Numerical Solidification

Analysis

of Solute

Redistribution

during

Accompanying

o/r Transformation*

By Sumio KOBA YASHI,* Tsuneaki NAGAMICHI** and Koki GUNJI** *

Synopsis A mathematical method is presented to quantify solute redistribution during solidification with a/' transformation; new methods to solve the equation of diffusion numerically and to estimate the equilibrium phase diagram of multi-componentlow alloyed steel are described. Thermal analysesof low alloyedsteels were made to verify the mathematical method described. It has been shown that the unequilibrium phase diagram of low alloyed steelfor a given cooling rate can be predicted by this method. Key words: mathematical modeling; numerical simulation; solidification; segregation; diffusion; carbon steel; o/' transformation; phase diagram.

Gn = kn/rCi, on the o/r phase boundary, ........................(1-2) where, Cn : the concentration of element n in p phase kn/q: the equilibrium distribution coefficient between p and q phases superscripts S, L : the solid and liquid phase, respectively. The definition of the concentration parameter introduced in the present paper, C,, is as the following : On _' Cn/kS/L.........................(2) The parameter Gn is singly valued and continuous everywhere, because kn/r _ kn/L/kr'L (3)

Introduction Solute redistribution during solidification affects the various aspects of the behavior of solidifying steel such as micro- and macro-segregation, formation of solidification crackings, depression of solidification point and initial alloy composition for peritectic reaction. However, mathematical analyses of the solidification with oIr transformation have not been understood."2~ The following problems still remain : (1) a method to predict the equilibrium phase diagram of steel with multiple alloy elements, and (2) a method to deal mathematically with the solute concentration on o/r phase boundary, where the solute concentration has two values. The present paper describes a mathematical model which overcomes the problems mentioned above. In the model, the equilibrium phase diagram of steel is predicted on the assumption that the steel exhibits the Raoultian ideal behavior, and the mathematical treatment of the solute concentration on a/r phase boundary is simplified by introducing a new concentration parameter which is singly valued and continuous everywhere. A computational method for the mathematical model is also presented. Further, thermal analyses of several steels were executed to validate the mathematical model proposed. II. Analytical Model In the present model for the dendritic solidification, the assumptions described below are adopted. (1) The local equilibrium is assumed on the phase boundary: Cn = kn/LCn, S = a or r, on the liquid-solid interface, ........................................(1-1) and,
* Based on the papers presented to the 110th ISIJ Meeting, October

I.

(2) Dendrite morphology is taken to be platelike and a volume element shown in Fig. 1 is considered. In Fig. 1, solidification starts at the position of X=O, and ends at X=Lo. The length of the volume element Lo corresponds to a half of dendrite spacing. (3) All of the equilibrium distribution coefficients are constant in the whole range of composition and temperature analyzed. (4) Solute diffusion in the liquid phase is complete and is represented in the solid phase by the following equation of diffusion :

a (knlLC = a Dn(T) a (kn/LGn), ......... (4) n) ax at ax

where Dn is the diffusion coefficient of element n in the solid phase and is a function of the absolute temperature of the volume element T. (5) The temperature T is uniform in the volume element. (6) Each phase has an identical and constant density throughout the solidification. (7) The volume element is closed to the solute transfer and the following equation of the solute conservation is assumed.

Fig.

1.

Analytical

model.

1985, 51066, at Niigata University in Nii gata

and

to the

111th

ISIJ Meeting, April 1986, S131, at The University of Tokyo in Tokyo. Manuscript received on June 17, 1987 ; form on January 14, 1988. 1988 ISIJ ** Technical Research Laboratories, Sumitomo Metal Industries, Ltd., Nishinagasu-hondori, Amagasaki 660.

