- Tests of the Weak Interaction and the Neutron Lifetime. The cold
neutron guide hall at the NIST Center for Neutron Research (NCNR) provides a
unique opportunity for the U.S. to compete for a leading role in research on
the physics of fundamental particles. High precision measurements at very low
neutron energies complement high-energy research at national and international
particle accelerator laboratories. Measurement techniques developed for this
research improve NIST's ability to provide measurement services and
calibrations. The Neutron Interactions and Dosimetry Group pursues a research
program of its own, as well as supporting a national user facility for
industrial and university researchers.
Two different neutron lifetime experiments, one a Harvard-led ultra cold neutron
(UCN) experiment, the other a NIST-led cold neutron beam experiment, are
currently able to take data on our polychromatic neutron beam at the NCNR.
Complete three-dimensional magnetic trapping of ultracold neutrons was
demonstrated by the Harvard/NIST collaboration for the first time, as reported
in the journal Nature in January 2000. Trapping of neutral and charged
particles is an invaluable tool for the study of both composite and elementary
particles. The main advantages of trapping are long interaction times and
isolation from perturbing environments. In the present work, inelastic
scattering in superfluid 4He is used to load neutrons into the trap,
and the helium also acts as a scintillator for detection of neutron decay. The
work described in the Nature article verified the theoretical predictions
of the loading process and the technique of magnetic trapping of neutrons.
During CY00 major upgrades to the
apparatus were installed including a larger trapping magnet and a monochromator
to prefilter the incident beam. These improvements should result in a precise
measurement of the beta-decay lifetime of the neutron sometime in CY01CY01.
The NIST-led lifetime experiment utilizes a Penning trap for decay protons and
a thin 6Li neutron fluence monitor to measure the lifetime of free
neutrons in a 30 K thermal neutron beam. During CY00 final data taking
runs of the experiment were completed. A major source of uncertainty in this
experiment comes from measurement of the neutron fluence. In the past the
neutron monitor calibration factor was calculated from a cold neutron capture
cross section, the areal density of the 6Li deposit through which
the neutrons pass, and the measured solid angle of the detector. Now in
collaboration with Indiana University, an independent calibration of the
neutron fluence monitor is being achieved by use of a totally absorbing
cryogenic calorimeter. Several absorbing targets are being intercompared: LiPb,
LiMg, and liquid 3He. The LiMg target results have verified the thin
6Li monitor results within about 0.4 %, as reported in a recent
Ph.D. thesis. When completed in early CY01, this work is expected to reduce the
uncertainty in the neutron fluence by at least a factor of two.
Preliminary work has begun on a NIST-led experiment to measure the
electron-antineutrino correlation in neutron beta decay using a novel asymmetry
technique that does not rely on precise proton spectroscopy. This correlation
coefficient was last measured in 1978 and has a 5 % uncertainty (by
comparison the other better known correlation coefficients are known to slightly
better than 1 %). This experiment requires an electron spectrometer with a
high degree of backscatter suppression to minimize the low-energy tail in the
response function. During CY00 a prototype electron spectrometer consisting of
a conical array of plastic scintillator detectors coupled to photomultipliers
was designed and constructed, and testing was begun on our 4 MeV electron
Van de Graaf.
In CY00 the large collaborations responsible for two previous experiments on
our polychromatic beam continued major drives to upgrade those experiments in
preparation for further running on our beam. Both projects, a search for
time-reversal symmetry violating correlations in neutron decay and a search for
parity violating spin rotation of neutrons in bulk media, are expecting to be
ready for beam time sometime in late CY01. These projects have produced three
recent Ph.D. theses and have already made modest improvements on the best
preceding results. The results of the time-reversal asymmetry experiment were
recently published in Phys. Rev. C.
