Actinide Research Los Alamos National Laboratory Quarterly · N u c l e a r M a t e r i a l s R e s...

Also In This Issue

■ Annual reviewassesses the state ofscience and technologyin NMT Division

■ Technology transferbetween Savannah Riverand the national labs

■ Plutonium Futuresconference speakers set

■ Mary Neu is intriguedby actinides

■ “Eye of the Beholder”

N u c l e a r M a t e r i a l s R e s e a r c h a n d T e c h n o l o g y

Quarterly Actinide Research

Researchers cast first “spiked” plutonium alloy

2nd quarter 2002

Nuclear Materials Technology DivisionMail Stop E500Los Alamos, New Mexico 87545

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Major success in replicating how the stockpile ages

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Nuclear Materials Technology/Los Alamos National Laboratory

Actinide Research Quarterly

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NMT Division DirectorTimothy George

Chief ScientistKyu C. Kim

Writer/EditorMeredith S. Coonley

DesignerSusan L. Carlson

Contributing WriterKathy DeLucas, IM-1

PhotographersMichael D. GreenbankJoe Riedel

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Actinide Research Quarterly highlights recent achievements and ongoingprograms of the Nuclear Materials Technology (NMT) Division. We welcome yoursuggestions and contributions. ARQ can be read on the World Wide Web at:http://www.lanl.gov/orgs/nmt/nmtdo/AQarchive/AQhome/AQhome.html.

In This Issue

1 Researchers cast first “spiked” plutonium alloy

8 Annual review assesses NMT Division

11 Technology transfer between Savannah Riverand the national labs

17 Plutonium Futures conference speakers set

18 Mary Neu is intrigued by actinides

20 “Eye of the Beholder”

About theCover

Actinide ResearchQuarterly is producedby Los AlamosNational Laboratory

LALP-02-061

Claudette Trujillo of theNuclear MaterialsScience Group(NMT-16) assists withrolling an enrichedplutonium cookie on alaboratory-scale rollingmill during the historiccasting of a “spiked”plutonium alloy May 13.Cold-rolling the as-castplutonium emulates theprocess used at theRocky Flats Plant tomanufacture weaponscomponents. To provideeven more credibility tothe process, the samegrade of oil previouslyused at Rocky Flats,Texaco Regal ®, wasused to lubricate theplutonium during rolling.The background imageis of an enrichedplutonium specimenmounted inside analuminum fixture thatwill be tested using a40-mm launcher. Thestory begins on thenext page.

photo by Joe Martz

2nd quarter 2002

Nuclear Materials Technology/Los Alamos National Laboratory 1

Major success in replicating how the stockpile agesResearchers cast first“spiked” plutonium alloy

The photo at rightshows the plutonium-238 metal button that

was used as thestarting material for the

May 13 enrichedcasting. Plutonium-238

is normally onlyavailable in the form of

plutonium oxidebecause its radioactive

decay produces somuch heat that the

material must bepresent as a ceramic

for it to be stable. Theplutonium-238 button

shown here wasreduced to the metal

form from oxideoriginally fabricated for

space-program heatsources. Personnel inthe 238Pu Science and

Engineering Group(NMT-9), who followeda procedure developed

at DP Site in the1970s, performed the

reduction. This wasthe first time that

plutonium-238 metalhad been fabricated at

TA-55. This buttonweighs about 100

grams and is sitting atabout 200 degrees

Celsius.

photos by J. David Olivas

Los Alamos researchers celebrated a major success May 13when they cast the very first “spiked” plutonium alloy, creat-ing an accelerated-aging alloy that should age at a rate sixteen

times faster than normal. As a result, in four years the researchers hopeto have a material representative of sixty-year-old plutonium.

Researchers will measure the spiked material to look for any age-related changes in key physics, engineering, and materials properties.On the basis of these experiments, they’ll determine if the nation’sstockpile pits will last at least sixty years.

“This is probably the most technically difficult project we haveever attempted, at least metallurgically, at TA-55,” said J. David Olivas,technical lead on theproject and formerRocky Flats scientist.

The experimentrequired years ofpreparation and in-cluded replicating theRocky Flats pluto-nium manufacturingprocess. To that end,Los Alamos research-ers had to set up acapability that hadnever existed before:a one-of-a-kind small-scale casting, rolling,and machining opera-tion at the Laboratory’sPlutonium Facility (PF-4). The researchers also had to reproduce keyprocess steps and produce a material that matched Rocky Flats specifi-cations in a number of important properties.

And they did it on the first try.The research endeavor, called the Accelerated Aging of Plutonium

(AAP) Project, is an experimental collaboration between Los Alamosand Lawrence Livermore National Laboratories. Besides Olivas, theAAP team at Los Alamos consists of Franz Freibert, principal investiga-tor; Richard Ronquillo, lead mechanical technician; Claudette Trujillo,materials accountability specialist; Chris Trujillo, mechanical technician;and David Dooley, graduate research associate. All are with the NuclearMaterials Science Group (NMT-16).

These Los Alamos scientists, working with others in NMT-16, theStructure/Property Relations Group (MST-8), and the DetonationScience and Technology Group (DX-1), will examine the spiked material


Nuclear Materials Technology/Los Alamos National Laboratory2

“Spiked”Plutonium

Alloy

The casting yielded nineenriched plutonium“cookies,” one of whichis shown here. Thethickness of thisminiature ingot dupli-cates the thickness ofthe Rocky Flats ingots,giving researchers agood simulant for thenext stage of process-ing: rolling the ingot intoa sheet.

Chris Trujillo of theNuclear Materials

Science Group(NMT-16) machines

a Kolsky testspecimen. A non-

water-based coolantis used to flood the

specimen duringmachining. Flooding

ensures that thesample is not

overheated duringthe machining

process, avoidingthe introduction ofnonaging-relatedartifacts into the

plutonium sample.

with advanced characterization tools to measureaging-related changes in physical and chemicalproperties. Scientists at Livermore are conducting aparallel materials production and sample preparationactivity. The two laboratories will exchange informa-tion and samples.

The AAP activities support the EnhancedSurveillance Campaign goal to protect the health ofthe stockpile by examination of aged plutoniumthrough the accelerated production of defects.

The information obtained from this research will beused to predict material and component aging rates asa basis for annual certification, refurbishment scopeand timing, and nuclear weapon complex planning.

