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PHYSICS

SONOLUMINESCENCE

AYSHA AZAH
XII
Acknowledgement

I am indebted to Mrs. Nandini for her guidance, without


which this project would have been incomplete. I am
grateful to my beloved friends and family for their evergreen
love and support. Last but never least, I give thanks to the
Universe for its ceaseless grace and mercy.
CONTENTS

s.no.
title page number

1 introduction 1

2 history 2 - 6

3 the paradox 7-8

single-bubble
4 9-12
sonoluminescence

multi-bubble
5 13-16
sonoluminescence

6 bubble dynamic 17-18

7 light emission 19-20

bubble shape and


8 21
stability

9 bubble surface 22-23

10 applications 24-25
introduction
Sonoluminescence is the production of light from sound. Sonoluminescence occurs
when a small gas bubble is acoustically suspended and periodically driven in a liquid
solution at ultrasonic frequencies, resulting in bubble collapse, cavitation, and light
emission. This effect has been and continues to be, the subject of considerable
experimental and theoretical research.
Sonoluminescence (SL) refers to the phenomena in which a micron size gas bubble is both
spatially trapped and oscillated by an acoustic field in such a way that on each
compression of the bubble, a small burst of light is emitted. This light emission is in the
form of extremely short bursts (< 100ps), but is periodic, occurring in phase with every
cycle of the driving pressure field. Each bubble collapse produces about 500,000 photons.

The bubble collapse is so violent that some predicted that the theoretical accelerations
are larger than those associated with a Black Hole! The actual emission mechanism has
not yet been explained, although theories are as plentiful as they are diverse.

'Neutron star'
(sonoluminescence) in a
test tube under
experimental conditions

1
history
The history of sonoluminescence (SL) begins with its discovery in 1934 by H. Frenzel and H.
Schultes. Motivated by recent advances in sonar technology, Frenzel and Schultes sought a
quicker development of photographic film by subjecting development fluid to ultrasonic
excitation. In the process, they observed tiny flashes of light emanating from within the fluid,
which they described as bubbles undergoing electric discharge. And thus, the field of SL was
born along with the first of many interpretations of a poorly understood phenomenon.
For the first 50 years after its discovery, SL was primarily generated by the non-resonant
acoustic excitation of a fluid. This arrangement creates a cloud of cavitating bubbles and is
now known as multi-bubble sonoluminescence (MBSL). After its initial discovery, the study of
SL progressed slowly, with dark-adapted eyes as the primary diagnostic as the photomultiplier
tube and oscilloscope were in their infancy. Even with this limitation, in 1939 E. Harvey
published a study of the effects of various parameters on SL emission. In fact, many of the
parameters under investigation would be revisited 50 years later using modern
instrumentation. It would take until the late 1950s before the publication of the SL spectrum
and bubble dynamics.

Article published by
The Science Journal
(1994)

2
A summary of these findings was published by P. Jarman in 1960, which noted a thermal-like
spectrum and light emission coinciding with the final stage of collapse.
Jarman noted a model for adiabatic compression and heating of the bubble to temperatures of
thousands of degrees, whereby thermal radiation is the source of light emission. It is
mentioned even in this early work that the bubble emission “resembles that of a blackbody”.
However, due to the spectrum being uncalibrated, the flash width and size of emission being
unknown, and the ensemble nature of MBSL, blackbody confirmation was not possible.
Jarman also proposed a model of “micro shocks” to describe the thermal-like spectrum waves
that form during the bubble’s final collapse stage and create shock heating similar to shock-
tube experiments. This description would persist through the years and it is still considered a
plausible model for SL in water. Jarman confidently ends the article with a bold prediction
that “another decade of experiments should settle these issues.” Sadly, it would take over 40
years before blackbody emission could be confirmed.

3
Similar to the decades preceding it, little research was conducted in the 60s and 70s.
However, the uncalibrated spectrum taken by Holroyd et al. showed excellent
blackbody fits with temperatures between 8,800 and 11,000 K . Without missing a
beat, Holroyd published work showing that the light emission occurs in the collapse
phase of the bubble, in the very next article of the same journal.