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1 Lo s knlLCndx,+fLCn = C .............(5) where, fL : the fraction liquid c : the initial alloy composition. Equation (5) is equivalent to the following boundary condition :
ax (knl LCn) = 0, for x = 0 and x = L0. (6)

ter X,, similar to Cn, we get XFe = 1n

Xn = 1n

kn/LX n . .........(10) potential of Fe is

When
n

~kn/LX n 1, the chemical by PFe = GFe-RTE

approximated

knlLXn .............(11)

(8) Enthalpies of transformation (4HLa, 4HLr and 4H5r) and heat capacity cp are constant and independent of the temperature. (9) Temperature of the volume element is given by

On the phase boundary between p and q phases, the following equation is valid, because GFe=,4e.
plL_ (kn q/L p q kn )Xn -= GFe - GFe ..............(12)

Applying the following relation to Eq. (12), T4Spq = 4Hpq1T pq ........................(13) represents

a -i;= Q ...........................(7) q = 4pqHGpe-GFe

............(8)

and H = cpT +4Harfa+4HLrfL, where, H: the enthalpy per volume in the volume element Q: the heat input per volume and per time which is given explicitly in this paper f a: the fraction o phase.

we can get the following equation which the phase boundary in the phase diagram.

?~

-7----+_R pq

pq

~(knlL_knlL)Xn, nn

.........(14)

III. Prediction of Equilibrium Phase Diagram The equilibrium phase diagram of steel with multiple alloy components is predicted on the basis of the Fe-C phase diagram shown in Fig. 2(a). Figure 2(b) is drawn in terms of the concentration parameter C~; it is necessary to predict the position of phase boundaries B1 to B3 for a given alloy composition. In the present analysis, it is assumed that the alloy exhibits the Raoultian ideal behavior and several thermodynamical relations3'4~ are used. The chemical potential of Fe in p phase GFeis given by the following equation. PFe- GFe+R T In XFe . ..................(9) where, GFe the Gibbs free energy of Fe in p phase : R : the gas constant XFe: the mole concentration of Fe in p phase. Denoting the mole concentration of the element n as X n, and introducing a mole concentration parame-

where, TTpq the temperature of p/q transformation : of pure Fe 4Hpq : the enthalpy of p/q transformation per mole 4Spq=4Hpq/Tpq: the entropy of p/q transformation per mole. Equation (14) can be rearranged as a function of Cn : 1 T = Tpq1 4H ~ (kplL_kglL)Cn .........(15) + Rpq n n n Wn where, 4Hpq: the enthalpy of p/q transformation per unit mass Wn: the atomic mass of element n. The phase boundaries in the diagram of Fig. 2(b) for multi-component alloys are given by the following equations.

+ =
T

Ti

1 +_R

4HLa n

(1-k)2n

Wn , for B1, .....................(16-1)

1 -:;-=--+_R T T1 Lr

4HLr n

(1-kn,L) Cn , for B2 Wn .....................(16-2)

1 T = T1 + R (kn/L_kn/L)Cn for B3 ar 4Har n Wn ~ .....................(16-3) VI. Thermophysical Data The thermophysical data adopted are listed in Table 1. Most of the data are taken from the literature,5-77 however the melting point of pure r iron TLr and the enthalpies of transformation, 4HLS, 4HLr and 4HSr were modified in order to be consistent with the model described. The assumption (8) yields the following equation.
Fig. 2.
Fe-C equilibrium phase d iagram.

4HLr = 4Har+4HLa ...................(17)

F n

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Table

1.

Thermophysical

data

adopted.

Fig.

3.

