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I. INTRODUCTION
intermetallics at the joint interface. It was shown that when the
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BRAUNOVIC AND ALEXANDROV: INTERMETALLIC COMPOUNDS AT ALUMINUM-TO-COPPER ELECTRICAL INTERFACES 79
OPTICAL (200
Fig. SEM and optical micrographs of the intermetallic phases formed in the bimetallic AI-Cu contact after 24 days of diffusion
annealing at C in a furnace.
TABLE I
IMFQRTANTCHARACTERISTICS PHASES
OF INTERMETALLIC FORMED IN THE BIMETALLIC
ALUMINUM-TO-COPPER
SYSTEM.
DATAFOR THE RESISTIVITY, D O ,ACTIVATION
RATECONSTANT ENERGYQ WERETAKENFROM [6]
microohmetre has been developed at IREQ and operates on Water-cooled and hydraulically driven contact plates,
current pulses of 10 A and 17 ms duration. A simplified pressed against the bimetallic samples at 2.5 kN, were used
schema used for resistance measurements is shown in Fig. to maintain the contact and current transfer to the samples.
1. The separation between the potential probes was approx- The current was generated through a step-down transformer,
imately 3 mm. The resistance changes due to the formation the primary of which was connected to a synchronous control
of intermetallic phases at the aluminumxopper interface were system. A thermocouple, located at the contact interface,
sufficiently large to be measured between the potential probes. was connected to this control system. When the interface
Following the resistance measurements, cross sections of temperature reaches the preset value, the control system shuts
bimetallic aluminumxopper samples were examined with the power. This procedure maintained temperature of the
optical and scanning electron microscope and the rate of for- bimetallic contact interface in the range 200 to at
f5"C.
mation of the intermetallic phases formed at the interface were
The contact resistance changes, the rate of formation and
determined. The chemical composition of the intermetallic
the chemical composition of intermetallic phases formed at
phases was determined using the X-ray fluorescent analysis
the Al-Cu interfaces were determined in the same manner as
(EDX). Microhardness of the different phases was determined
described above for the samples treated in thermal gradient.
at 0.4 N (40 g) load.
The effect of electrical current on the formation and
growth kinetics of intermetallic phases in aluminum-to-copper RESULTS
bimetallic joints was investigated by heating the bimetallic
samples 5 mm in diameter and 10 cm long machined from a A. Effect of Temperature
friction-welded AI-Cu bar. Diffusion annealing was realized Over the entire temperature range investigated, the interdif-
in air by heating the aluminum-to-copper bimetallic samples fusion layer consisted of five major bands. These are illustrated
with an ac electrical current ranging from 400 to 1000 A for in the SEM and optical microscope micrographs in Fig. 2,
different times. shawing the cross-section of &e aluminum-copper interface
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80 IEEE TRANSACTIONS ON COMPONENTS, PACKAGING. AND MANUFACTURING TECHNOLOGY-PART A, VOL. NO. I. MARCH 1994
TABLE I1
THICKNESSES
OF INTERMETALLIC
PHASES(IN MICRONS,pm) IN ALUMINUM-TO-COPPER
BIMETALLIC
JOINTS FOLLOWING
HEATTREATMENT AT DIFFERENT
TEMPERATUFSS
AND TIMES
0.5 1 9 20
5 18
24 22 30 60 102
10 60 120
I
Or
I 520”c
1
0 1
EB 470°C
425°C
380°C
Imole
3 800
5
(S l n )
Fig. Formation and propagation of the intermetallic phases in the AI-Cu Fig. 4. Arrhenius plot of the rate constant for growth of the diffusion layers
bimetallic contacts diffusion annealed in a furnace. in AI-Cu bimetallic samples diffusion annealed in a furnace and also by an
electrical current. and Q F indicate the activation energies for samples
treated by an electrical current and in a fumace.
