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polyampholytes

Y. Rabin*+, ++, S. Panyukov++, m and M. Wilhelm+++, mm

+

Yukawa Institute for Theoretical Physics, Kyoto University, Kyoto 606-01, Japan

Department of Physics, Bar-Ilan University, Ramat-Gan 52900, Israel

+++

Department of Materials and Interfaces, Weizmann Institute of Science, Rehovot 76100, Israel

m

On leave from: Theoretical Department, Lebedev Physics Institute, Russian Academy of Sciences, Moscow 117924, Russia

mm

On leave from: Max-Planck-Institut fur Polymerforschung, D-55021 Mainz, FRG

++

We study the interaction between randomly and irreversibly charged rigid objects. We consider arbitrary parallel displacements of two rod-like polyampholytes and of two plates and calculate the statistical properties of the resulting energy landscape, such as the distribution of energy minima and the depth, width and density of typical energy wells, as a function of the

separation between the objects and of the Debye screening length. The possibility that stickslip phenomena may arise during relative motion of the objects is discussed. Other cases considered in this work are that of random distribution on one rod

and a periodic one on the other, and that of local periodic order on both rods.

1. Introduction

The statistical physics of interacting manybody systems deals with a thermodynamically large number of elementary units (atoms, spins, etc.), each of which is

described by a small number of parameters. This leads to a

class of models in which complex physical behavior arises

due to cooperative behavior of a large number of such

simple units. There is, however, a different class of interacting complex systems, of the type encountered in biology, in which the number of parameters necessary to specify a single unit (e. g., a protein) is very large. Due to the

inherent complexity of the individual units, even a small

number of such interacting objects can exhibit very complex behavior.

In this work we investigate a generic model of the latter

type, i. e., that of two interacting rigid objects on which a

random distribution of charges is irreversibly placed. Such

objects are extremely complex in the sense that complete

specification of the charge distributions requires precise

information about the location of each of the charges, the

number of which can be arbitrary large, depending on the

size of the objects. We allow for charges of both signs and

the resulting combination of long-range attractive and

repulsive forces leads to the appearance of complex interaction energy landscapes. We would like to stress that our

model differs from that of usual polyampholytes (i. e.,

polymers carrying charges of both signs) since we assume

that the charged objects are rigid and therefore both the

charge distribution and the conformation are quenched.

Recall that all polyampholyte models to date deal with

flexible polymers [1] and consider the thermal fluctuations

and the associated entropic elasticity of the polymer

chains.

In Sec. 2 we study the statistical properties of the interaction energy landscape of two parallel rod-like polyampholytes, on which positive and negative charges were randomly and irreversibly placed. The detailed derivation of

these results was presented in [2]. New results are derived

Fax: +972-3-535 3298

E-mail: yr@rabinws.ph.bin.ac.il

544

interacting with a periodic charge distribution on the other,

and for the case where charge distributions on both rods

are locally periodic, up to some finite correlation length. In

Sec. 3 we present the analogous results for two parallel

randomly charged plates and discuss the possibility of

stickslip motion when force is applied to one of the plates.

In Sec. 4 we discuss our results and point out the limits of

validity of our approach.

2. Parallel rods

2.1. Random charge distributions

L and L9, respectively, on which positive and negative

charges with local charge densities qi x and qi x (the

index i takes the values 1 and 2; corresponding to the two

rods) are randomly and irreversibly placed. The frozen distribution of total charge on each rod is given by qi x

qi x qi x (i 1; 2). Note that although different realizations of the charge distribution will have, in general, a

different selfenergy, we will disregard the question of

how such charge distributions can be prepared and assume

that all possible realizations are equally probable.

The assumption that the charges are randomly distributed on the rods with average charge density q q q

leads to a Gaussian distribution of the quenched variations

of density dqi x qi x q, with the second moment

dqi xdqj x9 gdij dx x9

the bar denotes averaging over the ensemble of all possible

realizations of quenched disorder

R on the rods, with probability Wdq V exp2g1 dq2 dx.