Schematic grids.

representation

of

the

finite

difference

at

xc xwknlL dx = Dn ax (knlL x=x Cn a G'n) e

-D n ax (knlL(~n)Ix=x2U ........................(20)

Therefore, the requirement that Eqs. (16-1) through (16-3) are mutually consistent leads to 4HLr _ dHsr + dHLa T Lr Tor TLo By combining Eq. (17) with Eq. (18) and by using the data taken from the Fe-C equilibrium phase diagram shown in Fig. 2(a) : Tar=1 665 K, TL= 1 809 K, kg/L=0.1961, k~/L 0.3529 and T= 1 768 K for = O =0.005l, the numerical values of TILT, 4HLo, 4HLr and 4Hsr in Table 1 were determined. The data in Ref. 6) and 8) are shown in parentheses in the table. The mathematical model for the equilibrium phase diagram will be adequate, because the difference of the determined values shown in Table 1 from the data presented in the literature is slight. The diffusion coefficient of every element in the solid phase was assumed in the form of D11=D exp RT Qn , ...............(19)

The finite difference approximation in time is based on the completely implicit method. By denoting the values at a given time t; like C, and k i and the finite difference time interval as At, Eq. (20) can be approximated by the following finite difference equation.
xe kSIL,~~3dx_ n n
xw

xekSIL,~-iG.~-1dx dt n n
xw

Dn a x kn Cn x-xe Dn ax kn Cn x_x~ . ........................(21) On the other hand, the finite difference approximation in space is based on the assumption that the phase boundary coincides always with one of the preset finite difference grids and the terms in Eq. (21) are approximated as

Sxe k1LOfldX n= C72,p(kBE+kn;wBti~)

xw

and the values of D and Qn for each element are listed in Table 1. The diffusion coefficient of carbon in o phase is assumed to be equal to that in a phase, because it is not available in the literature. V. Method of Numerical Analysis

Dn a (kSILCn)x=xe Dn,eknle a AE(Cn E-On p)> etc. x ~ > ........................(22) where, BE =(XE-XE)!2, AE -1/(XE-xp) Bw = (xp-xw)/2, Aw =1/(XP-xw), .........(23) subscripts E, W, P, e, w : the positions. The parameters Ai and Bi (i=E or W) are set to be zero at the edges of the volume element considered. When the finite difference grids are numbered as i = 1, 2, ... , iN in the order from the leftside end of the volume element, AE(iN)=BE(AN)=0, A1~'(1) Bw(l) =0. = ........................(24) The variations of the several parameters are shown schematically in Fig. 4. Equation (5) is approximated by the following equation.

1. Finite Difference Equation Equations (4) and (5) are solved by the finite difference method. A portion of the finite difference grids is shown in Fig. 3. In the figure, xW, xp and xE represent the finite difference coordinates on the grids, and xw and xe indicate the midpoint coordinates of the finite difference grids. For the definition of the suffixes W, P, E, e and w, we refer e.g. to Forsyth and Wasow9~ and Gosman et a1.10' Application of the integral f xw[-] dx with Eq. (4) gives the following integral equation.

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Fig.

4.

Schematic physical

representation quantities in the

of finite

the

distributions method.

of

difference

aB-1

Cn(i)(kn,e (i)BB(i)+kn,w(i)BW(i))
1=1

+Cfl(2B)(LO-x(ZB)+kn;w(ZB)BW(ZB)) = CoL0, ........................(25) where, iB: the grid number of the solid-liquid interface. 2. Method of Computation The method of computation is shown in Fig. 5 as a flow chart. The finite difference time interval d t is set by iterative computation so that the liquidus temperature determined from the alloy composition coincides with the temperature of the volume element determined by thermal condition from Eqs. (7) and (8) during solidification. After the volume element is completely solidified, the time interval 4t is kept at a fixed value. The LU decomposition" is employed to solve the finite difference equations of Eqs. (21) and (25). 3. Finite Difference Grid The effects of the spacing of finite difference grids on the accuracy of computation were examined by using the Brody-Flemings model of dendritic solidification,12~because the exact solution has been derived for the Brody-Flemings mode1.13~ The numerical results of the finite difference method were compared with those of the exact solution. The Brody-Flemings model is based on a planar dendrite assumption as shown in Fig. 1, but it is more simplified than the present model. The assumptions in the BrodyFlemings are as follows. (1) of transformation does not take place during solidification. (2) The diffusion coefficient D and the equilibFig. 5.

