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A Mechanism for the Formation of Lower Bainite

G. SPANOS, H.S. FANG, and H.I. AARONSON

A diffusional mechanism for the formation of lower bainite is proposed based primarily on transmission electron microscopy (TEM) observations of isothermally reacted specimens of Fe- C-2 pct Mn alloys. The mechanism involves the initial precipitation of a nearly carbide-free ferrite "spine," followed by sympathetic nucleation of "secondary (ferrite) plates" which lie at an angle to the initial "spine." Carbide precipitation subsequently occurs in austenite at ferrite: austenite boundaries located in small gaps between the "secondary plates." An "an- nealing" process then occurs in which the gaps are filled in by further growth of ferrite and additional carbide precipitation; the annealing out of fenite: ferrite boundaries between impinged "secondary plates" completes this process. This annealing stage contributes to the final ap- pearance of lower bainite sheaves as monolithic plates containing embedded carbides. The pres- ent mechanism accounts for the single variant of carbides oriented at an angle to the sheaf axis repeatedly reported in lower bainite; it is also consistent with the previous observation of one "rough" side and one "smooth" side of lower bainite "plates."

I.

INTRODUCTION

ALTHOUGH there were many observations of the microstructure now known as bainite in steel prior to 1930 (as summarized by Hultgren[q) and the morphological features of this constituent, to the extent that they could be characterized by optical microscopy, were well de- scribed by Robertson t2j in 1929, it was not until the fa- mous paper published in the following year by Davenport and BainI31on the time-temperature-transformation (TTT) diagram that the bainite reaction was taken seriously as a major mode through which the decomposition of aus- tenite can take place. Mehl t4] made an important contri- bution to the nomenclature of this reaction in 1939 when he divided the morphology of ferrous bainites into two categories, "upper" and "lower" bainite, named in ac- cordance with the temperature regions in which each ap- pears. Although no such division of bainites formed in substitutional nonferrous alloys has so far been reported, this categorization has been widely accepted and utilized in steels. Lower bainite has occupied a position of particular prominence with respect to evaluations of the basic mechanism of the bainite reaction. These evaluations, which have been undertaken repeatedly since 1930, largely revolve around the issue of whether the unit atomic pro- cess through which iron atoms are transported across austenite:ferrite boundaries is one of shear or of diffu- sional jumps. That the driving force for these jumps is

G. SPANOS, formerly Graduate Student, Carnegie Mellon University, is with the Physical Metallurgy Branch of the Naval Research Laboratory, Washington, DC 20375-5000. H.S. FANG, formerly Visiting Professor, Carnegie Mellon University, is Professor, Division of Metallic Materials, Department of Mechanical Engineering, Tsinghua University, Beijing 100084, People's Republic of China. H.I. AARONSON, R.F. Mehl Professor, is with the Department of Metallurgical Engineering and Materials Science, Carnegie Mellon University, Pittsburgh, PA 15213. This paper is based on a presentation made in the symposium "International Conference on Bainite" presented at the 1988 World Materials Congress in Chicago, IL, on September 26 and 27, 1988, under the auspices of the ASM INTERNATIONAL Phase Transfor- mations Committee and the TMS Ferrous Metallurgy Committee.

METALLURGICAL TRANSACTIONS A

the chemical free-energy change attending the trans-

formation of austenite to ferrite is rarely disputed. There also seems to be general agreement that, at least in dis- tinctly hypoeutectoid alloys, the first formed product of

the transformation is

trum of opinion about the relative contributions of these 9two fundamental mechanisms of atomic attachment is now available, especially as a function of isothermal reaction temperature. At one extreme, Widmanst~itten ferrite (containing few if any carbides), upper bainite, and lower bainite are all considered to form by high-velocity shear. At the other extreme, all of these transformation prod- ucts are taken to develop through diffusional mecha- nisms, with only martensite forming by a shear process. Probably the majority opinion is that the contribution of shear increases with decreasing temperature. Numerous investigators thus adhere to the view that the formation of lower bainite, at the least, takes place by shear./6-91 Conversely, several criticisms against a shear mecha- nism for bainite formation have been made previ- ously;tl~ hence, only a few of the major topics of this debate which are pertinent to the present model of lower bainite formation will now be briefly considered. One of the strongest arguments for the growth of lower bainite plates by shear is the now "classic" presence of elongated carbides lying at an angle of approximately 55 to 60 deg to the longitudinal axis of the plates. I8,16-~9]An obvious mechanism through which these carbides form is by the precipitation from the (necessarily highly super- saturated) ferritic component of lower bainite. In view of the much higher diffusivity of carbon in ferrite [2~ than in austenite, [2q both acquisition and retention of suffi- cient carbon supersaturation to account for the large volume fractions of carbides often found within lower bainite require that its ferritic component grow at rates well above those allowed by the diffusion of carbon in austenite away from the growing bainite plates, i.e., by shear taking place at quite high velocities. [~,l~ How- ever, there is still no reliable experimental evidence for such high growth rates, as discussed in detail in another paper in this symposium, u3] One of the most puzzling features of this mechanism is the repeated observation