Throughout the year our group explored promising new ideas for experiments that
probe the weak interactions with scientists from Los Alamos National Laboratory
(LANL). The most promising ideas would lead to participation in a LANL-led
measurement of the parity-violating gamma-ray asymmetry in the
"npdγ" reaction (polarized
neutron plus proton goes to deuteron plus gamma-ray) at the spallation neutron
source at LANL, and to participation in a LANL-led measurement of the electric
dipole moment of the neutron using UCN. (M.S. Dewey, J. Nico,
P. Huffman, F. Wietfeldt, J. Adams, A. Thompson, with
M. Arif, T. Gentile, F. Bateman, D. Gilliam, D. Jacobson)
- Polarized 3He for Neutron Spin Filters. The primary focus
of the polarized 3He program is the development of neutron spin
filters and application of these devices to both materials science and
fundamental physics. We are developing two optical pumping methods,
spin-exchange and metastability-exchange, for producing the polarized
3He gas. In collaboration with materials scientists, we are
conducting experiments at the NCNR to demonstrate the advantages of
3He spin filters for certain materials science applications. In
addition, we are contributing to an experiment in weak interaction physics at
the Los Alamos National Laboratory, and we are collaborating with Indiana
University in applications at the Intense Pulsed Neutron Source (IPNS) at
Argonne National Laboratory.
Figure 2. Neutron Polarization Analyzer for Small Angle Neutron
Scattering (SANS) Experiments. Conventional neutron polarization analyzers
would destroy the delicate SANS signal, but the He-3 spin filter does not. This
permits differentiation of magnetic scattering effects and nuclear scattering
effects.
In May 2000, we employed polarized 3He-based neutron polarization
analysis for an experiment on the NCNR NG7 small angle
neutron scattering (SANS) instrument (Fig. 2). The goal was to separate
the magnetic and nuclear scattering obtained from a sample of the colossal
magnetoresistive (CMR) material
La0.85Sr0.15Mn03. Materials in this class are
of interest for application of polarized 3He because no other method
exists for isolation of the magnetic scattering. Data was acquired using cells
polarized by both optical pumping methods. The ferromagnetic transition of the
material at 235 K was clearly identified by depolarization of the neutron
beam by the sample. However, analysis of the scattering data has proved to be
problematic, which may due to the overwhelming structural scattering in this
sample. Hence we are planning experiments on other samples so that the method
can be demonstrated clearly in a simple case, before tackling such difficult
samples again.
Besides production of the polarized 3He gas required for spin
filters, an important issue in the application of spin filters is the
interaction with the sample and instrument environments. Relaxation of the
3He polarization in different holding field scenarios is being
studied with a diode-laser-based apparatus for metastability-exchange optical
pumping.
The 3He polarization achievable with the diaphragm compressor
apparatus has been improved using a more efficient optical pumping scheme. For
the SANS experiment the polarizations obtained from each of the optical pumping
methods were both just under 50 %, but the spin-exchange cell was the
better performer because of the extremely long relaxation time of the
spin-exchange cell (130 hours). Hence the focus of attention for the
metastable work will shift from improving the polarization to improving the
cell relaxation times by using alkali coatings.
We are also investigating spin-exchange optical pumping with spectrally
narrowed high power diode lasers. One of the reasons we typically use high
3He pressure (3.5 bar) for spin-exchange cells is to increase
the pressure-broadened absorption width to better match the broad spectrum of
high power diode lasers. Recently spectrally narrowed diode lasers have been
developed by other researchers, which might allow reduced pressures for
spin-exchange cells. In addition to relaxing the mechanical constraints on
spin-exchange cells, lower pressure cells would allow for the possibility of
extremely long cell relaxation times because of the reduced dipole-dipole
relaxation. We have recently produced a neutron-compatible cell at 1 bar
with a relaxation time of at least 400 hours, a world record to our
knowledge. Such cells would allow for quite stable polarization even in the
absence of continuous optical pumping.
NIST is collaborating with LANL in the application of 3He polarizers
to the proposed npdγ LANSCE experiment. A
recent test run at LANSCE (November 2000) utilized a NIST
"double" spin-exchange cell (i.e., separate volumes for optical
pumping and spin filtering). Indiana University recently employed a
metastability-exchange cell prepared and tested at NIST for an experiment to
demonstrate 3He-based neutron polarization analysis in polarized
neutron reflectometry. (T. Gentile, A. Thompson, and D. Rich)
- Neutron Interferometry and Optics Facility (NIOF). During the past
year at the NIOF a number of fundamental and applied physics experiments have
been started and/or completed with collaborators from the University of
Melbourne, Australia, the University of Missouri, the University of Indiana,
and the University of North Carolina: Phase Contrast Radiography,
Neutron-Deuteron Scattering Length in Gaseous Deuterium, Dynamical Diffraction
Measurement of the Neutron-Electron Scattering Length, and Visualization of
Lithium Ion Migration in Ion Conductors.
