Closing Report on Faculty Research Grant: “Development of an ultrasonic sensor

array for the PICASSO dark matter experiment”

Ilan Levine, Assistant Professor of Physics and Astronomy 5 November, 2004
1) Description of grant supported activity
I was asked to lead the effort in the PICASSO collaboration to develop acoustic detection
equipment and analysis techniques for this experiment. A 40 g version of the experiment has been
taking data in the SNO laboratory and a major upgrade to a 1kg detector is currently underway.
Eventually, this experiment will replace the SNO experiment in the INCO Creighton mine in
Sudbury, Ontario, as one of the major physics experiments in Canada, and one of the leading
astroparticle experiments in the world. The detector should be the best positioned experiment to
confirm or refute the controversial reported dark matter signal by the DAMA experiment in Italy,
and the work at IUSB will play a major part in the development of this detector.

The activity at IUSB this summer consisted mainly of the development of an externally mounted
ultrasonic sensor which will be used in the 1kg detector, as well as improvements of the amplifier
for these sensors. The amplification technique has been submitted for patenting through ARTI,
and we have now applied for a full international patent through the law firm of Leydig, Voit &
Mayer LTD.
2) Were you able to complete the project? Describe and difficulty you had.
We accomplished the goals of creating an inexpensive, externally mounted, ultrasonic sensor
which has more sensitivity than commercial units which sell for about $150/sensor. Our sensors
cost ~$15/sensor, an order of magnitude less than the commercial units. Since the 1kg detector
will require 200 sensors, this represents both a major scientific contribution to the experiment and
a major financial contribution. Our major difficulty has been to develop sensitivity at higher
frequencies ( ~100kHz ), and we are currently modifying various aspects of the construction of
the sensors to obtain this sensitivity.

3) Did, or will, the project result in a specific product -- a manuscript, composition,

syllabus, etc? If so, please describe and indicate state of development
.
There were several specific products:
1) An international patent for the circuit that we developed has been applied for.
2) Ed Behnke, an IUSB physics major and Ilan Levine both gave presentations at the annual
meeting of the American physical society.
3) A grant application (written this September) to the NSF was prepared based upon this
work, has been submitted. A copy of the one page scientific summary of this grant
application, and the full scientific description are appended to this report.
4) A new collaboration between the group at IUSB and Yale University has been formed
which will attempt to develop the superheated emulsion technique for various
applications.
I would like to thank the R&D committee for the support through the faculty research grant which
helped make this work possible.

Sincerely,

Ilan Levine
RUI: A Search for Dark Matter with Superheated Emulsions
Intellectual Merit: One of the most enduring mysteries in astrophysics is the explanation for the
compelling evidence that, on virtually all scales above the size of a star, far more gravitating material
exists in an invisible form than that which can be detected by all known types of radiation. This "dark
matter" is detected dynamically, through its effects on the structuring of galaxies, clusters of galaxies and
larger scale structures in the universe. Generic extensions of the standard model of subatomic particles
predict the existence of Weakly Interacting Massive Particles (WIMPS) which are excellent candidates
for the dark matter. These are expected to interact with ordinary matter as rarely as neutrinos and thus be
extremely difficult to detect.

The PICASSO group has undertaken the development of a new large dark matter detector based on the
well known bubble chamber technique. In this application, the detector consists of a uniform emulsion of
micron-sized halocarbon droplets suspended in a compliant material such as a polymeric or an aqueous
gel and kept in a superheated state (i.e. they are kept above their boiling point.) In this thermodynamically
metastable state, the droplets can be vaporized by exposure to radiation. Sound is emitted in the rapid
phase transition from liquid to vapor, and can be recorded using acoustic sensors. Superheated emulsions,
originally invented at Yale University, have now become a mature technique in neutron dosimetry. This
key feature, along with the ability to increase the target size inexpensively, and the possibility of tailoring
the response to specific types of radiation, based on chemical composition, droplet loading, and
temperature/pressure conditions, have brought superheated emulsions to the forefront of dark matter
investigations. It is anticipated that, within two years, PICASSO will be the world’s most sensitive
detector, if interactions between dark matter and WIMPs are predominantly spin-dependent.

Thanks to their expertise in nuclear electronics, radio-purification and assay, halocarbon chemistry, and in
the superheated emulsion technology, Indiana University South Bend (IUSB) and Yale University were
invited to join the PICASSO project. While the Canadian partners are funded in their efforts, IUSB and
Yale have no specific support for this research. The two universities hereby jointly seek NSF support for
this potentially groundbreaking research. In this project, IUSB would be responsible for designing new
sound sensors and their associated electronics, and for measuring the acoustic properties of the detectors.
IUSB and Yale would jointly explore and develop new pulse analysis algorithms for the identification of
bubble formation events. Yale would be in charge of extending its current models of the radiation physics
of superheated emulsions in order to optimize the operating conditions required for the detection of
WIMPS. Finally, while fluorine compounds are currently used for their favorable spin-dependent cross
section, Yale and IUSB would also jointly explore the incorporation of high-Z atoms, such as lead, into
the droplets in order to enhance coherent scattering interactions.

Broader impacts: Enhancing the education of science majors is an integral part of the program. Two
physics majors and one chemistry major have participated in the work at IUSB. They developed a data
acquisition system, designed a device to couple to piezoelectric sensors in a unique fashion which is now
being patented, and designed the preamplifier that will be used in the 1kg PICASSO detector in March
2005. One student presented this work at the 14th Argonne Symposium for Undergraduate Research in
Science Engineering and Mathematics, October, 2003, and at the 1st International Workshop on Bubble
Detectors in Applied and Fundamental Research, February, 2004. The chemistry student has produced the
first IUSB Scientific and Technical report for the PICASSO group on different pathways for the synthesis
of perfluoroalkyl lead.

