightforwardly be seen to be the following expression:

f

1

=

3

2

1

n

0

[w]

_

U

0

1

3

U

2

f

0

I

_

(69) :

1

2

_

r

+

_

r

_

t

_

.

If the equation of continuity, /r

= 0, is taken into

account, it is seen that the following relationship is satised:

(70) I :

_

r

+

_

r

_

t

_

= 0.

A. Satoh, T. Majima / Journal of Colloid and Interface Science 283 (2005) 251266 259

We now have obtained the zeroth and rst order solutions

of f

,

(71) f

=f

0

+f

1

,

in which f

0

and f

1

are given in Eqs. (60) and (69), respec-

tively.

4.2. Viscosity due to momentum

The viscosity due to momentum,

K

, can be obtained

from Eqs. (42) and (71) as

K

= n

0

_ _

U

_

f

0

+f

1

_

dv

= n

0

I +

3

2

_

1

2

_

3/2

n

0

[w]

_

U

_

U

1

3

U

2

I

_

exp

_

1

2

U

2

_

dU

:

1

2

_

r

+

_

r

_

t

_

(72) = n

0

I +

3

2

1

[w]

_

r

+

_

r

_

t

_

,

in which the following relationship has been used:

_

U

_

U

1

3

U

2

I

_

: D

exp

_

1

2

U

2

_

dU

(73)

=(2)

3/2

_

2D

11

D

12

+D

21

D

13

+D

31

D

12

+D

21

2D

22

D

23

+D

32

D

13

+D

31

D

23

+D

32

2D

33

_

.

In this equation, D

is dened by

(74) D

=

1

2

_

r

+

_

r

_

t

_

.

Hence, by comparing Eq. (72) with the general expression

of a stress tensor for Newtonian uids,

(75)

= P

I +

_

r

+

_

r

_

t

_

,

the viscosity due to momentum,

K

, can be expressed as

(76)

K

=

3

2

1

[w]

=

45

4

1

.

The dimensional expression for this expression is written as

(77)

K

=

3

2

mkT

r

3

c

[w]

.

4.3. Viscosity due to dissipative forces

We derive an expression for the stress tensor

D

. With

the following Taylor series expansion of the Dirac delta

function,

(r r

i

+e

ij

)

=(r r

i

) +e

ij

r

(r r

i

)

(78) +

1

2!

2

e

ij

e

ij

:

r

r

(r r

i

) + ,

the stress tensor due to dissipative forces can be written as

D

=

1

2

_

j

(i=j)

w

D

(r

ij

)(e

ij

v

ij

)e

ij

r

ij

(r r

i

)

_

+

1

4

r

_

j

(i=j)

w

D

(r

ij

)

(79) (e

ij

v

ij

)e

ij

r

ij

r

ij

(r r

i

)

_

+ .

The second term on the right-hand side in this equation is

negligible unless there is a signicant nonuniformity of the

system. Equation (79) is, therefore, rewritten as

D

=

1

2

n

2

0

_

_

R

w

D

(R

)

_

R (v

v

)

_

R

(80) f

(2)

(r

, r

+R

, v

, v

, t

) dR

dv

dv

.

By the assumption of molecular chaos, written in Eq. (53),

with Eq. (71) for f

(2)

can be written

as

f

(2)

(r

, r

, v

, v

, t

) =f

0

(r

, v

, t

)f

0

(r

, v

, t

)

+f

0

(r

, v

, t

)f

1

(r

, v

, t

)

+f

0

(r

, v

, t

)f

1

(r

, v

, t

)

(81) +

2

f

1

(r

, v

, t

)f

1

(r

, v

, t

).

By evaluating Eq. (80) with Eq. (81), the expression for

D

can be obtained, which is now shown in the following.

We rst derive the expression for the stress

D

0

due to the

rst term on the right-hand side in Eq. (81). From Eq. (80),

we get the following expression:

D

0

=

1

2

n

2

0

_

_

R

w

D

(R

)

_

R (v

v

)

_

R

(82) f

0

(r

, v

, t

)f

0

(r

, v

, t

) dR

dv

dv

.

If we take into account the relationship

(83)

v

v

=(v

) (v

u

) R

(r

, t

),

then Eq. (82) can be rewritten as

(84)

D

0

=

1

2

n

2

0

_

w

D

(R

)R

2

R

R : D

dR

.

