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Original Title: EnskogTheoryRigidDiskFluid J.chem.Phys 1971

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BLACK

16 T. G. Slanger and G. Black, J. Chem. Phys. 53,3717 (1970).

17 G. Black, T. G. Slanger, G. A. St. John, and R. A. Young, J.

Chem. Phys. 51, 116 (1969).

18 T. G. Slanger and G. Black, J. Chem. Phys. 51, 4534 (1969).

19 E. C. Y. Inn (private communication).

20 H. Wise (private communication).

21 T. G. Slanger and G. Black, 53, 3722 (1970).

22 W. Felder, W. Morrow, and R. A. Young, J. Geophys. Res.

75,7311 (1970).

23 K. Schofield, Planetary Space Sci. 15,643 (1967).

24 H. Yamazaki and R. J. Cvetanovic, J. Chem. Phys. 40, 582

(1964); 41,3703 (1964).

25 N. G. Moll, D. R. Clutter, and W. E. Thompson, J. Chem.

Phys. 45, 4469 (1966).

THE JOURNAL OF CHEMICAL PHYSICS

26 E. Weissberger, W. H. Breckenridge, and H. Tauhe, J. Chem.

Phys.47, 1764 (1967).

27 M. Arvis, J. Chim. Phys. 66, 517 (1969).

28 T. G. Slanger, J. Chem. Phys. 48, 586 (1968).

29 J. D. Simmons, A. M. Bass, and S. G. Tilford, Astrophys. J.

155,345 (1969).

30 C. A. Barth, Science 165, 1004 (1969).

31 D. A. Parkes, L. F. Keyser, and F. Kaufman, Astrophys. J.

149,217 (1967).

32 L. D. Gray Young, Icarus 11, 386 (1969).

33 D. M. Hunten, Can. J. Chem. 47, 1875 (1969).

34 S. I. Rasool, J. S. Hagan, R. W. Stewart, and L. H. Russell,

J. Atmospheric Sci. 27, 841 (1970).

VOLUME 54, NUMBER 5 1 MARCH 1971

Enskog Theory for a Rigid Disk Fluid*

DAVID M. GAsst

Lawrence Radiation Laboratory, University of California, Livermore, California 94550

(Received 3 August 1970)

The Enskog theory for a dense fluid of rigid disks is developed. The collisional contribution, which

dominates in liquids, is derived and added to the kinetic term, which describes a dilute gas. Expressions

for shear and bulk viscosity and for thermal conductivity are obtained. The initial correlations are evaluated

via the autocorrelation function approach, and the exponentially decaying functions which result are

related to the Enskog theory.

I. INTRODUCTION

Calculations in two-dimensional systems often serve

as prototypes. In the investigation of long-time correla-

tions by molecular dynamics computation, rigid disk

systems are within the practical limitations of present

day computers, whereas hard sphere systems are not.!

The density expansion of the transport coefficients,

based upon a generalized Boltzmann equation for a

two-dimensional system, breaks down in the triple colli-

sion contribution, affecting the first-order density cor-

rection.' In three dimensions the density expansion

breaks down beyond first order in the density, thereby

complicating the numerical evaluation of the diver-

gence. The Enskog theory for rigid disks can be used

as a handle on these and other rigorous calculations.

The Enskog theory for a hard sphere fluid

3

yields

transport coefficients over the entire density range and,

in the low density limit, goes over to the Boltzmann

form. The Enskog theory takes into account exactly

the term in the Boltzmann equation which arises from

the difference in position of colliding molecules. In

addition, the influence of triple and higher-order colli-

sions is approximated by scaling the Boltzmann collision

integral with the local equilibrium radial distribution

function at contact. The same observations also apply

to a rigid disk fluid. The kinetic contribution to the

transport coefficients of a rigid disk fluid has been ob-

tained by Sengers.2 This contribution arises from the

bodily movement of molecules between collisions. In

dense fluids the collisional or potential contribution is

dominant. This term, which derives from transport

between molecules while they are in contact, is the one

on which we focus in this paper.

In the Enskog theory, correlations in time among

many molecules are only estimated, while two-body

effects are calculated exactly. Correlations for short

times, as reflected in the various autocorrelation func-

tions, are expected to be more accurately described by

this theory than those which persist for many mean

collision times. This observation is important since

hydrodynamic and molecular dynamics calculations

4

suggest a slow decay for the autocorrelation functions,

while exponentially decaying functions result from the

low-density, zeroth-order Sonine polynomial solution

to the Boltzmann equation. As yet, only the velocity

autocorrelation function has been shown to possess a

long-time tai1.