The results of an experiment to produce quantitative Phase Contrast Radiographs
of small objects were reported in the journal Nature (November 2000).
This experiment was the result of collaborative efforts between NIOF, the
University of Melbourne, and the University of Missouri. This Phase Contrast
Radiography technique is novel since it provides a way of extracting phase
information in an image without the use of an interferometer. Images taken have
shown that this technique makes small and delicate features much more prominent.
Eventually this technique will be applied to neutron phase contrast tomography
as well.
Major progress has been made in the design and construction of a highly
sensitive experimental assembly for the precision measurement of the scattering
lengths of gases in a neutron interferometer. This will lead to an upcoming
experiment that will measure the scattering length of deuterium gas. This
achievement is important since the neutron interferometer represents the only
neutron optical device capable of precisely measuring the scattering lengths of
gaseous samples. Accurate knowledge of the scattering length is important in
many theoretical models of the neutron interaction in few body problems. By
using gaseous samples, one can avoid some of the difficulties encountered in
interpreting the results of similar scattering length measurements in solid
state systems, e.g., Bragg reflection interferences.
The results of an ongoing experiment to measure the neutron-electron
interaction amplitude via the scattering length bne have been
extremely promising. This very fundamental quantity bne is
critical to the understanding of the charge structure of the neutron and of the
deuteron charge structure in atomic physics. After four decades of sustained
effort discrepancies between different experimental values and between
experiment and theory persist. Using a novel dynamical diffraction effect for a
perfect single crystal inside a neutron interferometer, we are attempting to
measure bne directly and accurately. This measurement does
not suffer from many of the systematic errors common to most of the previous
experiments.
Ongoing ATP supported
experiments to image lithium ion conduction in batteries have shown that
neutron imaging is a very effect technique to reveal the isotopic lithium
concentration in ion conductors. This research effort aims at providing new
methods for evaluating the effectiveness of future battery technologies.
Finally, after a highly successful effort to design, construct, and operate a
mobile 3-D neutron imaging station, new funding has been secured to aid in the
construction of a more permanent neutron tomography facility. The DoE Office of
Transportation Technologies Fuel Cell Program is supporting the establishment
of a fuel cell test and evaluation facility here at NIST. This station will
afford industrial researchers the tools of neutron tomography to aid the future
development of advanced fuel cell related technologies. (M. Arif,
D. Jacobson, S.A. Werner, P. Huffman, T. Gentile, and
A. Thompson)
- Neutron Dosimetry. For the first time we provided a neutron survey
instrument calibration in an Am-Be neutron field. We still have some development
work to do on this capability, before we can provide these calibrations with
uncertainties as low as those done with 252Cf sources. Nevertheless,
the customer was very pleased to get a calibration that relates directly to his
own Am-Be transfer source.
Another important development was the initiation of accelerated testing for
neutron-induced soft failures in SRAM and DRAM chips. This accelerated testing
was done both with thermal neutrons and 252Cf neutrons. In this work,
it was shown conclusively that thermal neutrons at normal environmental levels
(from cosmic rays) have begun to be a serious problem for some batches of
SRAM and DRAM chips that incorporate
borosilicate glass films in their manufacture.
The neutron source calibrations this year included one calibration for a
secondary standards laboratory and two calibrations for industrial customers.
The radiation protection dosimetry calibration customers included one DoE fuel
processing facility and four industrial customers. Special tests for two neutron
detector manufacturers were performed with thermal neutron beams at the reactor
thermal column. (J. Adams, A. Thompson, J. Nico, and
D. Gilliam)
- Neutron Cross Section Standards. The NIST Neutron Cross Section
Standards Project has played an important role in the improvement of the
neutron cross section standards through both evaluation and experimental work.
