IEEE TRANSACTIONS ON ULTRASONICS, FERROELECTRICS, AND FREQUENCY CONTROL, VOL. 42, NO.

4, JULY 1995 619

Mechanisms of Removal of Micron-Sized

Particles by High-Frequency Ultrasonic Waves
Quan Qi and Giles J. Brereton

Abstract-In this paper, theories of particle removal by high-
frequency ultrasonic waves are discussed and tested against
recent experimental data. First, the principal adhesion forces
such as van der Waals forces are briefly reviewed and the
typical uncertainties in their size in particle-surface systems
are assessed. The different ultrasound-induced forces-linear
forces such as added mass, drag, lift, and Basset forces and
nonlinear ones due to radiation pressure, and drag exerted
by acoustic streaming-are discussed and their magnitudes are
evaluated for typical cleaning operations. It is shown that high-
frequency ultrasound can clean particles most effectivelyin media
with properties like water because: (1) the wavelength can be
made comparable to the particle radius to promote effective
sound-particleinteraction; (2) the viscous boundary layer is thin,
minimizing particle “hide-out;” and (3) both the added mass
and radiation pressure forces exceed typical adhesion forces at
high frequencies. Based on these analyses, possible mechanisms
of particle removal are discussed and interpreted in terms of
experimental observations of particle cleaning.
I. INTRODUCTION
forces generated by high-frequency ultrasonificationprocesses
and to identify the likely mechanisms whereby small particles
are removed from surfaces.
Small particles in an ultrasonic field near a solid surface
experience two kinds of forces of particular interest to this
study: adhesion forces; and cleaning forces that arise through
interactions of ultrasound with particles. Adhesion forces,
in general, comprise capillary forces, van der Waals forces,
electrostatic image forces, and electrical double-layer forces
[ 131, [ 2 ] .During cleaning operations, components are usually
immersed in a liquid to ensure good acoustic coupling, in
which case both capillary and electrostatic image forces be-
come insignificant. Consequently, the adhesion forces of most
importance are van der Waals forces and electrical double layer
forces.
In ultrasonic fields, the cleaning forces on particles are hy-
drodynamic ones which arise from linear as well as nonlinear
interactions between the ultrasonic field and particles in fluid.
Linear interaction forces include added mass, drag, lift, and

0 NE of the most important applications of particle- Basset forces while nonlinear ones include radiation pressure
removal technology is the cleaning of small particles forces and drag forces due to acoustic streaming. An important
from silicon wafer surfaces. The presence of particles on the difference between these two kinds is that linear forces are
surfaces of semiconductors has long been recognized as a time-dependent and have zero means while nonlinear ones
cause of reduced yields in the production of semiconductor have a time-independent component and, on average, take
devices through contamination of processes such as etching, nonzero values; linear interaction forces are usually much
photoresist stripping and prediffusion cleaning [ 171. As the larger than nonlinear counterparts in conventional applications
characteristic linewidths, and so the size of the particles which at moderate frequencies (up to, say, megahertz).
must be cleaned, continue to decrease, conventional cleaning There have been relatively few studies of mechanisms
techniques become less effective. of particle removal. Olson [ 191 conducted a finite-element
Conventional ultrasonic cleaning techniques depend on the computational study of the forces imparted by small-amplitude
mechanisms of (1) chemical solvation, and ( 2 ) acoustic cavi- plane waves to a sphere on a surface, at frequencies as high
tation, both of which can have undesirable effects. Solvents are as one gigahertz, and concluded that acoustic excitation at
often environmentally hazardous and cavitation thresholds are
wavelengths of the order of one radius led to the greatest
hard to predict, cavitation forces are difficult to control, and
amplitude of the surface-normal oscillatory force on a spheri-
may cause damage to the component being cleaned. Recently,
cal particle. Geers and Hasheminejad [7] considered a model
the removal of particles by high-frequency focused ultrasound
in which a spring and a damper were used to represent the
in water [4] has shown great promise as a technique which
adhesion force and proposed that a possible mechanism of
requires no solvents and may be applied below thresholds at
particle removal from the surface was through excitation of
which cavitation occurs. The goal of this paper is to analyze the
the particle at the resonance frequency of the particle-spring-
Manuscript received November 5 , 1993; revised November 16, 1994; damper system. These removal mechanisms are both linear and
accepted November 16, 1994. This work was supported by the Materials so have no provision for mean displacement of particles. In
Research Center of the University of Illinois (MRC MCM CTR). Q. Qi was the following sections, the principal adhesion forces and linear
supported by the Acoustical Society of America and the Hunt Fellowship. G.
Brereton was supported by IBM, T. J. Watson Research Center. and nonlinear hydrodynamic interaction forces are reviewed.
Q. Qi is with the Department of Theoretical and Applied Mechanics, Order of magnitude analyses are presented from which it
University of Illinois at Urbana-Champaign, Urbana, IL 61 801 USA. is shown that the combined effect of the interaction forces
G. Brereton is with the Department of Mechanical Engineering and Applied
Mechanics, University of Michigan, Ann Arbor, MI 48109 USA. and mechanisms of advection of the loosened particles must
IEEE Log Number 9409984. be considered if removal mechanisms are to be explained.
0885-3010/95$04.00 0 1995 IEEE
620 IEEE TRANSACTIONS ON ULTRASONICS, FERROELECTRICS, AND FREQUENCY CONTROL, VOL. 42, NO. 4, JULY 1995