Still, the characterization of the bubble dynamics was hindered by the convolution of many
bubbles collapses. In this time period, notable experiments were conducted that generated SL
from a single bubble in various ways.
An experiment by West and Howlett created SL by bombarding degassed tetrachloroethylene
with pulses of fast neutrons and thus seeding cavitation. The liquid was resonantly driven at
20 kHz with an amplitude of up to 20 atm, which brought about strong collapses after initial
bubble growth. This method would be revisited in 2002 by Taleyarkhan of “sonofusion”
infamy. An experiment was conducted by Buzukov and Teslenko where a large laser pulse was
focused in water, causing dielectric breakdown and an expanding bubble. This bubble would
collapse after its initial expansion and create a single SL flash.
This work would also be revisited 3 decades later and be known as laser-induced cavitation.
An effort to stabilize a single SL bubble was made by Saksena and Nyborg in 1970 where an
injected bubble rising in a column of viscous fluid were subjected to ultrasonic excitation.
This work confirmed SL’s periodicity with
the sound field and showed a single pulse of
light at the time of collapse for an isolated
bubble.
The concepts of bubble generation in this
work would be crucial to later experiments
involving water hammers and drop tubes.
Ultimately, the effort to stabilize a single SL
bubble was realized in 1970 by Temple. In
this experiment, SL was trapped at a velocity
node in a resonant field and emitted light at
the driving frequency. This work would pave
the way for the explosion of SL research later
in the 1990s. Although these experiments
showed great promise, detailed bubble
dynamics and spectral measurements in a Rusi Taleyarkhan
resonant system would not occur for another
two decades.
4
The 1980s belonged to the chemists as a whole new field arose known as Sonochemistry.
Exploration of MBSL in various liquids and gases produced spectra with atomic and molecular
excitation lines. These lines provided insight into the state of the heated gas bubble and showed
that the light is being radiated from plasma at temperatures of thousands of degrees. As a
consequence, high-temperature chemistry occurs within the contents of the cavitating bubbles,
which is otherwise difficult to achieve. The model of a rapidly collapsing gas bubble undergoing
adiabatic heating and compression became the consensus. However, the specific dynamics of the
bubble’s collapse and subsequent light emission were still unknown. This would all change with
the advent of single-bubble sonoluminescence (SBSL).

In 1989, F. Gaitan and L. Crum successfully trapped a single bubble in a resonant sound field,
which produced SL with every acoustic period. This newly discovered method opened the door
for measuring the bubble dynamics of SL and the properties of its light emission. Interest in SL
exploded in the following decades, due mostly to the arrival of stable SBSL. To put this in
perspective, the number of SL publications from 1990 to 1995 roughly equaled all publications
from its discovery in 1934 to 1989! This was truly an exciting time for the experimentalist as
access to SBSL was now available to any lab for little cost. Below are some of the key findings

made during this time, which provided insight into the properties of SL :

1. bubble dynamics
For the first time, time-resolved collapse dynamics were observed for a single bubble
using a technique called Mie scattering. This measurement showed that an air bubble in
water undergoes a slow expansion phase and grows to ten times its static radius. The
bubble then collapses at supersonic speeds and is compressed to near liquid densities! At
the time of minimum collapse radius, a flash of light is emitted. This process repeats itself
for every acoustic cycle with a clocklike synchronicity. In some cases, the flash-to-flash
jitter was below 50 ps!

2. flashwidth
Before the arrival of SBSL, the flashwidth of SL was known to be very short.
Even the fastest photomultipliers and oscilloscopes of the time could not
resolve its flashwidth, making it a subnanosecond phenomenon. However,
SBSL gave new life to this measurement through a technique called time-
correlated single-photon counting. Using this technique, the flashwidth of SL
was shown to be in the 100 ps timescale.

5
3. spectrum
The spectrum from SBSL in water was measured and found to be continuous in nature and
void of line emission. In all cases, the spectrum compared well to thermal emission and
particularly to blackbody radiation. These fits showed a gas emitting at temperatures greater
than and equal to 10, 000 K.

The most widely accepted theory for SL emission is the adiabatic compression model
proposed as early as 1950 by Neppiras and Noltingk.

Neppiras and noltingk's


adiabatic compression model
In this model, the gas bubble undergoes a rapid collapse and is adiabatically heated
to thousands of degrees. At thousands of degrees, the gas becomes ionized and
emits bremsstrahlung radiation which is a continuous spectrum. In addition to the
adiabatic compression theory, the shock-wave model suggested by Jarman in 1960
was also revisited due to the supersonic collapse speeds found in SBSL
experiments. This model continues to be a plausible mechanism for the very high
temperatures obtained in water SBSL.