Enhancing the science background of education majors is another focus of our group. Each semester, an
education major will work with the group on a well defined R&D project. The students will have an
inquiry-based science experience and will produce a written technical report that they will defend orally
at a collaboration meeting. The idea is that having participated in a real science project will inform their
teaching of science when they are in the classroom.
RUI: A Search for WIMP Dark Matter with Superheated Emulsions
1.1 Introduction
One of the longest standing and most important questions [1] in astrophysics and particle physics is “what
is the dark matter?” Since the mid 1930s [2] there has been evidence that there is more gravitating
material in objects larger than the scale of a star than can be accounted for by the amount of light coming
from those objects [3]. The evidence has become more convincing and more detailed, including for
example the observations of X-ray data from gravitationally bound heated gases [4] and the gravitational
lensing of distant galaxies [5]. Also, evidence has accumulated that the deficit of light from all of this
extra mass is not because the mass is concentrated in clumps of ordinary matter, such as high mass
planets [6]. Even more recently, WMAP’s studies of the asymmetries in the distribution of relic radiation
from the last scattering in the early universe [7] make a compelling case that a large fraction of gravitating
matter stopped interacting with ordinary matter (protons, electron, neutrons, etc) just after the Big Bang.
The neutralino, a particle predicted by generic extensions [8] of the standard description of particles and
their interactions, and assumed to have normal weak nuclear interactions with ordinary matter, is a prime
candidate for the dark matter. The lightest of the supersymmetric partners to ordinary matter, neutralinos,
should be the sole relic of this class of particles created in the big bang. There are a number of direct
search techniques [9] being developed to search for evidence of these primordial Weakly Interacting
Massive Particles (WIMPs). The common point of all these searches is to look for nuclei of ordinary
matter which are elastically scattered by an undetected projectile (The incoming WIMP would not be
detected, since it does not interact with ordinary matter through the strong force or the electromagnetic
force.) The rate of these interactions should change as a function of the time of year, since the earth
changes its direction of motion and thus relative kinetic energy of the detector target nuclei with respect
to the galactic cloud of WIMPS. This annual modulation of the scattering rate is a signal being searched
for by operating direct search experiments. (Some future experiments will also reconstruct the direction of
the incoming WIMPS, which ought to be correlated with the direction to the center of the galaxy.)
1.2 Coherent and Spin Dependent Interactions
The neutralino interaction with nuclei of ordinary matter has the general form given by

2
⎛ MχMA ⎞
σ A = 4G F ⎜⎜2
⎟ CA
⎟
M
⎝ χ + M A ⎠

where GF is the Fermi constant, Mχ and MA are the mass of the neutralino and the target nucleus,
respectively [10, 11, 12], and CA is an enhancement factor which depends on the type of neutralino
interaction. Spin independent (SI), or scalar, interactions proceed via Higgs, or sfermion exchange. For
equal couplings to neutrons and protons, the cross section is proportional to A2. Minimal supersymmetry
predicts cross sections ranging from between 10-8 – 10-11 pb per nucleon for neutralinos with masses from
70 GeV to 500 GeV. However destructive interferences can lead to cross sections lower than 10-13 pb
which will remain undetectable in the near future. If the neutralino is of the Gaugino or Bino type, then
CASI vanishes altogether. On the other hand, spin dependent interactions (SD) with axial coupling involve
sfermion and Z-exchange and cross sections depend on the nuclear spin of the target. The cross sections
in this case are smaller than the SI cross sections, and vary from 10-4 to 10-9 pb per nucleon, but
cancellations are much less likely. This is discussed more completely in the letter of interest (LOI) which
the PICASSO collaboration submitted to the SNOLAB long range planning committee.
(http://www.viktortec.com/loi).

1.3 The case for SD Sensitive Detectors.

The main efforts currently undertaken worldwide are searches in the SI sector. The most sensitive
experiments employ NaI scintillators (e.g. DAMA, NAIAD), bolometers (e.g. Edelweiss, CDMS,

1
CRESST) and liquid Xenon detectors (e.g. ZEPLIN). Their sensitivity is of the order of 10-6 pb per
nucleon with background levels of the order of 1 event/kg/d. Several of these projects aim at 1 ton
detectors with sensitivities at the level of 10-10 pb and background levels below 10-3 event/kg/d, by about
2010. However, if the dominant interactions are spin dependent, experiments with zero spin targets,
such as CDMS, will not detect a dark matter signal. Thus, experiments with non-zero spin targets
are strongly motivated.
1.4 Sensitivity in the SD sector.
Various targets useful for exploring the SD sector have been used (NaI, CaF2, A12O3, CnFm, C2ClCF5) by
different experiments (Tokyo, ELEGANT, SIMPLE, CRESST, ANAIS, DAMA, UKDMC, NAIAD and
PICASSO.) The state of the art sensitivity in the SD sector is of order 1 pb, obtained by NaI detectors
(DAMA, UKDMC, NAIAD.)

Figure 1: WIMP-proton axial coupling limits

Figure 1 (adapted from ref [13]) summarizes present and future limits and theoretically (MSSM) favored
regions. The shaded brown region shows the DAMA allowed region. The solid orange line shows
preliminary limits of the data taken by the PICASSO 40 g detector. These experiments need about two
orders of magnitude improvement to reach the SUSY predictions for relic neutralinos. The 1 kg
PICASSO detector (0.2 cts/g/d), to be installed in March, 2005, will have a sensitivity shown as
“PICASSO Phase 1”, with about 6 months of data. By the end of 2005, the PICASSO collaboration
should be able to confirm or exclude the DAMA results in the spin dependent sector. Phase 2 (~3 kg,
radioactive background down to 0.02 cts/g/d), which should be reached by the end of 2006, will just reach

2
the tip of the MSSM (green dots.) Phase 3 (10 kg) will reach well down into the 10-5 pb cross section
region by the end of 2007. Phase 3 R&D will prepare the technology for the first large detector (~100 kg,
0.001 cts/g/d.)

The DAMA group has claimed [14] that an annual modulation in count rate in their NaI experiment is
evidence for the direct observation of particulate dark matter. This modulation is consistent with a
neutralino with a mass between 40 and 110 GeV, interacting with an SI cross section between 10-5 and 10-
6
pb, or an SD cross section between 0.7 and 0.1 pb. With its first underground measurements [15], the
CDMS group has ruled out SI interacting WIMPS as the source of this signal. It has been argued [16, 17]
that SD neutralinos with the DAMA properties can also be ruled out, by noting the absence of high
energy neutrinos [18] coming from the sun in the Super-Kamiokanda neutrino telescope1. However, a
direct search in the SD sector would be less model-dependent. By the end of 2005, the PICASSO group
expects to either confirm the SD DAMA results or rule them out, using a 1 kg detector now being
built for installation in the Sudbury Neutrino Observatory (SNO) water purification drift. This detector is
a scaled up version of the 40 g detector, which is sufficiently low in radioactivity to be sensitive to the
entire allowed DAMA region with six months of data.
This proposal describes IUSB’s and Yale’s role in the PICASSO group’s plan to explore the DAMA
allowed region by the end of 2005(“Phase 1” in Figure 1), reach the tip of the MSSM (“Phase 2”) by the
end of 2006, explore a much larger region of the MSSM space by the end of 2007 (“Phase 3”), and to
begin the R&D required to design large scale detectors.
2 Superheated Emulsion Detectors, PICASSO Technique and Results
2.1 Superheated Emulsion Detectors
The PICASSO collaboration’s approach
(http://picasso.lps.umontreal.ca/ and ref. [ 19 ])
relies on the superheated drop detector, a
miniature replica of the bubble chamber [20 ]
invented at Yale University by Robert Apfel
[ 21 ]. These detectors consist of uniform
dispersions of superheated halocarbon and/or
hydrocarbon droplets suspended in a compliant
material such as a polymeric or an aqueous gel.
Charged particles liberated by radiation
interactions nucleate the phase transition of the
metastable drops and generate detectable
bubbles (Figure 2). Bubble chambers utilize a
pressurised homogeneous liquid that is suddenly
and briefly brought to a transient superheated
state by dropping the applied pressure.
Conversely, superheated emulsions are
continuously sensitive since the liquid is kept in
steady-state superheated conditions. This
metastable state is normally fragile and short- Figure 2. Superheated drop detector before and
lived due to the high number of "heterogeneous after irradiation.
nucleation" sites: microscopic particles and/or
gas pockets present at the interface with container surfaces, which act as seeds for the phase transition.
However, a liquid may be kept in steady-state superheated conditions by emulsifying it into droplets

1
Elastic scattering with protons in the dense core of the sun would stop the WIMPS, which would then
collect, over billions of years, and then annihilate to high energy neutrinos coming from the core.