Ultimately, this work will form the key basis forestablishment of pit lifetimes. Results of the research will also be usedto make improvements to the basic surveillance program (see ARQ 1st

quarter, 2001).The new casting and machining capability also will enable Nuclear

Materials Technology (NMT) Division to expand its research anddevelopment efforts in the study of weapons-related actinides and otherspecial isotopes and materials.

Aging weapons alloy and stockpile stewardshipResearchers spiked the plutonium alloy cast May 13 with isotopic

blends containing 7.5percent plutonium-238. The greater alphadecay rate of the plu-tonium-238 isotopeaccelerates the self-irradiation processand enhances the self-irradiation damage asa function of time.Accelerating the self-irradiation agingeffects in weaponsalloys should providecritical data atextended effectivelifetimes in the manifestation of aging effects on weapon design param-eters and component function, according to the researchers.

2nd quarter 2002


During the agingprocess, theenriched sampleswill be stored inincubators like theone in the photo atleft. The samples willbe cleaned beforebeing loaded in theincubator chamber,and then will bestored in a pristineatmosphere for up tofour years. Fouryears of storage inthe incubator inactual time isequivalent to sixtyyears of aging inaccelerated time.The samples will beremoved periodicallyfrom the incubatorsand tested to obtainaging information atintermediate times.The incubatorchambers weredesigned and built atLawrence LivermoreNational Laboratory.

The detection and prediction of changes in an aging stockpile areperhaps the most challenging and technically engaging aspects ofscience-based stockpile stewardship. Originally, weapons systems were

designed with theexpectation that thenuclear componentswould provide a rea-sonable lifespan andthat the systemswould be modern-ized or replaced ona consistent basis.Weapons systemswere not designedwith the goal of long-term (fifty or sixtyyears) robustness.

Given the currentconstraints and con-ditions in the nuclearweapons stockpile,systems will requireextended lifetimesfor various compo-nents with only amodest remanufac-ture capability toreplace excessivelydegraded units.

Determining an appropriate response (recertification, refurbishment,or remanufacture) ultimately depends on an accurate assessment ofindividual component lifetimes.

The most acute challenge lies with testing and certification ofplutonium components and the pits in which they reside. Previously,certification and recertification of the plutonium components reliedheavily on full-scale nuclear tests—an approach that is no longer viable.

Relevant properties of weapons-grade plutonium and its decayproducts that affect performance include equation of state, spall andejecta, material strength, density, geometry, corrosion resistance, andnuclear reactivity. Among the time-dependent phenomena that couldaffect the properties of weapons-grade plutonium are radiation-induced void formation and swelling; ingrowth of decay products suchas helium, americium, and uranium; and phase instability. These effectsmay well be synergistic, making it particularly difficult to assess theimportance of any one phenomenon by itself.




Alloy

Red or green? The New Mexico questionA note on nomenclature

Using plutonium-238 to enrich weapons-grade plutonium resulted in the creation ofa new material previously not used in theweapons complex. Addition of the plutonium-238 has led to the material being called byseveral names—spiked, enriched, anddoped—all of which are acceptable.

Because this material is significantlydifferent from other plutonium alloys, theresearchers have chosen to name thematerial “Hatch.” This is, of course, inhonor of the southern New Mexico citythat produces the regionally famous “hot”chile peppers.

Now, if they could just decide if Hatchqualifies as red or green.

Because of the lack of a suitable number and variety of agedplutonium samples, researchers sought to produce alpha-decay-induced damage at an accelerated rate. They accomplished this by add-ing relatively small amounts of the short-lived isotope plutonium-238,which has a half-life of 86.4 years, to weapons-grade plutonium-239.This technique simulates many years of aging in just a few years.

Experimental and theoretical approachesThe AAP researchers assume that the damage created by alpha decay

of plutonium-238 is comparable to the damage that occurs in the nor-mal material and that sensitive, fundamental measurement techniquescan be employed to characterize this damage.

The spiked plutonium is being made into samples for many differentexperiments, and the data will give researchers a composite image ofthe aging process. A suite of advanced techniques is being used to char-acterize the enriched material and track subtle changes as the agingprogresses. (See sidebar on page 7 for a description of the tests that arebeing used.)

“Most of these experimental techniques have been used in the past tostudy research-grade material, but this is the first time they will all beapplied to the same material, and one that has such a well-known pedi-gree,” said Freibert.

Testing diagnostic methods focus on assessing effects of extendedaging on important design properties. Tests include density, dilatom-etry, elastic constants and bulk compressibility, conventional and highstrain rate mechanical testing, x-ray diffraction, helium effusion, lightand electron microscopy, and others.

These experimental capabilities will be applied to measure materialproperties sensitive to the reversible and irreversible thermodynamics ofthis plutonium alloy, as well as to provide information on the kinetics ofaging-related processes. This information will provide a sound technicaland scientific foundation for predicting weapon component lifetimes.

Researchers know from the analysis of nuclear reactor materials thatthe most obvious consequences of radiation damage are helium bubbleformation and void swelling. The net effect is that the metal will swelland therefore reduce the density of the metal. Although there are othertime-dependent phenomena that may affect the properties of weapons-grade plutonium, helium bubble formation and void swelling willunquestionably affect weapon performance.

Experiments using transmission electron microscopy (TEM) to imagehelium bubbles in weapons-grade metal have provided evidence sup-porting this theory (see ARQ 4th quarter, 2001). So far, the accumulationof aging effects and the overall impression on important weaponsdesign properties are still quite speculative.

2nd quarter 2002


Personnel from theNuclear MaterialsTechnology (NMT)Division load ex-tended x-ray absorp-tion fine structure(EXAFS) and x-raydiffraction (XRD) testspecimens intospecial containers.The specimens wereshipped to theStanford LinearAccelerator fortesting. The contain-ers isolate theplutonium beneath aspecial window andfacilitate the testing ofplutonium-bearingmaterials in facilitieswhere nuclearmaterials are notnormally handled.

photo by Fred Hampel

Fabrication “blitz”The Los Alamos researchers are now in a fabrication “blitz” so that

they can get experimental data near time equals zero. “That kind ofdata was missing at Rocky Flats,” said Olivas. “It’s not that Rocky Flatswas not interested in scientific data, it’s just that they were more inter-ested in making the product to specifications. Information that was notpart of the specification typically was not collected.”

