Electrical and Interfacial Characterization of Conductors Under Tensile Strain

Jake Rabinowitz1,2, Gregory Fritz1, Caprice Gray1

1 C. S. Draper Laboratory, Cambridge MA
2 Northeastern University Dpt. Chemical Engineering, Boston MA
Abstract
An important step towards developing viable flexible hybrid electronic (FHE) platforms is qualifying the
performance of materials and processing methods under strain. Metal films on polymer substrates have
demonstrated elasticity under tensile strain, but standard methods to quantify performance of these
interfaces are only just starting to be developed in this emerging FHE industry. In this work, we have
developed a model to predict strain induced crack percolation and a method to electrically measure
conductor deformation. To validate the model, we measured conductor resistance while applying tensile
strain to various metal-polymer systems. Under such conditions, it is known that resistance will increase
!
geometrically according to the relationship
= 1 + ; any further resistance increase is caused by
!!

conductor deformation. On kapton substrates strained to = .07, evaporated gold films did not deform,
whereas deformation caused 29% and 72% of the resistance increase in evaporated and printed silver
films, respectively. On PDMS substrates, conductors were significantly less elastic. At strains of only =
.024, deformation caused 29% of the resistance increase in evaporated silver films and 86% of the
resistance increase in evaporated gold films. Printed silver films were inelastic, losing continuity nearly
instantaneously. The results suggest that rigid polymers and traditional fabrication techniques may be
more suitable to FHE applications than softer substrates and additively manufactured conductors.
1. Introduction
Soft materials and electronic systems offer intriguing and exciting possibilities when compared to their
conventional rigid counterparts. Flexible hybrid electronics (FHE) could enhance functionality and
introduce conformability to current electronic devices, while pioneering novel implantable and interfacial
biocompatible ones [1]. Current silicon-based microfabrication techniques are generally incompatible
with soft materials, which has spurred the development of additive manufacturing techniques that hope to
enable realization of flexible and stretchable devices [2,3]. Aerosol inkjet printing is of particular interest
to FHE because it enables precise deposition of any aerosolizable bulk material onto a variety of surfaces
rigid, curved, nonuniform, flexible, elastic, and hybrid [47]. Additionally, this method facilitates rapid
design prototyping and incorporation of novel materials into complex device geometries [810].
However, in order to determine their viability for many potential FHE applications, inkjet printed
materials must be characterized under mechanical strain, which will be intrinsically present in future FHE
systems.
Extant research has characterized a variety of conductors on non-silicon substrates under single strain
conditions., A number of studies have been done to quantify strain induced deformation of metal traces
applied to polymer films using more traditional evaporation and sputtering methods [1119]. When
considering conductive materials applied by alternative manufacturing methods, silver has been the most
heavily characterized. Researchers have demonstrated stretchable silver nanoparticle, microparticle, flake,
and reactive inks, as well as nanowire networks [4,7,10,2023]. Within the scope of these materials and
processes is a wide range of tolerances to mechanical strain and a universal increase in electrical
resistance while applying the experimental strain.
When applying tensile strain to a conductor, it is possible to derive the geometric rate of resistance
increase from the fundamental resistance definition and simple assumptions regarding strain conditions.
For any conductor, resistance is defined as

!"

(1)

where R is resistance, is resistivity, L is length, and A is cross-sectional area. If it is assumed that the
volume of a conductor under tensile strain is preserved, then the following relationship is maintained
= ! !

(2)

where A and L are the changing cross-sectional area and length during strain and A0 and L0 are the initial
cross-sectional area and length. If it is also assumed that the resistivity of the film remains constant
throughout strain, then dividing the dynamic resistance by the initial resistance yields the change in
resistance as a function of strain according to the relationship
!
!!

! !
!!

= (1 + )!

(3)