ferrite. I5] However, a broad spec-

VOLUME 21A, JUNE 1990-- 1381

that nearly all carbide plates or rods precipitate parallel to only one crystallographic variant of their habit plane in the ferritic component of a given lower bainite plate. I8,~6-191This is in contrast to tempered martensite, where carbide precipitation parallel to multiple members of the same crystallographic form is repeatedly ob- served. [23-261Insofar as the present authors are aware, the only explanation offered for this phenomenon on the basis of.precipitation wholly within ferrite is that the carbides form along parallel twins created in the bainitic ferrite plates while these plates grow by a shear mechanism. [271 However, twins have not been observed in lower (or in upper) bainite. 17'271 A substantial body of experimental evidence has now been accumulated suggesting that this view of lower bainite formation is incorrect. Smith et a1.128~have thus observed with hot-stage optical microscopy the forma- tion of martensite occurring with great rapidity, while that of lower bainite is simultaneously taking place very slowly at reaction temperatures below Ma. Speich I291 subsequently reported measurements of both the length- ening and thickening kinetics of lower bainite plates with the same technique in hypereutectoid Fe-C and Fe-C-X alloys. He satisfactorily rationalized these measurements in terms of diffusional growth. A more recent report based upon photoemission electron microscopy, that lower bainite plates in an Fe-0.34 wt pct C-2.02 wt pet Si-3.0 wt pct Mn alloy lengthen much more rapidly than carbon diffusion in austenite will allow, [9J may be due instead to bainite-stimulated martensite formation occurring well above the Ms temperature, as observed by Smith eta/. [281

and

Oka. [30]

recently characterized

in

detail

by

Okamoto

and

Crystallographic arguments in favor of carbide nucle- ation predominantly within the ferritic component of lower bainite [81 are often ambiguous. I31'32J In particular, Shackleton and Kelly I311showed that the Bagaryatski [331 orientation relationship between ferrite and cementite observed in lower bainite, [3~1which is the same as that found in tempered martensite, [33'34'351can be explained just as well in terms of precipitation of certain variants of both ferrite and cementite directly from austenite.~27~ Orientation relationship arguments that the ferrite forms by shear [6,36] are diminished by the finding that lower bainite and martensite formed in the same alloy have quite

different crystallographies. [371 The appearance of

shaped rather than invariant plane strain surface relief effects in association with lower bainite plates t29]further detracts from arguments in favor of a shear mechanism for the formation of lower bainite, since it has been dem- onstrated that diffusional transformation products can yield tent-shaped reliefsI38,39'4~ wheareas martens[tic products should not do so. On the basis of this background, the question of the mechanisms through which lower bainite develops is en- gaged in this paper. Instead of shear, purely diffusional ledgewise migration of partially coherent ferrite: austenite boundaries and sympathetic nucleation [411of ferrite crys- tals at the ferrite: austenite boundaries of previously formed ferrite crystals will be utilized to develop a new trans- formation mechanism capable of explaining the distri- bution and morphology of carbides within lower bainite. This mechanism will be based primarily on an optical

tent-

1382--VOLUME 21A, JUNE 1990

and transmission electron microscopy (TEM) investiga- tion of lower bainite morphology in both hypo- and hypereutectoid Fe-C-Mn alloys.

II.

EXPERIMENTAL

PROCEDURE

Six high-purity Fe-C- -2

pct Mn alloys* and a single

*All compositions are expressed in weight percent; the exact man- ganese content in each of these alloys is actually within -+0.2 pct of 2 pct.