6
the paradox

Although great experimental gains and theoretical insights were made during this decade, a
new paradox in SL would arise. This paradox was addressed by K. Yasui in 1999, Vazquez et al.
in 2001, and Camara et al. in 2004. The spectral measurements of SBSL had now been
calibrated due to the direct measurements of the SL flashwidth. The spectrum not only
showed excellent fits to a blackbody in shape but also in intensity as compared to the newly
measured collapse radius. The emission from SBSL appeared to be radiating from an opaque
plasma by these conclusions. However, to be a surface emitter (opaque), two conditions must
be met :
1. Light and matter must be in thermal equilibrium.
2. A photon must undergo many absorptions and re-emissions before leaving the body.
This second condition appeared to be unsatisfied by SL as estimates for the photon mean-
free-path were much larger than a micron. The big question in SL now became: How can SL
be a blackbody with such a small size? An answer to this question would come with the
arrival of SBSL in acids.
The study of SBSL has a vast parameter space such as temperature, gas mixture, driving
amplitude and frequency, etc. It was predicted that lowering the vapor pressure of the driving
liquid would increase the brightness of the SBSL emission by reducing the amount of vapor
inside the bubble, and thereby maintaining a pure noble gas. Inorganic acids such as sulfuric
and phosphoric acid proved to be excellent candidates with both very low vapor pressures
and high optical transparency. In 2005, Flannigan and Suslick generated xenon and argon
SBSL in concentrated sulfuric acid, which had an increased brightness of 1500 and 2700 times
that of water, respectively. Shortly thereafter, Hopkins et al characterized the bubble
dynamics, flashwidth, and spectrum of a xenon bubble in sulfuric acid. The results from this
experiment show that bubbles generated in sulfuric acid have much larger collapse radii (4
µm) and longer flashwidths (10 ns) which result in the increased brightness compared to
water. Once more, the spectrum is very well fit to a blackbody whose radius of emission also
matches the collapse radius. Although the collapse radius is much larger than water SBSL,
the plasma temperature is similar and therefore the blackbody paradox is again confronted.
This shows that under vastly different experimental conditions, blackbody emission is a
robust feature of SBSL. However, a firm explanation to the blackbody paradox still eluded the
field.
To gain further insight into the temporally and spatially-resolved properties of the SBSL
emission process, a larger and longer lasting bubble is required due to the experimental and
technological limitations. Advancements in the stabilizing methods of rotating water
hammers and the larger and longer SL emission from inorganic acids led to incredibly bright
and long lived bubbles. These conditions led to the groundbreaking experiment conducted
by Kappus et al. and the discovery of SL as a new phase of matter and a potential solution to
the blackbody paradox.
7
In this experiment, a trapped xenon bubble is made to oscillate at 40 Hz in a cylindrical quartz
tube filled with concentrated phosphoric acid. This configuration produced a very large bubble
with a collapse radius of 50 µm and a flashwidth of 1 µs. At the time, it was believed SBSL was
opaque due to its supersonic collapse speeds, which produced a very hot inner plasma core
through shock waves. However, the bubble created by Kappus had a collapse speed that was
slower than the speed of sound and therefore was not expected to create shock waves, and
therefore a transparent plasma. This was not the case as again, the spectrum was an excellent
blackbody fit, whose radius of emission matched the measured collapse radius! Once again, the
blackbody paradox was present as lv ∼ 10^4Rc. Owing to the much longer flashwidth, time-
resolved spectroscopy was performed and showed a strong Xe* line before and after the
minimum collapse radius. Using this line emission and the blackbody fit, a new theory was
presented where SL originates as a new form of matter, characterized by an unusually high
electron density. Previously in the field of SL, electron density had been calculated using Saha’s
equation, which applies to a dilute plasma. However, as we will see in the following section, SL
cannot be considered a dilute plasma. Recognizing this, Kappus et al. applied density
corrections to Saha’s equation and found that two solutions existed for a given temperature and
atomic density.
One solution is weakly ionized and optically transparent (dilute limit). The other solution is
completely ionized and optically opaque (dense limit). This dense limit is believed to be a new
state of matter and provides a potential solution to the blackbody paradox. In summary, SL is
produced by the emission of hot compressed gas. The phenomenon of SL exists in a large
parameter space resulting in a wide range of emission properties. The flashwidth can range
from 50 ps to as long as 1 µs. Similarly, the size of the emitting region can range from 100 nm to
as large as 100 µm. SL is very robust over this enormous parameter space which suggests its
intrinsic properties are fundamental. Indeed, over this parameter space, the blackbody
temperature remains between 6,000 to 20,000 K, and the atomic density is between 1 − 10 ×
10^21 cm^−3 . It is these two properties that make SL unique in nature and, as will be shown in
the next section, a part of a larger class of matter known as strongly coupled plasma (SCP).

8
single-bubble sonoluminescence

Single-bubble sonoluminescence occurs when an acoustically trapped and periodically driven


gas bubble collapses so strongly that the energy focusing at collapse leads to light emission.

Detailed experiments have demonstrated the unique properties of this system:


The spectrum of the emitted light tends to peak in the ultraviolet and depends strongly on
the type of gas dissolved in the liquid.
Small amounts of trace noble gases or other impurities can dramatically change the
amount of light emission, which is also affected by small changes in other operating
parameters (mainly forcing pressure, dissolved gas concentration, and liquid
temperature).

Sketch of a typical setup for


generating sonoluminescing bubbles.