Based on these analyses, mechanisms of particle removal are
proposed and used to interpret recent experimental results.
11. BRIEFREVIEWOF ADHESIONFORCES
For particles fully immersed in a liquid, the dominant
adhesion forces are van der Waals and double layer forces.
Van der Waals forces can be classified in the categories
of [23]: (1) dipole-dipole forces; (2) dipole-induced dipole
forces; and (3) dispersion forces. Of these, the nonpolar
As the adhesional distance z increases, (1) loses its validity
and the adhesion force becomes retarded. Strictly speaking,
the Hamaker constant is never a constant [lo] but decreases
progressively as z increases. The effect of retardation has been
accounted for [23] by introducing a second relation
2rBR
FvdW = ~ for relatively large z
323
where B is called the Hamaker constant for the retarded force;
a typical value is B 20-28 Jm. When elastic deformation of
N

dispersion force (also called the London-van der Waals force) the sphere and the surface takes place, there is an additional
is believed to be the most important [2], [3]. Under the contribution to the van der Waals force, given by [3] as
assumptions of “nonretardation” and “additivity,” the resulting
interaction force between a particle and a plane surface can (3)
be characterized by the conventional Hamaker constant. A
more satisfactory approach was developed later by Lifshitz The first term describes the nondeforming van der Waals force
[3] in which the principal parameter was the Lifshitz-van while the second accounts for deformation of the particle
der Waals constant, defined as an integral function of the and/or surface. The parameter h is the Lifshitz-van der Waals
imaginary parts of the dielectric constants of the adhering constant and p is the radius of the adhesive surface area.
materials. Israelachvili [lo] has shown that in some cases Comparison between (1) and the first part of (3) gives the
Hamaker constants can be calculated on the basis of the relation between the Hamaker constant and Lifshitz-van der
Lifshitz theory. Hence a one-to-one correspondence between Waals constant as
the Hamaker constant and the Lifshitz-van der Waals constant h
A=-. (4)
can be established. 8T
Electrical double layer forces are associated with particles A number of complications arise when using these models.
whose effective diameters are smaller than 5 microns [3]. First, in (1)-(4) the adhesional distance z cannot be calculated
A surface contact potential is created between two different from theoretical considerations and so is usually approximated
materials based on each material’s respective local energy as a constant. For example, a value of z = 0.4 nm is suggested
state. The resulting surface charge build-up needed to preserve in [13] while [ 101 uses z = 0.2 nm in numerical computations.
charge neutrality sets up a double-layer charge region, thus Moreover, particle asperity also complicates the choice of an
creating the electrostatic attraction. However, for particle appropriate value for z and the range of validity of (1) and (2)
adhesion, [ 131 concluded that the electrostatic double layer is not well known. Second, real particles are seldom spherical
force can at best be of the same order of magnitude as the van in shape and use of effective radii can involve considerable
der Waals force and can generally be neglected in favor of approximation. Third, the value of the Hamaker constant, as
the van der Waals force. Consequently, for order-of-magnitude obtained from the Lifshitz theory, does not always agree with
analyses of adhesion forces it is usually sufficient to consider those evaluated from experimental data on colloid stability
only the van der Waals force. [3]. Hence it is, in essence, an adjustable parameter describing
adhesion phenomena. Finally, the deformation of the particle
A. van der Waals Force or surface can induce an additional adhesion force which
There exist two different theories describing van der Waals may exceed the nondeforming van der Waals force [3]. The
forces: the microscopic theory of de Boer and Hamaker estimation of these forces is uncertain owing to the difficulties
and the macroscopic theory proposed by Lifshitz. These two in evaluating the contact area. These difficulties constitute
theories can be related, though many experimental results are sources of uncertainty in the prediction of adhesion forces.
in better agreement with the macroscopic one. Comprehensive The extreme importance of the van der Waals force to
treatments of both theories can be found in [13], [23], [lo]. micron particle removal can be appreciated by comparing its
For the purpose of this paper, we restrict attention to these size with the gravitational force on a spherical particle, which
interaction forces for the case of a spherical particle near a flat is given by
surface. The van der Waals attraction force is then modeled as 4
F,,, = -rR3pg.
F,,~W = $ for relatively small z
3
For particles on the order of a micron, FvdW 106Fg,,!
N

where A is the Hamaker constant for the nonretarded force;

R is the radius of the sphere, and z is the distance of
maximum force of adhesion (adhesional distance). A typical
value for A in a gaseous medium is A N J, although
immersion in a liquid usually reduces A by an order of
magnitude. Appropriate
_ .- values of the Hamaker constant for
different combinations of materials can be found in [IO].
111. CLEANING FORCESINDUCED BY ULTRASOUND
The transmission of ultrasound through a liquid has a
number of consequences. First, any particles suspended in
the liquid oscillate at the driving frequency and experience
significant acceleration at high frequencies. Second, a time-
invariant mean flow known as acoustic streaming is generated.
QI AND BRERETON: MECHANISMS OF REMOVAL OF MICRON-SIZED PARTICLES BY HIGH-FREQUENCY ULTRASONIC WAVES 62 1