3
dispersed in an immiscible host fluid. This procedure creates perfectly smooth spherical interfaces, free of
nucleating impurities or irregularities. Number, size and composition of the droplets can be varied in the
formulation of the detectors, and this permits a wide range of applications. In particular, halocarbons with
a moderate degree of superheat (i.e., a small difference between their operating temperature and boiling
point) can be used for neutron detection since they are only nucleated by energetic heavy ions such as
those produced by fast neutrons. These detectors may have sensitivity to neutron kinetic energies as low
as 10 keV. Halocarbons with an elevated degree of superheat can detect sparsely ionising radiations, such
as photons and electrons. Various techniques are used to record and count the bubbles forming in
superheated emulsions. The most immediate method is the visual inspection of the detectors, a process
that can be automated using video cameras and image analysis techniques. Other imaging techniques
based on optical tomography and nuclear magnetic resonance have also been successfully developed. In
addition, volumetric measurements are possible, in which case the number of bubbles is inferred from the
volume of gel that they displace into a graduated pipette. Finally, bubbles may be counted while they
form by detecting the acoustic emission accompanying their explosive expansion. The PICASSO
collaboration uses superheated emulsions of various fluorine-laden halocarbons (e.g. C4F10 and C3F8) and
the acoustic bubble registration technique in order to detect WIMP interactions.

2.2 The Advantages of the PICASSO Technique

This technique has many attractive features. First, the SD WIMP cross section with 19F is higher than for
any other nucleus [22, 23], meaning that a smaller amount of target material is required for a given
sensitivity. Second, the detectors can be made relatively insensitive to most background radiation. In
principle, radioactive contamination of detector materials is one of the biggest problems that this type of
experiment needs to overcome, since the decay products (α,β,γ, recoiling decay nuclei) can mimic the
signal. The superheated emulsion technique has the advantage that, with the proper operating pressure and
temperature, the detector is insensitive to β,γ and minimally ionizing particles. Third, the detector should
be relatively inexpensive to manufacture and purify (~50,000 USD/ton active material.) This should be
compared with the large costs for the other leading detection techniques, such as those based on purified
NaI and Ge. Fourth, the detector can be operated at room temperature. Fifth, complementary event
detection can be achieved with the addition of liquid scintillator to the droplet mixture. Sixth, the IUSB
group is exploring doping a fraction of the target molecules with Pb nuclei from Roman Lead samples (in
which the 210Pb has decayed.) Simple calculations show that this additive can make the detector a
competitor in the SI sector as well.
2.3 Past and Current WIMP limits measured by PICASSO.
PICASSO’s first published results [24], using data taken with sixteen 8 ml gel filled test tubes (and only 1
g of active mass), located in a basement room in the Université de Montréal (15 m water equivalent of
shielding), set limits that were competitive with limits set by other larger experiments (Figure 1, the curve
labeled “PICASSO 2000”.) Since then there has been much progress.
The experiment has been taking data, since fall 2002, in space allocated to it by SNO, which is a class
1000 clean room solar neutrino experiment housed in the 6800 foot level (6010 meters water equivalent)
of INCO’s Creighton Mine, near Sudbury, Ontario, Canada. There are six 1 liter detectors, each with an
active mass of about 7 g, with a level of contamination of about 10-11 gU/g(gel) and 10-12 gTh/g(gel),
which is 10 times cleaner than in the previously published data. To achieve this level of purity, some of
the SNO water purification techniques were used to clean the salt (CsCl), which is used to adjust the
density of the gel to equal that of the liquid Freon droplets. The preliminary results, shown in Figure 1
(labeled “PICASSO prelim”), are consistent with what would be expected from the measured level of
Uranium-chain and Thorium-chain contaminations. These results will soon be submitted for publication
in Physics Letters. Two instrumentation articles are also being prepared for submission to Nucl. Inst. &
Meth.

4
3 History, Funding and Management of the PICASSO group.
3.1 History
The PICASSO experiment was founded by Professors V. Zacek and L. Lessard, at the Université de
Montréal , in 1996. The group has been funded by NSERC, Canada’s National Science and Engineering
Research Council, since 1998. In 2000, PICASSO published WIMP limits, using data from a 1 g detector,
which were comparable with other state of the art detectors. The confidence in the progress of this group
led to their getting a share of a Université de Montréal 3 million CAD detector development grant. The
group has grown to include 5 members of the Montreal faculty. In 2002, Anthony Noble, a faculty
member from the department of physics of Queen’s University, in Kingston, Ontario (who is the leader of
the water purification program of SNO), joined the experiment. In 2003, two faculty members at Indiana
University South Bend and one faculty member from the University of Pisa joined the collaboration. In
2004, a world leader in superheated emulsion detectors, Francesco d’Errico (Yale University Medical
School), accepted an invitation to join the experiment.
The detector size, cosmogenic background environment, radiopurity, detection efficiency and all
systematic uncertainties have been improved upon, and the group is preparing to publish data taken with a
40 gram detector running since 2002 in the SNO lab. The detector systematics are all low enough and the
experimental techniques are robust enough that NSERC has funded a 1 kg detector for installation in the
SNO lab in March, 2005. The 1 kg detector will be the most sensitive experiment in the world in the
spin dependent sector. Using conservative projections, future instances of the detector are
anticipated to increase in sensitivity by about a factor of 10 every year for the next 3 years.

3.2 Management
Major group decisions are made by consensus whenever possible. If consensus cannot be reached,
decisions are made by a vote of members of the collaboration. Routine decisions are made by the
management board of the collaboration. The board will consist of the collaboration scientific
spokesperson, the project director, a spokesperson from each country funding the experiment, a
representative from each member institution, and two representatives of members of the collaboration
who are not yet in permanent or tenure track positions.

