Low-Temperature Solid-State Bonding of Copper PDF
Low-Temperature Solid-State Bonding of Copper PDF
Low-Temperature Solid-State Bonding of Copper PDF
Mechanisms associated with low-temperature solid-state bonding of copper were investigated. The low-
temperature bonding phenomena was observed to be time/temperature dependent and related to a defor-
mation process. An analytical technique for predicting bond strength and bonding behavior is presented.
Note: Bonding parameters, pressure = 68.9 MPa (10 ksi) held constant during all tests; sample roughness, 10 to 15 gin. (screw machined). N/A ---not
applicable due to bulk deformation occurring during bonding.
Temperature,
*C Time, sec
2 0 0 .................................................................. 0 300 600 1200 2400 4800
225 .................................................................. 0 300 600 1200 2400 4800
250 .................................................................. 0 300 600 1200 2400 4800
275 .................................................................. 0 300 600 1200 2400 4800
300 .................................................................. 0 300 600 1200 2400 4800
325 .................................................................. 0 300 600 1200 2400 4800
350 .................................................................. 0 300 600 1200 2400 4800
Note: Bondingparameters, pressure = 68.9 MPa (10 ksi) held constant during all tests; surface roughness,40 p.in. (mill cut). An isothermaltime of zero
seconds representsthe heatingcycle of the isothermalheat treatment.
IOO ! ! I I | | I I I | I I | I I I | I I | | | | | | | I
-r" 5 T=400*C
I- I:1 / J - . . " E T ~ T = 375 eC
2 ~~_.0._______----~ -T=35o'c
Z
LI.I
I---
(/) I0
5
03 4 (3 T= 400"C
O T= 375 ~
e T:350"C
A T=~00 eC
l i l I I 9 I | i I i | I | i J i l i i i i I I * i I
2 3 4 5 6 7 8 9 10 2 3 4 5 6 789100
TIME (sec)
Fig. 1 Preliminary data given as a log-log plot of bond strength as a function of time for various isothermal heat treatments.
O 200 deg.C
Q 225 deg.C o
9 250 deg.C
25000 9 275 aeg.C
300 aeg.C
A
O 325 deg.C
9 350 deg.C v o
' 20000
o
A &
c 15000 o
A
U
L II
O 99 9 n
o t0000
C
O n O
9 I:]
n
n i3 U
O
5000 0
0 ' i
0
I
500
~ I I
t000
I
t500
I I i I o
Fig. 2 Fraction of bond strength established during the isothermal annealing time, shown as a function of annealing time, for temperatures
from 473 to 623 K (200 to 350 ~
35000 . .. ! . !
' I ' ! 9 l '
I
l ' I ' I ' I ' I ' I 'f
0 200 deg.C
O 225 aeg.C
30000 9 250 cleg.C
9 275 (Jeg.C O
A 300 Oeg.C
0 325 Oeg.C
25000 9 3,50 Oeg,C V 0
m
20000 O O
c & A 9
L 15000
O
c 9 9 9 rl
o 10000
9 n n O
El O
n
5000 & O
O
i O l i L l l l l
t i I I I I I t I I I = 1 J 1
Fig. 3 Maximum bond strength plotted as a function of total heating time for temperatures from 473 to 623 K (200 to 350 ~
14000
12000
m
10000
c 6000
L
m 6000
C
O
m 4000
C
H 2000
0 i I ~ I i I i I i I
Temperature (deg.C)
Fig. 4 Bond strengths established during the time required to reach thermal equilibrium, shown as a function of final bonding temperature.
35000 i I ' I ' ! ' ! ' I ' I ' I ' I ' I ' I ' I i
25000
c
m 20000
L
c 15000
o
m
E
10000
E
X
m 8 8
x 5000
8 S
' lid ~ I i 1 i I I , i , I . i , I I I I I J
0
0 500 t 0 0 0 1500 2000 2500 3000 3500 4000 4500 5000
Time (sec)
Fig. 5 Comparison of maximum bond strength and the bond strength attributed to the isothermal annealing time, at 473 K (200 ~ shown
as a function of isothermal annealing time.
9 Bond S t r e n g t h ( B ) , 3 5 0 deg.C 9
0 B-Bo, 350 deg.C
30000
o
25000
c
m 20000 0
L
oc t5000
o 9 0
E 0
0
10000
E
0
X
x 5000
, i * l l l I * l t l l l l l J . l J l , l l *
Time (sec}
Fig, 6 Comparison of maximum bond strength and the bond strength attributed to the isothermal annealing time, at 623 K (350 ~ shown
as a function of isothermal annealing time.