Although its magnitude is usually of secondary importance to

that of the primary ultrasonic field, its role in mean particle
transport may be very important. Third, particles in the path of
the ultrasound scatter acoustic waves and reduce the acoustic
energy density through reradiation, leading to a reaction force
called radiation pressure force. Viscous boundary layers also
develop near the liquid-solid interface, the thickness of which
depends on the driving frequency and the kinematic viscosity
of the liquid.
Each of these phenomena involves different interaction
forces between the particle and the liquid. The acceleration Fig. 1. Schematic representation of a particle removal. Liquid density and
of liquid leads to the so-called added mass force, which viscosity of the liquid: p and p . Acoustic wave frequency: f and the intensity:
I . The radius of the particle: R and the thickness of the boundary layer: 6.
will be shown to play a key role in high-frequency particle-
fluid interaction. Both the time-dependent and time-invariant
flows of surrounding liquid relative to the particle generate propagates towards a surface, on which a particle rests, the
drag forces which have different scalings depending on the added-mass force is diminished, but still accelerates fluid
Reynolds number regime. Thus primary acoustic fields induce above and below the midplane through the particle. Hence
instantaneous drag forces and secondary acoustic streaming this force should be oscillatory in sign, alternatively promoting
leads to a steady drag force on particles. The radiation pressure removal and attachment.
also applies a net force on particles. This force increases Lift Force: Circulation of fluid around a particle generates
with frequency and hence plays an important role in particle a lift force of inviscid character, with a surface-normal com-
removal with high-frequency ultrasound. Finally, a so-called ponent acting to remove the particle. The pressure difference
Basset force is also present as a result of flow-particle inter- between the bottom and top of the particle may be estimated
action with a typical magnitude between that of added mass from the Bernoulli’s equation to yield an estimate of lift force
and Stokes drag forces. as
Our principal interest in these forces is to make assessments (7)
of the conditions under which one or more can reach the same
order of magnitude as the adhesion forces and hence can be For smaller particles at surfaces, viscous effects may become
utilized to remove particles adhering to a surface. For these important and estimates of lift from Navier-Stokes equation
purposes, we consider a spherical particle adhering to a plane solutions have been made by [16], [6]. It was concluded [6]
surface (Fig. 1). The radius of the particle is denoted by R , that the lift force is decreased by the presence of a wall for
the density of the particle by pp, the viscosity of the fluid particles sufficiently close to the wall. Equation (7) may be
by p, and the density of fluid by p. The ultrasound field is regarded as an upper limit for lift force.
characterized by a frequency f and an intensity I . When a Drag Forces: Drag forces take different forms, depending
viscous boundary layer is present, its thickness is denoted by on the regime of the flow Reynolds number, defined as
6. Derivation of exact expressions for the forces on a particle Re = - PRu
submerged in a sonofied liquid is rarely possible as analytic P
solutions are only known in idealized cases [8], [9]. More When Re << O( 1) the well-known Stokes drag is of the order
generally, solutions have to be obtained numerically. For the
purpose of this study, order-of-magnitude estimates of these Fs ~ R u .
N (9)
forces are of primary interest and are analyzed in the following On the other hand, when Re >> O(l), the drag force is of
sections. Similar analyses and discussions can be found in the the order
review on suspension mechanics by Kim and Lawrence [ 111.
Fo ~ ( u R ) ~ .
N (10)
A. Linear Interaction Forces The relative importance of viscous and inertial effects at
Added-Mass Force: The added-mass force Fa, on a con- different Reynolds numbers is reflected by the proportionality
taminant particle is an effect of the acceleration of the fluid. of Fs to the viscosity of the liquid, radius of the particle and
For a spherical particle, this force is parallel to the direction of the velocity, while Fo scales linearly on the density of the
acceleration, and its magnitude may be estimated as if it were liquid, and quadratically on velocity and particle diameter.
an isolated sphere. The exact value is expected to differ by a Basset Force: When the particle radius R is comparable
factor of order unity when the presence of the plane surfaces to the boundary layer thickness S ( p / 2 ~ f p ) l the
N / ~ ,added
is accounted for. The added-mass force is then mass force will be modified by a force of “Basset”-type from
the shear in the boundary layer and the resultant modification
of the pressure field. This force can be estimated, for particle
exposure to monochromatic acoustic waves, as
where U N [1/(pc)]’l2is the instantaneous fluid particle
velocity associated with the acoustic wave and I is the
intensity of the incident acoustic waves. When a plane wave
622 IEEE TRANSACTIONS ON ULTRASONICS, FERROELECTRICS, AND FREQUENCY CONTROL, VOL. 42, NO. 4, JULY 1995

from which FB is the geometric average of the added-mass TABLE I

and the Stokes drag forces. FORCES
(IN N) VERSUS PARTICLE SIZE R (RADIUSIN pm) FOR f = lo6/ 2T HZ
In ultrasonic fields, the time-averaged values of these forces R 0.1 1 .o 10.0
are zero. Furthermore, as the size of the particles decreases,
the Stokes drag becomes increasingly important-unlike other
F,,, 2x104 2 x 10-8 2 x 10-7
interaction forces, it depends on particle radius only linearly.
Fam 2~ 10-13 2 x 10-10 2 x 10-7
B. Nonlinear Interaction Forces
Radiation Pressure: The radiation pressure force on an FL9FD 4 x 10-13 4 x 10-11 4 x 10-9
isolated solid particle in an ideal fluid induced by a plane ~~

wave was deduced by King (1934) as F, 2x lo-” 2 x 10-10 2 x 10-9

FB 2 x lo-’* 2 x 10-10 2 x 10-8

R F,, 2 x 10-16 2 x 10-13 2 x 10-10

for 2 r f - << O(1) (12)
c
where c is the sound speed in the liquid medium. This solution
requires the particle to be small or acoustically “compact.” i.e. V u 2 / c . Therefore the drag force which results from
N

King also derived the related expression for larger particles boundary layer-generated acoustic streaming FST is given by
FRT - p ( ~ ) 1~ 95- - 48(P/PP)
89 5 + 6(P/P,)
+ 36(P/Pp)2
+ 2(P/PP) FST p R ;
N
U2
(15)
R where the Stokes drag is assumed to be the relevant one at
for 2 r f - N 0(1) (13)
C typically low Mach numbers in particle removal. The principal
The above equations are for traveling waves. For stationary difference between the nonlinear and linear forces is that
waves, King showed that nonlinear forces have nonzero time averages and so provide a
mean component to the removal force. Streaming is ordinarily
FRS N 8p (F) R3u2sin 2kl 1 + - P/PP>
2 +P/Pp
parallel to surfaces and so can potentially advect particles
along the surfaces.
R
for 2 r f << 0 ( 1 ) (14)
I v . ESTIMATION
OF FORCES
where 1 is the distance between the center of the particle
and a nodal plane of the stationary wave. For 2 r f R / c << A. Forces in Plane Wave Fields
O(l ) , it can be verified that FRS >> FRT. For 2 n f R / c N Based on the development of the previous sections, the
O(1); no analytic expression is available for FRS,We shall orders of magnitude of the forces in (1) and (6)-(15) will
nevertheless use (14) for approximate estimations. Yosioka be considered for particles with radii in the range 0.1-10
and Kawasima [25] extended King’s results by including the pm. For illustrative purposes, a mica particle is assumed
effect of compressibility of the particle, though the correction to adhere to a mica surface in water, in which case we
is small for solid particles and did not affect the outcome have A = 2.0 x J [lo], p = N sm-2, c =
of order-of-magnitude analyses. When particles are positioned 1500 ms-l and p = 1000 kgm-3. Material properties of
on surfaces, the radiation pressure imparted by plane acoustic mica are similar to those of silicon and other materials used
waves directed normal to the surface is into the surface. in semi-conductor processing. The intensity of the ultrasonic
Thus this nonlinear force would act to retain particles at the field is given by I 0.6 x lo5 WmF2, which is a value
N