The charges on the two rods interact via a screened Couq q

lomb potential

Vx x9 expj x x9 2 h2 = x x92 h2 ,

where j1 is the screening length and h is the distance

between the rods. When the two rods undergo parallel rela-

Acta Polym. 1998, 49, 544 548 i WILEY-VCH Verlag GmbH, D-69451 Weinheim 1998

0323-7648/98/1010-0544$17.50+.50/0

coordinates,

R R the interaction energy is given by

Eu

dx1 dx2 q1 x1 q2 x2 Vx1 x2 u, where the

integration is taken over all the points in the two rods. We

assume that L s L9 and consider only relative displacements for which the two rods overlap. In the following we

will not consider any effects associated with the presence

of counterions (other than Debye screening, which can

arise due to the presence of added salt), i. e., counterion

condensation, electrical double layers, etc. [3]. While such

effects may be of importance in reallife situations, they

are irrelevant to the main theme of this work: the interaction between randomly frozen charge distributions on rigid

rods and plates.

The energy Eu associated with a particular relative

shift of the two rods differs, in

R general, from the average

interaction energy E q2 L dx Vx, by an amount

dEu Eu E. In Fig. 1 we plot a typical energy landscape dEu that results from the relative shift u of two

rods. This plot was generated by a computer simulation of

the randomly frozen charge distributions on the rods, with

periodic boundary conditions on the random charge distribution on the longer rod (the period is much larger than

either L or h and should not have a significant effect on our

results).

In order to characterize the energy landscape in a statistical sense, we calculate the average number of energy

minima Nmin EDE with energy in the interval (E,

E DE). This yields

Nmin E

dE dEuhw2 dEu=wu2

extr

where the sum goes over the positions u of all the energy

extrema for which wdEu=wu 0 and the h-function

ensures that only minima are counted (w2 dEu=wu2 A 0).

For two parallel rods, u is a scalar and w2 dEu=wu2 is the

inverse squared radius of curvature of the energy minimum, which is a measure of the stiffness of the potential

Fig. 2. Plot of the number of minima per unit energy per unit

length, Nmin E=L9 , as a function of their energy dE , for different

vertical separations between the rods. The broken line corresponds

to h L and the solid line to h 0:1L (with g 1).

ensemble of randomly charged rods, of lengths L and L9 .

In order to calculate the average in Eq. (2) we express

the h-function as an integral over a d-function and exponentiate each of the two dfunctions in the resulting product. Since the energy dE is quadratic in the charge density

dq and the density distribution function Wdq is Gaussian,

the functional integration over dq can be performed analytically (the details are reported elsewhere [2]). For

unscreened Coulomb interaction between the charges on

the rods, we obtain the following universal form:

Nmin E

L9

p pmin y

g hL

where

p

y2

y2

2

pmin y 3

exp

5 exp

16p2

2p

25p

y erf

y

p

5 p

and

E

y3

g

function of the relative displacement u (in arbitrary units of length)

for a randomly chosen realization of disordered charge distributions

on the rods. The crosses corresponds to h 1 and the solid line correspond to h 0:5.

y

r

h

L

of energy wells per unit energy and unit length, Nmin =L9 , as

a function of dE, for several values of L=h. Although this

distribution is always peaked at a negative value of dE

there is a finite probability of observing a potential well

with a positive value of dE: This reflects the possibility of

having local energy minima located inside broad energy

maxima (see Fig. 1). Note that the probability of observing

an energy minimum with energy much lower than dEmin

545

such minima are statistically insignificant. The distribution

is very broad and its width increases with L as L=h1=2 .

In the presence of screening, the average concentration

of potential wells (total number of minima divided by L9 ) is

s

1

m2 h

c

4

2p

m1 h

Rv

where mk h 3 2 0 dr wk Vr=wr k 2 are the second

moments of the corresponding derivatives of the potential.