Flow chart of the computation (1 time step).

rium partition ratio k are constant throughout the solidification. (3) The local solidification rate is parabolic as expressed by X = K ~l t , ........................(26) where, K: a constant parameter t : the time from the beginning of the solidification. The solute distribution in the solid phase Cs at a fraction solid fs is given by CS( , x*) = kCp bn -nl ' 112' x 121 f s .f n=o F(-n12,1/2 ~ -1/2Y) and

n-1[ JLLl_kF(_m12,312; F(-m/2 -1121) , 1/2;-1 /2r)

where, x < x/X = r = 2D/K C,o the initial composition : F(a, b; z) : the confluent hypergeometric function. 14) The values of the parameters adopted for the comparison were : r = 0.05 and k=0.06. These are the same adopted by Clyne et a1.15~ calculate the segreto gation of phosphorus in r iron. The finite difference grids were determined by

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aiN-1- 1 x(i) = L01 - dxmiii-- a-1 i=1,2,...,iN ..............................(28) and the two cases marked by 10 and 20 in Table 2 and in Fig. 6 were compared. In Fig. 7, the numerical solutions for grids 10 and 20 are shown, together with the exact solution. The numerical solution for the equally-spaced grids 10 deviates appreciably from the exact one. The numerical solution for the unequally-spaced grids 2 agrees satisfactorily with the exact one, although the maximum spacing in the grids 2 seems to be too coarse. The finite difference grids 03 shown in Fig. 6 are finally adopted: 1) iN=45, 2) equally spaced with the spacing of 0.05L0 for i<18 (x(i)G0.85), and 3) set according to Eq. (28) with the values of a= 1.272 and 4xmin= 6 X 10-5 for i > 19.
Table 2. Finite difference grids examined.

VI, Experimental I.

and Simulation

Results

ExperimentalMethod The experimental method is shown schematically in Fig. 8. A specimen having a diameter of 20 mm and a weight of 80 g was remelted and held for 10 min at 1 600C in the furnace, and then cooled in the furnace with a constant cooling rate of 0.5 K/s. The temperature and its time derivative (cooling rate) of the specimen were recorded continuously. The composition of the specimen is shown in Table 3. Carbon content in the specimens was systematically changed within the range of 0.040.51 wt%. The equilibrium phase diagram estimated by the present model for the composition in Table 3 is shown in Fig. 9. The measured results were compared with the computed results of the mathematical model described in the previous sections. The heat transfer properties of the volume element considered were modeled by the following first-order lag equation, on the basis of the measured cooling rates of the specimens. dH/dt =cp(TF(t)T)/z ................(29) and TTF(t) TF(0) - Vt, ..................(30) = where, TF (t) : the furnace temperature T: the specimen temperature z : the time constant of the heat transfer between the specimen and the furnace (=58s) V: the cooling rate in the furnace (=0.5 K/s). The size of the volume element, Lo, was set to be 180 m on the basis of the measured average dendrite arm spacing in the specimens. Z. CoolingCurves Measured cooling curves of the specimens are compared with the calculated results in Fig. 10. Metallurgical phases calculated are also indicated in each figure. All the calculated temperature (T)-time (t) curves agree well with the measured results. With respect to the temperature derivative (d T/dt)-time (t) curves, the measured values correspond fairly well with those calculated, although the slight differences are observed in the figures. From the measured (dTT/dt)-t curves, a series of the characteristic temperatures can be extracted; the physical meanings of each characteristic temperature were interpreted in the following. (1) The temperature corresponding to dT/dt = 0 at the initial stage of solidification is indicated by the mark 0 in Fig. 10 and it corresponds to the liquidus temperature. (2) The physical meanings of the temperatures corresponding to the minima in (dT/dt)-t curve differ for various carbon contents in the specimens. Measured timing of the maximum cooling rate is indicated by the mark in each figure. (i) For 0.04 C steel, the first minimum point corresponds to the temperature at which oar transformation takes place (marked by E), and the second cor-

Fig . 6.