surfaces. When the incident wave is not normal or the particle
is at the edge of an ultrasonic beam, a force component due
to radiation pressure in the direction parallel to the surface
will also be present, which acts to remove the particle from
the contaminated area. A more detailed discussion of such a
removal is given later.
Drag Force Due to Acoustic Streaming: The acoustic
streaming motion generated by an ultrasonic field near a
solid surface leads to a drag force, caused by interaction
between the mean flow and particles. It is described by (9)
when the streaming velocity is substituted in place of the
instantaneous velocity. It can be shown [18] that, for streaming
near a solid surface, the magnitude of the streaming velocity
-
v is of the order of the product of Mach number and U ,
representative of those used in commercial ultrasonic cleaning
operations. Consequently U N ( I / p ~ ) l z / ~0.2 ms-l and
Re N 0.02, 0.2, 2 for R = 0.1, 1, 10 pm, respectively. At
an acoustic frequency of 106/2r Hz, 2 r f R l c N for
R = 1 pm. The corresponding orders of magnitude of forces
are given in Table I, assuming an adhesional distance z = 0.4
nm without particle or surface deformation. For this relatively
small adhesional distance, these estimates for van der Waals
forces are upper bounds on their approximate values.
These results illustrate the increasing difficulty experienced
in removing particles of decreasing size, for acoustic excitation
at megahertz frequencies. The reduction in van der Waals
force with increasing adhesional distance emphasizes that,
once the particle is dislodged and suspended in the medium,

QI AND BRERETON: MECHANISMS OF REMOVAL OF MICRON-SIZED PARTICLES BY HIGH-FREQUENCY ULTRASONIC WAVES
TABLE I1
FORCES(IN N) VERSUS PARTICLE IN pm) FOR^= 106/2a Hz
SIZER (RADIUS
R 0.1 1.0 10.0
Fam 2 x 10-IO 2 x 10-7 2 x 10-4
FRs 2~ 10-13 2x 10-10 2 x 10-7
the adhesion force decreases drastically. An important issue
in cleaning is therefore the prevention of dislodged particles
from readhering to the surface.
It is interesting to evaluate when the van der Waals force will
be comparable to the gravitational force. For a given particle
radius, this determines the separation distance at which the
adhesion force becomes insignificant. This distance can be
estimated from (l), (2), and (5). The following results are
given for a micron-sized mica particle
AR 4 particles are submerged (“hide-out”) in the boundary layer
622 = -7rpgR3
3 + z = 0.3 pm (16)
27rBR 4
3z3 = 57rpgR3 + z = 0.47 pm (17)
where we have taken B = Jm [23, p. 221. They indicate
that adhesive forces are no longer dominant when micron
particles are displaced from the surface by roughly one third
of a particle radius, at which point other hydrodynamics forces
determined subsequent particle motion.
At f = 106/27r Hz, the van der Waals force Fvdw in
Table I is at least an order of magnitude larger than all the
other forces for micron and submicron particles. As particle
size increases, the added-mass force first becomes comparable
to the van der Waals force. This is because the adhesion
forces are linearly proportional to the radius of the particles
while acoustically induced hydrodynamic forces (with the
exception of the Stokes drag force) are proportional to particle
diameter squared or cubed. Furthermore, the particle velocity
is limited by the ultrasound intensity level. Consequently, the
smaller the particle size, the more dominant the adhesion
forces. However, in ultrasonic cleaning applications, the choice
of acoustic frequency may be used to advantage-higher
frequencies generate higher acceleration of the liquid and
so larger added-mass forces as illustrated in the order-of-
magnitude estimates in Table 11. Except for radiation pressure
and added-mass forces, other forces are not affected by the
increase of frequency and hence are not reproduced in this
table.
For the case of acoustic excitation at gigahertz frequencies,
the force due to the radiation pressure field is still much
smaller than the van der Waals force for micron and submicron
particles. A comparison of Table I and Table I1 shows that
the added-mass force at f = 109/2.rr Hz dominates adhesion
forces for particles of micron size or larger. However, the van
der Waals force remains dominant for particles of the order
using 6 N (,~/27rfp)’/~:S -
of 0.1 pm. The boundary layer thickness can be estimated
1 pm for f = 106/27r Hz
and S 0.032 pm for f = 109/27r Hz. Consequently, small
N
~
623
\
e2nfir
Acoutic streaming components
displacement
Fig. 2. Acoustic streaming flows and their interaction with particles. The
horizontal streaming flow helps push the particle off the contaminated area,
and the vertical streaming flow helps prevent readhesion of the particle to
the surface (left). Particle removal (right): added mass force overcomes the
adhesion force and mean forces generate a net displacement. The accumulation
of displacement leads to removal.
at relatively low frequencies. In contrast, most particles are
outside the boundary layer at gigahertz frequencies and are
subject to the effective action of hydrodynamic forces.
The drag forces presented in Table I are for the instantaneous
local velocity near the particle. The drag due to streaming
flows, on the other hand, exerts a constant force on particles.
The order of magnitude of the drag force associated with the
acoustic streaming is estimated as follows.
The Reynolds number based on the streaming velocity is
given by Re” = ( p R u 2 ) / ( c p ) .For I = 0.6 x lo5 W/m2, we
find
Re” - 3x lop6, 3 x 3 x lop4
for R = 0.1, 1, 10 pm. (18)
Applying the Stokes drag relation of (9), the drag forces based
on the streaming velocity are
F, - 3x 3x 3x
for R = 0.1, 1, 10 pm (19)
which are larger than the gravitational force for submicron par-
ticles. Since the streaming velocity induced beyond a viscous
boundary layer is independent of acoustic frequency, these
results hold for both megahertz and gigahertz frequencies.
Recently, an improved description of acoustic streaming
near a plane boundary was obtained for plane waves [20].
It was shown that in addition to the streaming flows in the
travelling wave direction, a streaming flow perpendicular to the
plane surface is also generated because of compressibility of
the medium; its magnitude is of the order of u2d w / c 2 .
Although this component is usually small, it may play a
role in preventing particle readhesion once the particles are
loosened from the surface and suspended in liquid, especially
for neutrally buoyant particles. This effect is shown on the
left-hand side of Fig. 2.
Just as the drag force due to streaming motion is constant
with time, so is the radiation pressure force. However, un-
like acoustic streaming near a plane boundary, the radiation
pressure force does increase with frequency. In this regard,
624 IEEE TRANSACTIONS ON ULTRASONICS, FERROELECTRICS, AND FREQUENCY CONTROL, VOL. 42, NO. 4, JULY 1995