Fe-0.1 pct C-2.9 pct Mn alloy were employed in this in-

vestigation. In the former alloys, the carbon concentra- tion ranged from 0.34 to 1.37 pet. The composition and

alloys used are listed

in Table I. The TEM results presented here are centered on one hypoeutectoid alloy (0.34 pet C) and one hyper- eutectoid alloy (0.95 pet C). The heat treatment and TEM procedures utilized are described in Reference 43. [431

estimated Ms temperature [42Jof all

III. RESULTS AND PROPOSED MECHANISM

Before presenting the findings of the present investi- gation, it is necessary to note that the term "sheaf" was originally employed to describe a packet of precipitate plates, particularly of ferrite, formed by successive "face- to-face" sympathetic nucleation, [41,441 as shown sche- matically in Figure 1. Sympathetic nucleation has been defined as the nucleation of a precipitate crystal at the interphase boundary of another precipitate crystal of the same phase when the matrix and precipitate differ con- tinuously in composition. [41,441The dashed lines across these plates drawn perpendicular to their broad faces in- dicate that "edge-to-edge" sympathetic nucleation 144,45] has also occurred and has participated in their length- ening. Oblak and Hehemann [TJ have also reported this type of microstructure but interpreted it differently, as is

considered in Section IV.

mission electron micrographs [1~ indicate that the fer- ritic component of upper bainite consists primarily of single intragranular plates (or laths [271)and closely spaced sideplates (or laths I271) at higher temperatures but in-

creasingly of sheaves of sideplates and of intragranular plates at lower temperatures. These sheaves are predom- inantly of the type sketched in Figure 1. In the lower bainite region, we shall now demonstrate that the ferritic component also consists of sheaves of crystals but with a different and considerably more complex geometry. Unlike upper bainite, many of the individual plates in a sheaf will be shown to make an appreciable angle with respect to the axis of the sheaf as a whole. Given this background, the proposed mechanism for lower bainite formation will now be presented concurrently with the experimental observations. On the present model, the initial element of a lower bainite sheaf* is evidently a single, nearly carbide-free

Published optical and trans-

*For reasons which will become apparent, this paper uses the term lower bainite "sheaf" to refer to the microstructure which has in the past been termed a lower bainite "plate." [8,27,471

ferrite plate. Figures 2(a) and (b) are bright- and dark- field TEM micrographs of a lower bainite sheaf formed at 250 ~ in an Fe-0.95 pct C-1.93 pet Mn alloy. The

METALLURGICAL TRANSACTIONS A

Table I.

Alloy Compositions and Estimated M,* Temperatures

Wt Pct C

Wt Pct Mn

Wt Pct Si

Wt Pct P

Wt Pct S

Ms (~

0.10

2.90

0.02

0.004

0.005

448

0.34

1.90

0.003

0.004

0.005

337

0.57

1.99

0.007

0.003

0.003

243

0.77

1.94

0.003

0.002

0.003

185

0.95

1.93

<0.01

0.003

0.003

146

1.12

1.82

0.003

0.003

0.004

131

1.37

1.99

0.005

0.003

0.002

104

*Estimates were made from formulas compiled by Andrews. [42j

heavy arrow in each of these figures points out the ini- tiating ferrite plate. Once the initiating ferrite plate of a sheaf, which may be termed its "spine," has appeared, other ferrite crystals are then sympathetically nucleated at it but often on only one of its two broad faces, as in Figure 2. These crys- tals, whose morphology often appears to approximate that of a thick plate, frequently develop at a marked angle to the spine. Figure 3(a) shows another example of this structure near the tip of a lower bainite sheaf. In Figure 3(b), the higher magnification employed permits observation of serrations at the sides of the sheaf, de- veloped where the individual "secondary plates" have lengthened unequally, perhaps because they nucleated at different times. Figure 4 illustrates this type of structure in the 0.34 pct C alloy; gaps between adjacent "second- ary plates" are evident (indicated by arrows in Figure 4). The third step in this process is the precipitation of carbides in the small gaps between "secondary plates" (which may have already impinged along other portions of their interphase boundaries). In the present alloys, electron diffraction studies indicated that the carbide was cementite. A typical example of the diffraction analysis is shown in Figure 5. (Also note the ferrite spine in Figure 5(a).*) These carbides were presumably nu-

*The appearance of a few carbides in the region of the spine shown in Figure 5(a) is most likely due to a stereological effect in which the carbides associated with sympathetically nucleated ferrite plates over- lap the spine, either above or below the spine, within the TEM foil. However, it is also possible that some carbide precipitation occurred at austenite:ferrite boundaries of spines at boundary orientations where their growth was markedly slowed by a low density of growth ledges and later resumed, or reinitiated, by sympathetic nucleation, t44,451

cleated at the austenite: ferrite boundaries forming the sides of the gaps in the same manner that carbide precipitation occurs between ferrite laths in upper bainite. Extensive overlap within the austenite gaps of carbon diffusion fields associated with the adjoining ferrite must markedly in- crease the carbon concentration in the gaps and thereby diminish the migration kinetics of the ferrite:austenite

(

Fig.