4

However, since the stress and heat-flux

autocorrelation functions contain a term which depends

only on the velocity field at long times, it is reasonable

to suppose that these functions decay slowly at such

times.

The initial values and slopes of the autocorrelation

functions are evaluated. Then the assumption of expo-

nential decay yields transport coefficients which agree

with the ones calculated from the low-density, zeroth-

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ENSKOG THEORY FOR A RIGID DISK FLUID 1899

order Sonine polynomial solution to the Boltzmann

equation. Initial correlations are related to terms which

appear in the Enskog theory.

II. COLLISIONAL TRANSFER

In as much as the Enskog theory for dilute systems of

rigid disks is already known,2.5 only the collisional con-

tribution is required in order to evaluate the transport

coefficients for dense fluids. This term arises from the

instantaneous transfer of a molecular property across

a line, I, while two disks centered on opposite sides of

t are in contact.

Use of the molecular chaos approximation implies

that the probable number of collisions per unit time,

where c, CI, and k lie in the ranges dc, dCI, and dk, is

(uk) (uk) ]u

2

(gk)dkdcdcI(kn)dl;

(1)

c and CI are the velocities of the colliding molecules, k

is a unit vector in the direction of the line of centers,

x(r) is the Enskog scaling factor, f is the one-particle

distribution function, (uk) and (uk) are the

centers of the two molecules of diameter u, g= CI- c,

and n is the unit normal to t.

For each molecular property, if;, at each collision,

there is a net transfer of if;' -if; across I, where if; is the

value prior to collision and if;' is the value after colli-

sion. The total rate of transfer across I by all collisions,

per unit length, is

1fl (if;' (uk) (uk)]

gk>O

X (gk) (kn)dkdcdcl. (2)

The above expression, which is of the form Vrn, gives

the vector flux, V" of if;. Inasmuch as only linear trans-

port coefficients are of interest here, the distribution

functions in (2) can be expanded about the point of

contact of the disks, r, and only terms up to the linear

term in the gradien t are kept. Linearization yields the

collisional contribution to the flux

V,=I+i{ilx)J f fW-if;)fORk

. (a/ar) log(j/R) (gk)kdkdcdcI, (3)

where

fO is the local equilibrium single-particle distribution

function, and all quantities are evaluated at r.

III. MOMENTUM TRANSPORT

In order to evaluate the momentum transport, we

take if;=mC=m(c-co), where Co is the macroscopic

velocity at the point r. Substitution of if; into Eq. (3)

and integration with respect to k using the identities

(5) and (6) yieldEq. (7):

f(C'-C)k(gk)dk= Jkk(gk)2dk= t1l'(2gg+g2U),

(5)

Jkk(k V) (kg)2dk= (4/15)

X[V.g(gg+g2U)/g+g(Vg+gV)], (6)

where U is the unit tensor and V denotes a vector,

which will be taken as (a/ar) log(j/R):

V m = ft (1I'

mu2

x) ff fh (2gg+ U g2) dcdcI

(

a fO a fO)]

+ g g - log - + - log -0 g dcdcl.

ar R ar h

(7)

Since g= C

I

- C and the odd moments of C and C

I

are zero, and since Jfdc=N / A=nand ffCCdc=n[CC]I,

the first term in Eq. (7) can be written as

V

m

l=i{bp

2

x) (2[CC]I+[C2]IU), (8)

where the coarea, bp=H1I'nu

2

), and p=mn have been

introduced. The remaining term in Eq. (7), V m

2

, con-

tains the factor

(9)

The terms involving aT/ar in V

m

2 are odd functions of

C or CI and thus vanish on integration. The remaining

terms are more conveniently evaluated when the vari-

ables G

o

= (C+C

I

)/2 and g=CI-C are introduced.

The result is

V

m

2= - (2::TY ff exp [- (

G

0

2+tg2)]

X {aco : gg(gg+g2U)

ar g

+g .g) g+g .g)]} dGodg. (10)

Performing the integration indicated in Eq. (10)

yields

Vm2= -wIHaO[co]/ar)+Hl(a/ar) co), (11)

where w= (5n2ilx/8) (1I'mkT) 1/2 and

aO[coJii /ar= acdar

j

) + (acoj/ari) (a/ar) . COOij.

