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I. INTRODUCTION shear melting is controlled by the stress tensor rather than the
sliding velocity as assumed in Ref. 10. Making use of the
The nature of sliding friction is a fundamental physical generalized Lindemann criterion, we combine shear and ther-
problem of prime practical importance.1,2 While the possibil- modynamic melting within a unified description. Using this
ity to create low-friction surfaces and lubricant fluids has approach we describe the onset of stick-slip motion as a
been ubiquitous for almost all engineering applications, it function of the film thickness and temperature, and deter-
has become crucial for the design of modern microminiature mine the dynamic phase diagram. We demonstrate that ran-
devices such as information storage and microelectrome- dom nucleation of droplets of the fluid phase during the mo-
chanical systems, where low friction without stick-slip 共or tion leads to an irregular temporal distribution of slip events
interrupted兲 motion is necessary. and to ultrasound radiation. Admittedly, our approach is phe-
Studies of friction between atomically flat mica surfaces nomenological in nature; it is not justified from first-
separated by an ultrathin layer of lubricant have revealed a principles calculations and cannot be used for a precise esti-
striking phenomenon:3 in a certain range of experimental pa- mate of experimental parameters. Nevertheless, it captures
rameters the fluid exhibited solidlike properties, in particular, all observed experimental phenomenology, results in a cor-
a critical yield stress leading to stick-slips similar to that in rect order of magnitude estimate of the critical velocity, and
solid-on-solid dry friction processes5 with the transition to gives insights into the problem.
sliding above critical velocity V c ⬃1 m/s. This behavior The structure of the article is the following. In Sec. II we
was attributed to the confinement-induced freezing of the describe the general formulation of our model. In Sec. III we
lubricant and its recurring melting due to increased shear introduce the thin-layer approximation. Using this approxi-
stress: as the fluid thickness is reduced to several molecular mation, we reduce the model to a relatively simple system of
layers, it freezes, but when the shear stress exceeds some equations for averaged shear stress and deviation of the order
critical value, it melts. This behavior was confirmed by mo- parameter. In Sec. IV we study the stick-slip dynamics for
lecular dynamics 共MD兲 simulations,6,7 which indicated order- spatially uniform motion. In that section we also compare
ing of the fluid due to confinement by the walls. our results for the critical velocity with the experimental val-
A quest for the quantitative description of stick-slip lubri- ues. In Sec. V we study the nucleation dynamics of liquid
cant dynamics motivated several theoretical works.8 –10 An phase droplets in the overheated solid and connect it to ir-
important step has been made by Carlson and Batista10 who regularity in stick-slip sequences. Finally, in Sec. VI we in-
proposed a phenomenological constitutive relation connect- vestigate the generation of ultrasound by stick-slip events.
ing the frictional forces to velocity and coordinates via the
order-parameter-like state variable reflecting the degree of II. MODEL
melting. This model successfully described some of the ob-
served phenomenology of the experiment3 and gave insight The simplified setup of a friction experiment is shown in
into the dynamics. Yet many important questions including Fig. 1. The upper plate is sliding with the velocity V on a
the very mechanism of the onset of the stick-slip remain thin-layer of lubricant with thickness h. The ‘‘free end’’ of
unresolved. In particular, MD simulations of Ref. 6 give the the spring, representing the overall elastic properties of the
critical velocity V c ⬃10 m/s which exceeds the experimental friction device, is pulled with constant velocity V̄. The re-
value by many orders. This apparent disagreement was at- sulting friction force F is proportional to the deflection of the
tributed by Persson9 to complex nucleation dynamics of spring.