Working with the enriched plutonium has led to two independentchallenges. “First, we must fabricate the enriched plutonium quickly,because once you make it, it starts aging,” said Olivas. “To get time-equals-zero data, we need to make samples as quickly as possible, andthen get them to the test station equally quickly.” A twenty-three-day-old sample is about twelve months old in accelerated time.

Independent from the timing issue are the problems associated withthe additional heat present in the samples from the presence ofplutonium-238. Recall that plutonium-238 is normally used as a heatsource. For example, the spiked material also appears to oxidize at anaccelerated rate outside its storage environment.

“It started to oxidize within minutes of production, forcing us toconduct all our fabrication operations in very pristine atmosphere,”said Olivas. The extra heat also makes taking measurements more diffi-cult. “When we attempted to measure the density of one of the as-castdisks using the Archimedes method, we literally boiled the immersionbath fluid.”

Previous work on a control castingThe May 13 spiked casting comes one year after a “control” material

of the same chemistry, but significantly lower plutonium-238 isotopiccontent, was cast and machined to validatethe installed equipment andthermomechanical processing.

A portion of the control batches receivedspecial processing to create samples withminute yet finite differences in physical andmechanical properties. These samples arenow undergoing testing by a suite of diag-nostics on a blind-sample basis to discernminute differences in physical and mechani-cal properties of plutonium alloys. Resultswill be used to quantify the sensitivity of themeasurement methods.

Data from the spiked casting show thatthe density of the heat-treated spiked disksmatches the density of the control casting




Alloy

Tony Valdezof the Weapons

ComponentTechnology Group(NMT-5) loads the

casting furnace withthe precursor

materials for theenriched casting:

plutonium-239 metal“imported” from the

Rocky Flats Plantand plutonium-238

metal buttons madeat Los Alamos. Forthis casting, everyeffort was made to

duplicate theprocessing param-

eters, such asheating and cooling,that were previously

used at the RockyFlats Plant to castplutonium ingots.

The metal is placedin a tantalum

crucible, heatedabove the meltingpoint of the pluto-

nium, and thenpoured into the

mold. All operationswith molten pluto-nium are done in

vacuum because ofthe extreme

reactivity of theliquid plutonium.

One of the advancedcharacterization

techniques being usedat TA-55 to obtain data

on the acceleratedaging process is a

40-mm launcher, whichis the equivalent of a

cannon with a40-mm-diameter bore.

The big exception is thatthis cannon is located

inside a glovebox. In thephoto at the top of the

next page, an enrichedplutonium 40-mm

launcher test specimenis mounted inside an

aluminum fixture.Testing material

properties on thelauncher consists of

accelerating a quartzprojectile down thebarrel, impacting it

against the face of theplutonium sample

shown in the photo-graph, and using a

velocity interferometersystem for any reflector

(VISAR) on the backface of the sample to

observe the shock waveas it passes through the

sample. To producegood results, the facesof the sample must be

perfectly flat andparallel, typically to

within plus or minus0.0002 inches.

disks at the samepoint in the process-ing. This is goodnews, according toFreibert and Olivas,because it indicatesthat metallurgically,Los Alamos’ process-ing for the spikedmaterial was equiva-lent to that of the con-trol casting.

More important,the researchers say, italso suggests thatthere seems to be nosignificant physical

difference in the spiked material that may be attributed to adding theplutonium-238.

A work in progressProgress on the enriched casting is proceeding nicely, according to

Olivas and Freibert. As of this writing, all metallurgical processing hasbeen completed, samples are being fabricated, and time-equals-zerotesting has begun. The researchers have completed time-equals-zerotesting on most of the mechanical property tests (40-mm launcher testsat high strain rate, Kolsky tests at intermediate strain rate, and com-pression tests at quasi-static strain rate), resonant ultrasound spectros-copy (RUS) tests, and x-ray diffraction tests.

In addition, they have shipped enriched plutonium to the StanfordLinear Accelerator Center for extended x-ray absorption fine structure(EXAFS) and x-ray diffraction (XRD) tests. ■

—Franz Freibert, J. David Olivas, and Meredith S. Coonley

2nd quarter 2002


Diagnostic test Information obtained by the test

Analytical chemistry Isotopics, δ-phase plutonium stabilizers, and tramp elements (elements that arecontaminated)

Density Relative amounts of phases (α and δ) plutonium, helium, and void swelling

Optical metallography Grain size, relative amounts of phases (α,α′,δ) plutonium, Pu6Fe (an intermetalliccompound that typically forms at grain boundaries), and inclusions

X-ray diffraction Lattice parameters, relative amounts of phases (α, α′, δ) plutonium

Microprobe Gallium segregation

Resonant ultrasound Elastics constants, compressibility, and sound speeds

40-mm launcher Dynamic mechanical behavior (spall strength and phase transitions)

Kolsky bar apparatus Intermediate strain rate mechanical behavior

Tensile/compression Quasi-static strain rate mechanical behavior (elastic-plastic properties)

Dilatometry Thermal expansion, δ→α′ plutonium Martensite transition, and density changes

Part evaluation cycle Phase stability (e.g., Stockpile to Target Sequence [STS], which is the order of eventsinvolved in removing a weapon from storage and assembling, testing, transporting, anddelivering it on target)

Thermoelectric transport Transport properties andisochronal annealing(damage recovery)

Thermal gas desorption Gas species determin-ation and helium trapenergetics

Calorimeters Phase transformations,transformation enthalpies,and specific heat

Helium effusion Energetics of heliumdiffusion

Positron annihilation Location and distributionof atomic-scale defects

Other Surface science and localstructure techniques

In the photo below,an as-cast cookiesits in the immersionbath of the densitymeasurementstation. The decayfrom the plutonium-238 generates somuch heat that itcauses the immer-sion bath fluid,FC43, to boil. Theboiling point of FC43is 165 degreesCelsius. The bubblesare faintly visible asthey rise above thesurface of thecookie.

In metallurgy, the polymorphic phases of elements and alloysare identified by the Greek alphabet. Plutonium has sevenphases; six at ambient temperatures and a seventh underpressure. Room-temperature α-phase plutonium has thelowest temperature and is brittle. δ-phase plutonium is stableat high temperatures and is very ductile, so it is easily formedinto shapes.