Finite

difference

g rids

examined.

Fig.

7.

Effects ference

of grid

spacings

on

results

of the

finite

dif-

calculation.

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Fig.

8. illustration method. of the experi-

Schematic mental

Table

3.

Steel

tested.

responds to the finishing temperature of o/r transformation (marked by C). (ii) For 0.08 C steel, the minimum point corresponds to the ending temperature (C) of o/r transformation. (iii) For 0.13 C steel and 0.50 C steel, the minimum point () does not represent any phase change. (3) The temperature at the point where the gradient in (dTJdt)-t curve changes abruptly corresponds to the starting temperature of o/r transformation (~) for 0.08 C and 0.13 C steels. The solidus temperature could not be detected directly in any cooling curve. Unequilibrium Phase Diagram The characteristic temperatures obtained by the experiment are plotted on the calculated unequilibrium phase diagram shown in Fig. 11. The validity of the present mathematical model has been proved in the figure at least for the alloy tested. It is also shown that the carbon content at the peritectic point is lowered by the microsegregation effects in comparison with the equilibrium condition shown in Fig. 9. Figure 12 compares the measured temperature at the maximum cooling rate with fraction solid calculated. The temperature at the maximum cooling rate corresponds to the fraction solid of approximately 0.99 for the carbon range above 0.15 wt%, where r phase solid forms directly from the liquid phase.
VII. 1. Discussion Equilibrium Phase Diagram model diagram proposed in this paper, of a multi-component

3.

Fig.

9.

Equilibrium ent 3. model.

phase diagram estimated by the presComposition of steel is listed in Table

In the mathematical the equilibrium phase

alloy is predicted on the assumption that the alloy exhibits the Raoultian ideal behavior. The proposed model will be valid for low alloyed steels, because the unequilibrium phase diagram predicted by the present model agreed well with the results of the thermal analyses. The liquidus slopes in phase diagrams predicted by the model were compared with the experimental data available16~ for further verification. Equation (15) can be approximated by the following linear equation : 2
T pq- R pq Q (1-p/L_ ~n 11A7'" ....... (31) fin r-q/L n Li pq n n

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Fig. Typical

10. cooling curves.

thus, the liquidus slope mL for element n is given by mL1(K(wt%))_ - RT is(l -~n~~) S (3 or 1004H ISh n ' = r ........................(32) The calculation results of Eq. (32) are compared with the experimental data in Table 4. Most of the experimental data are close to the values predicted by Eq. (32). The present mathematical model to predict equilibrium phase diagrams has been proved

valid also by the experimental data. 2. Solidus Temperature Comprehensive results and interpretation of thermal analyses are presented in the literature.17~ The interpretation of the characteristic temperatures in Ref. 17) is almost the same as the present authors' except for the solidus temperature which represents the temperature at the maximum cooling rate in the reference. In order to examine whether such dis-

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Fig . 12.

Relationship maximum

of coolin

calculated g rate with

temperature fraction solid.

at

the

Fig . 11.

Estimated parison with

unequilibrium experimental

phase data.

diagram

in

com-

the cooling rate is maximum (fs>0.99 based present analysis) is subject to further research.
slope.

on

the

Table

Comparison

of

liquidus

(K/wt%)

3.