where R0 is the initial resistance and is the engineering strain. Because the above relationship assumes
that the conductor is not damaged during tensile strain, it will henceforth be referred to as the ideal rate of
resistance increase.
The work of Zuo, et al. confirmed the validity of the previous assumptions by demonstrating that the
resistance increase of copper on polyimide obeys the derived relationship up to tensile strain = 0.5 [11].
At large strains, they observed microcracking of the film but determined that the deformations had
negligible effect on the film resistance, based on close adherence to the ideal relationship. In conjunction,
they determined that macroscale cracking was initiated at some critical strain limit, c, where the
measured resistance surpassed the ideal resistance by 5% [12]. The findings supported the groups prior
finite-element analysis indicating that strong interfacial adhesion of a metal to a sufficiently stiff polymer
can enable metal elasticity during tensile strain by way of the substrate delocalizing strain in the overlying
film [24]. Crucial to their analysis was the need for a sufficiently stiff polymer, indicating that softer
materials would be less capable of delocalizing strain and preventing destructive deformation.
2. Theory of Dislocation Induced Resistance during Tensile Strain of Conductors
The present report relies on experimental observations and extant data to develop a model to quantify the
integrity of conductor-polymer interface under tensile strain. Conductor-polymer systems under tensile
strain experience resistance increase in excess of the ideal rate, expressed in equation 3. Resistance
increases beyond those caused by bulk geometric factors are caused by dislocations: cracks of varying
depths, sizes and distributions. These dislocations decrease the volume of the conductive path and gives
rise to a resistance increase beyond the ideal case in equation 3. In the following discussion, we will refer
to this excess resistance as dislocation induced resistance.
To evaluate the impact of dislocation on resistivity of strained traces on polymer substrates, we relied on
similar work that has been done to model the resistance of thin ITO films on PET substrates under tensile
strain based on crack initiation [25]. The research of Cairns, et al. calculates the increased resistance of a
cracked film as the summation of the incremental resistance added by all individual cracks initiated in the
strained film. Their model defined crack induced resistance as follows
!!
!

!!!
!

!
!!!(

!" )!

[4]

where Rc is the crack induced resistance increase, L is strained gauge length, is resistivity, is a length
scale, m is the number of cracks, is strain, ci is the strain at first crack initiation, and V is volume of the
cracked conductive path. Further, the work of Leterrier, et al. expands upon Cairns model to account for
nonlinear crack propagation and the rapid transition from initial crack formation to loss of continuity
observed within ITO films [26]. Their model accounted for nonlinear crack propagation as follows
! =

!!!
!

!
!!!

!!! !!
!!!

ln

[5]

where k is the crack density, N is the crack density at film delamination, and is an adjustable factor
influenced by material nonuniformity.
More so than ITO films, thin metal films can maintain continuity at very large strains, albeit typically
with a significant degree of dislocation induced resistance. Thus, prior models designed for ITO cannot
directly be applied to metal-polymer systems, necessitating a model to predict the dislocation induced
resistance of metal-polymer systems under tensile strain. The model calculates dislocation induced
resistance using the following equation
= ! + ! = ! (1 + )! +

!!(!!!)
!

!(!!!)

[6]

where R is measured resistance, Rg is geometry induced resistance increase, Rc is dislocation induced

resistance, R0 is initial resistance, is engineering strain, is metal film resistivity, D is characteristic
crack length along the direction of strain, A is the characteristic crack cross-sectional area, m is the
number of cracks in the metal film, and is a crack-percolating factor.
We have added the crack-percolating factor to the resistance calculation as necessitated by the increased
elasticity of metal thin films when compared with ITO. Any deformations in metal thin films under strain
will demonstrate a tendency to increasingly propagate and converge with other deformities as strain
increases. The crack-percolating factor accounts for this characteristic by predicting exponential crack
growth with increasing strain. Moreover, the response of any experimental system will be a complex
function of polymer, metal, and interfacial properties, allowing the crack-percolating factor to serve as a
metric to compare the relative performance of investigative systems.
It is possible to determine an appropriate value for and subsequently calculate m at any point during
strain. Solving Eqn. 4 for m generates the desired relationship

1+

(1+)
0
(1+)

[7]

where m grows exponentially with strain as cracks begin to percolate.

Characteristic crack dimensions were determined from scanning electron and atomic force microscopy
measurements of post-strained experimental metal films. Characteristic cracks were chosen from isolated
deformities representative of those observed during crack initiation. For simplicity, it was assumed during
calculation that all cracks were of the same dimension as the average characteristic crack, and that the
deformed conductive path had resistivity equal to the pure thin film resistivity. It was also assumed that
the cross-sectional area of the crack remained constant and the length along the direction of tensile strain
grew proportionally with the strain.

