LA-UR-12-22471

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Title: Weapons radiochemistry and nuclear forensics

Author(s): Burns, Carol J.

Intended for: Lecture at DHS-sponsored Nuclear Forensics Summer School, University

of Missouri, Columbia, 7/2/12

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Weapons radiochemistry and

nuclear forensics
Carol Burns
Nuclear and Radiochemistry, Los
Alamos National Laboratory
LA-UR-12-22471
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Technical Nuclear Forensics: Recognizes three main types of

forensic “events”, but includes other subclasses:

Post-detonation
Materials

Event
Class
Non-
Emplaced Explosive Nuclear
Interdiction Explosive
Source RDD Yield
RDD

Device IND
Fissile Rad Sealed Explosive Failed
Material Material Source RDD IND

Subclass
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For some classes of events, we have real case

examples…what about for a postdetonation event?

Source – Mayer et al., Actinide Resarch Quarterly, 2007

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The genesis of weapons radiochemistry

• Some time before the Trinity event, it

was proposed that radiochemistry
could determine the yield of a device:
– Assume that the yield is solely due to
fission in plutonium
– In a sample of the debris, determine
the amount of fission products relative
to “unburned” plutonium to determine
the efficiency
While many scientists predicted that the Trinity test
– Given a known mass of fuel, the total would be a“fizzle”, Teller predicted a yield of 40 kt, and
number of “fissions” can be Fermi was taking side bets that the test would ignite the
determined atmosphere
– This can be converted into energy
release:
1012 calories = 1 kiloton (~ ¼ mole of
fissions)

Until the radiochemical data was available, the best estimate of

the yield of the device was obtained by Fermi, who dropped small
scraps of paper as the blast wave went by
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Basics of nuclear explosive devices

• A nuclear explosive device generates a large amount of

energy from a small amount of fuel.
• “Yield” to mass ratio is much greater than conventional
explosives
• Leaves behind fissile material, fission products, activation
products
• Try to create a large multiplication factor – biggest increase in
the number of neutrons (fissions) from one generation to the
next.
• The resulting energy generated causes the explosion – the
trick is to keep the device assembled long enough.
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Types of nuclear explosive devices

Gun assembled Implosion assembled

• Like “Little Boy” • Like “Fat Man”

• Simpler – not tested prior to • Trinity test
use • More challenging to
• Not suitable for some fuels generate an even implosion

• Conditions must exist (quantity, shape, isotopic composition)

to have the material exceed the critical mass
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Fusion reactions
• Fusion of two very light nuclei can also release energy
• Multiplicity is small; not self-sustaining
• Fusion can be accomplished in accelerators, or at high
temperatures and pressures (stars)
• Fusion neutrons provide a high-energy assist, or “boost”, to
the fission process (increase fission efficiency)
• More complex design; requires special materials

Staged weapon

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What might be different about weapons

materials?
• Nonfissile components kept to a minimum:
– Maximum amount of fissile isotopes
– Moderators are bad
• For fast neutrons, fission (n,f) cross sections are much
lower than for thermal neutrons
• Capture (c) cross sections are also affected, but not as
much
• Certain alloying elements may be present (aids in
fabrication)

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Weapons radiochemistry was developed during

the history of the test program
US Nuclear Tests by Calendar Year
120
100
80
60
40
20
0
1945
1948
1951
1954
1957
1960
1963
1966
1969
1972
1975
1978
1981
1984
1987
1990

Source DOE/NV-209-REV15 (2000)

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Radiochemistry quantifies device performance, and

provides validation data for codes

• Radiochemical diagnostics are time

integrated measurements
• There are three major classes of
analytes that are determined by
radiochemistry
– Actinides
– Fission Products
– Activation Products

The radiochemical interpretation of a

nuclear event from fission products relies
on the ability to determines fissions :

Ni = FYi F = Ni / Yi FPY
(fission
product
Ni = number of atoms of fission product i
yield) %
Yi = cumulative fission product yield

Ai mass of fission product

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Forensic Investigation of Debris

To perform forensic analysis on debris, using developed data interpretation
techniques to learn about the device
Debris from an explosion
RDD or
nuclear Medium of
explosive detonation?
device?

Fissile
material? Design?
Efficiency?

The big difference: we can still measure the efficiency, but we don’t know the
ingoing mass/type of fuel - now we need to get yield some other way

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Requirements:
Technical approach •Collection tools
•Yield information
•Analytical methods/facilities
•Assessment of radchem
•Modeling

Prompt Device Technical

data assessment
modeling

Event

Debris/gas Radiochemical
collection analysis

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Collections during the Trinity test

Sherman tanks were fitted

with lead compartments to
protect personnel during
sample retrieval during the
first day

The radiation field at

ground zero was 700 R/h
at t0 + 1 day.

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Collections during the Trinity test

Samples for analysis were collected from the cloud by a rocket or manned airplane

The pilot was in a shielded cockpit; plane was decontaminated and samples
were removed before the pilot emerged to reduce dose

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Testing Underground
After ratification of the Limited Test Ban Treaty, nuclear testing was conducted
underground

Underground tests were conducted at

depths of up to a mile:

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Sampling in the underground environment

“Drillback” conducted to retrieve

samples

- Over a period of 1-3 weeks

- Gamma activity used to locate

samples

- Samples retried from multiple

locations through a main hole
and a sidetrack hole

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Collections now – where and what to measure?