3.3 Funding of the Canadian groups

Two institutions in Canada are currently funded by the NSERC to conduct the PICASSO experiment.
Since 2001, annual funding has been stable at 240,000 CAD. Their current funding cycle ends in April
2007. In addition, PICASSO has a portion of a major detector grant to the Université de Montréal
amounting to 370,000 CAD for detectors and infrastructure (including a clean room for detector
manufacture) and a 50,000 CAD/y supplement in funding for salaries. Queen’s university has annual
funding of 100,000 CAD for PICASSO. So, current annual funding in Canada is 390,000 CAD/y plus a
one time additional grant of 370,000 CAD. It is anticipated that the successful completion of the 1 kg
experiment will lead to doubled annual funding for both groups, plus a major detector single time award
of ~500,000 CAD.
4 Future of the PICASSO experiment.
The goal at each stage of the experiment is to improve all of the critical parameters, so that sensitivity
increases by an order of magnitude. The next stage (scheduled for March, 2005) in the experiment will be
to produce a 1 kg active material detector with a similar technique to that used to produce the 40 g
detector. The main improvement will be an increase in the total target mass. This detector will have a
sufficient target mass and radiopurity to completely explore the allowed region of the DAMA [14]
experiment (in the spin-dependent sector) with 6 months of exposure. This will be a useful milestone for
PICASSO’s technical development. As a side remark, we note that the detector, in addition to being
larger in size, will use preamplifiers designed by IUSB, and ultrasonic transducers also designed and
manufactured at IUSB.

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The following stage, scheduled for mid- 2006, is a 3 kg active mass detector using 30 liter containers, a
new uniform droplet size injection technique, with a dead layer near the container walls, a loading of
about 2% active material, an improvement in radiopurity (10-13gU/g gel and 10-12gTh/g gel) using a new
gel developed at BTI which does not require CsCl (the main source of radiocontamination) for density
balancing, and submergible ultrasonic sensors (to maintain high signal efficiency in the large containers.)
With a six month exposure, SD cross section limits as low as 4*10-3pb (Phase 2) will be achieved. An
upgrade from 4 of these containers to 12 containers, with a total active mass of 10 kg is scheduled for mid,
2007, and this detector would achieve a sensitivity of about 2*10-3 pb, with a six month exposure.
IUSB will be responsible for development of acoustic sensors (including both externally mounted sensors,
such as the ones for the 1 kg detector, and sensors for a future large detector, where signal attenuation
requires mounting sensors in situ.) and their associated electronics, a noise monitoring system, 3
dimensional event reconstruction algorithms, radon emanation studies of wetted materials, and, in
collaboration with Yale, both bubble formation characterization (to develop noise/bubble separation
criteria), and the development of a heavy metal doping technique which may make PICASSO competitive
in the coherent sector as well. In addition to the collaborative work with IUSB, Yale will be in charge of
extending its current models of the radiation physics of superheated emulsions in order to optimize the
operating conditions required for the detection of WIMPS.
5. Accomplishments of IUSB and Yale.
5.1 Electronics and Sensors
IUSB has made contributions to the collaboration using the PI’s
startup funds and with the generous support of the IUSB R&D
committee. IUSB began actively participating in the PICASSO
experiment in May, 2003. The first project was to build a low cost
bubble detection system consisting of two commercial
piezoelectric sensors, home-built preamplifiers, a two input
oscilloscope emulation card on loan from the Université de
Montréal, and a PC for data acquisition. The sensors were attached
to a commercial superheated emulsion dosimeter, purchased from
BTI (Figure 3), in which the emulsion had been spiked with 241Am
to cause droplet-bubble transitions at a rate of ~0.1 Hz. The signal
from a typical droplet-to-bubble event is shown in Figure 4. The
wave form is a slowly damped sinusoid. The events exhibit high
frequency peaks which are not present in noise events. The
locations of these peaks, in two containers of different size, shifted
by an amount consistent with the change in radius of the containers.
We are investigating whether these features are due to repeated
reflections from the container walls.
The main accomplishment that summer was to develop a
preamplifier for reading the piezoelectric sensors with little signal
loss, a flat gain over a wide frequency range, and with no DC
voltage difference established across the sensor. Typical circuits Figure 3. Photograph of the spiked 8
found to read these devices seem to rely on the Q value for specific ml BTI neutron dosimetry tube, and an
sensors. They discard a large portion of the signal (and thus require IUSB ultrasonic transducer (covered
more gain-which leads to noise and rolloff) and establish a voltage in duct-tape).
difference across the crystal, due to bias current of the op-amp. The group developed what is believed to
be a novel circuit which solves all of these problems, and delivers a low noise signal (with little
amplification needed) and a nearly flat gain from 1,500 Hz to 2 MHz. Although the response of the
particular sensor currently being used is much more restricted than this range, the preamplifier was

6
 Figure 4: (a) Waveform of a typical bubble event observed, in a standard BTI neutron dosimetry detector spiked
with 241Am, with the IUSB preamplifier, using a gain of only 300. (b) The Fourier transform of this signal showing
peaks in high frequency region of 100 kHz. Noise events typically seem not to have this high frequency
component. The amplifier gain of this device is flat out to a frequency of 2MHz.

developed with the intention of testing a wide variety of sensors. The circuit has been submitted to the
Indiana University office of technology transfer for possible patenting. In Figure 5a the performance of
the front end of the circuit is shown. The gain is flat from 50 Hz to 5 MHz. Figure 5b shows the
performance of the entire circuit from 50 Hz to 5 MHz. The gain is roughly constant from 1,500 Hz to 2
MHz. The flat response can easily be extended in both the high frequency and low frequency bands, if
desired, with appropriate capacitor and resistor selection.
During the academic year, improvements in the circuit, including moving to surface mount production in-
house, using the latest high speed, low noise components, and implementing high-pass and low-pass
filtering led to the circuit design being adopted for use in the 1 kg PICASSO detector to be built in 2005.

During summer 2004, the group succeeded in producing ultrasonic transducers which are both more
sensitive than the commercial ones used by PICASSO, and are about a factor of 15 less expensive than
the commercial sensors. IUSB is building 200 of these sensors for the 1 kg detector.

Figure 5: (a) The front end of the IUSB circuit is meant to couple to a piezoelectric sensor and maintain the DC voltage
drop across the sensor to be zero, while allowing very low current ac signals to be amplified. This portion of the circuit
has almost constant gain from 50 Hz to 5 MHz. (b) The amplification stage of the IUSB circuit. The measured gain of
the entire circuit, including the front end, is shown for frequency range 50 Hz to 5 MHz, using a signal generator.