9 200 C
0 225 C
4.25 9 25O C
0 275 C 9 i 9
rt 9 300 C 9 9
4.00 A 325 C 9 i
m 9 350 c dl = ~=
! 9 o o
m 0
9--, 3.75
t~ o
o
I-!
3.50
1-
4-)
01
cQ ) 3 25
s
4~
(Jr)
3.00
E
0
m
' 2.75
o
r-t
I I l 1 9 i i . i ! i i I I i * | 9 I 1 I I t i 9 9
log-Time (log-sec}
Fig. 7 Isothermal annealing bond strength (B-Bo), shown as a function of isothermal annealing time. Scales are in common logarithm form.
Temperatures range from 473 to 623 K (200 to 350 ~
0 200 geg.C 0
9 225 geg.C
0 250 deg.C
9 275 deg.C
0 300 aeg.C
15000 9 325 aeg.C
13
9 350 Oeg.C 0 0
Q.
<> 0 13
!
iO000
t"
4J 13
t~ t I . o
r-
Q)
L 13
9 o
U)
5000
"13
o
0 i i ~ , I i i , i i I i I i I i I
4.5 5.0 5.5 5.0 6.5 7.0 7.5 fl.O
0.25 0.25
( Time ) (sec)
Fig. 8 Isothermal annealing bond strength, plotted as a function of isothermal annealing time taken to n = 0.25. Temperatures range from
473 to 623 K (200 to 350 ~
others, it is difficult to achieve a mechanistic understanding of terms in the two equations are the constants that contain infor-
the rate-controlling process. Difficulty in the mechanistic inter- mation about the discontinuity relationship and the instantane-
pretation results from the continuous change in microstructural ous bond strength value for the specified temperature range.
details controlling the bonding process (a decrease in real stress If Eq 4 is set equal to zero, then the temperature at which the
at the bonding interface occurs, even though the bonding load is initial bond strength Bo becomes greater than zero can be deter-
constant). To achieve a physical interpretation of the apparent mined. By performing the calculation for this boundary condi-
activation energy, an experiment that maintained constant stress tion, a temperature of 184 ~ can be determined. The 184 ~
and constant material conditions at the bonding interface would temperature value represents the temperature for the initial
be required. measurable bond strength under this particular set of bonding
conditions. It is anticipated that with an increasing applied load
3.2 Interpretation of Results used during bonding, the minimal bonding temperature can be
lowered further.
The initial bond strengths established during the time re-
Comparing these bonding results to copper annealing
quired to reach thermal equilibrium were shown in Fig. 4 to
data, [38-40]several similarities can be observed. Clarebrough et
abruptly increase as the target bonding temperature was in-
al.[40] reported the importance of deformation in influencing the
creased through the 300 to 325 ~ temperature range. Although
recrystallization temperature of copper. The recrystallization
a distinct step or discontinuous increase in the bond strength was
temperature range observed by Clarebrough eta/. [4~ (325 to
observed, the slope or rate at which the initial bond strength, B o,
350 ~ was similar to the temperature range observed in this in-
increased with temperature appeared relatively constant in both
vestigation for a finite change in bonding mechanism. Bonding
the high- and low-temperature regimes, as shown in Fig. 4.
mechanism changes were observed at -325 ~ for both the pre-
The initial bond strength for these temperature regimes can
liminary tests (see Fig. 1) and for the more extensive primary
be empirically represented by the following equations:
bonding studies that followed (see Fig. 4). This comparison be-
Bo=31T-14,151 for T < 573 K [4] tween the present investigation and the work of Clarebrough et
al.[38-4~ suggests that low-temperature bond strength in copper
Bo=31T-7351 for T > 573 K [5] can be greatly influenced by dynamic recrystallization.
Understanding the processes that occur along the bonding in-
where T is the absolute temperature, and B o is given in units of terface prior to and during heating is important to further im-
pounds per square inch (psi). The temperature coefficient for the provements in low-temperature solid-state bonding. In general,
initial bond strength is identical in both equations. The second the morphology of the bond interface may be used to promote an
tO 14
I/3
GI
r-I iO t 3
113
I
9 "e-l--__ .-
Q= II K c o l/mo l/ - -,.
iO i 2
lO l i i i i I i I i i i I ~ I i
.0016 .00i7 .0018 .0019 .002 .002~
Fig. 9 Logarithmic rate constant K (see Eq 3) as a function of reciprocal absolute temperature, revealing the apparent activation energy for
the bonding of copper.
increase in contact area through the process of strain and defor- Bo=8.06t+5092 T>573K [7]
mation. The area of true interfacial contact is very small initially,
and the concentrated stress at the contacting asperities is greater A comparison of the calculated results for the initial bond
than the yield stress. These asperities plastically deform on con- strength to the experimental data is shown in Fig. 10, where the
tact, and the contact area increases until the local stresses de- empirical expressions represent the data quite well.