For unscreened Coulomb interaction between the rods

(j 0) m1 l 1=h3 and m2 l 1=h5 , and thus c l 1=h (i. e.,

the distance between the energy minima is of order h). We

conclude that the density of energy minima increases with

increasing proximity of the rods and approaches the number

density of charges g at a distance h x 1=g, which corresponds to the limit of validity of our model (at such separations the charge distribution can no longer be considered as

continuous). In the presence of electrostatic screening, the

above qualitative picture remains valid in the range

g1 f h f j1 . At separations exceeding the screening

length, m1 l j1=2 h5=2 exp2jh and m2 l j3=2 h7=2

exp2jh and therefore c l j=h1=2 . The conclusion

that screening increases the number of energy minima

(although their depth is exponentially decreased compared

to the unscreened case) is quite unexpected.

The average depth of an energy minimum is

s

gm1 h

pL

dEmin

5

4

m2 h

and its characteristic width is

m2 h 1=2

wx

m3 h

distance between the typical minima, c1 , we conclude

that the characteristic minima form a densely packed random lattice. At distances smaller than the screening length

the average spacing of this lattice is of the order of the

spacing between the rods h and at larger distances it is

h=j1=2 . Both the curvature and the width of shallow

energy wells are small and since the probability of observing uncharacteristically deep wells is exponentially small,

the resulting energy landscape does not havep

a fractal character (i. e., is smooth). Note that jdEmin j V L, and since

for sufficiently large systems the energy of attraction can

easily exceed the thermal energy kB T, the frozen randomness of the charge distribution on microscopic scales may

result in pinning, i. e., the system will be trapped in one

of the typical energy minima. Such effects can be observed

by keeping the rods at a fixed distance and monitoring their

stickslip response to externally applied tangential forces.

This phenomenon will be discussed in more detail in the

following when we consider the interaction of charged

plates.

546

Another important result is the dependence of the stiffness of the average potential well, K w2 dEu=wu2 , on

the distance h between rods,

Kh Kh0 m2 h=m2 h0 1=2

Equation (7) shows that the distribution of the radii of curvature of the energy minima is invariant with respect to the

change of the distance between rods. Thus, when the two

rods approach each other, existing minima become progressively stiffer and deeper, just as in the case of rods with

charges that form a regular periodic lattice. At the same

time, new shallow minima appear and grow in depth as h is

reduced. The appearance of new minima is a characteristic

signature of random charge distributions on the rods and

has no analog in the periodic case, i. e., when the frozen

charge distributions on both rods are periodic, with the

same period k. In the latter case, the number of minima is

independent of the distance between the rods, and their

depth increases monotonically with decreasing separation

h.

Our main analytical results for the unscreened Coulomb

case can be rederived by a simple scaling estimate. Let us

replace the microscopic charge distribution by one that is

coarse-grained over a length scale h (the distance between

the rods). Each electrostatic blob contains gh charges of

both signs and thus the total charge per blob is of order

Qh lgh1=2 . Since there are L=h such blobs and the

average interaction energy between the rods vanishes

(assuming that there is no net charge on the rods), dE can

written as the sum of interaction energies of L=h neighboring blobs on the two rods. Each one of the contributions is

a random function, which takes the values lQ2h =h, and

therefore the total interaction energy is also a random

quantity with zero average and characteristic deviation

dE x l L=h1=2 Q2h =h l gL=h1=2 , in agreement with

the exact result, Eq. (5).

We study the interaction energy landscape for two parallel rods: rod 2 is of length L9 with a randomly frozen density distribution q2 and rod 1 is of length L (L s L9 ) with a

frozen periodic density distribution

dq1 x qeiqx q eiqx ;

q 2p=d

In the following we will assume that both rods are very

long and neglect end effects. Introducing

the Fourier transR

ikxx9u

Vk

and

forms

Vx

x9

dke

R

dq2 x dk9eik9x dqk9 , the interaction energy can be

written as Eu

Eu Vq dqq qeiqu Vq dqq q eiqu

The calculation of the average number of minima is performed using the method described in [2] and the resulting

expression for Nmin is very similar to that in Eq. (19) in the

above reference,

Acta Polym. 1998, 49, 544 548

Zv

Nmin E L

3 Z

Y

dkj

dKK

6

2p

j1

"

2

#

Djl kj kl

10

jl

0

1

m0

0 m1

D @ 0

m1

0 A

11

m2

m1 0

period d on both rods, with a finite correlation length rc ?