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BRAUNOVlC AND ALEXANDROV: INTERMETALLIC COMPOUNDS AT ALUMINUM-TO-COPPER ELECTRICAL INTERFACES 81
TABLE In
THICKNESSES p m) IN ALUMINUM-COPPER
OF INTERMETALLIC PHASES (IN MICRONS,
JorWs FOLLOWING
BIMETALLIC DIFFUSION ANNEALING
BY ELECTRICALCURRENT
Diffusion Annealed by Electric Current
Time (hours)
200° c 250" C 300' C 350' C 400°C 450' C 5oO0 c
0.3 0.5 1 3.5 5.5 20
2 0.45 0.7 1.5 5 10 25 30
5 0.7 1.2 3 8 15 30 50
24 1.6 2.5 5 17 65 100
D (cm2/s) 3.0 x 7.3 x 3.0 x IO-" 3.3 IO-" 2.1 x 4.8 1.2 x10-!J
@/Do Q 13.2 D~ 5.9 x Q 26.5 Do 3.3 x lo-*
kcalhole kcal/mole
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82 IEEE TRANSACTIONS ON COMPONENTS, PACKAGING. AND MANUFACTURING TECHNOLOGY-PART VOL. 17, NO. I , MARCH 1994
AI
0 90
0 200 300
Fig. 7. SEM micrographs of the intermetallic phases formed in the bimetallic
AI-Cu contact after 2 h of diffusion annealing at C by an electrical
current. Fig. 9. Formation and propagation of the intermetallic phases in the A l Z u
bimetallic contact diffusion annealed by an electrical current.
0 30 90 150
Fig. 8. Cracks formed in the intermetallic layers illustrating the fragility of (pm)
intermetallic phases formed in samples heat treated by an electrical current.
Fig. 10. Growth of interface resistance with thickness of the intermetallic
phases formed at the AI-Cu bimetallic joints after heat treatment by an
a single activation energy over the entire temperature range electrical current at different temperatures and times.
studied but rather by considering the two separate regions,
i.e., 200 to 300°C and 350 to 500°C.The activation energy intermetallic layers formed follows (3) with the proportionality
corresponding to temperatures below approximately 350°C is constant A having the value
considerably lower, Q 13.2 kcal/mole, than that obtained The most important feature of these results is that both
for higher temperatures Q 20.5 kcavmole. It is important the rate and the total diffusion bandwidth of the intermetallic
to note that for the same temperature range, these values phases formed under the influence of electrical current are
are significantly lower than those obtained for the samples higher than in samples diffusion annealed in fumaces. Some
diffusion annealed in a furnace, i.e., Q 17.2 kcaYmole and plausible explanation for the observed effect will be provided
Q 32.2 kcdmole. in the discussion. These results are in contrast with those
The contact resistance rise resulting from the formation of obtained in the case of roll-bonded aluminum-to-brass since
the intermetallic phases at the Al-Cu interface was determined no effect of electrical current on the intermetallic growth was
by averaging ten resistance measurements made across this found in this system [8].
interface after selected time intervals at each of the diffusion
annealing temperatures. The results are shown in Fig. 10. IV. DISCUSSION
Within the scatter of experimental data, the rate of resistance The permissible operating temperature in electrical connec-
rise across the Al-Cu interface and thickness (x) of the tioas is generally within the range 100-150°C. However, it
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BRAUNOVIC AND ALEXANDROV: INTERMETALLIC COMPOUNDS AT ALUMINUM-TO-COPPER ELECTRICAL INTERFACES 83
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IEEE TRANSACTIONS ON COMPONENTS, PACKAGING, AND MANUFACTURING TECHNOLOGY-PART A, VOL. NO. MARCH 1994
under the low-current densities or ac conditions. Hence, since In summary it can be stated that electrical current exerts a
in the present work, ac current of comparatively low density pronounced effect on the morphology of the Al-Cu bimetallic
lo3 A/cm2) was used, electromigration alone is unlikely solid-phase joints, which, in tum, can dramatically affect the
to be the operating mechanism responsible for the observed current transfer across the contact interface and thus their
accelerated formation of the intermetallic phases in electrically reliability in electrical installations.
heat-treated Al-Cu, bimetallic joints.