7
5.2 Physics of Bubble Development
Superheated emulsions were invented by Prof. R. Apfel at Yale University in the late 1970's, and
investigated and developed jointly by Apfel and d'Errico since the mid-1980's. Over almost 3 decades, the
Yale group has refined the manufacturing technology of the emulsions as well as advanced the
understanding of the physics of radiation-induced bubble formation. In particular, Dr. d'Errico has
investigated the physics of these detectors both at the theoretical level [25, 26, 27, 28] and with major
experimental campaigns at a variety of accelerator and reactor facilities worldwide (among which: INFN
Legnaro, Italy; Physikalisch-Technische Bundesanstalt and University of Munich at Garching, Germany;
Université de Louvain la Neuve, Belgium; CERN and Paul Scherrer Institute, Switzerland; The Svedberg
Laboratory Uppsala, Sweden; iThemba Labs, Cape Town, South Africa) [29, 30, 31, 32, 33, 34, 35, 36].
The general workings of superheated emulsions are well known. Charged particles generate trails of sub-
microscopic vapour cavities inside the droplets. When these cavities exceed a critical size they keep
growing until the whole droplet evaporates. On the contrary, sub-critical cavities collapse back to the
liquid phase under the action of external pressure and surface tension. The energy and the critical size that
are necessary for bubble nucleation depend on the composition and the degree of superheat of an
emulsion. General agreement exists on this qualitative description of the nucleation process, but a
universally accepted quantitative theory is still elusive. In fact, the thermal fluid dynamics problem of
radiation-induced vaporization in a metastable liquid, common to superheated emulsions and to bubble
chambers [20] is extremely complex and has not yet been solved in general form.
In the absence of a detailed theory, semi-empirical models of the detection process have been developed
based on the thermodynamics of the isothermal spontaneous nucleation modified according to Seitz's
"thermal spike" theory [37]. The latter suggests that when a charged particle slows down crossing a liquid
its kinetic energy is transferred as heat, creating trails of vapour cavities. In this theory, it is further
assumed that embryonic bubbles can grow indefinitely if they exceed a critical radius, Rc, derived from
the condition of mechanical equilibrium between surface tension and pressure difference through the
walls of the cavity: Rc = 2σ / (p" - p') ~ 2σ / [(ps - p')(1 - v'/v")]
where σ is surface tension, p is pressure (ps saturation value), v is specific volume, while ' and " denote
the liquid and vapour phases. The energy, Wo, required in the radiation-induced nucleation in superheated
liquids can be calculated with the following expression developed by Skripov for bubble chambers [38]:
16π σ 3
WO =
v′
[ 1 + ( p − 2p′∆)(Hv" − v′ ) − 3 Tσ ddTσ ]
3( ps − p′ )2 ( 1 − )2 s
v"
where all symbols have been previously defined, except for ∆H the latent vaporisation heat of the fluid.
This theoretical expression has been verified extensively and shown to provide accurate values of the
measured bubble formation energies [26, 27]. In the formula, the first factor represents the work WG , or
Gibb's free energy [39] required for the isothermal spontaneous nucleation of a critical size bubble in
equilibrium with its surroundings, a process called homogeneous nucleation. WG amounts to the
difference between the surface free energy of the bubble and the work done in the expansion against the
pressure of the liquid, this difference is maximum for a radius Rc. The second, non-dimensional factor in
square brackets contains positive terms expressing the additional work required when the liquid is not
superheated enough to undergo homogeneous nucleation, and the vaporisation is heterogeneously
initiated by an ionising particle. The semiempirical assumptions underlying this factor are that the energy
is available in the form of heat and that the evaporation process is initially adiabatic, which is reflected in
the term containing dσ /dT.
Wo is over an order of magnitude higher than WG and increases further when we take into account the
irreversible energy losses occurring during the formation of the bubble. The ratio η = WG /Wo, typically ~
1/20 [40, 41], is an indication of the efficiency of the actual nucleation process as compared to the

8
reversible isothermal process of spontaneous nucleation of a critical bubble. Most of the energy is spent in
latent vaporisation heat, heat conduction, work against viscous forces and other irreversible terms
(including the emission of acoustic waves), so that only a relatively small fraction remains inside the
bubble during this process, which is consistent with the low values of η.
A unified parametrization of the properties of superheated emulsions based on light halocarbons was
proposed by d'Errico [26], whereby the previously reported theory is used together with a non-
dimensional quantity called "reduced superheat" and defined as: s = (T - Tb)/(Tc - Tb)

The reduced superheat represents the normalised operating point of an emulsion within the temperature
range corresponding to the metastable superheated state. At a given pressure, the boiling point Tb is the
temperature above which a fluid becomes either a vapour or a superheated liquid. Therefore, this
temperature represents the lower limit of superheat of an emulsion. On the other hand, the critical
temperature Tc is the value above which the liquid phase can no longer exist, the fluid cannot be liquefied

Figure 6. Computed bubble nucleation energy for superheated emulsions of dichlorofluoromethane (R-12),
monochlorodifluoroethane (R-142B), and dichlorotetrafluoroethane (R-114), plotted versus temperature and
superheat (left panel) and versus reduced superheat and. reduced temperature (right panel).

by compression and is then defined as a gas. Therefore, this is the theoretical upper limit for the
superheated state, although it is never reached in practice since spontaneous vaporisation starts occurring
at lower temperatures.
Total bubble formation energies W0 (Figure 6) and critical radii, Rc, have been computed for different
halocarbons for which a consistent set of thermodynamic parameters is available [42]. When results are
plotted versus reduced superheat, all data fall on a single curve, showing in part an exponential trend. On
the contrary, data are scattered if plotted against conventional thermodynamic parameters such as
superheat ∆T = T - Tb , or reduced temperature θ = T/Tc. The vaporisation curve allows us to predict the
radiation response threshold of the emulsions using a single parameter.
The reduced superheat concept has greatly enhanced our ability to design superheated emulsions with
specific response properties. In fact, based on the reduced superheat we can predict the fast neutron
detection thresholds of a given emulsion, its sensitisation to thermal neutrons, sensitisation to photons, as
well as its ultimate thermodynamic instability. However, as was mentioned above, the definition of
reduced superheat is a theoretical one, based on the use of the critical temperature Tc as the upper limit of
superheat for an emulsion. This definition is consistent with the theoretical computation of the minimum
vaporization energy W0. However, in practice a superheated liquid can only be raised up to a maximum
temperature, called superheat limit Tl , which is lower than the critical temperature. In the PICASSO
project, it is necessary to push the operating conditions of the superheated emulsions to the lower limits of

9
detection of WIMPs without trespassing into the detection of minimally ionizing radiations, such as
photons and electrons. For this purpose, it is proposed to investigate the opportunity of analyzing and
designing the emulsions based on the use of an "effective reduced superheat" seff = (T - Tb)/(Tl - Tb). The
degree of superheat of an emulsion depends both on its operating temperature and on its pressure. In
particular, the pressure exerted on the emulsion affects both its boiling temperature Tb and its superheat
limit Tl. Therefore, an investigation of the concept of effective reduced superheat should lead us not only
to a better determination of the response properties of the detectors but also to a better control of these
properties by modulating the pressure exerted on them.