Clearly, when rc s h,L the interaction energy landscape is

not sensitive to the local periodic order and is identical to

that obtained for random charge distributions on both rods.

However, new results are obtained in the range rc S h,

which will be considered below.

Consider the charge density profile

dq1 x qeiqxvx q eiqxvx ;

where

jvx vx9j2 d2

with

mi q2i jVq j2

12

q

13

c

2p

which depends only on the wavelength of the periodic distribution of charge and is independent of the distance

between the rods. Thus, the number of energy minima for

the randomperiodic case is the same as in the case of identical periodic charge distributions on both rods. However,

while in the latter case the depth of energy minima scales

like L, in the present case the average well depth is given

by

p

p=2 p

dEmin

14

q gLjVq j

2

For screened Coulomb potentials,

p

Z

j x2 h2

iqx e

Vq dxe p

x 2 h2

15

dEmin is a function both the wavelength 2p=q and the distance between the rods, h. Obviously, this expression

vanishes in the limit jh S 1 (strong screening). In the

opposite limit, jh s 1 (no screening), we have to distinguish between the cases qh S 1,

s

2p qh

e

Vq x

qh

and qh s 1, for which

Vq x 2 lnqh

Since, in the case of random charge distributions on

both

p

rods, the depth of a typical minimum is dEmin V g L=h,

we conclude that for g h s 1this depth is larger in the randomperiodic case than in the randomrandom case.

Another difference between the two cases is that the number of such typical energy minima is independent of the

distance between the rods in the randomperiodic case and

decreases with the separation in the randomrandom case.

Acta Polym. 1998, 49, 544 548

q 2 p=d

jx x9j

rc

gx x9 dq1 xdq1 x9 2 jqj2 e2p

2p x x9

cos

d

jxx9j=rc

random case, where we replace the expressions for the

moments by

2 jqj4 rc 2k 2

q Vq

mk x

p2

and set g 1. As in the randomperiodic case, the concentration of wells is given by

c 1=d

and the average well depth is

p

dEmin L q2 rc LjVq j

3. Parallel plates

the statistical properties of the interaction energy landscape produced by the relative displacement u (u is now a

vector in two dimensions) of two parallel plates of areas A

and A9 (A s A9 ) separated by a distance h shows that the

typical landscape consists of closely packed minima and

maxima of similar depth and width [2]. In the unscreened

Coulomb case the density of these minima is c x h2

(their width and the spacing between them are of order h).

At distances exceeding the screening length we obtain

c x j=h. At separations smaller than the screening length,

the depth of a typical energy minimum is dEmin x gA1=2 (g

is the average number of charges per unit area), independent of the distance between the plates. At distances

exceeding the screening length, the depth decays exponentially with the separation between the plates.

In order to illustrate how this energy landscape may lead

to stickslip behavior, we consider the following gedanken

experiment (the geometry is similar to that of the surface

force apparatus, operated in the shear mode [4]): A spring is

attached to one of the plates (say plate 2, with area A9 ) and

the other plate (plate 1, with area A) is moved by a distance u

547

parallel to it. If the distribution of charge on the plates is uniform, there will be no restoring forces associated with this

displacement and consequently plate 2 will not move. The

presence of frozen random charge distributions on the plates

leads to the appearance of a large number of energy minima,

which correspond to different relative parallel displacements of the plates. Since, for macroscopic plates, the typical energy associated with these minima scales as A1=2 , for

sufficiently large plates it may become much larger that the

thermal energy kB T and the plates will get stuck in one of

the minimal energy configurations. Plate 2 will move

together with plate 1 (stick phase) until the force on it

exceeds some critical value fcrit , at which point it will recoil

back (slip phase). This value can be estimated from the characteristics of the typical energy well and for h f j1 we

obtain fcrit x gA1=2 =h. At larger distances, screening comes

into play and this force decays exponentially with separation between the plates (no stick phase is expected at large

separations). Conversely, the stickslip phenomenon can

be suppressed by the addition of salt, even when the separation between the plates is fixed.