9
the discovery

Single-bubble sonoluminescence was discovered in 1989 by Felipe Gaitan, then a graduate


student at the University of Mississippi working with Larry Crum. Crum had seen hints of light
emission from a single bubble in 1985, and Gaitan’s objective for his thesis was to search
systematically for it. Gaitan was carrying out a set of experiments on the oscillation and
collapse of bubbles, using a flask of liquid lined with transducers tuned to set up an acoustic
standing wave at the resonant frequency at the jar. When the pressure amplitude Pa of the
sound waves is larger than the ambient pressure Po=1 bar, the pressure in the flask becomes
negative, putting the liquid under tension. At large enough tension, the liquid breaks apart (ca,
creating unstable bubble clouds in which the bubbles often self-organize into dendritic
structures. These cavitation clouds collapse with enormous force, powerful enough to do
serious damage to the surfaces of solid bodies in their vicinity.

In his search for single-bubble sonoluminescence, Gaitan at some point found a regime with a
moderate forcing pressure Pa /Po=1.2– 1.4 and with the water degassed to around 20% of its
saturated concentration of air. He then observed that :
‘‘as the pressure was increased, the degassing action of the sound field was reducing the
number of bubbles, causing the cavitation streamers to become very thin until only a single
bubble remained. The remaining bubble was approximately 20 mm in radius and was
remarkably stable in position and shape, remained constant in size and seemed to be pulsating
in a purely radial mode. With the room lights dimmed, a greenish luminous spot the size of a
pinpoint could be seen with the unaided eye, near the bubble’s position in the liquid’’
- Gaitan et al., 1992

At the time of Gaitan’s experiment, all previous work with light-emitting bubbles involved
many unstable bubbles being simultaneously created and destroyed. Using Mie scattering to
track the volumetric contractions and expansions of the bubbles, Gaitan and co-workers
demonstrated that their setup indeed generated a single bubble, undergoing its oscillations at
a fixed, stable position at a pressure antinode of the ultrasound field in the flask.
The oscillation frequency f is that of the sinusoidal driving sound
(typically 20–40 kHz), but the dynamics of the bubble radius are
strongly nonlinear. Once during each oscillation period, the
bubble, radius Ro is typically around 5 mm, collapses very rapidly
from its maximum radius Rmax = 50*10^6 m to a minimum radius
of Rmin= 0.5*10^6 m, changing its volume by a factor of 1*10^6.

10
Radius R(t), driving pressure P(t), and light intensity I(t)
from Crum (1994), as measured by Gaitan et al. (1992). A
negative driving pressure causes the bubble to expand;
when the driving pressure changes sign, the bubble
collapses, resulting in a short pulse of light, marked SL.

The bubble expansion


caused by the negative
pressure is followed by a
violent collapse, during
which light is emitted. The
process repeats itself with
extraordinary precision, as
demonstrated by
measurements of the phase
of the light emission
relative to the driving. Light
emission from collapsing
ultrasound-driven bubbles
had long been dubbed
sonoluminescence (SL).

A sonoluminescence bubble. The dot


in the center of the jar is the bubble
emitting light. From Crum, 1994.
11
Theoretical model

There are two types in models of bubble dynamics for SBSL. One is the shock wave model that
a spherical shock wave converges at the bubble center where extremely high temperature
plasma is formed. The other is the hot-spot model that nearly the whole bubble is heated by
quasi-adiabatic compression, where ‘quasi-‘ means appreciable thermal conduction takes
place between the heated bubble interior and the surrounding liquid.

Numerical simulations of bubble collapse by fundamental equations of fluid dynamics have


revealed that
Temperature and pressure are nearly spatially uniform inside a bubble
There is no shock wave formation inside a bubble under many conditions.

The reason for no shock formation is as follows:


As the temperature near the bubble wall is lower than that near the bubble center due to
thermal conduction between the heated interior of a bubble and the surrounding liquid,
sound speed is lower near the bubble wall. For the shock wave formation, a pressure wave
radiated inwardly from the bubble wall should overtake previously radiated pressure waves
which move with the sound speed plus radial fluid (gas) velocity. Typical bubble collapse is not
so violent to overcome the adverse gradient of sound speed for the shock formation. Thus, no
shock wave is formed inside a collapsing bubble under many conditions.
In the hot-spot model, temperature is assumed to be spatially uniform inside a bubble except
at the thermal boundary layer near the bubble wall. Thermal conduction takes place both
inside and outside a bubble. Non-equilibrium evaporation and condensation of water vapor
takes place at the bubble wall.