3. Materials and Methods

3.1 Kapton Substrate Preparation
Kapton was used as a polymer substrate. 125 m thick kapton polyimide type HN film was purchased
from DuPont and cut into 6 inch disks. Prior to deposition, the disks were washed in acetone and
isopropanol to remove any surface contamination and then rinsed in water and dried in nitrogen air to
remove organic solvents.
3.2 PDMS Substrate Preparation
PDMS was used as an alternate polymer substrate. 1mm thick PDMS disks were produced by mixing
Dow Corning Sylgard 184 in a 10:1 ratio of base:curing agent and pouring 20g of mixed solution onto the
backside of a 6 inch petri dish with a 1mm recess. Cross-linking was induced by curing in an oven at 75
o
C for 6 hours. Prior to deposition, the disks were washed in acetone and isopropanol to remove any
surface contamination and then rinsed in water and dried in nitrogen air to remove organic solvents.
When used as a substrate for inkjet printed conductors, PDMS was additionally treated for 1 minute with
120 W O2 plasma at a pressure of 0.6 mbar in order to increase the hydrophilicity of the surface,
improving wettability of water-based inks [27].
3.3 Metal Evaporation
Gold and silver metal films were electron-beam evaporated through shadow masks containing the
experimental geometry. Deposition chamber pressure was 2*10-7 T and thickness was 100nm.
3.4 Aerosol Inkjet Printing
Silver flake ink was used as-purchased from Novacentrix. Prior to printing with an Optomec Aerosol Jet
300 printer, silver ink was pneumatically atomized. Printing was done at a speed of 2.5 mm/s atop a
platen heated to 40 oC under atmospheric pressure. Following printing, silver ink was laser sintered with a
700 mW laser that followed the printing path at a speed of 2.5 mm/s.
3.5 Resistance Recording
4-wire resistance measurements were recorded during tensile strain using an Agilent 34970A Data
Acquisition Unit and the corresponding BenchLink Data Logger software. Different mechanisms were
used to contact the resistance pads according to the trace geometry and interfacial adhesion. For
evaporated metals on kapton, conductive copper tape was used to securely contact stripped wires onto the
resistance pads. For evaporated metals on PDMS, adhesion was such that the conductive copper tape
lifted off the metal; toothless alligator clips securely contacted the resistance pads and were shorted out to
the measurement device. For printed conductors on either substrate, small geometry inhibited the two
aforementioned contact methods; silver epoxy was used to contact small, stripped wires to the resistance
pads. Resistance recording began prior to strain initiation and continued beyond substrate failure.
3.6 Tensile Testing
Tensile strain was applied to conductor-polymer systems using an Instron 5982 tensile tester. Varying
sample lengths were normalized by controlling strain at a rate of = 0.1/min. Data recorded by BlueHill
software allowed for reliable alignment of strain data with resistance data based on the drop in load upon
substrate failure, which corresponded to a loss of electrical continuity.

4. Results & Discussion

4.1 Conductors on Kapton Substrates
The ideal resistance increase for metal thin films on stiff polymer substrates was initially verified by
applying tensile strains to gold thin films on kapton substrates. As depicted in Figure 1, resistance versus
strain curves for 100nm thick gold thin films on 125 m kapton substrates adhered closely to the ideal
curve until kapton failure, never differing by more than 0.5%. For gold thin film and all subsequent data,
error bars represent the minimum and maximum values across all experimental trials. Post-strain SEM
inspection corroborated the gold strain data by revealing no noticeable deformations or flaws in the poststrained films.

Figure 1: Resistance change versus strain for conductors on kapton substrates. Data for gold thin films
verifies ideal relationship as described for metal-polymer systems under tensile strain.
In contrast, silver thin films on the same substrate did not exhibit the same degree of elasticity. At <
0.02, deformation induced resistance is measured. Macroscopic cracking initiated, on average, at c =
0.07, just before the cutoff point of kapton failure. Upon inspection of post-strained silver films, it was
clear that strain localization and film debonding occurred. Figure 2 depicts the distinct contrast between
the undamaged portions of the post-strained silver film (left) and the deformed portions (right). The left
side of the figure was characteristic of the majority of the thin film and closely resembled the entirety of
the post-strained gold film. In contrast, small regions demonstrated a high density of localized film
wrinkling (inset) that occurred during spontaneous compressive strain of the system from failure length,
Lc, to initial length, L0, upon kapton failure. The phenomenon of wrinkling of an overlying film on a
compressively strained polymer has been characterized previously [28,29]. The observed wrinkling is
consistent with the measured deformation induced resistance, both of which indicate that some material

failure occurred during tensile strain. In the present case, the failure was interfacial debonding of the
silver thin film.