TABLE Ill radiation pressure forces are expected to be smaller than those
FORCES
IN (N) VERSUS PARTICLE SIZE (RADIUS IN pm) FOR f = 10' 2T Hz presented in Table 111. Nevertheless, the values of radiation
pressure forces give approximate estimates for submicron
R 0.1 1.o 10.0
particles. The increase of several orders of magnitude in
Fa" 4x 10-8 4 x 10-5 4 x 10-2
the drag force due to streaming emphasizes its dominance
over the gravitational force. Consequently, if the added-mass
and/or radiation pressure forces can move the particles out
FL'FD 4 X lo-' 4 x 10-7 4 x 10-5
of the region of influence of adhesion forces, the subsequent
particle motion will then be determined by steady drag alone.
FRS 2 x 10-8 2~ 10-5 2 x 10-2
This issue is discussed further when experimental results are
described.
FS, 3x10-1' 3 x 10-10 3 x 10-9

v. MECHANISMS
OF REMOVAL
The analyses in Sections 11-IV can be summarized as the
radiation pressure has been used successfully in particle frac- following.
tionation [24], in which particles suspended in a liquid are
The prediction of adhesion forces involves a number of
separated with the aid of radiation pressure force. At megahertz
uncertainties, including the proper choice of the adhe-
frequencies, the drag forces due to acoustic streaming and
sional distance and the estimation of particle asperities.
radiation pressure force are of the same order of magnitude
It is therefore more appropriate to describe a range of
for micron-sized particles. For smaller (larger) particles the
plausible adhesion forces for a given situation. Particle
drag force due to acoustic streaming is greater (smaller) than
removal is expected if the largest possible adhesion force
radiation pressure force. At gigahertz frequencies, however,
can be overcome by cleaning forces.
radiation pressure force dominates the drag force due to
High-frequency ultrasound in liquids like water can be
acoustic streaming.
generated with wavelengths that are comparable to the
size of particles being cleaned, which permits effective
B. Forces in Focused Wave Fields interactions between particles and the sound field. Fur-
The high values of forces such as added-mass forces attained thermore, increasing frequency also has the added benefits
of larger added-mass and radiation pressure forces, and
during high-frequency excitation are one reason for the success
of ultrasonic cleaning. However, one undesirable feature is the thinner viscous boundary layers, thus exposing particles
to the effective action of cleaning forces.
quadratic increase in attenuation with the driving frequency.
The drag force due to acoustic streaming generated near
It is therefore conceivable that a large part of the energy
in the plane wave would be attenuated when the driving the viscous boundary layer is independent of frequency.
The mean radiation pressure force increases with fre-
frequency was high, thus compromising the effective delivery
quency. Both forces have nonzero time averages and
of ultrasound energy for particle removal. One option for
improved cleaning effectiveness is to use focused ultrasound. promote displacements of particles.
Water may be used effectively as a cleaning medium,
When ultrasound is focused, energy can be purposely di-
thereby avoiding the use of environmentally hazardous
rected to the focal region and generate highly localized ve-
solvents. High frequency ultrasound can be used so that
locity and acceleration fields. Brereton and Bruno [4] have
the cavitation threshold is not exceeded and a focused
devised a focused ultrasound apparatus in which individual
particles can be manipulated selectively in this way. In this acoustic wave can be used to compensate attenuation loss.
apparatus the energy density at the focal point reaches a value
of ( E )M 390 x lo3 Jm-3. Consequently, if the sound speed is A. Proposed Removal Mechanisms
taken as c = 1500 ms-', then I = ( E ) cx 58.5 x lo7 WmP2 From previous discussions, the following particle removal
and U M 20 ms-'. Clearly, the local fluid particle velocity mechanisms are proposed.
at the focal region is much higher than in the case of a plane For micron-sized particles in close contact with the sur-
wave. Based on these estimates, we have Re = 2, 20, 200 and face, increasing frequency (to the gigahertz range) promotes
ReS = 0.027, 0.27, 2.7 for R = 0.1, 1, 10 pm, respectively. particle removal at commonly used intensity levels. Removal
The corresponding forces are given in Table 111. is accomplished by combined effects of the time-dependent
A comparison between Table I and Table I11 reveals that added-mass force and the time-invariant forces due to radiation
with the high-intensity focused beam even submicron par- pressure and acoustic streaming. During exposure to acoustic
ticle removal becomes possible. The significant increase of excitation, when the added mass force overcomes the adhesion
radiation pressure force implies that particles in the focal force and causes momentary removal, the particle is also
region may be forced out of the path of the ultrasonic beam subject to streaming and radiation pressure force which can
instantaneously, especially in the case of relatively large cause a net displacement in the direction of streaminghadiation
particles where cleaning forces overwhelm the adhesion force. pressure forces, before reversal of the direction of the added-
These conclusions are based on application of (14), which is mass force restores the particle to the surface. The cumulative
not strictly applicable in the large 27~f R/c limit; the actual displacement might amount to large-scale displacement over
QI AND BRERETON: MECHANISMS OF REMOVAL OF MICRON-SIZED PARTICLES BY HIGH-FREQUENCY ULTRASONIC WAVES
many acoustic cycles, as shown on the right of Fig. 2.
Additionally, the streaming motion may also remove particles
by advection.
If the contact between the particle and the surface is
imperfect, adhesion forces may be much smaller. In this case,
the radiation pressure force alone may be sufficient to re-
move particles, though particle displacement is not necessarily
tangent to the surface. The applied ultrasonic field and the