stress domains and the importance of thermally activated The flow of lubricant satisfies the momentum conserva-
processes in the shear melting transition. tion law
In this paper we develop a theory of stick-slip motion in
ultrathin liquids based on equations for the flow coupled to
D v i i j
the equation for the order parameter 共OP兲 for the melting 0 ⫽ , 共1兲
transition in the presence of shear stress. We propose that the Dt x j
0 t ⫽l 2 ⵜ 2 ⫺ 共 1⫺ 兲共 ␦ ⫺ 兲 . 共4兲
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STICK-SLIP FRICTION AND NUCLEATION DYNAMICS . . . PHYSICAL REVIEW B 65 125402
where T 02 ⫽c L2 a 3 . Substituting Eq. 共7兲 into the expression where v 0 ⫽ V/ 0 is the rescaled velocity of the top plate,
for the control parameter ␦ , Eq. 共5兲, one derives in the first and S⫽l 2 /( 20 0 ) x U, and ⫽ /(l/ 0 ) 2 ⫽O(1). The term
order S has been added to Eq. 共15兲 in order to account for radia-
tion losses of sound due to its leakage into the substrate. As
␦ ⫽ ␦ 0 ⫹ 2 / 20 , 共8兲 one sees from Eqs. 共14兲, and 共15兲, for A→0 共solid phase兲 the
where ␦ 0 ⫽(T⫺T 1 )/(T 02 ⫺T 1 ) and 20 ⫽ (T 02 ⫺T 1 )/ ␦ 0 a 3 is above system is reduced to the wave equation 2t S⫽ 2x S
the yield shear stress. ⫺ t S; i.e., it describes the propagation of shear elastic
waves with sound velocity c s ⫽ 冑 and radiation decay rate
III. THIN-LAYER APPROXIMATION .
The pulling velocity V̄ does not necessarily coincide with
In the thin-layer approximation, the thickness of the lubri- the upper plate velocity V; see Fig. 1. In a standard friction
cant layer h is small so that the dependence of the shear experiment, the upper plate is pulled via a spring with stiff-
stress and other stress components on the transverse coor- ness k. The relation between the position of the upper plate
dinate y is neglected in the leading order. Now we can further X, friction force F, and the position of the spring 共neglecting
simplify the OP dynamics. Since the walls favor the forma- masses of the spring and upper plate兲 reads F⫽k(V̄t⫺X).
tion of a solid, the boundary conditions for the OP are
Since F⬃ 兰 L0 (x)dx and V⫽dX/dt, the difference between
(0)⫽ (h)⫽1, and the bulk variations of the OP are small
as compared to 1. Let us seek the solution in the form the plate velocity V and pulling velocity V̄ can be neglected
for stiff enough springs.
where AⰆ1 is the slowly varying amplitude. Substituting First we discuss spatially uniform motion. In this case
Eq. 共9兲 into Eq. 共4兲 and making use of the standard orthogo- Eqs. 共10兲, 共14兲, and 共15兲 are reduced to a pair of coupled
nalization procedure leads to ordinary differential equations 共ODE’s兲:
冉
t A⫽ 2x A⫹ ␦ ⫺1⫺
2
h 2 冊 A⫹
16⫺8 ␦ 2 3 3
3
A ⫺ A , 共10兲
4 冉
t A⫽ ␦ ⫺1⫺
2
h 2 冊 A⫹
16⫺8 ␦ 2 3 3
3
A ⫺ A ,
4
共16兲
冕
slow and A being a fast variable. Stick-slips are described by
1 h
the limit cycle on the -A plane. The bifurcations among
U⫽ v y dy 共12兲
h 0 different regimes depend on the relative position of the
nullclines which are defined by the conditions d /dt⫽0 and
is the y component of the flow velocity averaged over the
dA/dt⫽0. The slow-motion nullcline determined by Eq.
width of the sample. Here we used nonslip condition for the
共17兲 is of the form
x component of the fluid velocity, which yields v x (h)
⫺ v x (0)⫽V⫽const, where V is the relative velocity of the 2
upper plate with respect to the bottom. * A⫽ v 0 /h. 共18兲
Now, integrating Eq. 共1兲 for the y component of the ve-
locity one obtains The manifold of fast motions consists of two separate curves
0 20 A⫽0, 共19兲
t U⫽ x . 共13兲
冉 冊
2
l
2 8 3
Here we assume that the hydrodynamic velocity is small and ␦ ⫺1⫺ ⫹ 共 2⫺ ␦ 兲 A⫺ A 2 ⫽0. 共20兲
h 2 3 4
neglect terms vⵜv. Thus, we obtain two coupled equations
Fixed points of Eqs. 共16兲 and 共17兲, i.e., steady sliding re-
2 v
t ⫽⫺ * A ⫹ 0 ⫹ S, 共14兲 gimes, correspond to the intersections of nullclines. The limit
h cycle can be approximated by two segments lying on two
different nullclines of fast motion and two lines ⫽const
t S⫽ 2x ⫺ S, 共15兲 which describe the rapid transitions from one branch of the