The model of bubble dynamics

12
multi-bubble sonoluminescence

Multi-bubble sonoluminescence (MBSL) is the light emission phenomenon from cavitation


bubbles in liquid irradiated by strong ultrasound. Cavitation is the appearance of bubbles in
liquid by a strong decrease in local instantaneous pressure by strong ultrasound or by some
hydrodynamic motion such as that around a ship propeller. In cavitation, a bubble collapses very
violently after bubble expansion under some conditions. There are two reasons for the violent
bubble collapse. One is the spherical geometry of a bubble collapse. According to the continuity
of the liquid, the speed of the bubble collapse increases as the bubble radius decreases because
the surface area of a bubble decreases. The other is the inertia of the surrounding liquid. Due to
the inertia of the ingoing liquid, the bubble collapse becomes very violent. The violent bubble
collapse is called the Rayleigh collapse.

Photographic image of MBSL from AR-saturated SDS solution


at an acoustic power of 4 W. Ultrasound at a frequency of
148 kHz was irradiated from the bottom of the beaker.

At the end of the violent bubble collapse, temperature and pressure inside a bubble significantly
increase to more than 4000 K and 300 bar, respectively, due to the quasi-adiabatic compression of a
bubble. As a result, water vapor inside a bubble is thermally dissociated and OH radicals are formed.
Furthermore, the faint light of sonoluminescence (SL) is emitted from a bubble. The duration of high
temperature and pressure inside a bubble is only less than 1–10 ns. Thus, the SL pulse width from a
bubble is less than 1 ns.

13
the discovery

MBSL was discovered in 1933 by Marinesco and Trillat who observed the fogging of the
photographic plate immersed in the liquid irradiated by ultrasound. MBSL was recognized as
the light emission from the cavitating liquid in 1934 by Frenzel and Schultes. A significant
development in SL research has been brought about after the discovery of single-bubble
sonoluminescence (SBSL) in 1990 by Gaitan and Crum. SBSL is SL from a stably pulsating
bubble trapped at the pressure antinode of a standing ultrasonic wave. In 1991, Barber and
Putterman reported in Nature that SBSL pulse width is less than 100 ps, which attracted many
researchers’ attention. After that, there has been significant development in SL research.
Before the discovery of SBSL in 1990, MBSL, which was simply called SL, had been considered
to originate mainly in the recombination of free radicals inside a bubble. The development of
the SBSL research has been reviewed by Brenner, Hilgenfeldt, and Lohse.
Another significant finding in SL research is the evidence of thermal plasma formation inside
a bubble in sulfuric acid in optical spectra of SBSL by Flannigan and Suslick in 2005.

vaporous and gaseous bubbles


When the bubble content is mostly water vapor even at the end of the bubble collapse, such
bubbles are called vaporous bubbles. On the other hand, when the bubble content at the end
of the bubble collapse is non-condensable gas such as air, such bubbles are called gaseous
bubbles.
According to numerical simulations, vaporous bubbles appear at relatively high acoustic
amplitudes at relatively low ultrasonic frequencies. For example, at 20 kHz and 5 bar in
ultrasonic frequency and pressure amplitude, respectively, a bubble expands dramatically
during the rarefaction phase of ultrasound. As a result, intense evaporation of water takes
place during the bubble expansion into a bubble in order to maintain the saturated vapor
pressure inside a bubble. Although intense condensation of water vapor takes
place at the bubble wall at the bubble collapse, still the main bubble content is
water vapor even at the end of the bubble collapse. It should be noted that
condensation at the bubble collapse is strongly in non-equilibrium,
and the partial pressure of water vapor inside a bubble is several orders
of magnitude larger than the saturated vapor pressure.

14
influence of bubble size

The linear resonance radius of an air bubble is 10.9 μm at 300 kHz. However, due to the strong
nonlinear nature of bubble pulsation, the expansion ratio (Rmax/Ro), where Rmax is the
maximum bubble radius and Ro is the ambient bubble radius which is the bubble radius when
ultrasound is absent, takes the peak value at smaller ambient bubble radius than the linear
resonance radius even at acoustic amplitude as low as 0.5 bar. As the acoustic amplitude
increases, the maximal response of a bubble shifts toward smaller ambient radius. At the
acoustic amplitude of 3 bar, the range of ambient bubble radius for higher expansion ratio
than 3 is from 0.27 to 7 μm.

The calculated expansion ratio (Rmax/Ro) as a function of ambient


bubble radius for various acoustic amplitudes at 300 kHz
The shape instability of a bubble is another important factor to determine the range of
ambient bubble radius for active bubbles observed experimentally. When the acoustic
amplitude is above the threshold for shape instability , a bubble disintegrates into daughter
bubbles in a few acoustic cycles. When the acoustic amplitude is larger than the Blake
threshold, bubble expansion becomes very strong, which is called transient cavitation. When
the threshold SL intensity and that for sonochemical production of oxidants is assumed as 10−7
pJ/collapse and 108 molecules/s, respectively, they are equal to or higher than the Blake-
threshold acoustic amplitude. The typical range of ambient radius for actual active bubbles is
from the SL threshold radius (or threshold for sonochemical production of oxidants) to slightly
above the threshold radius for shape instability because larger active bubbles disintegrate into
daughter bubbles in a few acoustic cycles. Indeed, Brotchie et al. reported experimentally that
the range of ambient radius for MBSL bubbles was from 2.9 to 3.5 μm at 355 kHz, which is a
relatively narrow range near the threshold for shape instability. Further studies are required
on this topic.