The sum of Eqs. (8) and (11) yields the collisional

contribution to the momentum flux and is the potential

part of the pressure tensor. The rate of transport due

to molecular motion between collisions is p[CCJ. There-

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1900 DAVID M. GASS

fore, the total pressure tensor is

F= p[l (bpx) J[CCJ+i (bp

2

x) [C2JU

-wi t(aO[coJ/ar) +tU(a/ar) col. (12)

To first order in the gradient,

p[CCJ = nkTU -x-

l

[l (bpx) J21)0(a

O

[coJ/ar), (13)

where 1)0= (1/20') (mkT/Tr)

I/2

b

o

(N) is the coefficient of

shear viscosity of the dilute gas. Further, the hydro-

static pressure, PO, is given by

P=knT(1+bpx) - (4w/5) (a/ar) co. (14)

The deviation of the pressure tensor from the hydro-

static pressure, from Eqs. (12)-(14) and the identity

[C2J=2kT/m is found to be

tlF= -I (21)0/x)[1+Hbpx)J2+twl (aO[coJ/ar). (15)

The definitions of wand 1)0 are used, and the identifica-

tion of the coefficient of -2(a

O

[coJ/ar) with the co-

efficient of shear viscosity yields

1)= 1)obp(l/bpx) + 1 + bpx Ii+ [2/Trb

o

(N) Jl). (16)

The third Sonine polynomial approximationS gives

b

o

(3) = 1.022 and therefore

1) = 1)obp[ (l/bpx) + 1 +0.8729bpx]. (17)

Vm2 depends on only the local equilibrium distribution

function and therefore does not depend on the Sonine

polynomial correction factor, bo(N).

The coefficient of bulk viscosity, c/J, is identified with

the coefficient of - (a/ar) coO in Eq. (12) and there-

fore

c/J= 4w/5 = [4x/ll'bo(iV) J (bp )21)0, (18)

which becomes

c/J = 1)

o

bp (1.246bpx) ,

when b

o

(3) = 1.022 is used.

s

IV. ENERGY TRANSPORT

(19)

In order to evaluate the energy transport, we take

1/I=mC2/2. Integration with respect to k in Eq. (3)

using Eqs. (20)-(22) yields Eq. (23), which is the

collisional contribution to the heat flux:

J (C

'

LC2)k(gk)dk= Jk (g+2C)k(gk)2dk

=2J(kG

o

)k(g.k)2dk, (20)

2J (k Go)k(gk) 2dk= ill'[2g(g Go) + g2G

o

J, (21)

J (C

'

2-C2) (k V) (gk)kdk

= !s{ Go g[g(g. V) +g2VJ/ g

+g[g(Go V) +Go(g V) Jl, (22)

Ve= /6 (ll'

mO'2

X) J Jffl[2g(g Go) + g2G

o

Jdcdcl

+ /5 (mO'3X)J JjOR[ (Go g) (gg+g2U) /g

+g(gGo+Gog)]- VdcdcI, (23)

where V= (ajar) log(f/R). As 2g(gG

O

)+g2G

O

=

![C

I

2C

I

+C2CJ, the first term in Eq. (23) is

(24)

Use of (9), where now the terms involving aco/ar

are the integrals of odd functions of C and C

I

, and the

introduction of the variables Go and g yield

+g(g.G

o

) (gGo+Gog). aT] dGodg. (25)

ar

Integration over Go and then g yields

(26)

where C

v

= kim and w= (uSn2x) (ll'mkT)I/2.

The collisional contribution of the heat flux, given

by Eqs. (23), (24), and (26), is augmented by the

energy transfer due to molecular motion, (p/2) [C2CJ,

and the total energy flux, Q, is thus found to be

Q= + (3bpx/4) J[C2CJ-c

v

w(aT /ar). (27)

To first order in the temperature gradient,

= - [1 + (3bpx/4) J(Ao/x)(aT /ar) , (28)

where Ao= (2/0') (k

3

T/mll')I/2al (N) is the low-density

formulation of the coefficient of thermal conductivity.

The insertion of (28) into (27) yields

Q= - ['\o/X[l+ (3bpx/4) J2+cvwJ(aT /ar) , (29)

and thereby the coefficient of thermal conductivity, A,

can be expressed as

A = (AD/X) [1 + (3bpx/4) J2+cvW

= Aobp(l/bpx) +!+bpx{ 1

9

6 + [l/ll'al (N) Jl). (30)

The third Sonine polynomial approximationS gives

al(3) = 1.029 and therefore

A= Aobp[ (l/bpx) +!+0.8718bpx]. (31)

V. AUTOCORRELATION FUNCTIONS

At low densities exponentially decaying autocorrela-

tion functions lead to coefficients of shear viscosity

and thermal conductivity equal to the ones calculated

from the zeroth-order Sonine polynomial solution to

the Boltzmann equation. This result was first observed

for the shear viscosity in rigid sphere systems.