(-

1-

i

)

 

i

)

 

I

I

!

 

C

 

"

'

'

)

!

I

Schematic representation of an upper bainite "sheaf."

METALLURGICAL TRANSACTIONS A

boundaries (partially) enclosing the gaps. More time is thus available for carbide nucleation at the austenite: ferrite interface. The fourth and final stage in the development of a lower bainite sheaf is further ferrite growth around the carbides, and perhaps additional carbide precipitation, until the small amount of austenite remaining in the gaps has been decomposed. If a significant proportion of Si is present in the alloy, though, both the third and fourth steps of this sequence can be greatly inhibited. The overall external shape of the sheaf will thus quickly lose its initial serrated appearance and will soon more nearly resemble that of a lenticular ferrite monocrystal

nearly resemble that of a lenticular ferrite monocrystal (a) (b) Fig. 2--A pct Mn reacted lower

(a)

nearly resemble that of a lenticular ferrite monocrystal (a) (b) Fig. 2--A pct Mn reacted lower

(b)

Fig. 2--A

pct Mn reacted

lower bainite sheaf formed in Fe-0.95 wt pct C-1.93 wt

for 15,000 s: (a) bright-field TEM micro-

at

250 ~

graph and (b) corresponding dark-field micrograph.

VOLUME 21A, JUNE 1990-- 1383

(a) (b) Fig. 3 -- Leading tip of a lower bainite sheaf in Fe-0.95 wt

(a)

(a) (b) Fig. 3 -- Leading tip of a lower bainite sheaf in Fe-0.95 wt pct

(b)

Fig. 3 -- Leading tip of a lower bainite sheaf in Fe-0.95 wt pct C- 1.93 wt pct Mn reacted at 250 ~ for 15,000 s: (a) lower magnification view and (b) higher magnification image showing serrations at the sides of the sheaf.

containing embedded carbides. As illustrated in Figure 6, this "smoothing" process occurs with sufficient rapidity

so that the polycrystalline nature of the sheaf can be de-

tected only near its leading edge, where this process was

terminated by quenching.* At the same time, migration

*Note that the long boundaries discerned near the center and lower right-hand portions of the sheaf in Figure 6 (and which lie parallel to the sheaf axis) are not the ferrite:ferrite boundaries between second- ary sideplates discussed throughout the text. The latter boundaries are only visible near the leading edge (e.g., see the higher magnification micrographs of Figures 3 and 4). The former boundaries apparently result from impingement of multiple ferrite "spines." Such spines have been "caught" at an earlier stage (before impingement) in the micro- graphs in Figures 2 and 8.

of small-angle grain boundaries formed by impingement

between adjacent ferrite crystals within a sheaf will soon remove much of the internal evidence that many crystals

were involved in the development of the sheaf, much in the same manner as an annealing or recovery process, e.g., during the tempering of martensite. I23~Addition- ally, after complete impingement has occurred along the

broad faces of ferrite sideplates, since their relative mis- orientation should be very small, such boundaries ex- hibit very weak contrast-- and may even be nonexistent.

A large portion of the sheaf shown in Figure 6 thus ap-

pears, except upon closest inspection, to be simply the product of the precipitation of carbide plates parallel to but a single habit plane within a large single crystal of ferrite.

Recapitulating this mechanism through the sequence

1384--VOLUME 21A, JUNE 1990

mechanism through the sequence 1384--VOLUME 21A, JUNE 1990 Fig. 4--Gaps (indicated by arrows) between ~secondary

Fig. 4--Gaps (indicated by arrows) between ~secondary ferrite plates" near the tip of a lower bainite sheaf in an Fe-0.34 wt pct C-1.90 wt pct Mn alloy reacted at 350 ~ for 40 s.

of sketches (which are greatly simplified for the pur-

poses of illustration) in Figure 7, a carbide precipitation process emerges which differs significantly from that of precipitation of a single variant of carbides entirely from ferrite. Carbide precipitation in lower bainite is now sug- gested to occur at the austenite: ferrite boundaries of the "secondary plates," predominantly from austenite (as will be considered further in Section IV). In effect, then, the sequence proposed in Figure 7 is essentially the same as the one which is widely accepted for upper bainite, i.e., precipitation of carbides at t~: y boundaries forming nar- row "pockets" or "gaps" of carbon-enriched austenite