Figure 2: Undamaged (left) and deformed (right) portions of post-strained silver thin film. Deformation
indicates that strain localization occurred within damaged regions, causing debonding at the film-polymer
interface. Where adhesion failed, debonded film wrinkled upon substrate failure and compressive
straining of the system. Scale bars 100 m and 2 m (inset).
Additionally, the performance of the evaporated metallic conductors under strain was compared to that of
an additively manufactured conductor, aerosol inkjet printed silver flake ink. The printed silver on kapton
fared the worst of all investigated conductors, exhibiting average c = 0.021 and a > 50% resistance
increase at the point of kapton strain failure. It should also be noted that initial resistivity of the printed
silver was nearly an order of magnitude greater than the other investigated materials.
Tape peel tests revealed that all conductors adhered strongly to the kapton, suggesting that material
properties drove the observed results. The difference in response to the tensile strain among the
evaporated metal films is most likely caused by the difference in modulus of gold and silver thin films on
kapton, which were measured to be _ GPa and _ GPa, respectively. The higher modulus of the silver
prevented it from demonstrating the same elasticity as the gold. The results similarly suggest that silver
thin films possess a lower strain hardening exponent than their gold counterparts, which is a similar
measure of material plasticity versus elasticity under strain. However, the present report did not have the
means to quantify the strain hardening exponent, nor could it find any values reported in literature.
There existed different governing mechanisms for electron transport within the printed silver under tensile
strain. Despite the poor elasticity of the printed silver when compared to the evaporated metals, inspection
of the post-strained printed conductor did not reveal discernable cracking (Figure 3). It is therefore likely
that the inks conducting silver flakes remain suspended in an aqueous medium that is loosely adhered to
the surface. Although the laser sintering process enables ink conductivity, it likely does not fuse the
grains into a cohesive film. As a result, when applying a tensile strain, the interconnected conductors are
pulled apart, reducing the number of electron transport pathways and correspondingly increasing the film
resistance.

Figure 3: Grain structure of post-strained silver flake ink on kapton. The lack of cracking indicates that
deformation induced resistance is caused by loss of grain overlap during tensile strain. Scale bar 1 m.
Consequently, the deformation induced resistance model was only applicable to one of three investigated
conductors on kapton. The gold thin films could not be applied because they did not demonstrate any
deformation induced resistance, and the printed silver thin films could not be applied because the
deformation was only discernable in resistance measurements. When trying to apply the model to the
evaporated silver films on kapton, an adjustment was needed based on interfacial debonding, rather than
surface cracking, causing deformation induced resistance. Applying the model required an inverted view
of the system, whereby cracking was initiated from the bottom of the film and propagated towards the
surface, with a depth of some distance less than the film thickness. There is no reliable means of
estimating the depth of these specific deformities, so it was only possible to determine a range for with
the assumption that the geometry of the observed wrinkles corresponded to bottom-up cracks whose
depths were somewhere within the range of the film thickness. Post-strain inspection typically yielded
370 (m) observed cracks across the entire metal film, with characteristic dimensions of 7 m (D) along
the direction of strain, 120 m width in the perpendicular direction, and depth of 0.01 0.09 m. As
such, the corresponding range for the crack-percolating coefficient for 100nm silver thin films evaporated
on kapton substrates is 1.1 < < 2.1, with the low corresponding to a 0.01 m deep characteristic crack
and the high corresponding to a 0.09 m deep characteristic crack.
4.2 Conductors on PDMS Substrates
Thin metal films on soft polymer substrates exhibited significantly less elasticity. As depicted in Figure
4, resistance versus strain curves for all experimental conductors demonstrated far more deformation
induced resistance than when strained on kapton substrates. 100nm thick evaporated gold and silver thin
films reached c at values of 0.006 and 0.042, respectively. Printed silver films on the same substrate were
completely inelastic, experiencing deformation induced resistance that was orders of magnitude greater
than R0 and losing continuity at < 0.005. Based on the previously referenced works, greater magnitude
of deformation induced resistance during tensile strain was expected for these systems because of both the
poor interfacial adhesion when depositing metal thin films on PDMS and the decreased efficacy of the
lower-modulus polymer when attempting to delocalize strain in the overlying film.

Figure 4: Resistance change versus strain for conductors on PDMS substrates and number of cracks
(orange) versus strain for evaporated gold and silver thin films on PDMS.
Because the evaporated thin films on PDMS exhibited extensive cracking, it was possible to apply the
deformation induced resistance model and determine a crack-percolating coefficient for the systems. For
the post-strained gold thin films, characteristic cracks were determined to be 0.2 m in the direction of
tensile strain (D) and 0.7 m x 0.05 m in cross-section (A); for the post-strained silver thin films,
characteristic cracks were determined to be 1.0 m in the direction of tensile strain (D) and 0.25 m x
0.03 m in cross-section (A). The difference in magnitude of the characteristic crack sizes when
comparing post-strained silver thin films on PDMS to those on kapton is demonstrative of the inability of
PDMS to delocalize strain in the overlying film. Shown in Figure 5 are SEM and AFM micrographs of
post-strained gold (left) and silver (right) thin films on PDMS. AFM data was used to determine the
typical crack depth and higher resolution SEM data was used to determine the planar dimensions of the
smaller, isolated cracks seen in the figure.