• Field deployed teams with equipment and
instrumentation for sampling
– Principal goal: field triage of samples

– Sample selection based on data

radiochemistry requirements

– Initial sample analyses provide preliminary,

low confidence characterizations

• We continue to develop:
– Models/tools to characterize the site
– Communications
– New tools for sampling in many
environments
– What can we tell in the field
– New signatures?

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Seismic monitoring
Old Regime -- Teleseismic

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Weapons radiochemistry in the test era

Collections consist of very

complex mixtures:
•Homogenization
•Dissolution
•Separation
Sample recovery •Assay

Not really fissions

ε=
this simple – Original atoms of fuel
other
F
corrections ε=
apply F+p
“Measure fissions” in the sample, F
If total fuel known, can calculate
Measure unburned fuel atoms, p
total fissions (FT), or energy
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Fixed laboratory analysis

Radiometric Analysis – Count Room Radiochemistry

•Gamma, beta, alpha, neutron •Standardized radiochemical

•Trace levels to >1013 fissions procedures
•Operates 24x7x365 •Refractory matrices
•Analysis codes •Segregated facilities for
handling different activity levels

Mass Spectrometry Sample Management and Quality Assurance

•Sample archives for Pu Assay in Plutonium Exchange Metal 442

Apr-01 Aug-01 Mar-03 Mar-04 May-05

•Clean laboratory environmental samples and 100

debris
99.8

•Modern Instrumentation 99.6

Pu Concentration (wt%)
•Specializing in actinide •Routine sample management 99.4

activities
99.2

isotopic analysis 99

•Years of routine •QA/QC for ongoing operational 98.8

missions
98.6

environmental and bioassay CORPEL CPC

Measurement Method
TIMS

monitoring experience •Intercomparisons with

otherlaboratories
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Fractionation
Chemical Fractionation:

- All elements initially exist within a plasma

- As the fireball cools, less volatile

(refractory) species condense first,
followed by the more volatile elements,
resulting in distortion of elemental
distribution

- Volatile fission products do not “track”

well with the debris; radiochemical
samples are selected for their refractory
character

Geometric Fractionation: Mixing may be

incomplete in the debris field
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Chemical fractionation
Chemical fractionation can occur if either precursor or final decay fission
products are volatile
While the lanthanides and most
actinides are refractory…

…The lighter rare earth

elements can come from
volatile precursors, and
appear volatile
For the mass 140 decay
chain associated with U-235
fission, most species come
from volatile precursors

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Geometric fractionation
Geometric fractionation can be determined through a “mixing analysis”, by
comparing several independent samples:

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Fission product distribution relates to energy, fuel

•Energy is generated at
different energies

•Energy distribution can

change during the event

•Other reactions occur, e.g.

neutron capture

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Assessment and modeling

Assessment Modeling

N49 = total mass of Pu

FT = Bx N49__ n49/f = fission per mass unit
n49/f B = 1/efficiency

- For a stockpile test, efficiency is characterized with

knowledge of the mass of fuel and the yield. Parameters of interest:
•Components/masses
- For an unknown event, we can essentially “go •Fission efficiency
backwards”: •Level of sophistication
With some independent estimate or measure of •Medium of detonation
yield, and efficiency provided by radiochemistry, we •Information about nuclear fuel
can determine the ingoing mass.

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Technical opportunities – forensic analysis of debris

Analysis:
Was the detonation nuclear? •Rapid/automated
separations
What was the fissile material? •New instrumental
Collections: methods
•Models/tools for site
How well did the device perform? •Fieldable analyses
characterization
•New signatures
•Communications
•Tools for sampling in What can we tell about the design?
differing environments
•New signatures What was the medium of detonation?

Modeling
•Code development
• Incorporating new nuclear data
• Modeling outputs
•Making tools more “usable”

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The ability to address these needs founded in experience and

infrastructure from enduring programs:

Our ability to
characterize nuclear Certification of
materials and materials in pit
processes relies on production
analytical methods
from:

Our ability to characterize Support for

signatures of worldwide international
nuclear materials safeguards
production relies on skills programs
built in:

Our ability to
characterize the origins Underground
of a nuclear explosion is test
based on: experience

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Strong research base advances these capabilities:

New materials characterization tools

Ground-based measuremetns Statistical models for interpretation,
confidence levels

Dispersion models to guide collections

Improving sensitivity of
measurements Improved nuclear data for models

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Capabilities supported by synergistic programs

Return to the weapons

program:
Analytical • Leverage support for
Interdicted chemistry plutonium sustainment
materials supporting
forensics certification • Support for the
development of
International
advanced analytical
Trace Environmental
materials safeguards methods
signatures
programs • Support for core
competencies not
Nuclear currently robustly
Post-det weapons
forensics assessment
supported
• Providing challenges
to help develop the
next generation of
scientists
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