Operated by the Los Alamos National Security, LLC for the DOE/NNSA

UNCLASSIFIED

Title Nuclear Forensics at Los Alamos

National Laboratory

David Podlesak, Robert Steiner, Carol Burns, Stephen LaMont, Lav Tandon

LA-UR-12-23987

Taiwan Experts Meeting, Taipei, Taiwan

August 13-15, 2012

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Overview

• Introduction to nonproliferation efforts

• Scope of activities at Los Alamos National Laboratory

• Facilities for radioanalytical work at LANL

• Radiochemical characterization capabilities

• Bulk chemical and materials analysis capabilities

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Los Alamos National Laboratory

• Over 65 years of actinide nuclear science

• Continuing mission – Develop and apply science and technology to ensure the safety and

reliability of the United States nuclear deterrent; reduce the threat of weapons of mass destruction, proliferation, and terrorism; and solve national problems regarding defense, energy, environment, and infrastructure.

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Los Alamos National Laboratory

• Analytical chemistry established in 1943 – plutonium R&D

• Special nuclear material recovery and processing (recycle or stabilization)

• Nuclear reactor fuel R&D

• Safeguards accountancy

• Space programs nuclear materials (Cassini, Galileo, Mars Rover, Mars Science Lab)

• Environmental management and remediation

• Destructive and non-destructive analysis standards

• Bulk nuclear material forensics

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LANL technical capabilities fostered by the nuclear weapons program support the evaluation of all categories of nuclear events:

Materials

Device

Post-detonation

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Nonproliferation Efforts

Combat the illicit trafficking of nuclear

materials

Detect activities indicating nuclear

proliferation

Monitor adherence to treaties and

international agreements

Characterize and catalog US nuclear material

attributes

Nuclear Material Analysis and Data

Assessment

Scope of Technical Activities

Certification of materials in pit

production

Support for international

safeguards programs

Our ability to characterize nuclear materials and processes relies on analytical methods from:

Our ability to characterize signatures of worldwide nuclear materials production relies on skills built in:

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

Underground test

experience

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Several facilities to work with materials of all quantities

RC-1, Sigma

Nuclear facilities (CMR, PF-4)

< 1011 atoms Pu-239 109 – 1022 atoms Pu-239

> 1022 atoms Pu-239

All facilities house ongoing missions that exercise analytical capabilities routinely

TA-48

CMR

Sigma

RC-45

TA-55

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Sample Matrices

PuBe neutron

pure impure

heat source power source

precursors

Plutonium Metal

pure impure

MOX fuels heat source

Uranium Metal

pure (EU) targets (NU)

Uranium Oxide

pure (EU) targets (NU)

MOX fuels (EU) reactor fuel (EU)

metal precursor (EU) ore concentrate (NU)

Plutonium Oxide

Rad Sources

Uranium Fluoride

tetrafluoride hexafluoride

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Radiochemistry

Elution of REs on Ln Resin

0

0.2

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1

0 2 4 6 8 10 12

mmol of HCl

Fra

cti

on

Elu

ted

La

Ce

Nd

Sm

Eu

Tb

9207

1

10

100

1000

10000

100000

1000000

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Tube Number (minutes)

To

tal

Co

un

ts

Tb Eu Pm Nd

0.075M -HIB 0.15M -HIB

Y Sm

0.13M -HIB

0.1

0M

-H

IB

Single or multi-element

Elementally separated radiochemistry

Standardized procedures

Refractory matrices

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Count Room capabilities

Provides qualitative and quantitative assay of gamma, beta, and alpha-emitting radionuclides in a variety of matrices and over a wide range of activity levels, – Trace levels to >1013 fissions

• Specializing in fission product measurements, • Operates 24x7x365 • Sample receipt and handling protocols • Makes ~ 70,000 measurements annually

– 30,000 high resolution gamma collections

• 30 non-automated high-resolution gamma-ray spectrometers, some highly specialized

• 10 custom automated high-resolution gamma-ray spectrometers, • 6 custom automated beta counters. • 6 custom non-automated beta counters (3 ~0.2 CPM Bkg) • ~ 90 Alpha spectrometers, • Batch and interactive analysis codes, • Relational database with web-based visualization tools.

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Clean chemistry and mass spectrometry

-State-of-the-art mass spectrometry instrumentation •TIMS NBS 1290 Sector 54 IsotopX Isoprobe-T •ICPMS HR-ICPMS (Element XR and Element 2) MC-ICPMS (Neptune and Neptune Plus) •IRMS MAT-253 Delta V

-10,000 sq. ft. of clean lab space, ideally suited for low-level routine analyses Perchloric acid hoods

Dry and wet ashing

- DOELAP accreditation; full quality envelope

- Many years of routine trace environmental and bioassay monitoring experience

-Expertise in the development and implementation of new procedures

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Radioanalytical capabilities - application to nonproliferation forensics

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Nuclear Materials Characterization

Analytical Method Information

High Resolution Autoradiography Number density of radioactive,

approximate size

High Resolution Gamma Spectrometry (Radiochemistry) Isotopic composition of Np, Am, U,

and Pu, fission products

Micro X-ray Fluorescence Elemental Distribution

Optical/Electron Microscopy Particle size, elemental distribution,

grain size, porosity, surface roughness.