Diagnostics used to assessplutonium-aging effects



DivisionReview Another outstanding/excellent rating

Annual review assesses the state ofscience and technology in NMT Division

Nuclear Materials Technology(NMT) Division is key to thenational mission of reestablishing

the capability to manufacture a pit and has the“awesome responsibility” of ensuring the reli-ability and safety of the nation’s nuclear stock-pile, said Rich Mah, associate director forWeapons Engineering and Manufacturing(WEM). Mah made the remarks at the openingsession of the annual NMT Division Review.

NMT Division received an overall rating ofoutstanding/excellent from the externalreview committee, which met with membersof NMT Division and upper management atLos Alamos May 14–16.

Areas under review were rated on fourcriteria: quality of science and engineering,relevance to national needs and agency mis-sion, operation of major facilities, and perfor-mance of programs.

Three of the categories received outstanding/excellent ratings. The review committee rateda fourth category, relevance to national needsand agency mission, outstanding.

The review, required under the Departmentof Energy’s (DOE) contract with the Universityof California, assesses the quality of thedivision’s science and technology programs.Because all science and technology activitiesconducted by the division must be covered bythe review within a three-year cycle, historically,about one-third of NMT Division’s program-matic activities have been looked at each year.

In a break with previous practice, this year’sreview focused on facility management, mate-rial control and accountability, informationmanagement, and waste management.

Because these critical activities are essentialto the success of so many of NMT’s program-matic missions, the entire NMT managementteam felt they should be submitted forexternal review.

‘Excellent progress’In giving NMT Division its outstanding/

excellent rating, the external review committeepraised division management for makingextensive changes and developing a morefocused approach. In particular, the committeecited the division’s making better use of statis-tical tools and numerical data to track pro-grammatic performance and learn newapproaches to operational excellence.

“The committee felt very strongly that theintegrated approach to research, production,and facilities operation is demonstrably criti-cal to programmatic success,” the review com-mittee members wrote in their report.

“Among its wide range of programmaticactivities, the division’s evidently successfulcommitment to pit production means that itscontributions to national needs are self-evident,” said the report. “Again, however, theintegrated approach will continue to be criticalbecause NMT has essential contributions tomake to the [pit] certification process.”

The committee cited the “excellentprogress” made by NMT Division in the pitmanufacturing area since the last review. Thir-teen pits have been fabricated, including oneearly development pit, seven of nine develop-ments, and five standard pits. The seventh de-velopment pit was fabricated fourteen monthsahead of schedule.

Pit certification is running ahead ofschedule, and the deadline has moved up twoyears from 2009 to 2007. Meeting the mile-stone two years early will save $450 million inthe certification process, Mah told the openingsession audience. The pit-manufacturingproject also is on track to meet a major mile-stone in April 2003 with the completion of theQual-1 pit.

While citing improvements in management,scientific excellence, and the success of thepit-manufacturing program, the committeerecommended that the division place more

2nd quarter 2002


photo by Mick Greenbank

Steve Yarbro (left),Tim George (center),and Rich Mah listento a speaker duringthe opening sessionof the annual NMTDivision review.

emphasis on the development of acomprehensive strategic plan. “This is bothurgent and important as programmatic suc-cess in the pit production area, for example,will likely mean that new responsibilities willbe assigned to NMT in the near future,” saidthe report.

Consequently, the report recommends thatNMT and ADWEM develop a strategic planthat will address issues of “how major pro-grams are expected to develop, space alloca-tion within the limited amount of nuclearfacility space, quality-of-life for the staff, andpromotion of basic science and engineering tounderpin the programs.”

As a result of these suggestions, NMTmanagers, scientists, facility managers, andprogrammatic leaders will be meeting overthe next two months to develop a comprehen-sive strategic plan for the division.

Aging facilities a major topicFacility infrastructure and management

were main topics of this year’s review anddiscussion naturally focused on the Lab’snuclear facilities: the TA-55 Plutonium Facility(PF-4) and the Chemistry and MetallurgyResearch (CMR) Building.

At 40,000 square feet in four wings, thingsare getting tight in PF-4. “The lack of spacedrives what we can do in that facility,” saidMah. “We require guns, gates, guards, andother special capabilities to work with actinidematerials; at a $10,000 per square foot replace-ment cost, these are expensive operations.”

NMT Division Director Tim George alsoemphasized the importance of theLaboratory’s actinide research facilities to thenation’s nuclear mission.

“PF-4 and CMR remain the nation’s onlyfacilities capable of handling all isotopes andchemical forms of plutonium, as well as otheractinides,” George told review committeemembers. “I would say that operation of these

two facilities, in the context of their age, andthe scope and significance of activities con-ducted within them, may be one of the mostchallenging tasks in the Department ofEnergy complex.”

George called the successful operation ofthese two nuclear facilities a major accomplish-ment of the division for the past year. WhilePF-4 is the nation’s newest plutonium researchand development facility, it is more thantwenty years old and is reaching the end of itsdesign life. And at fifty years old, the CMRBuilding must be replaced within a decade.

Critical missions and a milestoneGeorge told the review committee that

while the pilot production of pits is the



DivisionReview

division’s top priority, in the final analysis“stockpile surveillance and enhanced surveil-lance, or accelerated aging, may be the NMTmissions most critical to the nation’s security.”

George emphasized the point by announcinga major milestone in enhanced surveillancethat occurred the day before the review began:Researchers at Los Alamos have successfullydeveloped a way to replicate how the stock-pile ages by producing a “spiked” plutoniumalloy that will age at an accelerated rate. Thisfirst-of-its-kind feat will allow researchers toobserve the effects of plutonium aging in yearsinstead of decades. (See cover story.)

Mah and George both stressed to the reviewcommittee the importance of Los Alamosmaintaining a skilled work force. “We havethe largest pool of nuclear scientists in theworld,” said George, “and we have to main-tain that pool.”

To meet that priority, critical skills havebeen identified and strategic hiring is underway in the division. One hundred newemployees have been hired and at leastanother 100 are needed. One hitch is the lackof office space. “We want to hire additionalstaff,” said George, “but it’s very challenging;there’s no place to put them.”

In discussing the future, George talkedabout a two-year division initiative focusingon advanced nuclear fuels research to supporta DOE-sponsored endeavor called the Genera-tion IV Roadmap.

Generation IV, a DOE collaboration withnine other countries, will set out to identifynuclear power concepts and systems thatcan reach commercial viability by 2030.Generation IV will require extensive researchin advance fuels in the form of oxides,nitrides, metals, and salts, and NMT’s capabili-ties at the CMR Building and PF-4 will play akey role in research into these new fuel forms.