asperities and elastic properties of the surface and particle all
play a role in determining the trajectories of particles departing
from the surface.
For particles larger than 10 pm, the mean forces of stream-
ing and radiation pressure may be sufficient to remove particles
at gigahertz frequencies. At megahertz frequencies, the added-
mass force may again be needed to overcome the adhesion
force. In general, large particles are much easier to remove.
For particles of 0.1 pm or smaller, cleaning requires greater
forces. If the particles are truly spherical, they still may be
removed by the roll-off mechanism proposed by Bhattacharya
and Mittal [l]. However, if the particles are irregular in shape,
rolling may not take place and a focused ultrasonic beam of
high local intensity might provide sufficient force for removal.
Forces due to added mass and radiation pressure can reach the
same order of magnitude as the adhesion forces, as shown by
the comparison of Table I and Table 111. Successful cleaning
also depends upon preventing readhesion of particles, either
through convection patterns of surrounding fluid or by other
means.
B. Comparison with Experiments
Experiments have been carried out using both focused and
unfocused ultrasound to remove particles from surfaces. Be-
cause of the complexity involved, very few such experiments
have been performed. In general, the local contact conditions
of particles at surfaces cannot be measured and so one can
only use order-of-magnitude analysis to assess whether there
is rough agreement between experimental results and theory.
Imprecise knowledge of particle adhesional distance, and the
quadraticlcubic dependence of adhesion force on this distance,
make comparison of the adhesive and removal forces still more
difficult. Given these difficulties, general agreement to an order
of magnitude is the best one might hope for based on existing
experimental knowledge.
The studies of Kashkoush and Busnaina [14] addressed
the performance of standard unfocused ultrasonic cleaning
equipment which comprised steel tanks with surface-mounted
acoustic transducers. In these studies, particle counting equip-
ment was used to measure the efficiency with which con-
taminant polystyrene latex (PSL) particles could be removed
from wafer surfaces. Efficiencies were measured as functions
of particle size, excitation frequency, acoustic power density,
and exposure time. Experiments conducted with point-focused
ultrasound have been carried out by Brereton and Bruno [5]
who constructed a gigahertz system which allowed observation
of particle removal events (Fig. 3). They energized a commer-
cially available acoustic microscope objective, to which they
delivered as much as 1 W of power in pulses as long as 20
625
sapphire Cylinder
\;---“4
Water Drop
I -\
20 microns
Fig. 3. Acoustic transducer for spherical focusing of gigahertz-frequency
waves.
ps. The objective could focus an acoustic beam to an Airy
diameter of 1.2 pm. They observed different particle responses
to acoustic excitation at the beam focus and adjacent to it, and
studied particle behavior as functions of acoustic power and
proximity to the beam. For each of these series of experiments,
estimates of the acoustic forces were made and compared
with forces of attraction and experimental results on particle
removal. These data are compiled in Table IV.
In the studies of Kashkoush and Busnaina [ 141, clean wafers
were contaminated with PSL particles of 0.3, 0.5, 0.7, and 1.0
pm. Sonification was applied for time periods as long as 30
minutes, at power levels of 50 to 400 W, and at frequencies
of 40, 65, 80, and 100 kHz. Removal efficiencies typically
increased with exposure time and varied between 40% and
80% of the particle population. They also decreased with
decreasing particle size, with little dependence on frequency
over the range studied. These results were reported as the
net percentage of particles removed, so those remaining may
also have been removed but subsequently reattached. Since all
removal efficiencies were of the same order, these data are
summarized in a single column in Table IV.
From knowledge of the acoustic power delivered, the results
of the previous sections were used to estimate the relevant
acoustic forces. Of these, the Stokes drag force appeared to
be the largest N) and was within several orders of
magnitude of the upper estimate of the van der Waals adhesion
force. Thus a case can only be made for the reasonableness of
the theory if the van der Waals adhesion force of PSL particles
is a gross overestimation of the true particle-adhesion force.
Although the drag force is linearly proportional to the acoustic
power, Kashkoush and Busnaina [14] reported only a slight
increase in removal efficiency (10%) at 400 W, compared to
50 W. This result might be a consequence of a distribution
in particle size about its mean value, which could require
an increase in power by an order of magnitude to increase
removal efficiency by 10%.
626 IEEE TRANSACTIONS ON ULTRASONICS, FERROELECTRICS, AND FREQUENCY CONTROL, VOL. 42, NO. 4, JULY 1995

TABLE IV
COMPARISONS OF ACOUSTIC FORCEESTIMATES
WITH EXPERIMENTAL
OBSERVATIONS

Iiamond Diamond ,Diamond PSL Diamond

. ........
5-15
.. ."I-...
I
1 2-4
....................
2-4i
.
i 2-4 2-6

f (Hz)
1 4 x lo4
-105
I

1
.. .I . . . __
..... ....... ...
,

- .-

FRS
. ..

particle:
Observations removei

* Experiments of Kashkoush & Busnaina (1993); these experiments demonstrated particle removal
efficiencies of 60% to 90% over a range of frequencies, exposure times and power levels, using
unfocused ultrasonic excitation. PSL refers to polystyrene latex particles.
* Experiments of Brereton and Bruno (1994); this series of focused-beam experiments explored
single-particle response to streaming, away from the beam focus. Isurfoce is the local power density
estimated from the observed streaming, away from the beam.
#Experiments of Brereton and Bruno (1994);these focused-beam experiments concern single-par-
tick removal at the beam focus and could not accurately measure the likelihood of distant particle
re-attachment.