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I. S. ARANSON, L. S. TSIMRING, AND V. M. VINOKUR PHYSICAL REVIEW B 65 125402
t ⫹
2
L
* 冕 0
L
A 共 x 兲 dx⫽
v0
h
. 共21兲
abrupt with hysteresis between solid and dashed lines and smooth
otherwise. Below the dotted line (h 0 ) one has dry friction without
where ⑀ ⫽1⫹ 2 /h 2 ⫺ ␦ 0 ⬎0. From Eq. 共21兲, ⬇ v 0 t/h⫹ 0 ,
stick-slips. Inset: shear stress 共or friction force兲 vs sliding veloc- and A 0 and 0 are the values of amplitude and stress in the
ity v 0 corresponding to stationary sliding regimes in three different beginning of stick phase. We restrict ourselves to the case
regions. The falling part of line 2 corresponds to the unstable sta- h→h c , where 0 →0 and A 0 ⫽O(1). While is small, the
tionary solution; in this range of pulling velocities the system ex- amplitude A decays exponentially to very small values. It
hibit stick-slip oscillations. reaches a minimum A min ⫽exp(⫺2⑀3/2h/3v 0 ) at t min
⫽ ⑀ 1/2h/ v 0 . Then it starts to grow slowly and reaches the
crystals.13,15 In the case of driven vortex lattices the horizon- value O(1) 共slip event兲 at t⫽t m ⫽ 冑3t min . At t min ⬍t⬍t m
tal axis in Fig. 4, inset, represents voltage and the vertical the growth rate ⫺ ⑀ ⫹ 2 ⬎0, and therefore the lubricant is in
axes correspond to driving current. Then curve 1 describes an unstable 共‘‘overheated’’兲 state. The overheated solid is
the elastic depinning and curve 2 corresponds to hysteretic very sensitive to fluctuations, e.g., to thermal noise. Small
plastic depinning. nuclei of liquid can appear and expand within the solid, re-
Let us estimate typical values of the critical velocity for sulting in accelerated slip events. Since nucleation events
the transition to steady sliding. From Fig. 3 one finds a typi- have probabilistic character, one can expect spatio-temporal
cal value of the velocity v c ⬇0.1 . In physical units one randomness of the slip events. However, this randomness can
*
has V c ⬃0.1 0 0 c s 0 / . The ratio 0 / ⬃10⫺2 has the only manifest itself at low noise levels. At the higher level of
meaning of relative stress for onset of plastic deformation in the noise, the slips become more regular because the number
solids. Using the bulk value of 0 ⫽1010 s⫺1 one derives of nucleation sites increases, and the overall effect of the
V c ⬇1⫺10 mm/s, i.e., the value which is about 3 orders of noise averages out. This effect is somewhat similar to the
magnitude larger than the experimental value V 0 ⬃1 m/s. coherence resonance in noise-driven excitable systems where
Under high pressure 0 decreases by several orders of mag- increase of noise makes the oscillations more regular.17,18
nitude 共Refs. 3 and 4 report an effective increase of 0 by We studied Eqs. 共10兲 and 共21兲 numerically in a fairly large
4 – 6 orders for pressure of about 20 MPa兲, and one arrives at domain; see Figs. 5 and 6. Since during the slip phase the
V 0 ⬃0.1–1 m/s. shear stress rapidly drops, the domains do not necessarily
propagate through the entire system and in large systems one
V. NUCLEATION may observe ‘‘partial slips.’’ The random character of the
nucleation process manifests itself in the nonperiodicity of
The above analysis was based on the assumption that the slips and local amplitude A.
stick-slips occur simultaneously in the entire lubricant layer, In our simulations we used the value ⫽0.01, which
*
which may not be the case for large samples. It is natural to corresponds to the bulk value of 0 at normal pressure. For
expect that stick-slips occur via a series of nucleation events the experimental conditions,3 the value of 0 decreases by
when droplets of the liquid emerge in the solid phase and many orders of magnitude, which makes the simulations
then expand and merge throughout the system. Nucleation technically impossible. However, the qualitative picture of
can be responsible for the observed irregularity stick-slip se- phenomena does not change with a decrease of , which
quences 关notice that the second-order system of ODE’s 共16兲 *
even in our case is already sufficiently small.
and 共17兲 can only produce periodic oscillations兴.