The integral on the right-hand side in this equation can be

carried out using the polar coordinate systemto give the nal

260 A. Satoh, T. Majima / Journal of Colloid and Interface Science 283 (2005) 251266

expression for

D

0

,

(85)

D

0

=

n

2

0

15

[R

2

w]

1

2

_

r

+

_

r

_

t

_

,

in which

[R

2

w] =

_

R

2

w

D

(R

) dR

(86) =

1

_

0

R

2

w

D

(R

)4R

2

dR

.

Next, we have to evaluate the stresses due to the second,

third, and fourth terms on the right-hand side in Eq. (81).

From a similar procedure, it can straightforwardly be shown

that all these stresses become zero.

By taking into account all these results, the expression for

D

can easily be derived as

(87)

D

=

D

0

.

Hence, the comparison of Eq. (85) with Eq. (75) leads to

the nal expression for the viscosity

D

due to dissipative

forces:

(88)

D

=

n

2

0

30

[R

2

w] =

2

1575

n

2

0

.

The dimensional form is expressed as

(89)

D

=

n

2

0

30

_

r

3

c

R

2

w

_

.

The viscosity is nally obtained as the sum of

K

and

D

as =

K

+

D

in the present case.

It is clearly seen from the above discussion that the per-

turbation method with perturbation parameter using the

nondimensional basic equation written in Eq. (55) can be

signicantly understandable in notifying the validity range

of the analytical expression of the viscosity, Eq. (88) or

Eq. (89), although the result essentially agrees with that

which was derived by Marsh et al. [14].

4.4. Relationship with HK theory

In order to compare the present results with the HK the-

ory [3,4] more straightforwardly, we rewrite Eq. (89) as

(90)

D

=

n

2

0

30

_

r

2

_

1

r

r

c

_

2

dr =

n

2

0

30

_

r

2

w

D

(r) dr.

The viscosity due to dissipative forces,

D

HK

, in the HK

theory is written as

(91)

D

HK

=

mn

2

0

30t

_

r

2

w

HK

(r) dr,

in which w

HK

(r) is a weight function in the HK theory

and this weight function corresponds to w

D

(r) in the present

theory. However, it should be noted that w

HK

(r) does not

satisfy the uctuationdissipation theory [12,13], which is,

in constant, satised by the present theory. If we take into

account that the notation in the HKtheory is related to the

notations here as = t /m, it is seen that

D

essentially

agrees with

D

HK

. This clearly shows that the expression in

the HK theory,

D

HK

, has a similar validity range to the

present expression

D

, which has derived for the cases of

small values of .

5. Evaluation of viscosity by means of the

nonequilibrium dynamics method

5.1. Evaluation by GreenKubo expression

There are two methods for evaluating transport coef-

cients by means of simulations: the rst method is for

thermodynamic equilibrium and evaluates them using the

GreenKubo expression; the second one is the nonequilib-

rium dynamics method, shown in the following, in which

transport coefcients are evaluated under circumstances of a

simple shear ow.

The theory of the nonequilibrium molecular dynamics

method [20] for a molecular system is applicable to the

present case, if a simple shear ow is considered as a ow

eld. In this case, the viscosity

yx

is evaluated fromthe fol-

lowing equation in simulations [18,20],

(92)

yx

=

1

V

J

yx

ne

,

in which

J

yx

(t ) =

N

i=1

_

mv

iy

(t )v

ix

(t ) +y

i

(t )F

ix

(t )

_

(93) =

N

i=1

mv

iy

(t )v

ix

(t ) +

N

i=1

N

j=1

(i<j)

y

ij

(t )F

ijx

(t ),

and F

ijx

is the x-component of the force vector F

ij

. In the

dissipative particle dynamics method, the force acting be-

tween particles, F

ij

, is taken as F

ij

= F

C

ij

+ F

D

ij

. Also, is

the shear rate, and J

yx

ne

is the time average of J

yx

under

circumstances of a simple shear ow, which is assumed to

act in the x-axis direction.