When the critical force is exceeded, plate 2 will recoil

back to a position in which the spring force becomes sufficiently small. The process will repeat itself as long as we

continue to drag plate 1, and stick-slip motion of plate 2

will be observed. Note that each time the critical spring

force is exceeded, plate 2 recoils to a different new equilibrium state, which corresponds to an energy minimum that

differs in general from the initial one (such minima are

densely distributed in the space of relative displacements

of the two plates) and, therefore, a statistical spread of

equilibrium positions of the lower plate will result.

4. Discussion

by relative translation of two random frozen charge distributions interacting through long-range electrostatic forces.

Two simple geometries were considered, for which the statistical properties of this energy landscape can be calculated analytically, namely, two parallel rigid rods and two

parallel rigid plates. When the total charge on each of the

objects vanishes and the Coulomb interaction between

them is unscreened (i. e., when there is no characteristic

length scale associated with the interaction potential), the

interaction between the objects becomes significant and

energy minima appear when the separation between these

objects becomes of the order of their dimensions (when the

two objects are of different sizes, this happens when the

separation is of the order of the linear dimensions of the

larger of the two). When the separation is further

decreased, these energy wells deepen and new wells

appear. We calculated the corresponding energy distributions, the depth and the width of the characteristic energy

wells and the spacing between them and found that both

the width and the spacings are of the order of the separation

between the objects. This indicates that the typical energy

wells are densely packed in the space generated by the

relative translation of the objects.

548

interaction between a randomly charged rod and one on

which a periodically varying charged distribution is irreversibly placed. In this case, the density of typical energy

minima depends only on the wavelength of the periodic

distribution and not on the separation between the rods.

Yet another case considered in this work is that of local

periodic order on both rods. As expected, the energy landscape reduces to that of the randomrandom case at

separations that exceed the charge correlation length. At

smaller separations between the rods, the landscape is qualitatively similar to that of the randomperiodic case.

We would like to comment on the limitations of our

model. The theory is applicable to separations down to the

average distance between the charges (h F g1 for rods

and h F g1=2 for plates), at which point our assumption

of continuous charge distributions on the objects breaks

down. There is also an upper cutoff of the distance between

the objects: as shown elsewhere [2], the method of averaging over frozen disorder used in this work becomes inaccurate for separations that exceed the linear dimension of

the longer rod, h F L9 . The resulting corrections are of limited physical interest since in this limit the average number

of energy minima is of order unity and their depth tends to

zero. A more restrictive condition follows from the fact

that we did not explicitly introduce the constraint of fixed

total charge on each of the rods (we assumed that it is fixed

and, consequently, did not average over the distribution of

total charge on the rods). It can be shown that accounting

for the fixed total charge constraint leads to corrections of

order h=L (L is the length of the shorter rod) to our results.

Finally, in this work we considered only parallel rods and

plates. Although analytical results can be obtained for

other geometries as well, this increases the number of free

parameters and obscures the simple physical picture presented here.

Acknowledgements

A. Tkachenko for helpful comments. SP acknowledges the

hospitality of the Department of Physics, Bar-Ilan University, and MW acknowledges the hospitality of the Department of Materials and Interfaces, Weizmann Institute of

Science, and the support of the Minerva Foundation. YR

acknowledges financial support through a grant from the

Israel Science Foundation and expresses his gratitude to

the Yukawa Institute for Theoretical Physics, Kyoto University, where this work was completed.

References

[1] Y. Kantor, M. Kardar, Phys. Rev. Lett. 1991, 14, 421.

[2] S. Panyukov, Y. Rabin, Phys. Rev. E 1997, 56, 7053.

[3] J. Israelachvili, Intermolecular and Surface Forces, 2nd ed., Academic Press, London 1992.

[4] J. Klein, D. Perhia, S. Warburg, Nature 1991, 352, 143.

Final version June 10, 1998

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