15
bubble-bubble interaction

In contrast to the case of the single bubble system (SBSL), some complexity arises from the
bubble–bubble interaction in the multi-bubble system (MBSL). In a bubble cloud, bubble
pulsation is strongly influenced by the pulsations of surrounding bubbles because they
radiate acoustic waves into the liquid, which is called the bubble–bubble interaction.

acoustic field

MBSL has been used to visualize acoustic fields through the spatial distribution of active
bubbles in SL. Sonochemiluminescence (SCL) has also been used to visualize acoustic fields,
where SCL is the light emission from an aqueous luminol solution by chemical reactions of
luminol with oxidants such as OH radicals and H2O2 produced from cavitation bubbles. An
example of the SCL image is shown for a half plane of a rectangular cell (5 cm × 5 cm × 14.5 cm)
at 140 kHz. Horizontal stripes of pressure nodes and antinodes are seen in the photograph,
where pressure antinodes are the bright regions in blue by SCL. In addition, there is a vertical
narrow dark region, where acoustic amplitude is relatively low (or number density of bubbles
is relatively low).

The calculated spatial distribution of the acoustic amplitude for glass wall (7 mm in thickness) for various
attenuation coefficients of ultrasound. The full-width at half maximum for the Gaussian distribution of the
vibration amplitude of the vibrating plate at the bottom is 5 cm. The wall height is 20 cm. A half of the width
(the full width is 7 cm) of the liquid container is shown. The photograph of sonochemiluminescence from an
aqueous luminol solution is also shown for the corresponding half plane

16
bubble dynamics

These equations were made using five major assumptions, with four of them being common
to all the equations:
1. The bubble remains spherical
2. The bubble contents obey the ideal gas law
3. The internal pressure remains uniform throughout the bubble
4. No evaporation or condensation occurs inside the bubble
The fifth assumption, which changes between each formulation, pertains to the
thermodynamic behavior of the liquid surrounding the bubble. These assumptions severely
limit the models when the pulsations are large and the wall velocities reach the speed of
sound.

Keller–Miksis formulation

The Keller–Miksis formulation is an equation derived for the large, radial oscillations of a
bubble trapped in a sound field. When the frequency of the sound field approaches the
natural frequency of the bubble, it will result in large amplitude oscillations. The Keller–
Miksis equation takes into account the viscosity, surface tension, incident sound wave, and
acoustic radiation coming from the bubble, which was previously unaccounted for in
Lauterborn's calculations. Lauterborn solved the equation that Plesset, et al. modified from
Rayleigh's original analysis of large oscillating bubbles. Keller and Miksis obtained the
following formula:

where R is the radius of the bubble, the dots indicate first and second time derivatives, ρı is
the density of the liquid, c is the speed of sound through the liquid, pB(R,t) is the pressure on
the liquid side of the bubble's interface, t is time, and pA(t+R/c) is the time-delayed driving
pressure.

17
Prosperetti formulation

Prosperetti found a way to accurately determine the internal pressure of the bubble using the
following equation:

where T is the temperature, K is the thermal conductivity of the gas, and r is the radial distance.

Flynn's formulation

This formulation allows the study of the motions and the effects of heat conduction, shear
viscosity, compressibility, and surface tension on small cavitation bubbles in liquids that are set
into motion by an acoustic pressure field. The effect of vapor pressure on the cavitation bubble
can also be determined using the interfacial temperature. The formulation is specifically
designed to describe the motion of a bubble that expands to a maximum radius and then
violently collapses or contracts. This set of equations was solved using an improved Euler
method.

where R is the radius of the bubble, the dots indicate first and second time derivatives, ρı is the
density of the liquid, c is the speed of sound through the liquid, dpB(R,t) is the pressure on the
liquid side of the bubble's interface, t is time, and pA(t) is the driving pressure.