By nondimensionalizing the shear rate by (kT/m)

1/2

/r

c

,

the dimensionless form of Eq. (92) can be written as

(94)

yx

=

yx

(mkT )

1/2

/r

2

c

=

1

_

J

yx

_

ne

,

in which

(95) J

yx

(t

) =

N

i=1

v

iy

(t

)v

ix

(t

) +

N

i=1

N

j=1

(i<j)

y

ij

(t

)F

ijx

(t

).

The LeesEdwards boundary condition [18,20] has to be

used in order to generate a simple shear ow, and, further-

more, the equation of motion is slightly modied in many

A. Satoh, T. Majima / Journal of Colloid and Interface Science 283 (2005) 251266 261

cases for a molecular system. According to the nonequi-

librium molecular dynamics method, the nite difference

equations of the equation of motion for the present system

are modied as [20]

x

i

=

_

v

ix

+

i

_

t

, y

i

=v

iy

t

,

(96) z

i

=v

iz

t

,

v

ix

=

_

F

ix

iy

_

t

, v

iy

=F

iy

t

,

(97) v

iz

=F

iz

t

,

in which F

i

denotes the force acting on particle i.

5.2. Parameters for simulations

Simulations have been conducted under various condi-

tions in order to clarify the characteristics of the equation

of motion for dissipative particles dynamics by comparing

simulation results with theoretical solutions. Typical cases

such as n

0

= 0.5, 3.16, and 10.0 were taken for the number

density, and the particle number N was 500, unless specif-

ically notied. From sufcient numbers of simulations for

a small system, the time interval t

was taken as t

=

0.0001, and the total time steps were adopted as 5,000,000,

which ensures sufcient accuracy of average values. The er-

ror analysis [20] concerning almost all simulation results

was conducted to show the error ranges of simulation data;

the error ranges of

K

and

D

are denoted by

K

error

and

D

error

, respectively, and these values will be shown with

results in Section 6. Also, the parameters

and

, which

have appeared in the equation of motion for dissipative parti-

cles, were taken as

= 10, 25 and

/10, unless

specically noted.

6. Results

6.1. Inuence of

on viscosity

Figs. 1 and 2 show the inuence of the values of

on

the viscosity, which were obtained by the nonequilibrium

dynamics method. Fig. 1 is for the viscosity

D

due to dis-

sipative forces and Fig. 2 is for the viscosity

K

due to

momentum.

It is seen from Fig. 1 that the results obtained by the

nonequilibriumdynamics simulations are in good agreement

with the theoretical solutions shown in Eq. (88) for both

cases of

/10 and

of small number densities such as n

0

= 0.5, the simula-

tion results have signicant errors and, therefore, qualitative

properties are relatively difcult to identify. That the num-

ber density n

0

is smaller than unity means that a sufciently

large number of particles do not exist around an arbitrary

particle within the range of the radius r

c

from its center. In

this situation, the accuracy of the viscosity data is strongly

dependent on whether or not there are other particles which

interact with the particle of interest. Hence such a situation

(a)

(b)

Fig. 1. Inuence of

by nonequilibrium dynamics method (a) for

(

D

error

= (5.2, 1.5) for n

2

0

tively, for n

0

= 10, (1.5, 0.32) for n

2

0

for n

0

= 3.16, and (0.049, 0.022) for n

2

0

n

0

=0.5, in (a); similar errors are included in (b)).

causes signicant errors of the simulation results of viscos-

ity, which has been seen for n

0

= 0.5 in Fig. 1. We may

conclude from this fact that it is desirable to take the number

density as n

0

1.0 in simulating a ow problem by means

of the dissipative particle dynamics method.

Fig. 2 clearly shows that the simulation data are larger

than the theoretical solutions, and this tendency becomes

more signicant for larger values of

of dissipative forces is of the same order of the momentum,

that is, when

K

agree

well with the theoretical solutions. On the other hand, at

the momentum, the discrepancy between the simulation re-

sults and the analytical solutions has a tendency to increase

with values of

dial distribution function does not signicantly change for

values of

to the mechanism other than the assumption of molecular

chaos, adopted here. Some researchers attempted to explain

the discrepancy between simulation results and theoretical

solutions concerning the viscosity due to the momentum, in

terms of the pair collision theory [21].

262 A. Satoh, T. Majima / Journal of Colloid and Interface Science 283 (2005) 251266

(a)

(b)

Fig. 2. Inuence of

equilibrium dynamics method (a) for

(

K

error

= (0.57, 1.47) for 1/

0

= 10,

(0.40, 0.62) for 1/

0

= 3.16, and

(0.44, 0.12) for 1/

0

= 0.5, in (a);

similar errors are included in (b)).