5.3 Pb doping
The IUSB group has studied techniques for incorporating lead atoms into fluorocarbon molecules. Pb
nuclei, are a very attractive target to search for coherent interactions, since the cross section scales as the
number of nucleons squared. WIMP–Pb interactions which occurred in the liquid droplet would cause the
same explosive phase transition described above.

The problem is to detect the interaction and to eliminate radioactive background present in samples of
lead, due to the troublesome isotope 210Pb which has a 22 year half-life. If ancient lead, smelted by the
Romans 2000 years ago, were used, then most of the 210Pb would be removed. In fact, ancient lead
samples owned by INFN in Milan, Italy, have been found to have activities of less than < 4 mBq/kg [43].

The group is studying whether the Pb can be incorporated into a fraction of the Freon-like targets which is
small enough to not change the thermal properties of the liquid, but large enough to make a detector of
manageable size. There is good reason to believe that lead can be successfully incorporated into the target
fluids used by PICASSO. Organometallic compounds, those compounds in which an organic carbon
group is directly bound to a metal center [44], are well studied and often made on industrial scales. A
particularly well-known example is tetraethyl lead, the rather infamous anti-knock additive used in
gasoline. While the industrial scale synthesis of tetraethyl lead typically involved the reaction of a lead
sodium alloy with ethyl bromide or in an electrolytic process involving lead and organomagnesium
(Gringard) [45] reagents, there are a variety of laboratory scale synthetic pathways available [46].
Typically, these involve the reaction of an active metal based ethylating agent with a lead salt to form the
desired product (Rxn. 1).

4(C2H5)nMXm + PbX4 ==> nPb(C2H5)4 + 4MX(n+m) Rxn. 1

where M = Li, Mg, or Cd; X = Cl, Br, or I; n = 1, 2; and m = 0, 1, 2.

In a similar fashion, the synthesis of a series of perfluoroalkyl lead compounds is proposed. These new
perfluoralkyl lead complexes are expected to be completely compatible and soluble in the fluorocarbon
solvent used in the superheated droplet detectors and are not expected to change the thermal properties of
the fluid in a low enough concentration (order 1%)

Compounds that contain only perfluoroalkyl groups bound to a lead center have not yet been synthesized,
although the mixed perfluoroalkyl, alkyl lead compounds, such as (CH3)3PbCF3 and (CH3)3PbC2H5, are
known [47]. In fact, a review of fluorocarbon derivatives of metals states that “now that such reagents as
n-C3H7Li, C6F5Li, and CF2:CFMgBr have been obtained there seems no reason why a variety of
fluorocarbon-lead compounds cannot be prepared...” [48]. The proposed synthetic scheme will involve
the synthesis of active-metal perfluoronated derivatives (particularly those of Lithium and Cadmium) and
reaction of these with an appropriate lead salt (halide or acetate) to produce the desired perfluoronated
lead comound (Rxn. 2).

10
4M(RF)n + nPbX4 ==> nPb(RF)4 + 4MIn Rxn. 2

where RF is the perfluoroalkyl group (e.g. CF3, C2F5, C3F7); X = halide or acetate; and M = Li, n = 1 or M
= Cd, n = 3.

The synthetic route using the Cd-perfluoroalkylating agent is seen as a likely successful, high yield route
to the target lead compounds; the synthesis of analogous perfluoronated bismuth compounds has been
reported using Cd reagents [49]. In fact, a relatively large number of perfluoronated cadmium reagents are
available [50]. The availability of the perfluoroalkyl derivatives of cadmium, as well as those available
for lithium [51], bodes well for the successful synthesis of the perfluoronated lead compounds. Indeed,
preliminary results obtained in our laboratory, based on IR spectral comparisons to reported
perfluoronated metal complexes [49, 50, 52], indicate that the perfluorobutyl lead compound, Pb(n-C4F9)4,
can be synthesized by both the lithium and cadmium intermediate route, while the route using magnesium
(Gringard) reagents proved unsuccessful.

Once the target lead compounds are synthesized and characterized, an important aspect of the project will
be the purification of the products and the measurement of the thermal properties of the
fluorocarbon/perflouroalkyl lead solutions. It is expected that the shorter perfluoroalkyl chain compounds,
Pb(CF3)4 and Pb(C2F5)4, will be liquids and that the longer derivatives, e.g. Pb(C3F7)4 and Pb(C4F9)4, will
be liquids or volatile solids. Therefore, products will primarily be purified by distillation or sublimation.
As noted, the perfluoronated lead compounds are expected to be very soluble in the fluorocarbon droplets
of the detectors. In order to determine the thermal properties of the solutions, both the boiling point and
the vapor pressure of the solutions will be measured for a variety of perfluoroalkyl lead concentrations.
These measurements will provide data for the optimum operating conditions of the superheated droplet
detectors containing lead nuclei.

6: Personnel at IUSB.
In addition to the PI and Co-PI, the group will typically employ four IUSB students. An undergraduate
chemistry major will work with the Co-PI. Ms. Cynthia Muthusi, has worked with the Co-PI for the last
two summers and has produced a scientific and technical report for the collaboration on the unsuccessful
attempts to synthesize the lead compound using magnesium reagents, as well as the apparently successful
initial attempts to use the lithium and cadmium routes. She will likely continue her collaboration for the
next two years. A senior physics student will work with the PI and assist in guiding the less experienced
students. Ed Behnke was an undergraduate student who completed his BS, with a thesis on the
preamplifier designed for the experiment. He presented his work at an undergraduate research conference,
as well as at an international conference on droplet detectors. He also worked with the PI in obtaining a
provisional patent for this device. Mr. Behnke has enrolled in the applied mathematics and computer
science MSc. program at IUSB (there is no MSc degree in the physics department.) He will be writing a
thesis for this degree on acoustics work done with the PICASSO group. The physics group will also
employ two less experienced students, one of whom will be an education major.
7: An outline of a 3.5 Year plan:

Short term: Next 6 Months.(to be complete by March, 2005)

The main focus of the physics group at IUSB in the next six months will be on the production, testing and
characterization of ultrasonic transducers for the 1 kg detector. Ed Behnke and the PI are training two
undergraduate physics students in the techniques of production of transducers and the techniques used to
produce surface mount circuits.

The main focus of the Yale group will be preparing the investigations of the "effective reduced superheat",
seff = (T - Tb)/(Tl - Tb), by performing an extensive literature search for the published limits of superheats

11
of metastable liquids and for other thermodynamic parameters required in the computations planned for
this project.