An alternative is that accelerated formation of the inter-
metallic phases is a result of an enhanced diffusion of some
species, most probably copper. The enhancement may result V. CONCLUSIONS
from the concentration of vacancies and interstitials exceeding 1) The results show that the formation and growth of
their respective equilibrium values, thus increasing proportion- intermetallic phases in aluminum-to-copperbimetallic friction-
ally the contributions from the vacancies and interstadials to welded joints a pronounced effect on their mechanical and
the diffusion rates. electrical integrity.
Indeed, an extensive experimental and theoretical work 2) The deleterious effect of intermetallic phases is mani-
in the general area of the behavior of irradiated materials fested by an increased brittleness of the contact interface.
showed that the atomic mobilities can be increased under 3) The formation of intermetallic phases induce significant
ion irradiation by many orders of magnitude. This, although increase in contact resistance which is found to increase
being a rather attractive possibility, is unlikely since it is linearly with the thickness of the intermetallics formed.
inconceivable that a relatively low density current can produce 4) The intermetallic phases can form relatively rapidly
marked changes in the vacancy and interstitial concentrations at temperatures generally accepted as normal operating and
as in the case of irradiated materials. overload temperatures for the connectors on the network.
Another possible mechanism is that accelerated diffusion oc- 5) The presence of an electrical field greatly accelerates
curs via some short-circuit diffusing paths rather than through the kinetics of formation of intermetallic phases and alters
the lattice. Such short diffusion paths, called “pipe diffusion,” significantly their morphology.
can be dislocations, grain and subgrain boundaries. Diffusion
along these paths is found to be considerably faster (several
orders of magnitude) than diffusion of the same species ACKNOWLEDGMENT
through the lattice [lo].
The authors wish to express their thanks to A. Joly, J.
If the “pipe diffusion” is the operating mechanism, then
Larouche, P. Dufresne, and J. St-Onge for the technical
the kinetics of the intermetallic phase formation and growth
assistance and successful execution of this work.
leads to the conclusion that the mobility of diffusing species,
probably copper, is much greater in the presence of an electric
field than in the temperature gradient. Hence, it is believed REFERENCES
that interaction between the applied electric field and lattice
[I] C. R. Dixon and F. G. Nelson, “The effect of elevated temperature
defects notably dislocations and grain boundaries, enhance on flash-welded aluminum-copper joints,” Trans. AIEE /I, vol. 78, pp.
the migration of the diffusing species along these short- 4 9 1 4 9 5 , 1960.
circuit diffusion paths and thus accelerate the formation of [2] E. R. Wallach and G. J. Davis, “Mechanical properties of aluminum-
copper solid-phase welds,” Metals Tech.. pp. 183-190, Apr. 1977.
the intermetallics. [3] “Joint resistance and current paths in heat-treated alu-
The absence of certain phases, in samples heat-treated by an minudcopper solid-state welds,” Metals Sci.. pp. 97-102, Mar.
electrical current, can be attributed to the increased incubation 1977.
[4] D. M. Rabkin, V. R. Ryabov, A. V. Lozovskaya, and V. A. Dovzhenko,
time of some phases caused by the presence of an electrical “Preparation and properties of copper-aluminum intermetallic com-
field. In other words, the growth of these phases from their pounds,” Sov. Powder Metall. Ceram., no. 8, (92), pp. 695-700, 1970.
[5] M. M. Nakamura, Y. Yonezawa, T. Nakanishi, and K. Kondo, “Dura-
critical nuclei is suppressed by diffusion interaction with the bility of AI-Cu hot-pressure welding joints,” Wire J., pp. 71-78, Apr.
critical nuclei of neighboring phases having greater diffusion 1977.
permeability This agrees well with the results of the study [6] J. A. Rayne and C. L. Bauer, “Effect of intermetallic phase formation
on electrical and mechanical properties of flash-welded AI-Cu couples,”
dealing with the effect of electrical current on the formation in Proc. 5th Bolton Landing Con$ Weldments, General Electric, 1979,
and growth of intermetallic phases in AI-Au system [12] pp. 353-363.
where it was shown that electrical current can accelerate or [7] C. L. Bauer and G. G. Lessmann, “Metal-Joining Methods,” Rev.