between upper

ference between the development patterns of sheaves of upper bainite plates and those of lower bainite plates ap- pears to be that the ferritic component of lower bainite sheaves is composed of one or a few long "spines" plus a number of shorter plates making a substantial angle with respect to the spines, while the ferrite plates (or laths) in upper bainite form by face-to-face sympathetic nucleation. The fine scale on which the sympathetic nucleation and the growth of ferrite plates occur in the lower bainite region and the swift obscuration of the initial micro- structure are probably the principal reasons why pre- vious investigators have not discerned the present mechanism for the formation of lower bainite. Addi- tionally, the thin ferrite spines are often difficult to de-

tect even by TEM unless the lower bainite sheaf is prop- erly oriented in the microscope such that the secondary sideplates (and the corresponding carbides which form between them) do not overlap the spine in the field of view. Nevertheless, some common features between the current mechanism and previous models will be consid- ered in Section IV. Two complications in the morphology of ferrite within lower bainite sheaves must now be briefly noted. Figure 8, an enlargement of a portion of Figure 2(a), demonstrates that multiple ferrite "spines" (pointed out by arrow- heads) are present in some sheaves. These are often both

bainite plates, t8,46~Thus, the major dif-

METALLURGICAL TRANSACTIONS A

Fig. 5--Fe-0.95 wt pct C-1.93 wt pct Mn reacted at 250 ~ reflection, and (c)

Fig. 5--Fe-0.95 wt pct C-1.93 wt pct Mn reacted at 250 ~

reflection, and (c) corresponding diffraction pattern. Small circles in (c) represent cementite reflections.

for 15,000 s: (a) bright-field TEM, (b) dark-field TEM taken from a 113 carbide

shorter and thinner than the spine first formed. Length- ening rapidly, such spines would physically prevent fur- ther lengthening of large numbers of secondary plates (formed earlier), as shown in Figure 8. Several ferrite "spines" can thus be discerned in the lower bainite sheaf

can thus be discerned in the lower bainite sheaf Fig. 6--Lower magnification bright-field TEM image of

Fig. 6--Lower magnification bright-field TEM image of the lower bainite sheaf corresponding to Fig. 4, illustrating the smooth character of the sheaf boundary further from the tip.

METALLURGICALTRANSACTIONS A

shown in Figure 5 of Hehemann's tS] well-known review of the bainite reaction, reproduced here in Figure 9. The second complication in the morphology of ferrite in lower bainite sheaves to be noted is the strong ten- dency for individual ferrite crystals within these sheaves to form facets diagonally across their leading edge. This feature is, of course, most readily observed at the lead- ing tip of a sheaf, as illustrated in Figure 10; arrowheads point out prominent examples of such facets. Ohmori et al. t48]also drew attention to facets of this type in their sketches of bainite sheaves, emphasizing their potential for serving as nucleation sites for bainitic carbides. Car- bides growing "allotriomorphically" or as plates along

growing "allotriomorphically" or as plates along Fig. 7-- Sketch of the proposed mechanism for lower bainite

Fig. 7-- Sketch of the proposed mechanism for lower bainite formation.

VOLUME 21A, JUNE 1990-- 1385

I
I

Fig. 8--Enlargement of Fig. 2(a) revealing multiple ferrite spines.

such facets probably contribute to the carbide population whose long axis lies at about 55 to 60 deg with respect to the longitudinal axis of the sheaves. In regard to the carbide morphology within lower bainite sheaves, the dark-field micrographs of Figures 1l(a) and (b) indicate that the aligned carbides are not monolithic plates but, rather, are individual carbide crystals nu- cleated side by side, presumably along austenite:ferrite boundaries. Some have probably grown laterally into contact, while others may have been sympathetically nu- cleated at the edges of carbides formed a little earlier along these boundaries. The morphology of an aggregate

along these boundaries. The morphology of an aggregate Fig. 9--TEM micrograph of lower bainite in 4360

Fig. 9--TEM micrograph of lower bainite in 4360 steel reacted at 275 ~ taken from Ref. 8 (magnification was not reported).

1386--VOLUME 21A, JUNE 1990

was not reported). 1386--VOLUME 21A, JUNE 1990 Fig. 10--Facets at crystals at the leading tip of

Fig. 10--Facets at crystals at the leading tip of a lower bainite sheaf in Fe-0.34 wt pct C-1.90 wt pet Mn reacted for 40 s at 350 ~

of many such individual carbide crystals seems better described as interphase boundary allotriomorphs than as plates.

IV.