Rayleigh–Plesset equation

The theory of bubble dynamics was started in 1917 by Lord Rayleigh during his work with the
Royal Navy to investigate cavitation damage on ship propellers. Over several decades his work
was refined and developed by Milton Plesset, Andrea Prosperetti, and others.
The Rayleigh–Plesset equation is:

18
light emission
The inertia of a collapsing bubble generates high pressures and temperatures capable of ionizing
a small fraction of the noble gas within the volume of the bubble. This small fraction of ionized
gas is transparent and allows for volume emission to be detected. Free electrons from the ionized
noble gas begin to interact with other neutral atoms causing thermal bremsstrahlung radiation.
Surface emission emits a more intense flash of light with a longer duration and is dependent on
wavelength. Experimental data suggest that only volume emission occurs in the case of
sonoluminescence. As the sound wave reaches a low energy trough the bubble expands and
electrons can recombine with free ions and halt light emission. Light pulse time is dependent on
the ionization energy of the noble gas with argon having a light pulse of 160 picoseconds.

relative
radiance (W/nm)
brightness

1 1.5*10^-12 bright

2 9.00*10^-13 semi-bright

3 1.75*10^-13 dim

4 7.00*10^-14 very dim

5 2.00*10^-14 extremely dim

solution in water average max. radiance (W/nm)

1 xenon in water 1.04*10^-9

2 krypton in water 8.00*10^-10

3 argon in water 7.75*10^-10

4 neon in water 5.40*10^-10

5 helium in water 4.45*10^-11

19
electrical processes

In 1937, the explanations for the light emission favored electrical discharges. The first ideas
have been about the charge separation in cavitation bubbles, which have been seen as
spherical capacitors with charges at the center and the wall. At the collapse, the capacitance
decreases and voltage increases until electric breakdown occurs. A further suggestion was a
charge separation by enhancing charge fluctuations on the bubble wall, however, a breakdown
should take place during the expansion phase of the bubble dynamics. These discharge
theories have to assume that the emitting bubble undergoes an asymmetric collapse because a
symmetric charge distribution cannot radiate light.

Thermal processes

Because the bubble collapse occurs within microseconds, the hot spot theory states that the
thermal energy results from an adiabatic bubble collapse. In 1950 it was assumed that the
bubble internal temperatures were as high as 10,000 K at the collapse of a spherical symmetric
bubble. In the 1990s, sonoluminescence spectra were used by Suslick to measure effective
emission temperatures in bubble clouds (multibubble sonoluminescence) of 5000 K, and more
recently temperatures as high as 20,000 K in single bubble cavitation.

20
Bubble shape stability

The limit for the ambient size of the bubble is set by the appearance of instabilities in the
shape of the oscillating bubble. The shape stability thresholds depend on changes in the radial
dynamics, caused by different liquid viscosities or driving frequencies. If the frequency is
decreased, the parametric instability is suppressed as the stabilizing influence of viscosity can
appear longer to suppress perturbations. However, the collapses of low-frequency-driven
bubbles favor an earlier onset of the Rayleigh-Taylor instability. Larger bubbles can be
stabilized to show sonoluminescence when not too high forcing pressures are applied. At low-
frequency, the water vapor becomes more important. The bubbles can be stabilized by cooling
the fluid, whereas more light is emitted.

Upon the collapse of a bubble experiencing cavitation, a hot spot


is produced for a small amount of time. That hot spot contains a
high temperature core that is surrounded by a cooler outer shell.

21
Bubble surface

The surface of a collapsing bubble like those seen in both SBSL and MBSL serves as a
boundary layer between the liquid and vapor phases of the solution.

Generation

MBSL has been observed in many different solutions under a variety of conditions.
Unfortunately, it is more difficult to study as the bubble cloud is uneven and can contain a
wide range of pressures and temperatures. SBSL is easier to study due to the predictable
nature of the bubble. This bubble is sustained in a standing acoustic wave of moderate
pressure, approximately 1.5 atm. Since cavitation does not normally occur at these pressures
the bubble may be seeded through several techniques:
1. Transient boiling through a short current pulse in nichrome wire.
2. A small jet of water perturbs the surface to introduce air bubbles.
3. A rapidly formed vapor cavity via focused laser pulse.
The standing acoustic wave, which contains pressure antinodes at the center of the
containment vessel, causes the bubbles to quickly coalesce into a single radially oscillating
bubble.

Collapse

Once a single bubble is stabilized in the pressure antinode of the standing wave, it
can be made to emit pulses of light by driving the bubble into highly nonlinear
oscillations. This is done by the increasing pressure of the acoustic wave to disrupt
the steady, linear growth of the bubble which cause the bubble to collapse in a
runaway reaction that only reverts due to the high pressures inside the bubble at its
minimum radius.

Afterbounces

The collapsed bubble expands due to high internal pressure and experiences a
diminishing effect until the high pressure antinode returns to the center of the vessel.
The bubble continues to occupy more or less the same space due to the acoustic
radiation force, the Bjerknes force, and the buoyancy force of the bubble.