Materials Sci., vol. 6 , pp. 361-387, 1976.
suppress the growth of certain phases. [8] R. Timsit, “Electrical connectihility of aluminum wire,” CEA Report
It is obvious that further studies are needed to elucidate the 76-19, pp. 84-89, 1985.
[9] H. B. Huntington, “Electromigration in metals,” in Diffusion in Solids:
exact nature of the observed effect of an electric current on Recent Developments, A. S. Nowick and J. J. Burton, Eds. New York:
the kinetics of formation and growth of intermetallic phases in Academic, 1974. ch. 6.
Al-Cu bimetallic welded joints. This is of particular interest [lo] N. Gjosten, D@sion, ASM, 1973, p. 241.
[ l l ] A. M. Gusak and K. P. Gurov, “Kinetics of phase formation in a
since there is mounting evidence indicating that mechanical diffusion zone during interdiffusion. Phase formation in an electric
properties such as creep, stress relaxation, flow stress and field,” Phys. Metal. Metallography, vol. 53, no. 5, p. 12, 1982.
also recrystallization, recovery and.grain growth can be sig- [12] V. N. Pimenov, K. P. Gurov, K. I. Khurdyakov, S. S. Dol’nikov, R.
A. Milievskii. V. S. Khlomov, and Yu. G. Miller, “Effect of electrical
nificantly altered and the structure changed by the action of current on the phase transformation in the diffusion layer,” Fiz. Khim.
electrical current. ‘Obrabotki Materialov, p. 10”1,?7978(in Russian).
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BRAUNOVIC AND ALEXANDROV: INTERMETALLIC COMPOUNDS AT ALUMINUM-TO-COPPER ELECTRICAL INTERFACES
M. BraunoviC (SM'9.3) received the Dipl. Ing. N. Alexandmv received the B.S. degree in engi-
degree in technical physics form the University of neering from the Higher Institute of Mechanical and
Belgrade, Belgrade, Yugoslavia, in 1962. and the M. electrical Engineering, Sofia. Bulgaria. in
Met. and Ph.D. degrees in physical metallurgy from From 196.5 to 1979 he was working for different
the University of Sheffield, England. in 1967 and companies in Bulgaria and Crechoslovakia, where
1969, respectively. he supervised the work in the field of welding.
He joined the Institute of Metallurgy, Zenica, design, and industrial robotic applications. From
Yugoslavia, in 1962, where he was working in to he was associated with the Canadian
materials science research until 1965. From 1965 Welding Institute, Varennas, and in 1983 he joined
to 1969 he was asaociated with the Department of IREQ, Hydro-Quebec Research Institute. his main
Metallurgy, University of Sheffield. and from 1969 areas of activity are resistance welding. electrical
to 1971 he was associated with the Department of Mines and Metallurgy. contacts, robotics, and amorphous metals applications.
Lava1 University, Quebec, Canada. he joined IREQ in 1971, where he is Mr. Alexandrov has 22 inventions related to automation and improvement
presently a Senior Member of the scientific staff. His principal areas or olelectrical resistance welding. He also has a number of patents on amorphous
research are surface and interface phenomena in solids, phenomena related metal transformers and has presented a number of scientific papers at
to electrical contacts, shape-memory materials, and tribology. international conferences in the field of welding.
Dr. Braunovit has presented many papers at various intcmational confer-
ences and has published a large number of papers in the of his scientific
interests, including contributions to encyclopedias and books. He was the
Chairperson of the 15th International Conference on Electrical Contacts, held
in Montreal, August 2&24, 1990. he is a member of the American Society
for Physics, the American Society for Metals, the Materials Research society,
the Planetary Society, and the New York Academy of Sciences.
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