In the focused-beam experiments of Brereton and Bruno
[4], observations were made of manipulation and removal
of micron-sized particles on flat surfaces, for varying power
levels and duty cycles. The acoustic lens achieved beam waists
of approximately 1.2 pm so that individual particles could
be interrogated by exposure to ultrasonic waves propagating
normal to the surface. Particle response was recorded using
video microscopy at 30 frames per second, allowing resolu-
tion of streaming effects, particle presencehonpresence, and
sometimes particle position during displacement. The effect
of the focused beam on the surrounding liquid was to set up
circulatory streaming motions, as shown on the left of Fig. 4.
Thus both the direct effect of the acoustic beam and the indirect
effects of streaming on particle removal could be studied by
positioning the focus of the beam at different distances from
particles. When small (1 pm) tracer particles were introduced
into the flow, their frame-to-frame displacement could be used
to estimate velocities of streaming motions.
When the power of the focused acoustic wave was adjusted
to induce near-surface streaming at around 0.1 d s , it was
found that diamond particles of 5-15 pm in diameter could
be dislodged and occasionally rolled away. Typical removal
events are shown in the companion videotape to Brereton
and Bruno [ 5 ] . The relative insensitivity of this effect to
distance from the beam focus suggested that streaming might
drive this effect. Streaming patterns have been computed by
Brereton and Bruno [5] using a decomposition by the method
of successive approximations and a spherical model for the
acoustic beam, leading to the patterns shown on the right of
Fig. 4. This streaming pattern illustrates that, for the conditions
of this study, streaming motions along the surface were of
comparable velocity as far from the beam focus as 25 pm.
Similar patterns were computed for all power densities used
in these experiments.
By using the streaming velocity to estimate the local power
density, estimates of the acoustic forces beyond the acoustic
beam could be made. Beyond the beam, the intensity of
scattered acoustic radiation would be small and so the radiation
pressure and added mass forces were neglected. An upper
estimate of the van der Waals adhesion force was 2 x N. It
QI AND BRERETON: MECHANISMS OF REMOVAL OF MICRON-SIZED PARTICLES BY HIGH-FREQUENCY ULTRASONIC WAVES
Fig. 4. Streaming velocity field driven by a focused ultrasonic beam in an axisymmetric cavity model of a water drop. The beam focus is at the 0, 0
coordinate. The accompanying sketch on the left shows the motions observed experimentally.
is conceivable that the actual value is smaller and comparable
to a mean Stokes drag force of lo-' N (Table IV). This point is
partly verified by the experimental observation that streaming
rolls away many particles of this scale. Since diamond particles
are clearly not spherical, considerable variability in the ease
of removal was observed, and this was thought to be due to
the local contact conditions of individual particles. When 1 pm
particles were studied under the same experimental conditions,
it was not possible to dislodge or roll away any. From the
models developed earlier, the upper limit of the adhesive force
would be reduced by about five, while the Stokes drag would
be lowered by about 10 (third column, Table IV). Thus the
Stokes drag may not be sufficient to overcome the adhesion
force for particles 1 micron in size under these conditions.
In these focused-beam experiments, the acoustic intensity at
the surface was believed to be approximately 100 times greater
within the beam than beyond it. The acoustic intensity within
the beam, at the surface, was deduced from the attenuation
of the acoustic signal when it had reached the surface, and
the Airy diameter of the beam. The attenuation was found by
measuring the power to the transducer, and by observing on an
oscilloscope the strength of the acoustic signal reflected back
from the surface, through the transducer. By using attenuation
properties of water, we assume a 3 dB loss at the surface
and reciprocity in attenuation losses in the forward and return
directions, the signal strength at the surface could be deduced
[4]. The acoustic intensity beyond the beam was estimated
from the observed magnitude of the stream velocity. When
the power supplied to the transducer was reduced from its
removal level by a factor of 10 and the point of focus was
repositioned over a particle, an effective increase in local
power density experienced by the particle of about 10 was
achieved. These power densities relate to the fourth and fifth
621
(rm)
columns in Table IV. Under these conditions, particles at the
focus could be either manipulated or occasionally dislodged a
short distance from the focus. It was possible to manipulate
individual particles about their point of contact with the surface
through remote translation of the acoustic transducer. This
capability is also demonstrated in the companion videotape
to Brereton and Bruno [4]. Single particles such as diamond
and polystyrene latex particles 2-4 pm in diameter positioned
at the beam focus appeared to rotate to align themselves to
present the most streamlined shape towards the axis of the
acoustic beam. At slightly higher power levels they were swept
away from the acoustic axis, beyond the field of observation.
Within the beam, the unsteady added-mass force appears to
exceed the upper limit on the force of adhesion by several
orders of magnitude. However, this force has no component
which causes mean displacement. Of the nonlinear forces
which would cause mean motion, the radiation pressure force
appears to be the greatest and exceeds the estimated adhesion
force by a couple of orders of magnitude. Since this force
is localized within the beam and would taper off sharply at
the beam edges, the observed alignment of particles might be
with this radiation pressure field. From the estimates of the
magnitudes of acoustic forces, one might expect the radiation
pressure force to account for complete removal of particles.
However, this force is so localized in the focused beam
experiments that additional farfield forces may be necessary
to effect complete removal.
At the highest power levels possible in the focused beam
studies, all visible particles (1-4 pm diamond, 2-4 pm alu-
minum, 2-6 pm micron polystyrene latex) in the 1 pm-wide
path traced by the transducer could be removed, following
trajectories almost normal to the acoustic axis. Fig. 5 shows
a possible trajectory in this direction. Photographs of the
628 IEEE TRANSACTIONS ON ULTRASONICS, FERROELECTRICS, AND FREQUENCY CONTROL, VOL. 42, NO. 4, JULY 1995
Focused Acoustic Wave ( g H z )
Streaming Motions
~~~~~~~~~~~~~~~~~~~~~
Fig. 5. Suggested trajectory for removal by the combined action of the
added-mass, radiation pressure, and streaming induced drag forces.