In its report, the review committee agreedthat the advanced fuels trial program is animportant priority for the division butrecommended that the trial be lengthened tothree years.

Labwide assessment due in AugustThe NMT Division report, as well as the

individual reports of all other technicaldivisions at Los Alamos, will be rolled up intoa Laboratory-wide report called the Scienceand Technology Assessment, which will besent to the UC president’s office in August.The Science and Technology Panel of the UCPresident’s Council on the National Laboratoriesalso assesses Lawrence Berkeley and LawrenceLivermore National Laboratories.

Anthony (Tony) Rollet chaired the externalreview committee for the second year. Rollet,of Carnegie Mellon University, is a formerdeputy leader of Los Alamos’ MaterialsScience and Technology (MST) Division.

Other members of the review committeeincluded Richard Bartsch, Texas TechUniversity; Darleane Hoffman, LawrenceBerkeley National Laboratory and formerhead of Los Alamos’ Isotope and NuclearChemistry (INC) Division; AlexandraNavrotsky, University of California, Davis;Lee Peddicord, Texas A&M University; GeorgeWerkema, retired, DOE; and William Weston,Boeing Co., Rocketdyne Division.

Steve Yarbro, NMT deputy division leaderfor plutonium research and technology, wascoordinator of this year’s review. ■

—Meredith S. Coonley

2nd quarter 2002


GuestEditorial

photos courtesy ofSavannah River Site

This editorial wascontributed bySusan Wood,director of theSavannah RiverTechnologyCenter.

PAR Pond is a man-made lake, constructed in 1958 as acooling pond for the Savannah River Site’s P and Rreactors, hence the name. “RAP Lake” was also consid-ered as a name, but the site’s location near Augusta, Ga.(home of the Masters golf tournament), prompted siteofficials to choose the acronym PAR instead. It serves asa natural habitat for a variety of aquatic animals, makingit a “living laboratory” for studying alligators, severalspecies of fish, and migratory birds.

Susan Wood

The opinions in this editorialare the author’s. They do notnecessarily represent theopinions of Los AlamosNational Laboratory, theUniversity of California,the Department of Energy,or the U.S. government.

Integrating research and development with production missionsTechnology transfer betweenSavannah River and the national labs

Throughout its long history, the SavannahRiver Site (SRS) has benefited from close re-lationships with the national laboratories,

not the least of which is a special relationship withLos Alamos, based on our complementary capabili-ties in tritium and plutonium. These partnerships areessential in enabling this key Department of Energy(DOE) site to fulfill its current and future missions.

The SRS is a DOE industrial complex dedicated tostewardship of the environment, the enduringnuclear weapons stockpile, and strategic nuclear ma-terials. The SRS processes and stores nuclear materi-als in support of national defense and U.S. nuclearnonproliferation efforts.

With its applied research and development (R&D)lab, the Savannah River Technology Center (SRTC), the site also devel-ops and deploys technologies to improve the environment and treatnuclear and hazardous wastes left from the Cold War.

The site—with its five nuclear reactors (now shut down) and twochemical separations plants, plus numerous other production andwaste-management facilities—was built in the 1950s to produce materi-als used in nuclear weapons, primarily tritium and plutonium-239.

The SRS complex covers about 310 square miles encompassing partsof three South Carolina counties along the Savannah River, on theSouth Carolina–Georgia border.

Science and technology at SRSScience and technology (S&T) have always been important at SRS

because they support plant operations, enhance environmental cleanup,reduce cost, enhance safety, and enable new missions.

The S&T for SRS needs may come to the site fromSRTC, one of the national laboratories, or elsewhere.Whatever the origin, it typically is transmittedthrough SRTC, which then assumes responsibility for



GuestEditorial

An operator works on the Defense Waste Processing Facility’s (DWPF)equipment through a shielded window with the aid of video monitors.Remote operations, coupled with five-foot-thick walls, are necessary tokeep workers from being exposed to high levels of radiation produced bythe waste going through the facility. DWPF is the largest radioactivewaste glassification plant in the world. It is where high-level liquid nuclearwaste currently stored at the Savannah River Site is converted into asolid glass form suitable for long-term storage and disposal. Sinceradioactive operations began in March 1996 at DWPF, more than 1,300canisters of glassified waste have been poured. It is expected to takeseventeen to twenty-five years to turn the entire site inventory of high-level waste into glass.

ongoing support; hence our slogan, “We Put Science to Work.” It isessential that we work closely with the national laboratories to leverageand integrate our respective capabilities as well as to provide a seamlesstransition from a “lead lab” to a production site. Each mission areanecessitates different partnerships and relationships tailored to its spe-cific needs and the S&T strengths of respective laboratories. Optimizingsuch integration requires mutual respect of each other’s capabilities anda willingness to share and team.

Tritium missionsTritium, with a half-life of 12.5 years, must be replenished, and SRS is

the nation’s only facility for recycling and reloading tritium fromnuclear weapons reservoirs returned from service. All tritium unload-ing, mixing, and loading is performed in a facility that went into opera-tion in 1994, replacing older facilities that processed the nation’stritium for thirty-five years. A new facility is being built to extract tri-tium created in the Tennessee Valley Authority’s light-water reactors.

SRS and Los Alamos have a fully integrated S&T roadmap, whichsupports both short- and long-term production mission objectives.Together, we represent the nation’s core tritium capability. In addition,the Accelerator Production of Tritium (APT) team leveraged the jointcore competencies in R&D and technology application to mutual benefitand success. This was an ideal role model for future work, which notonly enabled rapid technology deployment, but broadened career op-portunities as well.

Pacific Northwest National Laboratory(PNNL) also played a key role by performingexperimental and modeling work to demon-strate tritium extraction from Tritium Produc-ing Burnable Absorber Rods—or TPBARs.

2nd quarter 2002


For more than three decades, the Receiving Basin forOffsite Fuels (RBOF) has been safely receiving and storingon-site fuels and fuels from domestic and foreign researchreactor programs. Until 1988, it was routine for foreignresearchers to return U.S.-origin spent fuel to this country.At the urging of the U.S. Department of State and the

International Atomic Energy Agency, the Department ofEnergy renewed that policy in 1996. Plans are under way todeinventory RBOF, transferring spent fuel to SavannahRiver Site’s L Area Disassembly Basin, a much largerfacility. That basin was modified and received its firstshipment of foreign spent fuel in January 1997.