6.2. Inuence of

Fig. 3 shows the inuence of

dissipative forces. It is seen from Fig. 3 that the values of

cases of n

0

= 3.16 and 10.0. As will be shown later in Fig. 9,

the radial distribution function changes signicantly for dif-

ferent values of

to dissipative forces,

D

, is not strongly dependent on the

shape of the radial distribution function.

Fig. 4 shows the dependence of the viscosity on the num-

ber density of particles: Fig. 4a is for the viscosity

D

due

to dissipative forces, and Fig. 4b is for the viscosity

K

due to momentum. Since the theoretical solutions are valid

for n

ment with the analytical solutions for the values of n

0

which

satisfy the condition n

.

This agreement becomes worse with decreasing values of n

0

smaller than unity; especially, the results for

= 10 and

large error ranges. As already pointed out, this is presumed

to be due to the situation in which the ambient particles of an

Fig. 3. Inuence of

D

error

=

(1.2, 3.1) for

0

= 10 and

n

0

= 3.16 and

= 10).

(a)

(b)

Fig. 4. Inuence of number density on viscosity: (a) for viscosity due

to dissipative forces and (b) for viscosity due to momentum (

D

error

=

(2.7, 0.12) for n

0

= (10, 1), respectively, in the case of

= 25 and

0

= (10, 0.5), respectively, in the case

of

= 10 and

= 1, in (a);

K

error

= (1.1, 0.24) for n

0

= (10, 1),

respectively, in the case of

= 25 and

n

0

= (10, 0.5), respectively, in the case of

= 10, and

= 1, in (b)).

arbitrary particle come to be less for decreasing the number

density smaller than unity, which leads to the large uctu-

ation in the contribution of dissipative particles to physical

A. Satoh, T. Majima / Journal of Colloid and Interface Science 283 (2005) 251266 263

quantities such as transport coefcients with time. Although

the viscosity

K

due to momentum shown in Fig. 4b has a

large error range, it is clearly seen that there is a signicant

discrepancy between the simulation and theoretical values,

and this tendency does not strongly depend on the values

of n

0

. As already pointed out in Fig. 2, since the radial distri-

bution function does not signicantly deviate from g(r) = 1

(shown later in Fig. 10a), it is presumed that this discrepancy

for

= 10 and

than the invalidity of the molecular chaos assumption.

6.3. Inuence of time interval on mean velocity of particles

and viscosity

Fig. 5 shows the inuence of the time interval h

(=

t

nite difference equations, on the mean velocity of particles

and the viscosity. It is seen from Fig. 5a that the viscos-

ity

D

does not strongly depend on the time interval for

h

cosity due to momentum,

K

, is signicantly dependent

on the values of h

appear from h

K

signicantly

increase with increasing values of the time interval. A sim-

ilar tendency can be observed in Fig. 5c, in which the mean

velocity of particles signicantly increases from h

0.01

with the values of h

mensionalized in such a way of being v

= 1, this condition

has to be satised in actual simulations. We may, therefore,

conclude that the simulations have to be conducted using a

sufciently small time interval such as h

= 0.0001, adopted

here.

6.4. Inuence of shear rate and number of particles on

viscosity

Fig. 6 shows the inuence of the shear rate of a simple

shear ow and the number of particles on the viscosity. It

is seen that the simulation results come to have signicant

errors with decreasing shear rate, since just a weak simple

shear ow is generated for such situations. This character-

istic is observed for both cases of

D

in Fig. 6a and

K

in Fig. 6b, especially in the results of

K

. It is seen from

Fig. 6c that the mean velocity v

the shear rate after

range for the shear rate

satisfying the condition of v

generating a simple shear ow with an appropriate shear

strength. By taking account of these constraints, we here

adopted

Fig. 7 shows the inuence of the number of particles on

the viscosity

D

due to dissipative forces. It is seen from

Fig. 7 that a larger system is required for a smaller num-

ber density to remove the dependence of the results on the

number of particles. This means that the interactions of the

(a)

(b)

(c)

Fig. 5. Inuence of time interval on (a) viscosity due to dissipative forces,

(b) viscosity due to momentum, and (c) average velocity of particles

(

D

error

= (0.43, 2.7) for h

of n

0

= 10,

= 25, and

h

0

= 3.16,

= 10, and

K

error

= (0.34, 1.1) for h

= (0.01, 0.0001),

respectively, in Case A, and (1.1, 0.62) for h

tively, in Case B, in (b)).

particle of interest with the ambient particles come to de-

pend on the dimensions of the system, unless a sufciently

large system is used for the cases of small number densities.