22
Surface chemistry

The effect that different chemicals present in solution have on the velocity of the
collapsing bubble has recently been studied. Nonvolatile liquids such as sulfuric
and phosphoric acid have been shown to produce flashes of light several
nanoseconds in duration with a much slower bubble wall velocity, and producing
several thousand-fold greater light emission. This effect is probably masked in SBSL
in aqueous solutions by the absorption of light by water molecules and
contaminants.

Surface tension

It can be inferred from these results that the difference in surface tension between
these different compounds is the source of different spectra emitted and the time
scales in which emission occur.

Bubble oscillations correspond


to pressure anti-nodes

23
applications
Industrial and Medical Applications

The growing understanding of shock physics phenomena has led to numerous industrial
applications. M. Sanai of SRI International discussed two recent applications at the SCCM
Meeting: a method of assessing explosion safety in industrial plants, and a bomb-resistant
baggage container for wide-body aircraft.
Explosion safety usually employs computer simulation techniques to model the details of the
detonation of energetic materials. Using a general load-damage analysis technique known as the
pressure-impulse method, Sanai and his colleagues have developed a PC-based computer
algorithm that incorporates a continually expanding library of load and damage curves.
Sanai also described SRI's development of a patented hardened luggage container that can
protect the aircraft from a terrorist bomb hidden inside the baggage. The container relies on
blast management and debris containment provided by a flexible flow-through blanket woven
from threads made with a strong lightweight material, such as Spectra or Kevlar. "When an
explosion occurs, the mitigation blanket expands into a nearly circular shell that contains the
flying debris while directing the flow into the adjacent containers," said Sanai. "This redirecting
of the flow and slow venting of the detonation products dissipate the explosive energy without
damaging the structural shell of the aircraft."
In addition, promising new medical therapies are being developed which use concentrated
energy deposition via lasers and ultrasound. According to Livermore's M.E. Glinsky, an
understanding of stress wave propagation and material response is vital to design these new
techniques for maximum efficiency and minimal damage. He discussed ongoing experiments to
explore such issues as the structure of several generic hard and soft composite tissues and the
impact of thermal destruction on their structural integrity.

Shock Temperature Measurements


of Liquid Hydrogen

Scientists at Livermore have developed a new model to determine the final pressure and volume
of double-shocked liquid deuterium and hydrogen, after a series of measurements produced
temperatures as much as 40 percent lower than predicted by theory. According to N.C. Holmes,
the lower temperatures are a result of a fraction of the available shock energy being used to
dissociate some of the hydrogen molecules. In the new model, molecular dissociation energy
decreases with volume, and subsequent double-shock experiments, which reach higher densities
than equivalent-pressure experiments, were in overall agreement with this hypothesis.

24
Shock Wave Properties of
Brittle Solids
Using planar impact methods and velocity interferometry diagnostics, scientists at Sandia
National Laboratories have performed extensive experiments in large-amplitude, nonlinear wave-
profile measurements which manifest the shock strength and equation-of-state properties of
brittle solids. They also provide controlled, shock-induced motion histories that validate existing
computational models.
These high-resolution shock-profile data are providing a window into the physics of emerging
understanding of the compression and deformation behavior of high-strength brittle solids. The
shock wave data suggests that both crystalline plasticity and brittle fracture may play important
and interconnected roles in the dynamic failure process.

Numerical Anomalies Mimicking


Physical Effects
Numerical simulations of flows with shock waves typically use finite difference shock capturing
algorithms, which give a shock an artificial width proportional to the cell size to generate the
entropy increase that occurs across a shock wave. But numerical anomalies can occur when shock
waves interact or a shock wave is formed. Examples include strong shock reflected from a rigid
wall and errors that occur when a shock impacts a material interface.
This class of anomalies can be explained by the entropy generation that occurs in the transient
flow when a shock profile is abruptly formed or changed. When a shock wave has a profile, its
position can be defined to match the mass of an idealized continuous shock. However, in a shock
interaction, the shift in the energy of the wave profiles between the incoming and outgoing shocks
leads to an entropy anomaly in the spatial region where the incoming wave profiles overlap,

Time-Resolved Molecular Changes

Researchers at Washington State University (WSU) have conducted time-resolved Raman


scattering experiments to probe molecular changes in shocked materials. According to G.I.
Pangilinan, a good understanding of the molecular mechanisms governing shock-induced
chemical decomposition in condensed energetic materials is fundamental to the field of
detonation science, as well as to the development of new energetic materials.
To this end, Pangilinan and his colleagues made time-resolved Raman spectroscopy
measurements that enabled them to monitor in real-time the molecular changes associated with
the onset of a chemical reaction in shocked nitromethane. Raman spectra of nitromethane at high
peak pressures exhibited irreversible changes indicative of chemical reactions. It appears that the
activation energies of the initial reaction steps are lowered and this impacts the microscopic
models of decomposition of the material.
25
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https://core.ac.uk/download/pdf/4824488.pdf
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