6

We next consider the shear and bulk viscosity in

some detail. The presentation is based on that of Ref.

6. The coefficient of shear viscosity, 1), for long-wave-

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ENSKOG THEORY FOR A RIGID DISK FLUID 1901

length, zero-frequency processes is given by

71= (AkT)-ll'" (jXy(t)jXy(t+r) )dr

o

I

t

J'" = (AkTts)-l jXy(t)dt jXY(s)ds,

o t

(32)

where ergodic theory considerations and a variable

change from t+r to s allow the passage to the second

formulation of Eq. (32), and where

N N

JXY(t) = m L Ci""(t)Ciy(t) + L Rix(t)Fiy(t)

i=l i=l

N

= m L Cix(t) Ciy(t)

i=l

m

+"2?;j uki/kil(kij"gij)O(t-te), (33)

Cix(t) and Ciy(t) are the x and y velocity components of

particle i at time t and Fiy(t) is the y component of the

force on i at time t. The direction of the line of centers

from j to i is given by kij and the relative velocity

gij=Cj-Ci' The second formulation of Eq. (33) is a

specialization to rigid disk systems where te is the time

of collision c. The zeroth-order Sonine polynomial solu-

tion of the Boltzmann equation for the coefficient of

W(O), 5(0), and (Rc

xY

)2> can be evaluated exactly:

shear viscosity yields

7Joo=7Jo/bo(N) = (1/2u) (mkT/rr) 1/2,

and the Enskog expression for the collision rate of rigid

disks is r= (2Nbpx/u) (kT/rrm) 1/2. With the help of

these expressions Eq. (32) can be converted into

71 [srl'" - = X-I - W(t)dt

710 N 0

(34)

The effects of considering rigid disks, as compared to

hard spheres, are included in the coefficients of the

integrals of Eq. (34), which can be compared to Eq.

(S) of Ref. 6. The definitions of W, 5, and R/Y are

given in Eq. (7) of this reference.

'"

(Re

XY

)2) and L (RexYRe+kXY)

k-l

arise from correlations of molecular forces. The former

term is a zero-time correlation effect and represents

the contribution of instantaneous correlations to the

transport coefficient.

m2 N

W(O)= 4N(kT)2E (c/c/)=t,

(35)

(

m )3/2 J J J dcdc1dk exp[ - (m/2kT) (C

2

+CI

2

) ] (gk)2kXkY(cXCY+ClxCIY)

5(0) = - 2kT J J J dcdc

1

dk exp[ - (m/2kT) (C

2

+CI

2

) ](gk) .

(36)

First, the coordinate transformations, c_= C-Cl and C+= C+Cl, are made and the integrations over C+ are carried

out. Next k is projected onto L and a vector orthogonal to it, CJ.:

k=(L/i Li) coso+(cJ./i cJ.i) sinO, (37)

where 0 measures the angle between c_ and k. The expression of k

x

and k

y

in terms of 0 using (37) and the use of

the identity (gk)2= (cOS

2

0)C

2

allow the integrations in (36) to be carried out with the result

5(0) = - (1r)1/2/SV2,

(Re

xY

)2)= ~ ) J J J dcdc1dk exp[ - (m/2kT) (C

2

+CI

2

) ](gk)3(kXkY)2

2kT If J dcdc

1

dk exp[ - (m/2kT) (C

2

+CI

2

) ](gk)

_lc

-4'

The contribution of the (Re

XY

)2) term to 71 is given by Eqs. (39) and (34), and is

71(0) = 7Jobp[2bpx/1rbo(N)],

(3S)

(39)

(40)

where the zero in the parentheses indicates it is the zero-time contribution. 71(0) is identical to the unperturbed

single-particle distribution function's contribution in the Enskog theory.

The initial slope of Wet) can be calculated exactly and that of Set) can be calculated using the molecular

chaos approximation. It is then found that both decay as e-', where s is the mean number of collisions per particle.

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1902 DAVID M. GASS

The diagonal elements of the stress autocorrelation function characterize the coefficient of bulk viscosity, :

+1)= (AkT)-! [" (Jq,XX (O)Jq,xx (t) )dt,

o

(41)

where Jq,xx(t) =Jxx(t) - (px(t, with pI given by (33) when x replaces y, leads directly to

P+1)P= 1)

0

0 [16 (b

pX

)2 o (Rc

xx

)2)+ f (R/xRc+kXX].