As already pointed out, the number density has to be taken

as sufciently large, and a large system such as N = 500,

adopted here, at least has to be adopted to remove the de-

pendence of results on the system size.

264 A. Satoh, T. Majima / Journal of Colloid and Interface Science 283 (2005) 251266

(a)

(b)

(c)

Fig. 6. Inuence of shear rate on (a) viscosity due to dissipative forces,

(b) viscosity due to momentum, and (c) average velocity of particles

(

D

error

= (0.055, 2.7) for

and (0.0064, 0.32) for

K

error

= (0.028, 1.1) for

(0.017, 0.62) for

6.5. Inuence of

distribution function

Finally, we show the results of the radial distribution

function [18] in Figs. 810 in order to clarify the quantitative

dependence of the internal structure on

ber density of particles. Figs. 8, 9, and 10 show the inuence

of

It is seen from Fig. 8 that the radial distribution function

is almost independent of the values of

Fig. 7. Inuence of number of particles on viscosity due to dissipative forces

(

D

error

= (1.7, 6.1) for N = (1372, 108), respectively, in Case A, and

(0.19, 0.68) for N =(1372, 108), respectively, in Case B).

(a)

(b)

Fig. 8. Dependence of radial distribution function on

for

= 10 (a) for

n

0

= 3.16 and (b) for n

0

= 10.

of n

0

= 3.16 and 10.0. Although the theoretical solutions of

the viscosity have been derived under circumstances of ne-

glecting the internal structure of the system, that is, under

the molecular chaos assumption, it is very interesting that

the theoretical solutions agree well with the simulation re-

sults (Fig. 1), irrespective of the system being in a gas-like

or liquid-like internal structure, as shown in Fig. 8.

Fig. 9 clearly shows that the radial distribution function

strongly depends on the values of

. A more signicant

repulsive force acts between particles with increasing the

A. Satoh, T. Majima / Journal of Colloid and Interface Science 283 (2005) 251266 265

(a)

(b)

Fig. 9. Dependence of radial distribution function on

(a) for n

0

= 3.16

and

0

= 10 and

= 25.

values of

liquid-like structure for

= 25 and

of

of dissipative and random forces is much smaller than that

of repulsions due to conservative forces. This means that the

merits of the dissipative particle dynamics method cannot

function effectively under such circumstances. It is, there-

fore, presumed that

has to be taken as

<

to make

the dissipative particle dynamics method effective. It is seen

from Fig. 9a that the molecular chaos assumption is satised

to a certain degree for

for

Nevertheless, as already shown in Fig. 3, the viscosity

D

due to dissipative forces is almost independent of the values

of

forces do not strongly depend on the internal structure of the

system.

It is seen from Fig. 10 that the radial distribution function

is not strongly dependent on the number density. However,

the curve for the case of n

0

= 6.0, in which the particle of

interest can interact with a sufcient number of ambient par-

ticles, slightly deviates from the results for n

0

= 0.2 and 1.0,

in which there are not sufcient particles around the particle

of interest.

(a)

(b)

Fig. 10. Dependence of radial distribution function on number density of

particles (a) for

= 10 and

=25 and

=2.5.

Fig. 11. Results of radial distribution function obtained by Espanol et al.

[22].

Finally, we compare the present results of the radial distri-

bution function with other simulation results obtained by Es-

panol et al. [22]. They investigated the relationship between

the dissipative particle dynamics and the smoothed particle

dynamics methods. In the concrete, the behavior of the clus-

ters of particles, which correspond to dissipative particles

in the present study, was investigated by means of conduct-

ing equilibriummolecular dynamics simulations of a system

composed of particles with repulsive interactions. Fig. 11

266 A. Satoh, T. Majima / Journal of Colloid and Interface Science 283 (2005) 251266

shows one of the results concerning the radial distribution

function, which were obtained by Espanol et al. [22]. From

the potential curves of the mean force in their paper [22], it

is seen that R in their notation roughly corresponds to 3r

sults for a larger value of

see fromcomparing Fig. 9 (also Fig. 10) with Fig. 11 that the

shape of the curves are quite similar between the present and

their results, in which a small increase at very short distances

can be observed more signicantly with decreasing values

of

approaches a usual

system such as a molecular one, so that dissipative parti-

cles cannot penetrate each other due to a high-energy barrier.