DISCUSSION

A. Origin of the Transition from Upper to Lower

Bainite Sheaves

The most likely explanation of why edge-to-face sym- pathetic nucleation of secondary plates against a broad face of the ferrite spine appears in the lower but not in the upper bainite region is as follows. The higher driving force for ferrite nucleation available in the lower bainite regime simply makes the higher work of formation (AF*) of edge-to-face critical nuclei for sympathetic nucleation of ferrite, relative to the AF* for face-to-face sympa- thetic nucleation, t441 a competitively surmountable bar- rier at these temperatures. For example, calculations of the driving force for nucleation of ferrite have shown that a decrease in temperature from 500 ~ (in the upper bainite range) to 350 ~ (within the lower bainite range) in the Fe-0.34 wt pct C-1.90 wt pct Mn alloy can lead to a 50 pct reduction in AF* for a given critical nucleus geometry and interfacial energy. 143j

B. Some Questions Associated with the Present

Mechanism for Formation of Lower Bainite Sheaves

Speich t291has found that lower bainite plates formed in an Fe-0.66 pct C-3.32 pct Cr steel yield a tent-shaped surface relief effect. This appears inconsistent with the present view that lower bainite consists of sheaves of secondary plates sympathetically nucleated at one broad face of (usually) a single or a few ferrite spine(s).* How-

*Speich also concluded that sympathetic nucleation does not appear to be operative during the formation of the lower bainite structures he studied. However, the lesser resolving power of the observational techniques he employed, optical and replication electron microscopy, may have prevented observation of the fine (and easily obscured) structural features which led the present authors to the opposite conclusion.

METALLURGICALTRANSACTIONSA

Fig. 11--Lower bainite formed in 0.95 wt pct C-1.93 wt pct Mn re- acted at

Fig. 11--Lower bainite formed in 0.95 wt pct C-1.93 wt pct Mn re- acted at 200 ~ for 130,000 s: (a) dark-field micrograph taken from a carbide reflection and (b) lower magnification dark-field image.

ever, since the spines have a thickness of about 0.2/xm or less and may often lie below the plane of polish, they are not resolvable with optical microscopy. Conse- quently, the reliefs observed should be those produced by the array of parallel secondary plates. On the other hand, such an array ought to introduce a considerable

substructure into the surface relief effect, again on a very fine scale, and perhaps also not detectable with optical interference microscopy. A further question about lower bainite sheaf mor- phology is why do secondary plates often form on only one side of many of the ferrite spines? Hehemann has long emphasized that lower bainite "plates," which the present authors refer to as sheaves, often have one smooth side and one rough, with growth evidently occurring only

observation, made mainly with

on the rough side. tS~This

METALLURGICAL TRANSACTIONS A

replication electron and optical microscopy, is com- pletely consistent with the present TEM observations. The "smooth" side is now shown to correspond to an initiating ferrite spine, and the "rough" side is formed by the leading edges of the secondary plates. Hence, this question becomes one of explaining the asymmetry of sympathetic nucleation on opposite sides of the initiating spine. Although the current experimental findings do not provide a direct answer to this question, a possible ex- planation will now be offered. On a recent analysis of sympathetic nucleation, t44~it may be postulated that the nominally smooth side of the spine actually has a higher density of growth ledges than the side at which second- ary plates are sympathetically nucleated. The larger the average intededge distance, the longer is the time avail- able for sympathetic nucleation on the terraces and, thus, the smaller is the probability that the newly formed crys- tals will be overrun by an advancing ledge. ~44jHowever, the origin of the postulated unequal densities of growth ledges on opposite broad faces of a "spine" remains un- certain--a somewhat unsurprising situation in view of the difficulties being encountered in explaining the for- mation kinetics of growth ledges.j491

C. On the Crystallography of Secondary

Sideplate Formation

An obvious question which arises is why the broad faces of "secondary sideplates" lie at a characteristic angle of approximately 55 to 60 deg [47,5~ to the "spine" when the {111}~ atomic habit planes of ferrite plates tS~j form 70.5 deg angles with respect to one another (within a given matrix austenite grain). A survey of published thin foil and replication TEM micrographs [7,27'46,48,521of lower bainite sheaves showed that the apparent angle (i.e., not corrected for stereological effects) between the carbide direction and the sheaf axis actually varies between 46 and 67 deg, with 70 pct of the angles lying between 55 and 61 deg; a determination of the true angle by trace analysis procedures from a statistically acceptable num- ber of plates has yet to be reported. Nevertheless, the often quoted angle of 55 tS~ or 60 deg [471appears to be somewhat restrictive. Previous optical microscopy studies of lower bainite "plates" have shown considerable scatter in the habit plane at a given temperature as well as a change in the range of habit planes observed with decreasing tempera- ture. t4,531The habit planes measured by optical micros- copy are now seen to be those averaged over all the crystals comprising a given lower bainite sheaf; both structural and growth ledges at ferrite:austenite inter- faces can cause even further deviation of the atomic habit plane from that observed by optical microscopy, rS1}As far as the present authors are aware, the only study in which the atomic habit plane between ferrite and aus- tenite has been deduced is that of Rigsbee and AaronsontSl~ for ferrite plates formed at 450 ~ to 475 ~ in an Fe- 0.62 pct C-2.0 pct Si alloy. They reported triatomic structural ledges spaced between 2.2 and 3.6 nm apart, which cause the apparent habit plane, observed by con- ventional TEM techniques, to deviate by as much as 18 deg from the atomic habit plane, which was found to be {111}~/{110}~. Thus, if the atomic habit plane of the