Year 1 of grant (April 2005-March 2006)

Acoustics: The physics group at IUSB will assemble a VME based acoustics data acquisition system in,
identical to the type used in the underground experiment, capable of handling 20 separate inputs. This
change will be both much more cost effective than simply multiplying the current two input system, based
on commercial oscilloscope emulators, and will allow a more direct comparison with data coming from
the PICASSO detector. This system will first be used to take data from a 4.5 liter PICASSO unit identical
to the units in the 1kg detector, with the one difference being that a spike of 241Am will be added to the
active fluid in a well defined region in the detector to allow studies of resolution of 3-dimensional event
reconstruction and overall detection efficiency of the 1kg units in the experiment. The detector will also
be used in testing designs of transducers (bandwidth for bubble events, overall sensitivities, angular
sensitivities, etc.) for making noise measurements, systematics studies on event selection criteria. Studies
of the required sensor density for larger detectors will be initiated. Studies of a multiple device sensor
system will also be made (that is, the ideal sensor system may be composed of a few types of microphone,
each with response in a different frequency range.)

Radon emanation: A radon emanation chamber, cryogenic radon concentration device, and a
photomultiplier-based counting system will be assembled and calibrated. The system will be based on a
cryogenic radon collector which was optimized by Dr. Levine for SNO. Dr. Levine was responsible for
the protection of the SNO detector from radon in laboratory air (222Rn concentration in laboratory air is
about 106 times higher than the target level for the fiducial volume of the SNO detector.), developing
methods to measure the efficacy of these efforts, and was the corresponding author of a paper on the
method for radon measurement in the SNO detector [53]. A sensitivity level of ~0.1 222Rn atoms per liter
of gas (STP) was achieved. The limit on sensitivity was set by the cryogenic trap size and by the volume
of CO2 which was collected in the trap. Both of these will be addressed in the system at IUSB, and the
sensitivity of this system should improve. The system will be used first for measuring the emanation rate
and radon diffusion rate for prospective components of the PICASSO detector. When possible, the group
will offer to make measurements for other low background experiments.

Detector physics: A series of detectors will be manufactured in Dr. d'Errico's laboratory at Yale using the
light halocarbons listed below.

Chemical name Chemical Refrigerant Empirical Boiling point Critical point

abstracts nr number formula Tb (°C)* Tc (°C)
1,2-dichlorotetrafluoroethane 76-14-2 R-114 C2Cl2F4 3.65 145.7
Octafluorocyclobutane 115-25-3 C-318 C4 F 8 –6.99 115.22
Dichlorofluoromethane 75-71-8 R-12 CCl2F2 –29.76 111.8
1,1,1,2-tetrafluoroethane 811-97-2 R-134a C2H2F4 –26.07 101.2
Hexafluoropropylene (HFP) 116-15-4 — C3 F 6 –29.40 85.0
Monochloropentafluoroethane 76-15-3 R-115 C2CIF5 –39.17 79.9
Decafluorobutane 355-25-9 R-31-10 C4F10 -3.00 112.20
Octafluoropropane 76-19-7 R-218 C3F8 -37.75 70.90
* at atmospheric pressure (101 kPa)

12
The detectors will be 12 ml vials containing about 50,000 halocarbon droplets of 100 µm diameter,
suspended in a tissue-equivalent gel matrix. The emulsifier gels used in the detectors are immiscible and
inert, so that droplets neither dissolve nor loose their properties through chemical reactions. A suitable
elasticity of the matrix is also necessary in order to prevent the radiation-induced "explosive" bubble
formation from triggering the boiling of adjacent drops. These gels will be examined at IUSB in terms of
their radiopurity, according to the methods described above. An additional series of detectors will be
manufactured using an emulsifier gel spiked with 241Am.

Instrumentation will be set up in order to determine the detectors' response to different radiations as a
function of operating temperature and pressure. The formation of bubbles in the detectors will be recorded
in real time by means of piezo-electric transducers picking up the acoustical pulses which are emitted
when drops suddenly vaporize. Temperature controllers will be put together to stabilize the vials within ±
0.5 °C of set points in the range 20-60 °C, using thin heating foils and neoprene foam insulators. The
heaters will be operated by controllers of the proportional-integral-derivative type and will be monitored
by platinum resistance temperature sensors (Pt100). Regulated compressed air will be used to pressurize
the detectors up to 200 kPa, whereas a vacuum pump will be used to reduce the pressure down to ~20 kPa.
The operating pressure will be monitored using a high-precision piezoresistive transducer and a
membrane isolator will be inserted between the pressurization/depressurization devices and the detectors
to prevent diffusion of air into the emulsions.

Pb-doping: The majority of the work in the first year will be the synthesis, characterization, and
purification of perfluoroalkyl lead complexes. The synthesis is not trivial: both the lithium and cadmium
reagents must be synthesized initially, and then the lead compounds can be produced. The starting metal
salts and perflouroalkyl iodides are commercially available. While the final lead product is expected to be
quite stable and unreactive toward air and moisture, the lithium and cadmium intermediates are both air
and moisture sensitive. Products will be purified by distillation or sublimation, where appropriate. The
characterization of new products will primarily be made using IR and NMR spectroscopy, with purified
products sent out for commercially available elemental and/or mass spectral analysis.

Year 2 of grant (April 2006 – March 2007)

The PI and Ed Behnke will begin serving PICASSO detector shifts at the SNO site.
IUSB and Yale will begin to jointly conduct an independent anaylsis of the PICASSO data.

Acoustics: The machining and filling of a 30 liter module identical in construction to the units to be used
in the 3 kg and 10 kg detectors will be complete. In this detector, the improved loading techniques being
developed at BTI will be employed to deposit droplets which will be of a much more uniform size than in
the current detectors, and a new placement technique which will allow this spiked region to be confined to
an order 1cc volume. This will allow for more precise measurement of event location uncertainties. This
will be used to create fiducial volume cuts on the data to eliminate events originating from microscopic
defects on the detector walls, and will help to find possible radiocontaminated “hot spots” within the
detector. In situ tests of the system of submergible and external sensors will be conducted. Assuming that
radio-contamination is held to the target of 10-14 gU/g(gel), and that the WIMPS reside in the grey region
of parameter space in Figure 1, the true event rates will be below 0.1 events/kg/d, and the elimination of
radio-background events by rejection of “hot spots” will be essential to successful measurements.
An instrumentation paper on the above acoustic properties will be written by IUSB and Yale.

Radon emanation: Assays of materials used for transducers mounted inside the 30 liter containers. Other
PICASSO material measurements as required by the group. An instrumental paper on radiopurity
measurements of wetted materials will be written by the IUSB and Queen’s University teams this year.