If the sample size L is not very large and the ‘‘acoustic VI. SOUND EMISSION
shear time’’ a ⫽L/c s is much smaller than any characteristic
time scale of the problem 共e.g., slip time兲, we can simplify In this section we will briefly discuss the radiation of
the problem by neglecting the dependence of on the lon- sound during phase slip events. Although the physical
125402-5
I. S. ARANSON, L. S. TSIMRING, AND V. M. VINOKUR PHYSICAL REVIEW B 65 125402
mechanisms of ultrasound generation in friction experiments FIG. 7. Space-time plots of and A for ␦ 0 ⫽1.1, h⫽4,
*
are not well understood, it is believed that sound waves in ⫽0.01, v 0 ⫽0.0002, and ⫽1 in the system of length L⫽1000,
the range from 106 to 1011 Hz are excited.2 In most of the obtained from solution of Eqs. 共10兲 and 共14兲. Small ripples on the
mechanisms proposed earlier, the frequency of the ultra- (x) vs time plot show sound radiation.
sound is proportional to the pulling velocity.
The sound generation can be described within the frame- It should be noted that sound generation is an interesting
work of the full Eqs. 共10兲, 共14兲, and 共15兲 in the regime of phenomenon which can be observed experimentally. Accord-
‘‘partial slips.’’ Indeed, as follows from Eq. 共14兲, inhomoge- ing to our results, it is not the reason for stick-slips but their
neity in A(x) also creates inhomogeneity in the shear stress consequence. Our investigation shows that there is no quali-
distribution (x), which in turns generates elastic waves due tative difference with the nucleation dynamics described in
to the wave nature of Eqs. 共14兲 and 共15兲. Sec. V, where wave propagation effects are neglected.
We studied Eqs. 共10兲, 共14兲, and 共15兲 for the same param- Let us now estimate the frequency of the ultrasound. Ac-
eter values as in Sec. V. Indeed, as one sees from Fig. 7 and cording to our results, the ultrasound is generated during the
8, sound waves are emitted during the slip events. They are slip event. Since the duration of slip T slip is of the order
manifested as propagating ripples in Fig. 7 and high-
frequency modulation in vs t profiles.
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STICK-SLIP FRICTION AND NUCLEATION DYNAMICS . . . PHYSICAL REVIEW B 65 125402
1/ , the representative frequency of sound waves will be depinning transitions of flux-line lattices in type-II supercon-
*
⬃ . The parameter changes by several orders of mag- ductors, charge density waves, and other structures driven
*
nitude as a function of applied pressure, and one obtains for through disorder.13 Our results may also shed light on vari-
the frequency ⬃ ⫽106 –107 Hz for the conditions of ous phenomena related to shear thickening and memory ef-
experiment.3 Moreover, our results indicate that the fre- fects in complex fluids.19
quency of ultrasound practically does not depend on the pull- This theory is similar in spirit to our recent analysis of
ing velocity. This prediction is worth testing experimentally. partially fluidized flows in granular materials.21 That theory
also operates with an order parameter equation that is con-
VII. CONCLUSION trolled by the shear stress tensor. When applied to the de-
scription of granular friction experiments 共see, for example,
In this paper we have proposed a continuous theory for Ref. 20兲, it also reproduces the observed stick-slip dynamics.
friction dynamics in ultrathin films. Experimentally observed The important difference, however, is that the thermody-
layering and crystallization of ultrathin films near atomically namic temperature, which is essential here, is irrelevant for
flat surfaces 共see, for example, Ref. 3兲 can be phenomeno- the granular dynamics.
logically described as an ordered state with the correspond- It is also interesting to note the analogy between nucle-
ing order parameter close to 1. Under shear stress, crystalline ation dynamics of ‘‘partial slips’’ in the systems with the
structure breaks, and the film ‘‘melts,’’ thereby releasing the lubricated friction and the creation of defects during rapid
stress. This process of shear-induced melting and freezing quench 共‘‘cosmological scenario’’兲.22–24 In the vicinity of the
leads to the stick-slip behavior of thin liquid films to shear- phase transition the defects, e.g., domain walls in the one-
induced melting and freezing processes. Our theory is based dimensional case, are created from small fluctuations of the
on the Ginzburg-Landau equation for the order parameter order parameter on the background of essentially unstable
which describes the melting transition under shear stress. state 共overheated solid in our case兲.
The order parameter then enters the stress relaxation rate so
that it approaches zero in the solid state. The developed ap-
proach allowed for a quantitative description of dynamic ACKNOWLEDGMENTS
nucleation effects leading to slip events and sound genera-
tion. The proposed theory can be applied to a wide range of This research was supported by U.S. DOE Grant Nos.
phenomena including friction in nanoscale devices, friction W-31-109-ENG-38, DE-FG03-95ER14516, and DE-FG03-
on ice, etc. A similar approach can be used in describing 96ER14592.
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