VOLUME 21A, JUNE 1990--1387

spine and the sideplates in lower bainite sheaves are dif- ferent variants of {11 1}J{1 10}~, the presence of such ledges could account for the presence of angles smaller than 70.5 deg between the apparent habit planes of these variants.* The variations of the apparent habit plane re- ported by Rigsbee and Aaronson could thus explain the range of apparent angles between the carbides and the overall sheaf axis observed in the literature.**

*The almost invariable presence of martensite above and below the bainite sheaves, especially in the vicinity of the tip and the thin initiating "spine," and the high volume fraction of carbides resulted in the appearance of so many superimposed spots in the selected area diffraction patterns that the misorientation between the thin initiating spine and the "sideplates" could not be determined with any confidence. **The precise magnitude of the true angle is not critical to this explanation; the pertinent issue is that a single variant of carbides (lying at an appreciable angle to the sheaf axis) has been repeatedly observed in lower bainite. 17,~7,'z-45.5~

D. Mechanism and Kinetics of "Subunit" Growth and the Origins of Bainitic Carbides

As noted in the Introduction, the present mechanism for lower bainite formation is based upon diffusional

growth of ferrite (and, implicitly, also of carbides). Also,

Hehemann tT] have

postulated that individual ferrite plates (which they termed "subunits') within sheaves grow at much higher than diffusion-limited velocities, sufficient to provide the high carbon supersaturation in ferrite which is a prerequisite to extensive carbide precipitation within ferrite plates. Kinsman and Aaronson employed thermionic emission electron microscopy to demonstrate that individual fer- rite plates (a term the present authors prefer to "sub- unit," with its connotation of subboundaries formed by polygonization) within upper bainite sheaves grow at ap- proximately the rates permitted by the diffusion of car- bon in austenite, tl~ Equivalent experiments are now required on lower bainite. A useful deduction can be made, though, from the failure of lower bainite to grow at high velocities below Ma. [28] Strain energy is consid- ered to be the factor limiting the growth of individual ferrite plates or "subunits" to small fractions of the ex- ternal dimensions of a sheaf. [7a~ However, sufficient driving force should be available below Ma to permit these plates to grow swiftly to the much greater lengths characteristic of martensite plates, which are also ob- served at these temperatures. [28]The failure of the overall growth kinetics of lower bainite sheaves to increase greatly below Ma, while martensite plates simultaneously grow at much greater velocities, t28] strongly implies that their

as previously remarked, Oblak and

component plates do not grow more rapidly than diffu- sion control allows, even for a short distance (e.g., the length of a "subunit'). On the diffusional growth mechanism, ferrite should contain no more carbon than that corresponding to the extrapolated ferrite/(ferrite + austenite) phase bound- ary. [l~ Analysis of X-ray diffraction data on the com- position of retained austenite associated with partial transformation to both upper and lower bainite indicates that the average carbon concentration in bainitic ferrite is even smaller than this. [~~ While these carbon concen- trations are higher than those of the extrapolated ferrite/

1388--VOLUME 21A, JUNE 1990

(ferrite + carbide) phase boundary, the portion of car- bide which can precipitate from within ferrite must, ac- cording to the Lever Rule, be very small under this circumstance. Most of the bainitic carbides should thus precipitate from austenite at ferrite:austenite interfaces. Perhaps the most striking outcome of the present mechanism is its ability to explain the "single variant" of carbides oriented at an angle with respect to the lon-

direct and natural con-

gitudinal sheaf axis [8,~6-19] as a

sequence of (interphase boundary) carbide precipitation in gaps between the broad faces of the secondary (fer- rite) plates (and, to a lesser extent, along facets of ferrite crystals at the edges of the sheaf). The single "habit plane" of these carbides is thus a consequence of the predom- inance of one orientation of secondary ferrite plates in a bainite sheaf.