X-ray Diffraction Composition/phase

Pycnometry Density

Laser-Based Particle Size Analysis Particle size distribution

Analysis and characterization of actinide materials

Assay and Classical Chemistry Onsite Analytical Chemistry and Sample Management

Coulometric titration

Ceric titration

Pu (III) and Pu (IV)

U Assay by Davies Gray

Fe and Si determination

Loss on Ignition (LOI)

Free acid determination

Standard preparation

X-Ray Fluorescence (XRF) and X-Ray Diffraction (XRD)

Fingerprint Detection Technology

Plasma Spectroscopy

Inductively Coupled Plasma-Mass Spectrometry

Inductively Coupled Plasma- Atomic Emission Spectrometry

DC Arc Emission

Cold-Vapor Atomic Fluorescence

Coordinate sample receiving, shipping, and distribution at TA-55 and CMR

Onsite radiochemical and trace analysis

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UNCLASSIFIED Operated by the Los Alamos National Security, LLC for the DOE/NNSA

UNCLASSIFIED

Analysis and characterization of actinide materials

Radiochemistry and

Nondestructive Analysis Mass Spectrometry

Laboratory Information Management

System and Quality Assurance

Interstitial Analysis & Ion

Chromatography

High-Precision

Gas Mass Spectrometry

Alpha and gamma spectrometry

Gross alpha, liquid scintillation

Fluoride, chloride, nitrite

nitrate, phosphate, sulfate

oxalate and perchlorate

carbon, oxygen, hydrogen

sulfur, moisture, and tritium

Oracle SQL*LIMS

Sample/nuclear material

tracking and data

management

Quality Assurance and Control

Record Management

Document Control

Training

XRD

Electron Probe

SEM

XPS Auger

EDAXS

Micro-XRF

Physical characterization tools for bulk materials

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Are

a F

ractio

n

Grain Size (Diameter) [microns]

Grain Size (diameter)

100 m

Materials processing techniques leave unique signatures in microstructures:

•Grain Size/Morphology •Inclusion Distribution/Morphology •Microstructural Texture •Mechanical Properties •Surface Features

O Kα U Mα

Na Kα U Mβ

SEM

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Materials analysis

Origin?

Production Method?

Intended Use?

Age of Material?

History

Cl

Fe

Pb Si

S

UO3

0

150

300

450

600

750

1 1.5 2 2.5 3

Aspect Ratio (a.u.)

Nu

mb

er

of

Pa

rtic

les

Nuclide Sample

( g/g)

234U 5.5 x 101

235U 5.7 x 103

238U 7.9 x 105

238Pu 7.4 x 10-4

239Pu 2.5 x 101

240Pu 1.0 x 10-2

242Pu 2.5 x 10-4

0

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1

Sample,

Original

Cladding

Sample,

New

vial

TIMS

U-235

Weig

ht

%

90

95

100

105

U-238

Weig

ht

%

Sample

Original

Cladding

Sample,

New

vial

TIMS

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Sample,

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Cladding

Sample,

New

vial

TIMS

U-235

Weig

ht

%

90

95

100

105

U-238

Weig

ht

%

Sample

Original

Cladding

Sample,

New

vial

TIMS

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Sample management, QA/QC

• Bulk analysis and radiochemistry analytical capabilities operate under specific quality programs funded by sponsors. These include DOELAP, NQA-1

LANL Performance on Pu Blind QC Swipes240

Pu / 239

Pu

240Pu /

239Pu LANL Value

0.0 0.1 0.2 0.3 0.4 0.5

24

0P

u /

23

9P

u R

efe

rence V

alu

e

0.0

0.1

0.2

0.3

0.4

0.5

All curves:Coefficients:b[0]=4.1712162264e-4b[1]=0.9965635121r ²=0.9998786666

• Some operations will move toward ISO 17025 compliance

• Need for expanded SRM program, laboratory intercomparisons

Performance on NWAL Pu Isotopic Blind QC Samples

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• Neptune MC-ICP-MS

• IsotopX Isoprobe-T MC-TIMS

• FEI SEM w/WDS & EDS

• Element XR ICP-MS

• Dual-Clover high resolution gamma-ray spectrometers

Investments in modern capabilities

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8O

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Day 2

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• Analytical chemistry measurements on plutonium and uranium matrices are critical to numerous defense and non-defense programs including safeguards accountancy verification measurements.

• Los Alamos National Laboratory operates capable actinide analytical chemistry and material science laboratories suitable for nuclear material forensic characterization.

• Actinide analytical chemistry uses numerous means to validate and independently verify that measurement data quality objectives are met.

• Numerous LANL nuclear facilities support the nuclear material handling, preparation, and analysis capabilities necessary to evaluate samples containing nearly any mass of an actinide (attogram to kilogram levels).

Conclusions