Assumption Planar Geometry of Solute content in the liquid phase will take an intermediate value between the values estimated by the Scheil equation and the equilibrium equation. Thus the error in the solute content estimated by the present method is expected within the order of dC __ Cl- fs)k_i-Cl-CI-~)fs)-~ C (l- fs)k_1+(1--(1--k)fs)-1

crepancy is due to the problem of the adopted mathematical model itself or not, the cooling curves (dT/ dt-t curves) of 0.51 C steel of which composition is shown in Table 3 were calculated on the basis of the equilibrium equation18~and the Scheil equation,18~respectively. The maximum cooling rate for the equilibrium equation was calculated after the solidification was completed, while that for the Scheil equation was obtained at a fraction solid of 0.9. It seems that the disagreement of the solidus temperature with the temperature at the maximum cooling rate is a general phenomenon due to microsegregation effects. The validity of the solidus temperature predicted by the present model is indefinite, because no characteristic change was found in both the measured and the calculated cooling curves after the cooling rate became maximum. The solidification behavior after

It is within 10 % for f8<0.7. The maximum expected error is shown in Fig. 13. The assumption of any geometry including the planar one is adequate for the initial stage of the solidification, because both the results of the Scheil equation and those of the equilibrium equation are independent of the geometry of the solid-liquid interface. On the other hand, the morphology of the liquid phase will affects the microsegregation effects, at the final stage of the solidification (f8N 1). If the morphology of the liquid phase is film-like, the assumption of the planar geometry will be adequate. If the morphology of the liquid phase is spot-like or line-like at the final stage of the solidification, the assumption of the planar geometry will overestimate the microsegregation effects. For the alloys tested in the present paper, the assumption of the planar geometry will be valid within the range

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Fig.

13.

The

maximum

error

expected,

dGJC, in the

cal-

culation.

that the latent heat of the solidification is detectable by the thermal analysis (that corresponds to a fraction solid less than 0.99 based on the present analysis). Other geometries have been analyzed by Matsumiya et a1.19~ and by Ohnaka.20~ Their geometries are essentially cylindrical due to their assumptions of one dimensional mass flow. The difference between the model of Matsumiya et al. and that of Ohnaka is the geometry of the liquid phase at the final stage: line-like for Matsumiya et al. and film-like for Ohnaka. The present model can be easily modified to include those geometries analized by Matsumiya et al. or by Ohnaka, although there is no evidence that the assumption of planar geometry is not valid. It is to be desired that many reliable data become to be available, in order to assume the most realistic geometry of the liquid phase in dendritic solidification. 4. Predictionof UnequilibriumPhase Diagram The unequilibrium phase diagram of the alloy tested was predicted by the present mathematical model with fairly good accuracy. The experimental evidence has not been completely conclusive, it has been shown that the model is adequate. The model will be applicable to predict unequilibrium phase diagrams of various steels under a given cooling condition. In order to predict the unequilibrium phase diagram of steels which have higher sulphur contents than the steels tested in the present paper, a method to predict the precipitation of MnS may be needed. Schwerdtfeger21 has included MnS precipitation in a numerical description of microsegregation. The prediction method of MnS precipitation will be easily incorporated into the present model. Yasumoto et a1.22~ have carried out a series of thermal analysis for various steels and concluded that the temperature at the maximum cooling rate (` Tr ' by their designation) has a good correlation with the r grain size in the steel. Since the present model can predict ` Tr ' with a good accuracy as mentioned in the previous section, it will be also applicable to predict r grain size in various steels solidified under various cooling conditions. VIII, Conclusions A mathematical model quantifying solute redistribution during solidification with considerations on 3/Ttransformation and a computational method of the model have been derived. Features of the mathematical model are as follows :

(1) The morphology of the dendritic solidification is approximated by the planar geometry. (2) The equilibrium phase diagram of multi-component alloy is predicted on the assumption that the alloy exhibits the Raoultian ideal behavior. (3) The local equilibrium at the solid-liquid interface is assumed. (4) The equilibrium distribution coefficients are constant throughout the solidification and independent of the alloy temperature. In the computational method, mathematical treatment of the phase boundary has been simplified by introducing a new parameter which is defined as the ratio of the solute concentration to the equilibrium distribution constant. Accurate finite difference grids have been chosen based on the exact solution of the Brody-Flemings solidification model. The thermal analyses of 0.04-0.51C-2Mn-0.02P0.005S-O.Ol Si steels were carried out to validate the mathematical model. The cooling curves obtained by the experiments agreed well with those calculated and the results of the thermal analyses were interpreted by the theory. Unequilibrium phase diagram of various steel for a given thermal condition of solidification will be estimated by the present mathematical model. However, the sensitivity of the thermal analysis was restricted within the range where estimated fraction solid is less than 0.99. It is needed further research to quantify the solidification behavior of steel at the final stage of solidification. Acknowledgements The authors would like to acknowledge Dr. Y. Maehara and Messrs. K. Yasumoto and H. Ichihashi for their valuable discussion. Thanks are also due to Mr. Y. Sakamoto for his assistance in the computational work.