Spent fuelSpent fuel currently stored at SRS is from the site’s production reactors

and from domestic and foreign research reactor programs. All of this fuelis stored in water-filled concrete storage basins, which were intendedoriginally for interim storage while spent fuel awaited processing in achemical separations facility. In addition, studies are under way to findalternative technologies, such as dry cask storage, for the spent fuel.

SRS is the DOE’s Center of Excellence for the dispositioning ofaluminum clad fuel, an effort supported by Los Alamos.

Plutonium and other canyon missionsSavannah River Site’s two primary separations facilities, called canyons,

are located in F and H areas. F Canyon and H Canyon—together with theFB Line and HB Line, which are located atop the canyons—are wherenuclear materials historically have been chemically recovered and purified.



GuestEditorial

In addition to defense materials, HB Line has produced plutonium-238 forLos Alamos, which NASA used for the 1997 Cassini mission.

F Canyon completed its PUREX processing mission in March 2002.PUREX is an extraction process in which fuel elements are dissolved innitric acid and the uranium and plutonium are chemically separated outwith solvents. H Canyon continues to stabilize and manage most of theremaining inventory of plutonium-bearing materials at SRS. Inaddition, DOE has determined that H Canyon should be used to converta large quantity of weapons-usable highly enriched uranium (HEU) tolow-enriched material suitable as fuel in commercial power reactors.

Additionally, the H Canyon role in plutonium stabilization will beexpanded to include materials from dismantled weapons and surplusesfrom other DOE sites. SRS is also the announced location for the DOE’splutonium pit disassembly and conversion (PDCF) and mixed-oxide(MOX) fuel fabrication facilities. Technology development for the plu-tonium immobilization facility, which has been suspended, involved astrong partnership with Lawrence Livermore National Laboratory,which had the technology lead.

Both the past and the future of SRS plutonium missions involve closeinteraction between Los Alamos and SRS. Traditionally, we have syner-gistically shared and used actinide chemistry and process knowledge.

Savannah River Site (SRS) has two primaryseparations facilities where nuclear materialshistorically have been chemically recovered andpurified. Called F and H “canyons” for their long,narrow shapes, these large, remotely operated,heavily shielded facilities were constructed in theearly 1950s to provide materials, initiallyplutonium-239, for the U.S. nuclear arsenal. Asthe chemical separations processes developedand matured, these canyons showed a versatilitywell beyond their original scope, processing avariety of materials, including uranium-235 andneptunium-237 (which, when irradiated, producedplutonium-238, which is used in power systemsfor the U.S. deep space exploration programs).In recent years, the canyons have been used tostabilize and manage legacy materials at SRS,including plutonium-bearing materials and highlyenriched uranium. F Canyon completed itsscheduled production mission in March 2002;H Canyon continues to operate.

2nd quarter 2002


The plutonium-238 mission was a joint program, which was transferredto Los Alamos in 1995. Furthermore, Los Alamos is the lead lab for thePDCF, but we have not achieved the level of integration in plutoniumthat has been accomplished with the tritium mission.

SRS has a vital role in plutonium management for DOE. In itssupport of SRS missions, SRTC has a vital role in plutonium research,development, and technology (RD&T), as does Los Alamos. I believethat improved teaming and integration of RD&T would provide ben-efits for the customer and the technical staff at both locations. Certainly,it would facilitate technology transfer and ongoing support to the pro-duction site.

Waste management and environmental restorationWeapons material production created unusable byproducts, such as

radioactive waste. About 38 million gallons of high-level radioactiveliquid waste are stored in tanks at SRS. The Defense Waste ProcessingFacility (DWPF), which began operations in 1996, is processing thehighly radioactive waste by bonding radioac-tive elements in borosilicate glass. Much of thevolume in the tanks ultimately will be sepa-rated as relatively low-level radioactive salt

solution, which is mixed with cement, ash,and furnace slag, and poured into permanentconcrete monoliths for disposal at a facilitycalled Saltstone.

A technician works inside a glovebox on the HB Line, located on top ofH Canyon. HB Line was built in the early 1980s to support the production of

plutonium-238, a power source for the nation’s deep space explorationprogram. Decisions announced between December 1995 and October

1997 concluded that HB Line should be used to stabilize solutions stored inH Canyon. HB Line consists of three process lines. The Scrap Recovery

Line is used to recycle legacy plutonium scrap (sometimes mixed withother radioactive materials) for purification and concentration to a solidform. The Neptunium-237/Plutonium-239 Oxide Line can produce solid

oxide material from neptunium-237 or plutonium-239 nitrate solutions. (Thisline started operations for the first time in November 2001. The plutonium

material is shipped to FB Line for storage and eventual disposition. Theneptunium material will be shipped offsite for further processing.) The

Plutonium-238 Oxide Line can produce plutonium-238 oxide from nitratesolutions; there is not a current mission for this line.



Savannah River Site’s working relationships with national laborato-ries in support of the high-level waste mission are many and varied.They include strong teaming with PNNL on vitrification and wastepretreatment, together with Oak Ridge National, Argonne National,and Idaho National Engineering and Environmental Laboratories.The key has been to identify the best capabilities and integrate themto support mission needs, assisted by the Tanks Focus Area (part ofthe Environmental Management R&D Program).

The integrated technology roadmap is, however, more near-termthan the tritium model described earlier. Thus, while resources are bestused and networking relationships are strengthened by this approach,it does not promote long-term partnerships.

Similar relationships are in place to support the mission to remediatethe site’s 515 inactive waste and groundwater units. Waste sites rangein size from a few square feet to tens of acres and include basins, pits,piles, burial grounds, landfills, tanks, and associated groundwater con-tamination. While there are many common factors across SRS contami-nation sites that also extend to other parts of the DOE complex, thereare also many site-specific factors that impact chosen remedies. Thus,rapid knowledge-sharing and technology reapplication skills are key tosuccessful technology reuse at multiple sites.

In all of these activities, teaming with the national laboratories is partof everyday life at Savannah River. A continued strengthening of thespecial relationship between SRS and Los Alamos will be beneficial toall of us, as we jointly pursue our enduring missions. ■

Construction began on the first high-level wastetanks at the Savannah River Site (SRS) in 1951,while the last waste tank was constructed in 1981.The waste tanks vary in size, from 750,000gallons to 1.3 million gallons. There were fifty-onetanks originally constructed at SRS. However, in1997 SRS closed the first two high-level wastetanks in the nation by filling them with a specialgrout mixture and concrete, bringing the numberof waste tanks available to forty-nine. There areabout 37 million gallons of waste stored in thesetanks awaiting processing. The highly radioactiveportion of the waste stored in the tanks will be sentto the Defense Waste Processing Facility, where itwill be immobilized by converting the liquid wasteinto glass. The low-level portion of the wastematerial will be treated and stored on site in aspecial grout-cement mixture until its radioactiveconstituents decay to harmless levels.

2nd quarter 2002


The next Plutonium Futures—The Science Conference will beheld July 6–10, 2003 at the

Albuquerque Marriott.The conference addresses scientific and

technical issues surrounding plutonium andother actinides and attempts to educate thepublic and students on these topics. The plan-ning committee has already received a signifi-cant number of responses from scientists andresearchers throughout the world who areeager to attend the 2003 conference.

The conference committee expects a verysuccessful scientific and academic conferencesimilar in format to the last conference in2000. More than 400 international participantsfrom sixty institutions and fifteen countriesattended the July 2000 conference.

Next year’s venue will feature speakers suchas Pierre D’Hondt, director of Reactor Safety,Belgian Nuclear Research Center (SCK-CEN),who will speak about advances in mixed-oxide (MOX) fuel technology; and RolandSchenkel from the Institute for TransuraniumElements, who will speak about the recenthighlights of actinide research at ITU.

Teresa Fryberger from the Department ofEnergy (DOE) Office of Science will discussenvironmental aspects of plutonium and otheractinides. Helen Caldicott, founder ofPhysicians for Social Responsibility, will bethe banquet speaker. She will discuss medicalimplications of plutonium research.

Other guest speakers who have beeninvited but not yet confirmed includeMargaret Chu, DOE’s director of CivilianRadioactive Waste Management, and NikolasPonomorev-Stepnoi, vice president of theRussian Research Centre Kurchatov Institute.

The conference will kick off with a specialtutorial for students on Sunday, July 6. Theconference committee is encouraging studentparticipation and the conference will paytravel expenses for students who present papers.

Monday, July 7, will feature the plenaryspeakers. The plenary lectures establish themotivational, historical, and scientificreasons for holding the conference. The follow-ing days will include presentations by techni-cal experts and poster sessions. The banquet isscheduled for Wednesday evening, July 9.

Registration is $350 if received beforeJune 5, 2003. After June 5, the cost is $450. ForAmerican Nuclear Society members, the cost is$300 for early registration and $400 afterJune 5, 2003. The second announcement andcall for papers will be mailed in early August.

To register or express an interest formailings, access the conference Web site atwww.lanl.gov/pu2003. ■

Plutonium Futures 2003conference speakers set

For further information visit our web site at http://www.lanl.gov/PY2003.html or contact us at 505-665-5981 Plutonium Futures—the science, Los Alamos, national Laboratory, P.O. Box 1663 ms e500, Los Alamos, New mexico, usa 87545

Background photo: cone nebula, NASA and the ACS Science Team/Pu-238 Heat Source (NE/NASA)

July 6–10, 2003Albuquerque New Mexico, USA



Profile

photos by Mick Greenbank

Mary Neu is intrigued by actinides

“I t is human nature to believe that thephenomena we know are the onlyones that exist, and whenever some

chance discovery extends the limits of ourknowledge, we are filled with amazement,”Marie Curie wrote when she pondered thelack of knowledgeabout radioactivity inCentury Magazine,January 1904. “Wecannot become accus-tomed to the idea thatwe live in a world thatis revealed to us onlyin a restricted portionof its manifestations… how numerous andvaried may be thephenomena which wepass without a suspi-cion of their existenceuntil the day when a fortunate hazard revealsthem.”

It was this intrigue that interested MaryNeu in actinide chemistry as a graduate stu-dent and later prompted her to come to LosAlamos. “Actinide chemistry,” Neu says, “isvery complicated and underexplored. There ismuch room for many important discoveries.”

Neu performed her undergraduate work atthe University of Alaska at Fairbanks, startingout as a geology major. She soon discoveredthat other physical sciences were also interest-ing to her and switched her major to inorganicchemistry and mathematics.

She completed her doctorate at the Universityof California–Berkeley with her dissertation,“Coordination Chemistry of Two Heavy Metals:Ligand Preferences in Lead Complexation,Toward the Development of Therapeutic

Agents for Lead Poisoning; PlutoniumSolubility and Speciation in the Environment.”

Working on her doctorate, Neu conducted awide range of synthetic inorganic chemistryand solution thermodynamic studies.

She conducted the lead chemistry on theUC Berkeley campus under the direction ofProfessor Ken Raymond and did plutoniumchemistry at Lawrence Berkley and LawrenceLivermore National Laboratories under thedirection of Professor Darleane Hoffman andin collaboration with Bob Silva, HeinoNitsche, and Richard Russo.

She completed her doctorate at the firstGlenn Seaborg Institute established atLivermore in the early 1990s.

As a UC President’s postdoctoral fellow, shecame to Los Alamos in 1993 and worked withDave Clark in a group that was then in the In-organic and Nuclear Chemistry (INC) Divi-sion. Her early research here was on thesynthesis and characterization of actinide car-bonate species. Neu studied the processes andmeans that actinides form chemical bondswith other molecules.

Currently, Neu is deputy group leader ofthe Actinide, Catalysis, and SeparationsChemistry Group (C-SIC) and is conductingresearch in three general areas.

In the first research area, fundamentalcoordination chemistry, Neu is studyingligand preferences of actinides in different oxi-dation states and the resulting geometries ofactinide compounds that may be used in newseparations and processing technologies.

A second area of research is environmentalspeciation and behavior—studying and pre-dicting the nature of contaminant plutonium.Neu’s research, performed in collaborationwith several colleagues at Los Alamos, helpedidentify the common oxide of plutonium(IV)as the chemical species that is prevalent insoils at Rocky Flats.

To determine how important and stableparticular species are, Neu studies the

Actinide chemistry is complicated, underexplored,and has room for important discoveries

Mary Neu

2nd quarter 2002


formation and thermodynamics of plutoniumcomplexes of carbonate, hydroxide, chloride,and other ligands under environmental condi-tions. These studies, together with actinide-mineral interactions and geochemicalcalculations, support the development of pre-dictive contaminant mobility models and newcleanup technologies.

Neu’s third area of research is actinideinteractions with microorganisms and micro-bial chelators—with the goal of using thosemicroorganisms to stabilize or otherwisetransform plutonium. For these researchprojects Neu works in close collaboration withcolleagues in the Biosciences (B) Division, pri-marily Larry Hersman.

Her most exciting recent research resultsinvolve the reduction of plutonium(VI) and (V)by a common bacteria, shewanella putrifaceans.Although the exact mechanism is not well un-derstood, these are the first results that indicateplutonium can be reduced through bacterial res-piration to less environmentally mobile forms.Neu plans to further study this relationship andwill submit a paper to the journal Science. Shealso has applied for Laboratory DirectedResearch and Development funds for the project.

An outcome of this research with bacteria isthat she and her team have found that the tox-icity of plutonium and uranium to microor-ganisms is generally less than that of some ofthe more common hazardous metals, such aszinc, nickel, and cadmium.

Her work brought her to Los Alamosbecause it is one of the few places in the coun-try where she can research what she enjoys—fundamental actinide science.

She sees real difficulties in the future ofactinide research and radiochemistry becausethere aren’t many professors teaching these top-ics any more. The biggest challenge to actinidescience, Neu believes, is that bureaucracy, oldequipment, and aging facilities impede actinideresearch here as well as at other facilities.

Most of her work is done in the fifty-year-old Chemistry, Metallurgy, and Research(CMR) Building. Hope is on the horizon: Anew facility is planned. Neu is enthusiasticabout the CMR Replacement project and hope-ful that research space will be included andimproved in the new facility, which is sched-uled to be built around 2010.

“There is a tremendous need for modernradiological facilities across the Department ofEnergy complex and especially at Los Alamos,where such facilities are essential to both ourcore missions and to our research excellence,”Neu said.

She has a passion for actinides, and doesn’tdo it any differently than she did ten yearsago. “I wanted to be safe ten years ago and Iwant to be safe now,” Neu said. “I’m optimis-tic about the science and the incredible infor-mation we have yet to discover, but I’m alsoknowledgeable of the nontechnical challengesassociated with actinide research.” ■

—Kathy DeLucas



Award

“Eye of the Beholder,” the photo on page 21, is an inside view of a

vacuum chamber that will be usedfor laser-ablation, matrix-isolation studies ofactinide metal atoms and ions with smallgaseous molecules such as oxygen, nitrogen,carbon dioxide, and hydrogen.

The research is the postdoctoral project ofSteve Willson of the Actinide ChemistryResearch and Development Group (NMT-11)and is sponsored jointly by Kirk Veirs ofNMT-11 and Joe Baiardo of the Nuclear Materi-als Science Group (NMT-16).

Inside the vacuum chamber, a small actinidemetal target is supported by a post insertedinto the port through which the camera islooking (the post has been removed for thephotograph).

A neodymium:yttrium aluminumgarnet—or Nd:YAG—laser beam passingthrough the port where Greenbank has digi-tally added an eye is focused onto the surfaceof this metal target.

The resulting laser-induced plasma of metalatoms and ions are co-deposited with neon orargon and a small amount of reactant gas ontothe mirrored copper surface visible in the cen-ter of the photograph. This surface is cooled to6 Kelvins (six degrees above absolute zero) bya closed-cycle helium refrigerator.

The resulting thin film contains the reactionproducts of the metal atoms and ions with thereactant gas frozen into the inert gas matrix.The reaction products are detected using infra-red spectroscopy, which results in a series ofvibrational bands.

Precise identification of the chemical for-mula of the reaction products is obtained byrepeating the experiment with the same reac-tant gas containing a different mix of isotopes,which results in the vibrational bands shiftingin predictable ways.

The chemical behavior of these reactionproducts are further studied by warming thematrix to a still chilly 10 to 35 K elvins, byphotolysis of the products with ultravioletlight, or both.

Willson expects the system to be online thissummer in the Plutonium Facility (PF-4),where it will be used to experimentally probesome of the simple reaction chemistry ofactinide atoms with common atmospheric con-stituents. He designed the apparatus based onhis graduate work with Lester Andrews at theUniversity of Virginia and adapted it for safeoperation with actinides and optimal use ofthe available space.

He anticipates that his research will bevaluable for the exploration of some of theunderlying processes that occur in largersystems. The data collected will provide aspectroscopic catalog that he and his sponsorshope will simplify the identification of actinidecompounds in larger systems, with applicationfor corrosion studies of actinide-containingcomponents.

The components were fabricated by ArtMontoya of the Chemistry FacilitiesManagement Group (C-FM) in the TA-48machine shop and welded by Johnny Quintanaof the Weapons Materials and ManufacturingGroup (ESA-WMM) at the main shop. Duringthe design stage, Willson received assistancefrom John Morris of NMT-11.

Several adjustments made during thefabrication stage at the suggestion of Montoyaimproved the design and have been instru-mental in an invention disclosure filed on oneof the fabricated components. ■

The science behind“Eye of the Beholder”

2nd quarter 2002


Los Alamos National Laboratory, an affirmative action/equal opportunity employer, is operated by the Universityof California for the U.S. Department of Energy under contract W-7405-ENG-36. All company names, logos, andproducts mentioned herein are trademarks of their respective companies. Reference to any specific company orproduct is not to be construed as an endorsement of said company or product by the Regents of the University ofCalifornia, the United States Government, the U.S. Department of Energy, nor any of their employees. Los AlamosNational Laboratory strongly supports academic freedom and a researcher’s right to publish; as an institution,however, the Laboratory does not endorse the viewpoint of a publication or guarantee its technical correctness.

This photo, called “Eye of the Beholder,” by Mick Greenbank won third place in the Scientific/Industrial category at the Imaging Professionals of the Southwest (IPSW) Conference 2002.Greenbank and Joe Riedel, both with the Nuclear Materials Information Management Group(NMT-3), each came away with several awards from the conference, held in Albuquerque inApril. Besides his award for “Eye,” Greenbank received first place in the Commercial/Industrialcategory and honorable mention in the Special category. Riedel received both first place andhonorable mention in the Special category.

Actinide Research Los Alamos National Laboratory Quarterly · N u c l e a r M a t e r i a l s R e s...

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