systematic depletion of particle population by this cleaning
technique are shown in [5] with video evidence in [4]. In
these experiments (the last three columns in Table IV), the
dominant forces again appear to be the added-mass and
radiation-pressure ones. Since the direction of the primary
acoustic waves is towards the surface, the nonlinear Stokes
drag and radiation pressure forces are also in this direction. The
impenetrability of the surface obviously modifies estimates
of these forces, which are for a plane wave acting on a
particle in an infinite medium. Nonetheless, they are adequate
first approximations and, for the acoustic intensity levels at
the beam focus, the corresponding radiation pressure force is
large at gigahertz frequencies, and is estimated from (14) as
2x N. It is interesting to note that the amplitude of the
oscillatory added mass force, which produces no mean removal
effect, is only slightly larger. Thus what are ordinarily thought
of as secondary forces appear to play a very significant role
in particle removal under gigahertz-frequency excitation.
It appears likely that the combination of oscillatory added-
mass forces and the mean radiation-pressure forces produces
the mechanism of momentary detachment and outward dis-
placement which removes particles by sweeping them away.
Off-axis components of radiation-pressureforce arise wherever
there is wavefront curvature (i.e., everywhere but at the focus
of an acoustic lends without astigmatism). With any typical in-
tensity distribution within the beam (i.e. Gaussian), radiation-
pressure forces decrease with distance from the acoustic axis,
leading to gradients in radiation-pressure force normal to the
acoustic axis. When particles interfere with the beam, they are
subjected to radiation pressure forces parallel to the acoustic
axis, and to axis-normal components, both of which vary
around the particle, especially in the vicinity of the beam focus.
Solution of around complex particle-acoustic beam interaction
is beyond present capabilities. However, unless the acoustic
axis coincides with the particle’s axis of symmetry or some
other chance symmetries occur, there should exist radiation
pressure forces away from the acoustic axis, as well as towards
the surface adhesivehepulsive force while forces away from
the acoustic axis are opposed by the shear component of the
adhesive force. When this can be overcome, there exists a
mechanism for mean displacement of particles away from
the acoustic axis. When the trajectory given to particles by
these forces has both a surface-normal component and one
normal to the acoustic axis, they would follow an outward
path, relaxing from their oscillatory motion towards the motion
of the streaming field as shown in Fig. 5. When the intensity
at the beam focus reached 10’ W/m2, streaming motions were
noticeably more vigorous beyond the beam; this may be the
reason why complete removal is observed in the near field,
rather than particle rotation or manipulation, since the principal
forces are otherwise comparable to those discussed in the
previous paragraph.
While complete removal was seen in near-field observations,
when the microscope objective was changed to allow a broader
view, it was found that many particles (as many as 50%)
reattached after displacement of some 30-50 pm from their
original position. It has been shown [4] that this distance is
comparable to the scale of the recirculating streaming motions,
with reattachment probably taking place at the outermost
parts of streaming orbits. This point emphasizes again that
particle removal must be viewed as the combined processes
of overcoming adhesion forces, lifting particles from surfaces
and convecting them away.
VI. CONCLUDING
REMARKS
By considering orders of magnitude of various forces in-
volved in an ultrasonic cleaning operation, particle removal
mechanisms are proposed and compared with experimental
results. It appears that removal of particles attached to a
plane surface at high-frequency is achieved by the combined
effects of added-mass forces and time-independent forces due
to radiation pressure and acoustic streaming: the added mass
force overcomes the adhesion force instantaneously and mean
forces cause particle displacement. In the event that the particle
can be forced away from the plane surface momentarily,
the effective entrainment of the particle in the streaming
flow then determines the path of the particle, because the
adhesion force is reduced significantly by the increase of the
separation distance. These deductions would be strengthened
substantially with corroboration from further experiments,
designed to access the sizes of both adhesive and removal
forces.
The goal of the analysis presented here is to identify the
particle removal mechanism during an ultrasonic cleaning
operation and provide guidance for more detailed investigation
of the problem. As can be seen from the work by Goldman et
al. [8] and Goren and O’Neill [9], even for Stokes flows and
spherical particles, rigorous analysis of the forces on particles
becomes complicated if the presence of the plane surface
is to be accounted for. However, these analyses strongly
suggest that (6)-( 11) evaluate the relevant force to the correct
order of magnitude, which is as much as one should expect
without more detailed description of individual particle-surface
contact conditions. Thus these analyses and experiments lend
considerable insight into the mechanisms of particle removal
by ultrasonic waves. They provide means for estimating the
effectiveness of existing systems for cleaning prescribed high-
frequency systems for specific particle-removal tasks.
QI AND BRERETON: MECHANISMS OF REMOVAL OF MICRON-SIZED PARTICLES BY HIGH-FREQUENCY ULTRASONIC WAVES
ACKNOWLEDGMENT
John G. Harris, Robert E. Johnson, and William D. O’Brien
are thanked for fruitful discussions.
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Quan Qi, for photograph and biography, see p. 36 of the January issue of
this TRANSACTIONS.
Giles J. Brereton was awarded the BSc. in Me-
chanical Engineenng at Imperial College, Univer-
sity of London, in 1980. He subsequently earned
the M.S. in Mechanical Engineering at Stanford
University, in 1983, and completed the Ph.D. degree
in expenmental turbulence research at Stanford in
1987.
He joined the faculty of the University of Michi-
gan in 1987, where he is an Assistant Professor. His
interests in unsteady fluid mechanics have grown
to include research into internal combustion engine
emissions, nonlinear acoustics, optical diagnostics techniques, and measure-
ment and modeling of unsteady turbulent flows.
Dr. Brereton is a Member of the American Physical Society and the
Amencan Society of Mechanical Engineers, and is faculty advisor to the
ASME student section at the University of Michigan. He received the Silver
Medal of the Royal Society of A r t s in 1980 and was a Fulbright scholar in
1981.