crease to a value below that of the yield strength. Substitution of Eq 6 and 7 into Eq 3 will quantify the bond
To understand the limits of the low-temperature bonding strength for each temperature regime. However, the appropriate
process and to assist in bond strength predictions, it is desirable time intervals to be used must be considered carefully. The time
to develop an empirical expression. This expression must allow in Eq 6 and 7 begins at the moment when the two specimen
for the prediction of bond strength through the complete bond- halves are brought together and the heating cycle begins. The
ing thermal cycle, encompassing both heating and isothermal end of the heating time occurs when the isothermal temperature
segments. In considering the functional relationship of the initial is reached, or when the value dT/dt becomes zero. The time in Eq
bond strength, Bo, it is assumed that the minimum temperature at 3 begins when the heating cycle ends and continues at constant
which bonding has been determined to occur is 457 K (184 ~ temperatures until cooling is initiated. Thus, the total time (tt) of
The initial bond strengths are given by Eq 4 and 5 for the two the bonding cycle is the sum of the heating segment (th) and the
distinct isothermal bonding temperature ranges. By incorporat- isothermal segment (tt). The final form of the bond strength
ing the heating rate into these equations, a time-dependent equa- equation can be written for two temperature ranges:
tion for the bonding process can be expressed.
The expression for the determination of the initial bond B = (8.06 t h - 1708) + [Kt/] ~ T < 573 K [8]
strength in the temperature range 457 to 573 K for this specific
heating rate (0.26 K/sec where T > 573 K) becomes: B = (8.06 t h + 5092) + [Ktz]~ T > 573 K [9]
B o = 8.06 t - 1708 T < 573 K [6]
where K is an exponential expression (see Eq 2) with the appar-
Similarly, the initial bond strength for the upper temperature ent activation energy of 11 kcal/mol. Equations 8 and 9 are plot-
range 573 to 673 K can be determined by considering the dis- ted in Fig. 11 for bonding temperatures of 475 and 623 K, re-
crete increase in bond strength, ABo, that occurs over the tem- spectively. The model represents the data reasonably well. The
perature range of 573 to 623 K. This high-temperature initial experimental bond strength data for seven temperatures be-
bond strength equation becomes: tween 473 and 623 K are also shown in Fig. 11.
14000
12000 , . . 9 ,.-" 9
"-'~ t 0 0 0 0
c BOO0
L
6000
C
o
m 4000
0
H 2000
0 I, "~'I i I I I i i i I i
200 250 300 350 400
Temperature (deg.C)
Fig. 10 Initial bond strength data of tough pitch copper for temperatures and equilibration time indicated. Solid lines are the empirical equa-
tions given in the text (Eq 6 and 7).
References
4 Conclusions 1. R,F. Tylecote, The Solid Phase Welding of Metals, St. Martins
Press, New York (1968).
Bond strengths of low-temperature copper bonds have been 2. D.R. Milner and G.W. Rowe, Metall. Rev., 7(28), 433-480
characterized in copper for the temperature regime of 473 to (1962).
3. N. Bay, Weld.J, 62(5), 137s-142s (1983).
623 K. Low-temperature solid-state bonding of copper is a
4. N. Bay, Brit. Weld. J. Met. Const., 18(6), 369-372 (1986).
time/temperature-dependent process that is primarily controlled
5. N. Bay, Brit. Weld. J. Met. Const., 18(8), 486-490 (1986).
by deformation. A time-dependent exponent of 0.25 and an ap- 6. C. Clemensen, O. Juelstorp, and N. Bay, Brit. Weld. J. Met.
parent activation energy of approximately 11 kcal/mol were de- Const., 18(10), 625-629 (1986).
termined. 7. C.H. Hamilton, Titanium Science and Technology, Proc. 2nd Int.
Separation of the various stages in the bonding cycle--initial Conf., R.I. Jaffee and H.M. Butte, Ed., Vol. 1, Plenum Press, New
contact, nonequilibrium heating, and the isothermal a n n e a l - - York, 625 (1973).
are essential in determining an understanding of the mechanistic 8. R.A. Nichting, G.R. Edwards, D.L. Olson, and B.B. Rath, "Theo-
nature of low-temperature solid-state bonding. An empirical ries of Low Temperature Solid State Bonding," Proc. Int. Conf.
on Trends in Welding Research, Gatlinburg, TN, May 19-22,733-
equation for predicting low-temperature solid-state bond
738, ASM, Metals Park (1986).
strength for copper as a function of bonding time and tempera-
9. D.L. Olson and A.L. Liby, Joining III: Diffusion Bonding, inBe-
ture was determined. ryllium Science and Technology, Vol. 2, Plenum Press, New
York, 275-296 (1979).