X 7r k=!

(42)

Only the term involving intermolecular forces in px has been written in Eq. (42), as it is the only nonzero con-

tribution to in the Enskog theory. Further,

(

)2

(

m )fffdCdCldkexp[-(m/2kT)(C2+C!2)](gok)kX4

Rxx )- -

c - 2kT f f fdcdc!dk exp[ - (m/2kT) (C

2

+CI

2

) ](gok)

=1

(43)

A comparison of Eq. (18) with Eqs. (42) and (43) indicates that the only contribution to the bulk viscosity in

the Enskog theory arises from zero-time correlations of the diagonal elements of the stress tensor. The only non-

zero contribution to from the initial autocorrelation of the microscopic stress tensor is due to the correlation

of the impulsive force term with itself at the time of collision of two molecules. Evidently the deviations from

local equilibrium (in the distribution approach) give rise to correlations of more than two particles and to cor-

relations separated in time.

Similar calculations can be performed for the coefficient of thermal conductivity. The results again show an

agreement between an exponentially decaying autocorrelation function and the zeroth-order Sonine polynomial

solution to the Boltzmann equation. For the heat flux autocorrelation function the decay is found to be ~ e / 2 .

VI. DISCUSSION

This paper presents the Enskog theory for a dense

fluid composed of rigid disks. The collisional contribu-

tion, which dominates in dense fluids, is derived and

added to the low-density kinetic term. By determining

the initial values of the autocorrelation functions, we

conclude that, at low density, an exponential decay of

the microscopic stress tensor and microscopic heat flux

autocorrelation functions gives results identical to the

zeroth-order Sonine polynomial solution to the Boltz-

mann equation. The exponent of the decay agrees with

that found for the cross term (which is first order in

the density) under the molecular chaos approximation.

The collisional contribution to 1) and to A contains

one term dependen t upon the single-particle equilib-

rium distribution function and one term dependent

upon deviations from this distribution. The former

term, which is more than twice the latter for 1) and

more than half the latter for A, is equal to the contribu-

tion of the instantaneous correlations of the stress

tensor and heat flux to the transport coefficients. Thus,

the integration of the exact autocorrelation functions

from time zero to a few mean collisions times, when e-

S

and e-

s

/

2

are essentially zero, should give transport co-

efficients not unlike those predicted by the Enskog

theory. The early time behavior of Wet) and S(t) is

not expected to be greatly dependent on the density,

whereas

(Rc i.iRc+! i.i)

might vary by a factor of 2 over the fluid density range,

as it does in systems of hard spheres.!

At long times in rigid disk systems, correlations are

not believed to decay rapidly. This discrepancy from

the Enskog theory reflects the approximate treatment

of multiple correlations by the scaling of two-body

interactions. It is hoped, however, that the Enskog

theory, which represents the "best" scaled, binary colli-

sion theory, might be grafted onto a realistic long-time

description, involving a hydrodynamic model. The

availability of such a theory will provide the means

for the accurate determination of transport coefficients

for rigid disk systems.

ACKNOWLEDGMENTS

The author would like to express his appreciation to

T. E. Wainwright, W. G. Hoover, and B. J. Alder for

helpful discussions.

* Work performed under the auspices of the U.S. Atomic

Energy Commission.

t Present address: Physics Dept., University of Toronto,

Toronto 5, Ontario, Canada.

1 B. J. Alder, D. M. Gass, and T. E. Wainwright, ]. Chem.

Phys. 53, 3813 (1970).

2]. V. Sengers, in Lectures in Theoretical Physics, Kinetic

Theory, edited by W. Brittin (Gordon and Breach, New York,

1967), Vol. IXC, p. 335.

3 S. Chapman and T. G. Cowling, The klatlzematical Theory of

Non-Uniform Gases (Cambridge U. P., London, 1939). The

notation of this reference is used throughout this paper.

4 B. J. Alder and T. E. \Vainwright, Phys. Rev. 1, A18 (1970).

5 ]. V. Sengers, "Triple Collision Effects in the Thermal Con-

ductivity and Viscosity of Moderately Dense Gases," Arnold

Engineering Development Center, Tenn., 1969, Tech. Rept.

AEDC-TR-69-68.

6 T. Wainwright, J. Chem. Phys. 40,2932 (1964).

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