We are leading an effort that will result in a new international evaluation of
the neutron cross section standards. This has involved motivating and
coordinating new standards measurements, examining the standards database, and
pursuing the extension of the standards over a larger energy range. This work
is taking place through participation in the U.S. Cross Section Evaluation
Working Group and two international committees, the International Atomic Energy
Agency (IAEA) and the Nuclear Energy Agency Nuclear Science Committee. An IAEA
Coordinated Research Project has been formed to provide resources to allow
meetings of the contributors to this evaluation process. An objective is to
complete the evaluation in time for the major international cross section
evaluation projects to use the improved standards in forming new versions of
their libraries.
This NIST project has continued to maintain a limited experimental role in the
measurements of the standards. This role has led to a new, NIST-LANL-Ohio University
collaborative measurement of the H(n,n) angular distribution at Ohio University
at 10 MeV neutron energy. The final results of the data indicate
differences with the most recent U.S. evaluation of this angular distribution.
As a result of these differences measurements are planned at about 15 MeV
neutron energy to determine the energy dependence. This work was initiated as a
result of concerns about that evaluation expressed by European standards groups.
The H(n,n) angular distribution is one of the most important neutron cross
section standards. Also, plans are being made for a new measurement, which will
lead to an improvements in the 10B(n,α) standard at low neutron energies. This work will be done at the
new NIST monochromatic neutron beam facility on NG6. (A. Carlson and
D. Gilliam)
- Dissemination of National Standards of Radioactivity. The
Radioactivity Group disseminated the National Standards of Radioactivity mainly
through the following three activities: (1) over 650 Radioactivity
Standard Reference Materials (SRMs) were sold in 2000. (2) over 200
comparative measurements and Reports of Traceability were provided to federal
regulatory agencies, radiopharmaceutical manufacturers, commercial suppliers of
calibration sources and services, and the nuclear-power industry. Industrial
steering committees guided the work of four research associates in cooperative
testing programs. (3) over 50 calibrations of customer sources were
provided. (L.L. Lucas, J.C. Cessna and L.R. Karam)
- Calibration of 68Ge/68Ga Source for NIST Time and
Frequency Division. The radionuclide 69Ge and its
positron-emitting daughter, 68Ga, are often used as long-lived
(270 d) sources to calibrate detector systems for positrons as well as the
511 keV radiation that results from their annihilation. A NIST Physics
Laboratory Researcher in Boulder was using such a commercially available source
to calibrate his instrumentation and observed a factor of three discrepancy
between expected yields based on the activity certificate from the manufacturer
and experimental data. We performed an activity measurement on the source using
high-purity germanium gamma-ray spectrometry. The expanded uncertainty was
7.6 % and was mainly due to uncertainties in fitting the 511 keV
annihilation peak and the uncertainty in the decay data. Despite the relatively
large uncertainty, we were able to determine that the manufacturer's certified
value was not the source of discrepancy, although the manufacturer had
understated their uncertainties by a factor of about five. (B.E. Zimmerman,
L. Pibida, and L.R. Karam)
- Calibration of Pure-Beta-Emitting Intravascular Brachytherapy Sources.
Considerable work has continued on providing NIST-based activity calibrations
for manufacturers of intravascular brachytherapy sources. These sources are
intended for use in the prophylactic inhibition of restenosis following balloon
angioplasty in heart-disease patients. Their use has an ultimate potential of
possibly serving over 600,000 patients per year in the US alone, with an
economic value in excess of a billion dollars. In the past year, three sets of
nondestructive ionization-chamber-based calibrations were performed for
32P "hot-wall" angioplasty-balloon catheter sources that
are manufactured by Radiance Medical Systems Inc. (Irvine, CA). These
calibration measurements utilized previously established ionization-chamber
calibration factors that were in turn derived from destructive assays. The
results of the calibrations were used by Radiance for internal quality control
and to transfer the NIST calibrations to two other calibration laboratories,
viz., the Radiation Calibration Laboratory at the University of
Wisconsin-Madison and the Physikalisch-Technische Bundesanstalt (PTB) in
Braunschweig, Germany. Independent destructive assays of the 32P
content of balloon catheters by PTB were in agreement with the NIST to within
less than 1 %. Ionization-chamber-based calibrations were also performed
the Novoste Corp. (Norcross, GA) sources. These are stainless-steel-encapsulated,
ceramic-based 90Sr-90Y sources whose calibration factors
were also derived from earlier destructive radionuclidic assays by NIST.