10. W.H. King and W.A. Owczarski, Weld. J., 47(10), 444s-450s
(1968).
Acknowledgments 11. J.M. Gerken and W.A. Owczarski, "A Review of Diffusion Weld-
ing," Welding Research Council, Bull. 109, Oct (1965).
12. V.D. Taran, SvarProizv, 11, 12-14 (1958).
The authors appreciate and acknowledge the support of the 13. B. Derby and E.R. Wallach, Met. Sci., 16(1), 49-56 (1982).
Office of Naval Research and the technical services of Jim Aris 14. E. Elliott, E.R. Wallach, and I.A. Bucklow, J. Mater. Sci., 15,
and Dr. T. Schiling of EG & G (Rocky Flats Plant). 2823 (1980).
%,, 9
c 15000
L
Or 9
9 9 Q
oc t0000
o 9 9 o.,.
9 Q 0Q .......- "
o n, .... L - 200"C
5000 A o _ . . . - ~ "-" . . . . Eqn. 8
~
1 A I I I I I I I l I I I 1 1 l I i
0 500 1000 1500 2000 2500 3 0 0 0 3500 4000 4500 5000 5500
Time (sac)
Fig. 11 Comparison among experimental data and the empirical equations given in the text (Eq 8 and 9).
15. D.J. Allen and A.A.L. White, Sintering Processes in Diffusion 26. A.A.L. White and D.J. Allen, Elimination of Voids and Oxide in
Bonding, in The Joining of Metals: Practice and Performance, Diffusion Bonding, in Advances in Welding Processes, Vol. 1,
96-103, The Institution of Metallurgists, London, (1980). Harrogate, England (1975).
16. A.C. Moore and D. Tabor, Brit. J. Appl. Phys., 3,299-301 (1952). 27. H.A. Mohamed and J. Washburn, Weld. J., 54(9), 302s-310s
(1975).
17. S.B. Ainbinder andE.F. Klokova, LatvijaspsrZinatnuAkadVes-
tis, 10(87), 113-128; Brutcher Translation No. 3755, Mechanism 28. B. Derby and E.R. Wallach, Met. Sci., 18(9), 427-431 (1984).
of Bonding in Cold Welding (1954). 29. H. Kellerer and L.H. Milacek, Weld. J., 49, 219s (1970).
30. B. Derby and E.R. Wallach, The Joining of Metals: Practice and
18. FP. Bowden and G.W. Rowe, Proc. Roy. Soc., 233A, 429-442
Performance, 96-103, The Institution of Metallurgists, London,
(1956).
(1981).
19. T. Spalvins and D.V. Keller, Trans. Vac. Met. Conf. 1962, R.F.
31. B.N. Chapman, J. Vac. Sci. Technol., 11(1), 106-113 (1974).
B unshah, Ed., American Vacuum Soc., Boston, 149-155 (1963).
32. D.M. Mattox, J. Vac. Sci. Technol., 10(1), 47-52 (1973).
20. W.H. King and W.A. Owczarski, Weld. J., 46, 289s-298s (1967). 33. J. Ayers, private communication, EG & G Rocky Flats Plant,
21. M.G. Nicholas and D.R. Milner, Brit. Weld. J., 9(8), 469-475 Golden, CO (1989).
(1962). 34. J. Engl and G. Heidtkamp, Zeit. Physik., 95, 30 (1935).
22. K.J.B. McEwan and D.R. Milner, Brit. Weld. J., 9(7), 406-420 35. P. Ludwik, Zeit. Physik. Chem., 91,232 (1916).
(1962). 36. E. Hart, Acta Metall., 5,597 (1957).
23. J.S. McFarlane and D. Tabor, Proc. Roy. Soc. London, Ser. A, 37. N.H. Nachtrieb and G.S. Handler, Acta Metall., 2,797 (1954).
202(1069), 224-243 (1950). 38. L.M. Clarebrough, M.E. Hargreaves, D. Michell, and G.W. West,
24. G. Schoeck, Theorie s o f Creep, in Mechanical Behavior of Mate- Proc. Roy. Soc. (London), 215A, 507 (1952).
rials at Elevated Temperatures, J.E. Dorn, Ed., McGraw Hill, 39. L.M. Clarebrough, M.E. Hargreaves, and G.W. West, Proc. Roy.
New York, 79-107 (1961). Soc. (London), 232A, 252 (1955).
25. P.H. Kammer, R.E. Monroe, and D.C. Martin, Weld. J., 48(3), 40. L.M. Clarebrough, M.E. Hargreaves, and G.W. West, Philos.
l16s-124s (1969). Mag. Set. 7, 44(355) (1953).