Figure 5: AFM (a,b) and SEM (c,d) micrographs of gold (a,c) and silver (b,d) thin films on PDMS
substrates following tensile strain. Scale bars 2 m.
The deformation induced resistance model was employed to further quantify the performance of the
metal-PDMS systems under strain. Based on extrapolation of the number of cracks counted in SEM
micrographs across the entire area of the silver film, the characteristic crack dimensions, and the known
final resistance and strain values, the crack percolating factors of = 1.4 and = 1.9 were determined for
gold and silver thin films, respectively. It is consistent with material properties that the value for a
silver-PDMS system would be within the high-end of the previously stated range for the silver-kapton
system based on the decreased substrate modulus and interfacial adhesion when employing PDMS as the
polymer substrate. Additionally depicted by the orange curves in Figure 4 is the exponential increase in
crack initiation at large strains. From the calculated values, it was possible to determine the number of
cracks, m, found in the gold and silver films at all degrees of strain.
From the curves, it is clear that the gold cracked significantly more than the silver at equal strain. The
calculation is derived from the greater magnitude of deformation induced resistance in the gold film, but
is in contrast to the previous material responses when deposited on kapton. Interfacial analysis suggests a
possible explanation for the substrate-dependence of the metal responses. Even after curing, PDMS has a
significant presence of oxygen on the surface, which will chemically bond to reactive metals during
evaporative deposition. Whereas inert gold will only exhibit physical interfacial adhesion, silver seems to
possess a more robust interface with PDMS because of surface chemical bonding. Thus, the gold interface
debonds and cracks to a greater degree than the silver interface at comparable strain. Additionally of note
is the greater value of for silver films when compared to gold counterparts. The model suggests that the
significance of the disparity is that silver cracks tend to propagate to a greater degree than gold cracks, a
finding that seems to be mostly consistent with the SEM micrographs of Figure 5. The magnitudes of the
largest gold cracks exceed those of the largest silver cracks, but local percolation is more prevalent in the
silver, where far fewer isolated cracks were observed. Future analysis will serve to more definitively state
whether qualitative inspection of gold and silver films under strain is consistent with the calculated crack
percolation factors.
As was the case with the printed silver on kapton substrates, the deformation induced resistance of the
same conductor on PDMS was not caused by destructive cracking. Silver ink on PDMS did not
demonstrate visual cracking unless strained to extreme levels ( > 0.3) far beyond the loss of continuity.
The current belief is that when strained on the softer polymer, the lack of substrate support drastically
emphasizes the previously discussed loss of silver flake interconnection, resulting in conductor
inelasticity at very low strain. Also of note is that despite the inelasticity of the printed silver, it was able
to retain values close to the initial R0 upon compressively straining the substrate back to L0. Based on this

characteristic, is it conceivable that inkjet printed silver be employed as a strain switch on soft polymerbased electronic systems. The ink could serve as a crucial interconnection that disables sensitive device
components when the system is under strain and reconnects the same components when the strain has
been released.
5. Conclusion
In conclusion, various conductor-polymer systems have been compared under tensile strain for the
purpose of qualifying the systems for future use in FHE applications. Of the investigated polymer
substrates, kapton and PDMS, it was clear that the kapton enabled far more conductor elasticity due to a
combination of stronger interfacial adhesion and greater rigidity. Traditionally deposited conductors,
evaporated gold and silver thin films, outperformed printed silver flake ink, a finding indicating that
adapting traditional tooling to emerging needs may be more appropriate than relying on novel additive
manufacturing techniques for FHE applications.
Moreover, a model has been provided to predict deformation induced resistance of metal-polymer
systems under large tensile strain. Embedded in the model is a crack-percolation factor, , and a
determination of the number of cracks in a system, m, at any given strain. Future work should determine
for additional metal-polymer systems in order to verify the factor as a figure of merit for FHE
applicability, with favorable materials combinations possessing a low value. The deformation induced
resistance model was specifically applied to gold and silver thin films on PDMS, providing crackpercolation factors of = 1.4 for gold and = 1.9 for silver, although gold experienced significantly more
cracking based on weaker interfacial adhesion. The results suggest that improved adhesion would allow
the performance of the gold thin films under strain to surpass silver thin films. