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RecrystallizationandRelated AnnealingPhenomena

ThirdEdition

Elsevier

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PrefacetotheFirstEdition

Recrystallizationandtherelatedannealingphenomenawhichoccurduringthe thermomechanicalprocessingofmaterialshavelongbeenrecognizedasbeingbothof technologicalimportanceandscientificinterest.Thesephenomenaareknowntooccur inalltypesofcrystallinematerials;theyoccurduringthenaturalgeological deformationofrocksandminerals,andduringtheprocessingoftechnicalceramics. However,thephenomenahavebeenmostwidelystudiedinmetals,andasthisisthe onlyclassofmaterialforwhichacoherentbodyofworkisavailable,thisbook inevitablyconcentratesonmetallicmaterials.Althoughthereisavastbodyofliterature goingback150years,andalargecollectionofreviewswhicharedetailedinChapter1, therehaveonlybeentwomonographspublishedinrecenttimesonthesubjectof recrystallization,thelatestnearly20yearsago.Sincethattime,considerableadvances havebeenmade,bothinourunderstandingofthesubjectandinthetechniques availabletotheresearcher.

Metallurgicalresearchinthisfieldismainlydrivenbytherequirementsofindustry, andcurrently,amajorneedisforquantitative,physicallybasedmodelswhichcanbe appliedtometal-formingprocessessoastocontrol,improveandoptimizethe microstructureandtextureofthefinishedproducts.Suchmodelsrequireamore detailedunderstandingofboththedeformationandannealingprocessesthanwehave atpresent.Thedevelopmentoftheunderlyingsciencetoalevelsufficientforthe constructionoftherequiredmodelsfromfirstprinciplesprovidesagoalforperhaps thenext10 20years.

Thebookwaswrittentoprovideatreatmentofthesubjectforresearchersorstudentswho needamoredetailedcoveragethanisfoundintextbooksonphysicalmetallurgy,anda morecoherenttreatmentthanwillbefoundinthemanyconferenceproceedings.Wehave chosentoemphasizethescientificprinciplesandphysicalinsightunderlyingannealing ratherthanproduceacomprehensivebibliographyorhandbook.

Unfortunatelythegenerictermannealingisusedwidelytodescribetwometallurgical processes.Bothhaveacommonresultinthatahardenedmaterialismadesofter,butthe mechanismsinvolvedarequitedifferent.Inonecase,associatedwiththeheattreatment

PrefacetotheSecondEdition

Thissecondeditionhasasimilarphilosophyandformattothefirst,although developmentsinthesubjecthavenecessitatedsomesignificantchanges. Recrystallizationremainsaveryactiveresearcharea,judgingbythenumberof publicationsandconferencesonthisandrelatedareas,andthecontinuingdevelopments inmanyareasmakeitadifficultsubjecttocapture.Asintheprefacetothefirst edition,weaskthereadertorememberthatthisbookpresentsapersonalviewofthe subject,ataparticularmomentintime.

Therehavebeentwoimportantchangesinmethodsofinvestigatingandanalyzing recrystallizationsincethefirstedition.Thefirstisintheexperimentaldeterminationof microstructureandtexture,wheretheincreaseinthepowerandapplicationofthe ElectronBackscatterDiffraction(EBSD)techniquehasprovideddataofatypewhich waspreviouslyunavailable,andmanyexamplesofitsuseareincludedinthebook. Theotherchangeisintheincreasedamountofmodelingandsimulationofannealing processeswhichisnowcarriedout.

Intermsofthesubjectareas coveredinthefirstedition ofthebook,therehasbeen significantnewactivityintwoareasoffundamentalimportancetotheunderstandingof recrystallization;thecharacterizationofthedeformedstate,andthemeasurementof grainboundaryproperties.Somenewareashavealsoopenedup.Inthefirsteditionwe brieflymentionednewresearchwhichindicatedthatdeformationtoverylargestrains mightleadtomicrostructuralstabilityonsubsequentannealing.Thishasnowbecomea majorresearchareawhichisnotonlyofscientificinterest,butisalsoapotential methodofproducingstrongalloys,andthis isgivendetailedcoverageinthisedition. Developmentsinthisandotherareashavehighlightedthedifficultiesofapplyingthe traditionalterminologiestonewphenomena,anditisnowconsiderednecessaryto subdividerecovery, recrystallizationandgraingrowthinto“discontinuous”and “continuous”variants.

Changesinthelayoutofthebookincludeaseparationofdeformationmicrostructure (Chapter2)anddeformationtexture(Chapter3),introductionofasimpleanalyticalmodel whichembracesrecovery,recrystallizationandgraingrowth(Chapter10),aconsideration

ofcontinuousrecrystallizationduringandafterlargestraindeformation(Chapter14),anda summaryofthemethodsofmeasuringrecrystallization(Appendix2).

Finally,accesstovideoclipsofsomeinsituannealingexperimentsandsimulationswhich maybeofinterest,isprovidedattheWebsite: http://www.recrystallization.info.

JohnHumphreys MaxHatherly April2003

PrefacetotheThirdEdition

Thisthirdeditionhewscloselytoitspredecessorswithsignificantadditionsincertainareas wheresubstantialadvanceshaveaccumulated.Inallareas,thetexthasbeenreviewedand, whereappropriate,re-writtentoaccountforrecentadditionstotheliterature.Concerning theauthorship,MaxHatherlyisnolongerwithus,sadly;JohnHumphreyshasretiredandis nottobeblamedforanyerrorsormistakesthatwemayhaveintroducedinthisnew edition.Intermsofcontent,computermodelingofgrainboundarieshasresultedinnew insightsabouttheirproperties,especiallyenergyandmobility.Thecombinationof automatedserialsectioningandsynchrotron-basedcharacterizationhasprovided3-Dmaps ofmicrostructureandadditionalnewinsights.Thedescriptionsofworkhardeningand texturehavebeenstrengthened.

AnthonyRollett

GregoryRohrer

August2017

fromMichaelFerryandRobertMoonoftheUniversityofNewSouthWaleshavebeen extremelyvaluable.

ThethirdeditionowesmuchtotheresearchconductedatCarnegieMellonUniversityon interfaces,largelyunderthesupportfromtheUSNationalScienceFoundationofthe MaterialsResearchScienceandEngineeringCenter.ADRandGSRaregratefultothe manyindividualswhohelpedwithdiscussion,data,figures,etc.

Symbols

Thefollowingnotationisgenerallyusedinthetext.Thesubscripts i or n indicatetheuseof lettersornumbersforparticularsymbols.Onrareoccasionswherethelettersorsymbolsare usedforotherpurposes,thisisspecificallystated.

b Burgersvectorofadislocation

c,cn,C,Cn,Kn Thesedenote“local”constantswhicharedefinedinthetext

d Diameterofsecond-phaseparticle

D Grainorsubgraindiameter

Di Diffusivity(s ¼ bulkdiffusion,b ¼ boundarydiffusion,c ¼ core diffusion)

Ei Energy,e.g.,storedenergyofdeformationED

Fv Volumefractionofsecond-phaseparticles

G Shearmodulus

k Boltzmannconstant

M Boundarymobility

n Exponent,e.g.,intheJMAKequation

Nv Numberofgrainsorsecond-phaseparticlesperunitvolume

Ns Numberofparticlesperunitarea

PorPi Pressureonaboundary

QorQi Activationenergy,(fordiffusion:s ¼ bulk,b ¼ boundary,c ¼ core)

R Grainorsubgrainradius

s Shearstrain

t Time

T,Tm Temperature,meltingtemperature(K)

v Velocityofdislocationorboundary

V Volume

X Fractionrecrystallized

a, b Constants

g Energyofaninterfaceorboundary

gSFE, gRSFE Stackingfaultenergy,reducedstackingfaultenergy

gb Energyofahigh-angleboundary

gs Energyofalow-angleboundary

ε Truestrain

_

ε Truestrainrate

q Misorientationacrossaboundary;also,workhardeningrate

l Interparticlespacing(definedinEq.A2.13)

n Poissonratio

n0 Atomicvibrationalfrequency

r Dislocationdensity

Sn Coincidencesitelattice(CSL)grainboundaries.1/nisthefraction ofsitescommontobothgrains

s Truestress

s Shearstress

41, F, 42 Eulerangles,Bungeconvention(definedinAppendix1)

U Orientationgradient

Abbreviations

ARB Accumulativerollbonding

CA Cellularautomata

CLS Cahn,Lu¨cke,Stu¨we(theoryofsolutedrag)

CPFEM Crystalplasticityfiniteelementmodeling

CSL Coincidencesitelattice

DDW Densedislocationwall

DRX Dynamicrecrystallization

EBSD Electronbackscatterdiffraction

ECAE Equalchannelangularextrusion

ECD Equivalentcirclediameter

FE Finiteelement(modeling)

FEGSEM Fieldemissiongunscanningelectronmicroscope

GBCD Grainboundarycharacterdistribution

GBE Grainboundaryengineering

GNB Geometricallynecessaryboundary

HAGB High-anglegrainboundary

HSLA High-strengthlow-alloy(steel)

HVEM High-voltagetransmissionelectronmicroscope

IDB Incidentaldislocationboundary

IF Interstitialfree(steel)

JMAK Johnson Mehl Avrami Kolmogorovkineticmodel

LAGB Low-anglegrainboundary

MD Moleculardynamics

MLI Meanlinearintercept

ND,RD,TD Normal,rollingandtransversedirectionsinarolledproduct

ODF Orientationdistributionfunction

PSN Particle-stimulatednucleationofrecrystallization

SEM Scanningelectronmicroscope

SFE Stackingfaultenergy

SIBM Strain-inducedboundarymigration

SMG Submicron-grained(alloy)

SPF Superplasticforming

TEM Transmissionelectronmicroscope

Table1.1: Examplesofstaticannealingphenomena.

RecoveryRecrystallizationGrainGrowth ContinuousSubgraingrowthContinuousrecrystallizationNormalgraingrowth DiscontinuousDiscontinuoussubgraingrowthPrimaryrecrystallizationAbnormalgraingrowth

growth,inwhichthesmallergrainsareeliminated,thelargergrainsgrow,andthegrain boundariesassumealowerenergyconfiguration(Fig.1.1e).Incertaincircumstancesthis normalgraingrowth maygivewaytotheselectivegrowthofafewlargegrains (Fig.1.1f),aprocessknownas abnormalgraingrowthorsecondaryrecrystallization.

Recentresearchhasshownthatborderlinesbetweenthevariousannealingphenomenaare oftenunclear,anditisknownthatrecovery,recrystallization,andgraingrowthmayoccur intwoways.Theyoccurheterogeneouslythroughoutthematerial,suchthattheymaybe formallydescribedintermsof nucleation and growth stages,andinthiscase,theyare describedas discontinuous processes.Alternatively,theymayoccuruniformly,suchthat themicrostructuresevolvegraduallywithnoidentifiablenucleationandgrowthstages.In thiscase,theprefix continuous isusedtocategorizethephenomena.Itshouldbe emphasizedthatthisisaphenomenologicalcategorizationthatdoesnotimplythe operationofanyparticularmicromechanism.The“continuous”phenomenainclude recoverybysubgraingrowth,continuousrecrystallizationandnormalgraingrowthand the“discontinuous”phenomenaincludediscontinuoussubgraingrowth,primary recrystallization,andabnormalgraingrowth.Therefore,asshownin Table1.1,thereare atleast six staticannealingphenomenathatneedtobeconsidered.Notethemodern approachtophasetransformationsdistinguishesbetweenfirst-orderwithlatentheat,i.e., discontinuitiesinthefirstderivativeoffreeenergy(withlatentheat)versussecond-order withdiscontinuitiesinthesecondderivative.Again,primaryrecrystallization,forexample, certainlyreleasesheat(asmeasuredbycalorimetry)likeafirst-ordertransitionbutthere clearlyisnosenseinwhichonecandefineathermodynamicequilibrium.Therefore,all annealingprocessesare,strictlyspeaking,second-ordertransitions.

Althoughtheseprocessesareanalyzedseparatelyinlaterchapters,therearecircumstances whentheycanbeconsideredwithinaunifiedframework,asdiscussedinChapter10.This hasthemeritofnotonlyemphasizingthecommonfeaturesofthevariousprocesses,but, inbreakingdowntheconventionaldistinctionsbetweenthevariousannealingphenomena, allowsalsofortheemergenceofnewphenomenawhichmaynotconvenientlyfitintothe traditionalcategories.

1.1.2ImportanceofAnnealing

Manymetallicmaterialsareproducedinitiallyaslargecastings,whicharethenfurther processedinthesolidstatebyforging,rolling,extrusion,etc.,toanintermediateorfinal

In1898,Steadproposedthatgraingrowthoccurredbygrainrotationandcoalescence,and althoughEwingandRosenhainpresentedconvincingevidencethatthemechanismwas oneofboundarymigration,Stead’sideawasperiodicallyreviveduntiltheworkof CarpenterandElamfinallysettledthematterinfavorofboundarymigration.

1.2.1.3ParametersAffectingRecrystallization

By1920,manyoftheparametersthataffecttherecrystallizationprocessandtheresultant microstructurehadbeenidentified.

Kinetics:Therelationshipoftherecrystallizationtemperaturetothemeltingtemperature wasnotedbyEwingandRosenhain(1900)andHumfrey(1902)showedthattherateof recrystallizationincreasedwithanincreaseinannealingtemperature.

Strain:Sauveur(1912)foundthattherewasacriticalstrainforrecrystallization,anda relationshipbetweengrainsizeandpriorstrainwasreportedbyCharpy(1910).Carpenter andElam(1920)laterquantifiedbothoftheseeffects.

Graingrowth:Inaveryearlypaperonthecontrolofmicrostructureduringannealing, Jeffries(1916)showedthat abnormalgraingrowth inthoriatedtungstenwaspromoted inspecimensinwhichnormalgraingrowthhadbeeninhibited.

Furtherdevelopmentsintheunderstandingofrecrystallizationwerenotpossiblewithouta moredetailedknowledgeofthedeformedstate.Thiswasprovidedbythedevelopmentof thedislocationtheoryin1934,andanotableearlyreviewofthesubjectfollowingthe adventofthedislocationtheoryisthatofBurgers(1941).

Fromaboutthisperioditbecomesdifficulttodistinguishthepapersofhistoricalinterest fromtheearlykeypapersthatarestillrelevanttocurrentthinking.Thelatterarecitedas appropriatewithinthevariouschaptersofthisbook.However,itmaybehelpfultothe readertohaveasourcelistofbooks,reviews,andconferencesonthesubjectfromthe past50years,whichisgivenbelow.

1.2.2SelectedKeyLiterature(1952 2003)

MonographsonRecrystallization

Byrne,J.G.(1965), Recovery,RecrystallizationandGrainGrowth.McMillan, NewYork.

Cotterill,P.andMold,P.R.(1976), RecrystallizationandGrainGrowthinMetals. SurreyUniv.Press,London. Novikov,V.(1997), GrainGrowthandControlofMicrostructureandTexturein PolycrystallineMaterials.CRCPress,BocaRaton.

Multiauthor, EditedCompilationsonRecrystallization

Himmel,L.(ed.),(1963), RecoveryandRecrystallizationofMetals.Interscience, NewYork.

Margolin,H.(ed.),(1966), Recrystallization,GraingrowthandTextures.ASM, Ohio,USA.

Haessner,F.(ed.),(1978), RecrystallizationofMetallicMaterials.Dr.RiedererVerlag,G.m.b.HStuttgart.

ReviewArticlesandBooksContainingChaptersonRecrystallization

Burke,J.E.andTurnbull,D.(1952), RecrystallizationandGrainGrowth.Progressin MetalPhys., 3,220.

Beck,P.A.(1954), AnnealingofCold-workedMetals.Adv.Phys., 3,245.

Leslie,W.C.,Michalak,J.T.andAul,F.W.(1963), Theannealingofcold-workediron In: IronanditsDiluteSolidSolutions.(eds.)SpencerandWerner.Interscience. NewYork.119.

Christian,J.W.(2002), TheTheoryofTransformationsinMetalsandAlloys.Second edition,Pergamon,Oxford.

Jonas,J.J.,Sellars,C.M.andTegart,W.J.McG.(1969), StrengthandStructureUnder HotWorkingconditions.Met.Revs., 130,1.

Martin,J.W.andDoherty,R.D.(1976), TheStabilityofMicrostructureinMetals. CambridgeUniversityPress. Cahn,R.W.(1996),in PhysicalMetallurgy.(eds.)CahnandHaasen.Fourthedition. North Holland,Amsterdam. Hutchinson,W.B.(1984), DevelopmentandControlofAnnealingTexturesinLowCarbonSteels.Int.Met.Rev., 29,25. Honeycombe,R.W.K.(1985), ThePlasticDeformationofMetals.EdwardArnold. Humphreys,F.J.(1991), RecrystallizationandRecovery.In: ProcessingofMetals andAlloys.(ed.)R.W.Cahn.VCH.Germany.371. Doherty,R.D.,Hughes,D.A.,Humphreys,F.J.,Jonas,J.J.,JuulJensen,D.,Kassner, M.E.,King,W.E.,McNelly,T.R.,McQueen,H.J.andRollett,A.D.(1997), Current issuesinrecrystallization:areview.Mats.Sci.&Eng., A238,219. Verlinden,B.,Driver,J.,Samajdar,I.,andDoherty,R.D.(2007), Thermomechanical ProcessingofMetallicMaterials,Elsevier.

ProceedingsofInternationalConferences

InternationalRecrystallizationConferenceSeries(1990 1999)

Chandra,T.(ed.),(1991), Recrystallization’90.TMS,Warrendale,USA. Fuentes,M.andGilSevillano,J.(eds.),(1992), Recrystallization’92.Trans.Tech. Pubs.Switzerland.

The force, F,ontheboundaryisgivenby dG/dx,andthe pressure, P,ontheboundary,is givenby F/a,andthus

If DGin Eq.(1.2) isgiveninunitsofJ/m3,thenthepressureontheboundary(P)isin N/m2.Thereissomeconfusionintheliteratureregardingterminology,andtheterms force onaboundary and pressureonaboundary arebothusedfortheparameterthatis definedaboveby P.Since P hasunitsofN/m2,whicharethoseofpressure,thereissome logicinusingtheterm pressure,andthereforeweadoptthisterminology.

1.3.2UnitsandtheMagnitudeoftheDrivingPressure

Althoughwewillbediscussingtheforcesandpressuresactingonboundariesinsome detailinlaterchapters,itisusefulatthisstagetoexamine,withexamples,someofthe forcesinvolvedinannealing.Thiswillservetodemonstratethe units usedinthebookand alsotogivesomeideaoftherelativemagnitudesoftheforcesinvolvedinannealing.A gooddiscussionofforcesarisingfromavarietyofsourcesisgivenbyStu ¨ we(1978).

1.3.2.1Recrystallization:DrivingPressureDuetoStoredDislocations

Thedrivingforceforrecrystallizationarisesfromtheeliminationofthedislocations introducedduringdeformation.Thiscanbeestimatedbyformingtheproductofthe energyperunitlengthofadislocation(i.e.,thelinetension)andthedislocationdensityas linelengthperunitvolume.Accordingly,thestoredenergyduetoadislocationdensity r is w0.5 rGb2,where G istheshearmodulusand b theBurgersvectorofthe dislocations.Adislocationdensityof1015 1016 m 2,whichistypicalofthecold-worked stateincopper(G ¼ 4.2 1010 N/m2, b ¼ 0.26nm)thereforerepresentsastoredenergy of w2 106 2 107 J/m3 (w10 100J/mol)andgivesrisetoadrivingpressurefor primaryrecrystallizationof w2 20MPa.

1.3.2.2RecoveryandGrainGrowth:DrivingPressureDuetoBoundaryEnergy

Recoverybysubgraincoarseningandgraingrowthfollowingrecrystallizationareboth drivenbytheeliminationofboundaryarea.Iftheboundaryenergyis g perunitarea and theboundariesformathree-dimensionalnetworkofspacingD,thenthedrivingpressure forgrowthisgivenapproximatelyas3g/D.Iftheenergyofalowanglegrainboundary (gs)is0.2J/m2,andthatforahighangleboundary(gb)is0.5J/m2,wefindthat

P w0.6MPa forthegrowthof1 mmsubgrainsduringrecovery,andthat P w10 2 MPa forthegrowthof100 mmgrains.

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