This leads to the fact that the curves of the radial distribution

function comes to have an ordinary shape for a liquid or gas,

which has no small increase within a short distance range.

7. Conclusions

In order to investigate the validity of the dissipative par-

ticle dynamics method, which is a mesoscopic simulation

technique, we have derived expressions for transport coef-

cients such as viscosity, from the equation of motion of

the dissipative particles. In the concrete, we have shown the

FokkerPlanck equation in phase space, and macroscopic

conservation equations such as the equation of continuity

and the equation of momentum conservation. The basic

equations of the single-particle and pair distribution func-

tions have been derived using the FokkerPlanck equation.

The solutions of these distribution functions have approx-

imately been solved by the perturbation method under the

assumption of molecular chaos. The expressions of the vis-

cosity due to momentum and dissipative forces have been

obtained using the approximate solutions of the distribution

functions. Also, we have conducted nonequilibrium dynam-

ics simulations to investigate the inuence of the parame-

ters, which have appeared in dening the equation of motion

in the dissipative particle dynamics method. The theoreti-

cal values of the viscosity due to dissipative forces in the

HK theory are in good agreement with the simulation re-

sults obtained by the nonequilibrium dynamics method, ex-

cept in the range of small number densities. There are restric-

tion conditions for taking appropriate values of the number

density, number of particles, time interval, shear rate, etc., to

obtain physically reasonable results by means of dissipative

particle dynamics simulations.

References

[1] P. Mazur, W. van Saarloos, Physica A 115 (1982) 21.

[2] W. van Saarloos, P. Mazur, Physica A 120 (1983) 77.

[3] P.J. Hoogerbrugge, J.M.V.A. Koelman, Europhys. Lett. 19 (1992) 155.

[4] J.M.V.A. Koelman, P.J. Hoogerbrugge, Europhys. Lett. 21 (1993) 263.

[5] G. Bossis, J.F. Brady, J. Chem. Phys. 80 (1984) 5141.

[6] J.F. Brady, G. Bossis, J. Fluid Mech. 155 (1985) 105.

[7] L. Durlofsky, J.F. Brady, G. Bossis, J. Fluid Mech. 180 (1987) 21.

[8] A. Satoh, R.W. Chantrell, G.N. Coverdale, S. Kamiyama, J. Colloid

Interface Sci. 203 (1998) 233.

[9] A. Satoh, G.N. Coverdale, R.W. Chantrell, J. Colloid Interface Sci. 231

(2000) 238.

[10] A. Satoh, J. Colloid Interface Sci. 243 (2001) 342.

[11] A. Satoh, J. Colloid Interface Sci. 255 (2002) 98.

[12] P. Espanol, P. Warren, Europhys. Lett. 30 (1995) 191.

[13] P. Espanol, Phys. Rev. E 52 (1995) 1734.

[14] C.A. Marsh, G. Backx, M.H. Ernst, Phys. Rev. E 56 (1997) 1676.

[15] E.S. Boek, P.V. Coveney, H.N.W. Lekkerkerker, P. van Schoot, Phys.

Rev. E 55 (1997) 3124.

[16] P. Espanol, Europhys. Lett. 40 (1997) 631.

[17] J.B. Avalos, A.D. Mackie, Europhys. Lett. 40 (1997) 141.

[18] A. Satoh, Studies in Interface Science: Introduction to Molecular-

Microsimulation of Colloidal Dispersions, Elsevier Science, Amster-

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[19] K.E. Novik, P.V. Coveney, J. Chem. Phys. 109 (1998) 7667.

[20] M.P. Allen, D.J. Tildesley, Computer Simulation of Liquids, Claren-

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[21] A.J. Masters, P.B. Waeewn, Europhys. Lett. 48 (1999) 1.

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