(R. Collé)
- Development of Radioactivity Standards for New Brachytherapy Device for
Brain Cancer Therapy. Proxima Therapeutics is developing a new radiation
treatment technique to prevent the recurrence of aggressive brain tumors after
surgical resection. This new treatment modality involves the implantation of a
small balloon device, named the "GliaSite," in the cavity that
remains after the tumor is removed. The balloon is subsequently filled with a
solution containing radioactive 125I, marketed under the trade name
"Iotrex". The Radioactivity Group has experimentally analyzed the
response of Capintec CRC-12, CRC-35R, and Vinten 671 dose calibrators to
NIST-calibrated solutions of Iotrex. The use of new NIST data for dial settings
and correction factors significantly improves the accuracy of Iotrex assays.
Furthermore, these data constitute an important part of the documentation that
must be submitted by Proxima in order to receive FDA approval for the device.
(B.E. Zimmerman and J.T. Cessna)
- Development of Radioactivity Standard for
188W/188Re. The availability of the
188W/188Re generator has increased interest in using
188Re for a wide variety of nuclear medicine applications. The
daughter, 188Re, is milked from the generator and is currently under
investigation for radioimmunotherapy, radiation synovectomy, intravascular
brachytherapy, and as a bone palliation agent. Wires containing 188W
are currently being studied for possible applications in intravascular
brachytherapy. Because of its short (t1/2 = 17 h)
half-life, it is impractical to produce a Standard Reference Material (SRM) of
188Re to distribute to the large number of users worldwide. Rather,
by producing a standard of 188W in secular equilibrium with
188Re, users can calibrate their instrumentation for
188Re with a source that has a relatively long
(t1/2 = 69 d) half-life. Using liquid scintillation
counting, we have succeeded in calibrating solutions of 188W in
equilibrium with 188Re with an expanded uncertainty (k=2) of
0.79 %. This calibration was transferred to the NIST
"4π" γ ionization chamber to facilitate subsequent calibrations.
Calibration factors were also derived for the Capintec CRC-12 and
CRC-35R dose calibrators maintained at NIST in the standard 5 mL ampoule
geometry. (B.E. Zimmerman and J.T. Cessna)
- Resonance Ionization Mass Spectrometry. RIMS has been evaluated for
measuring 135Cs/137Cs isotopic ratios. Spectroscopic
measurements of 6s 2S1/2(F = 4) → 6p 2P3/2(F = 5)
transition frequency shifts for 135Cs and 137Cs confirmed
existing values and demonstrated that it is possible to perform such
measurements on sub-picogram samples. Optical isotopic selectivity of
~103 for both 135Cs and 137Cs against stable
133Cs was observed and, when combined with a quadrupole mass
spectrometer, overall selectivity of greater than 109 was
demonstrated. This selectivity appears to be limited by neutral particles
generated during the atomization of the samples and could possibly be improved
by using a non-axial geometry that prevents direct line-of-sight transport
between the atomization source and the ion detector region. Because of the
inherent elemental selectivity of the resonance ionization process, no
interference could be observed from barium isobars in the RIMS measurements.