13
Detector physics: Experiments will be performed with gamma rays from 241Am and 137Cs sources (~60
keV and 662 keV, respectively) and with 5.5 MeV alpha particles, in the case of Am-241 spiked detectors.
Additional experiments will also be conducted using 252Cf and Am-Be neutron sources. The experiments
with alpha particles provide the best defined energy deposition pattern. Experiments with photons, which
initially trigger bubble vaporisation via secondary electrons at their peak ionisation density, are required
for the optimization of the operating parameters of the PICASSO detectors. Experiments with neutron
sources are proposed since a wealth of data on the temperature-dependent responses is available, whereas
the complementary pressure-dependent response data are scarce.
In order to analyze our data in terms of the "effective
reduced superheat", seff = (T - Tb)/(Tl - Tb), knowledge of
the limit of superheat Tl of the emulsions will be required
as a function of temperature and pressure. The approach
that we will follow to determine Tl for our liquids is based
on the mechanical stability condition of classical
thermodynamics, summarized hereafter. The superheated
liquid states are found in the region of the P-V isotherm
situated between the saturated liquid and the minimum in
the van der Waals “loop.” The locus of all the maxima and
all the minima in the fluid isotherms is the spinodal, which
separates the metastable and unstable fluid states. The
condition (∂P/∂V)T = 0 is satisfied along the entire length
of the spinodal which has two branches. The locus of the
minima of all the isotherms, along which (∂2P/∂2V)T > 0,
provides the upper bound to the limit of superheat for the
liquid as a function of ambient pressure. Skripov and
Ermakov [54] observed that if the experimental limits of
superheat, Tl vs. P, are plotted on reduced scales (i.e., θ1 =
T1/Tc is plotted against π = P/Pc, where Tc and Pc are the Figure 7. Stability diagram for a fluid.
critical temperature and pressure) then all data are nearly
superimposed. Eberhart and Schnyders [55] reported that a two-parameter equation of state with n = 1/2
can provide a spinodal curve which represents these data reasonably well:

[P+ a
T nV 2
](V − b ) = RT (1)
where V is the molar volume, R is the gas constant, and a and b are constants. If the conditions (∂P/∂V)T =
0 and (∂2P/∂2V)T = 0 are applied at the critical point then Equation 1 can be put in the reduced form:
[ π + 3 ]( φ − 1 ) = 8 θ
θ nφ 2 3 3
(2)

where all symbols have been defined except for φ = V/Vc , the reduced volume. Everywhere along the
spinodal (∂π/∂φ)θ = 0, and applying this condition to Equation 2, we find:
θ1n+1 = (3 φ - 1)2 / 4φ3 (3)
The spinodal (θ1 and its respective π) will be calculated parametrically by assuming a series of values for
φ, calculating θ1 from Equation 3, and then calculating the associated value of π from Equation 2. Prior
knowledge of the Tc for our emulsions will allow us to derive Tl from θ1 and thus compute the "effective
reduced superheat", seff = (T - Tb)/(Tl - Tb). Finally, a comparative analysis of our results will be
performed in terms of "effective reduced superheat" as well as in terms of the "theoretical reduced
superheat", s = (T - Tb)/(Tc - Tb).

14
Pb-doping: After the lead compounds have been successfully synthesized and purified, the boiling points
and vapor pressures of solutions of the lead compounds in the fluorocarbon solvent will be determined.
Using in-house equipment, the boiling points of these solutions can be measured to ± 0.1 oC and the vapor
pressures can be measured to an uncertainty of < 1 mmHg. These data will allow for the selection of the
best perfluoroalkyl lead compound to use in the detectors.

Temperature, pressure, and volume measurements of the perfluoroalkyl lead/fluorocarbon mixtures at

different loadings of perfluoralkyl lead will allow for the estimation of the critical parameters (Tc, Pc, Vc)
by, for example, fitting to a Van der Waals equation of state [56]. This data will then be used to determine
the mixtures to be tested experimentally for performance in the detectors.

Year 3 of grant (April 2007- March 2008)

General: IUSB and Yale personnel will continue to share experimental shift duty with the collaboration
and conduct an independent data analysis. The detector physics investigations will be completed and
results fully analyzed. Based on these findings, optimized temperature (and pressure) operating conditions
for the PICASSO instrumentation will be implemented.

Pb-doping: Based on the results of the synthetic reactions and the testing in solution, it will be necessary
to “scale-up” the production of at least one of the perfluoroalkyl lead complexes so that it can be tested in
actual detectors. If lead is still considered an attractive additive, a small amount of Roman lead would be
purchased or borrowed from INFN for chemical processing and radio-assay testing, Pb would be
incorporated into the Monte Carlo in detailed way.

Instrumental papers on the acoustic properties and radiopurity measurements of the 30 liter detectors
would be written this year.

8 Conclusions:
In summary, the PICASSO technique offers the special advantages of high WIMP-target cross section,
intrinsic discrimination of most radioactive background, room temperature operation, and low purification
costs. PICASSO promises to be a leading experiment in the search for spin-dependent interacting WIMPs,
and may become a contender in the spin-independent search as well. This project represents an excellent
opportunity for IUSB and Yale to collaborate and participate in an exciting research with a high
likelihood of success. The students and faculty at IUSB eagerly look forward to doing the kind of science
not usually possible at an undergraduate institution. The contributions that IUSB and Yale are able to
make to the experiment are likewise eagerly sought after by our Canadian colleagues. We also look
forward to continuing our fruitful contacts and exchanges with other US scientists, such as Juan Collar at
the University of Chicago, developing the superheated emulsion technique for dark matter studies and
other fields, such as high energy experiments and Homeland security.

15
References: RUI: A Search for WIMP Dark Matter with Superheated Emulsions

1 Connecting Quarks With the Cosmos: Eleven Science Questions for the New Century, committee on
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2 F. Zwicky, “ On the Masses of Nebulae and of Clusters of Nebulae” Helv. Phys. Acta 6, 110, F.
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4 Lewis, Aaron D.; Buote, David A.; Stocke, John T. “Chandra Observations of A2029: The Dark
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13 V. A. Bednyakov, “Aspects of spin-dependent dark matter search” hep-ph/0310041. The red hashed
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Wichoski, V. Zacek, Université de Montréal, Montreal, QB, Canada., A.J. Noble, Queens University,
Kingston, ON, Canada., E. Behnke, W. Feighery, I. Levine, and C. Muthusi, Indiana University
South Bend, IN, USA. S. Shore, University of Pisa, Pisa, Italy. F. d’Errico, Yale University School of
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22 J. Ellis, R. Flores, “Elastic Supersymmetric relic-nucleus scattering revisited” Phys. Lett. B 263 (1991)
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45 There have been numerous articles written about the history of tetraethyl lead, its discovery, and its
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49 “The Preparation and Properties of tris(perfluoroorgano)bismuth compounds Bi(Rf)3 (Rf = CF3,

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Group 2B Compounds: Bis(trifluoromethyl)cadmium·Base. New, More Powerful Ligand-Exchange
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51 Preparation and Reactions of Perfluoroalkyllithiums”, Pierce, O.R., McBee, E.T., and Judd, G.F.,
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52 “Vibrational spectra and structures of fluoroalkyl and fluoraryl compounds of tellurium: Te2(CF3)2,
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54 V.P. Skripov and G.V. Ermakov. “Pressure dependence of the limiting superheating of a liquid” Russ.
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