E. Comparisons with Some Previous Proposals for

Lower Bainite Formation Mechanisms

Most of the previous proposals are based upon a shear mode for the formation of the ferritic component of bain- ite, followed by carbide precipitation within the ferrite. (Some authors have proposed that even the carbides in lower bainite form by shear. [54]) Attention will now be restricted to those mechanisms containing one or more elements of the formation sequence proposed as a result of the present investigation. Huang and Thomas [18]used crystallographic and mor- phological observations to conclude that carbides formed in association with lower bainite precipitate predomi- nantly from austenite at austenite:ferrite boundaries, in agreement with the present model. They particularly em- phasized that the single habit plane operative is char- acteristic of interphase boundary precipitation [47,55]rather than of carbide precipitation wholly within the ferrite phase, though their mechanism, if based upon precipi- tation at a single, essentially planar a:y boundary, is necessarily incomplete, as will now be described. Ex- plaining the single carbide "habit plane" as a result of precipitation at the broad faces of a monolithic lower bainite plate, tl8] as represented schematically in Figure 12,

-

/

~ '

' ~ "

Fig. 12--Sketch illustrating carbide precipitation at the broad face of a monolithic bainite plate.156]

METALLURGICAL TRANSACTIONS A

fails to account for the long, semicontinuous sheets of such carbides making a "55 to 60 deg" angle with re- spect to the interface, rather than lying parallel to the interface, as occurs during interphase boundary carbide precipitation at the broad faces of (nearly) monolithic grain boundary ferrite allotriomorphs. [47]As was briefly mentioned in Section III, Ohmori et al. t4sl also sug- gested that the carbides precipitate from the austenite phase

at a: y boundaries. In particular, they proposed that car-

bide precipitation may occur at facets on these bound- aries (at the edges and faces of ferrite plates) which make

a marked angle with respect to the overall sheaf axis

(Figure 13). Both investigationst~8,481were apparently made

on heavily transformed specimens in which many bainite sheaves had impinged; hence, detailed observations were not reported on the morphology of the leading edges of the sheaves.

Insofar as the present authors are aware, the only pre- vious investigation in which the tips of lower bainite sheaves were imaged by TEM at reasonably high mag-

nifications is

graphs also reveal one smooth side and one serrated side of lower bainite "plates" (at magnifications -<20,000 times); they indicated that a "substructure" of thin ferrite plates appears to be present. However, they essentially adhered to Hehemann's tsl proposal that the carbides pre- cipitate solely within ferrite which has formed by shear.

that of Yada and Ooka. t571 Their micro-

V.

CONCLUSIONS

In this paper, a diffusional mechanism for the for- mation of lower bainite sheaves has been proposed based

on TEM observations on specimens of Fe-C- ~2 pct Mn alloys which usually contained a relatively low (less than about 30 pct) volume fraction of bainite. The mecha- nism can be summarized in four steps (depicted schematically in Figure 7): (1) precipitation of a nearly carbide-free ferrite "spine"; (2) sympathetic nucleation of "secondary plates" of ferrite, usually on only one side

of and at an angle of approximately 55 to 60 deg to the

initiating "spine"; (3)precipitation of carbides in aus- tenite at a: y boundaries forming gaps between adjacent "secondary (ferrite) plates"; and (4) an "annealing" pro- cess in which the gaps are filled in with further growth of ferrite and additional carbide precipitation, causing the sheaf to lose its initial serrated appearance not far behind its leading edges. Annealing out of ferrite: ferrite boundaries formed by lateral impingement of adjacent "secondary plates" further contributes to the appearance of lower bainite sheaves as monolithic ferrite plates containing embedded carbides. The ferrite "spine"

Cementite

Fig. 13--Schematic representation of the mechanism of carbide pre- cipitation suggested by Ohmori et al. 1481

METALLURGICAL TRANSACTIONS A

corresponds to the "smooth" side of lower bainite "plates" first observed by Oblak and Hehemann t71 and sub- sequently reported by others, t571 The present mech- anism accounts for the single variant of carbides at an angle to the sheaf axis observed repeatedly in lower bainite, ts'16-191as a direct consequence of carbide precip- itation at the broad faces (and, to a lesser extent, on facets) of "secondary ferrite plates" lying at a large angle to the initiating ferrite spine.

ACKNOWLEDGMENTS

The authors express their appreciation to the National Science Foundation for support of this work through Grant No. DMR81-1907 to the Carnegie Mellon University Materials Research Laboratory. Appreciation is also ex- pressed to Professor W.T. Reynolds, Jr. for his careful review of this manuscript and Professor Helio Goldenstein for many helpful discussions.

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METALLURGICALTRANSACTIONS A