Overall detection efficiency for the RIMS process was found to be
1 - 2x10-6,
limited in approximately equal parts by the efficiency of converting Cs salts
in the atomization source to neutral gaseous Cs atoms and the efficiency of
ionizing the Cs atoms entering the laser beams. Test measurements on samples
containing as much as 4x108 excess of
133Cs were performed and demonstrated detection limits of 1 - 2x108 atoms. While this
only corresponds to ~100 mBq for 137Cs, the activity equivalent
for 135Cs is ~10-3 mBq, which could not be detected
by normal decay counting methods. Further, both radioisotopes can be measured
simultaneously by the same method, and this method is independent of the
nuclear decay properties. Isotope ratios for 135Cs/137Cs
were compared using both RIMS and conventional TIMS and found to be in excellent agreement. The isotope
ratio measurements were able to precisely date a standard sample whose isotopic
composition had been accurately measured two decades previously; however,
measurements on another standard with unknown 135Cs content yielded
an anomalous ratio that illustrates problems that may arise because of the
neutron-flux dependent fission yield of 135Cs. However the
neutron-flux dependence for the fission yield of 135Cs can provide
information about the origin of the samples studied. (L. Pibida,
L.R. Karam, and J.M.R. Hutchinson)
- Status of Low-level Radiochemical Analysis in the U.S. The NIST
Radiochemistry Intercomparison Program has four years of performance evaluation
data from fifteen commercial, university, advocacy, National, and Federal
Agency laboratories across the US for 90Sr, 238U,
238Pu, 240Pu, 241Am, at 0.03 Bq to
0.3 Bq per sample in water, air-filters, soil, synthetic urine, and
synthetic feces. A systematic evaluation of the data provides a glimpse at the
status of low-level radiochemical analyses in the U.S. The relative mean
difference from the NIST massic activity values across all matrices and
radionuclides ranged from –1 % to –6 % with standard deviation of the
means from 2 % to 7 %. Although there is an improvement in laboratory
performance since the inception of NRIP, analysis of variance indicated that
the analytical methods used was a factor in the difference of measured
241Am and 90Sr values from the NIST massic activity
values, whereas the test matrix was a determining factor for 238U
analyses. Furthermore, about 90 % of traceability evaluations were
acceptable when compared to the ANSI N42.22
criteria for performance evaluations. The majority of the failures to pass the
ANSI N42.22 criteria were due to unrealistically small estimates of
measurement uncertainties. The Radioactivity Group has provided workshops to
assist the NRIP participants with estimating their measurement uncertainties.
(Z.Y. Wu, C. McMahon, Z. Lin, and K.G.W. Inn)
- NIST Radiochemistry Intercomparison Program (NRIP). The NIST
Radiochemistry Intercomparison Program NRIP marks the successful completion of
the fourth year of its measurement traceability program for low-level
environmental radioactivity measurements. Four rounds of testing (five total
matrices were offered: water, air-filters, soil, synthetic urine, and synthetic
feces) were completed. The analyte list includes 90Sr,
234U, 238U, 238Pu, 240Pu,
241Am, at 0.03 Bq to 0.3 Bq per sample. Participants in
the program include: NM State Carlsbad Environmental Monitoring and Research
Center, Evaluation Group, Martin Idaho Technologies Company, Institute of
Nuclear Energy Research (Taiwan), Los Alamos National Laboratory, EPA Air and Radiation
Environmental Laboratory, Oak Ridge National Laboratory's Bioassay Laboratory,
Oak Ridge National Laboratory's Intercomparison Studies Program, Oak Ridge
Institute for Science and Education, STL Richland Laboratory, Sandia National
Laboratory, and Westinghouse Waste Isolation Pilot Plant. The program is vital
for relating low-level radioanalytical measurements to the National Standards.
The test matrices and analytes for each fiscal year are to be determined at the
upcoming Annual Conference on Bioassay, Analytical and Environmental
Radiochemistry. Continued growth in the number of participating laboratories is
anticipated from the commercial national and international communities.
(K.G.W. Inn, C. McMahon, Z.Y. Wu, and Z. Lin)
- International Equivalence. As part of NIST's efforts in the
international arena of measurement activities, the Radioactivity Group has
prepared a listing of calibration capabilities for Appendix C (list of
calibration and measurement capabilities, or CMC's) of the Mutual Recognition
Arrangement and submitted it to our RMO. The final version of the Group's CMC's
had nearly 400 entries covering a range of dozens of nuclides, geometries
and measurement techniques and will be part of a much larger database which
will include the CMC's from National Metrology Institutes around the world.
(L.R. Karam and L.L. Lucas)