REFERENCES 1) 2) 3) Y. K. Chuang, D. Reinish and K. Schwerdtfeger: Metall. Trans. A, 6A (1975), 235. Y. Ueshima, S. Mizoguchi, H. Kajioka and T. Matsumiya: Tetsu-to-Hagane, 71 (1985), 5202. D. R. Gaskell: Physical Metallurgy, ed. by R. W. Cahn and P. Haasen, Elsevier Sci. Publ., B.V., Amsterdam, (1983), 371. A. D. Pelton: Physical Metallurgy, ed, by R. W. Cahn and P. Haasen, Elsevier Sci. Publ., By., Amsterdam, (1983), 327. T. Takahashi: Iron and Steel Handbook, I: Fundamental Theory of Iron and Steel, 3rd Ed., ed, by ISIJ, Maruzen, Tokyo, (1981), 193. I. Ohnaka: Iron and Steel Handbook, I: Fundamental Theory of Iron and Steel, 3rd Ed., ed. by ISIJ, Maruzen, Tokyo, (1981), 213. K. Hirano: Iron and Steel Handbook, I: Fundamental Theory of Iron and Steel, 3rd Ed., ed. by ISIJ, Maruzen, Tokyo, (1981), 343. T. Nishizawa and M. Hasebe: Tetsu-to-Hagane, 67 (1981), 1887. G. E. Forsyth and W. R. Wasow: Finite Difference Methods for Partial Difference Equations, John Wiley and Sons, New York, (1960).

4)

5)

6)

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8) 9)

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10) A. D. Gosman, W. M. Pun, A. K. Runchal, D. B. Spalding and M. Wolfstein : Heat and Mass Transfer in Recirculating Flows, Academic Press, London, (1969). 11) G. E. Forsythe and C. B. Molar: Computer Solution of Linear Algebraic Systems, Prentice-Hall, New Jersey, 12) 13) 14) 15) (1967). H. D. Brody and M. C. Flemings: Trans. TMS-AIME, 236 (1966), 615. S. Kobayashi: J. Crystal Growth, 88 (1988), 87. E. T. Whittaker and G. N. Watson : A Course of Modern Analysis, Cambridge Univ. Press, Cambridge, (1927). T. W. Clyne, W. Wolf and W. Kurz: Metall. Trans. B, 13B (1982), 259.

16) 17) 18) 19) 20) 21) 22)

Y. Miyashita: Tekko-Binran, ed. by ISIJ, Maruzen, Tokyo, (1981), 205. A Guide to the Solidification of Steels, Jernkontret, ed., Ljungberg Tryckeri AB, Sodertalje, (1977). W. Kurz and D. J. Fisher: Fundamentals of Solidification, Trans. Tech. SA, Switzerland, (1984), 126. T. Matsumiya, H. Kajioka, S. Mizoguchi, Y. Ueshima and H. Esaka: Trans. Iron Steel Inst. Jpn., 24 (1984), 873. I. Ohnaka: Trans. Iron Steel lnst. Jpn., 26 (1986), 1045. K. Schwerdtfeger: Arch. Eisenhuttenwes.,41 (1970), 923. K. Yasumoto, T. Nagamichi, Y. Maehara and K. Gunji: Tetsu-to-Hagane, 73 (1987), 1738.

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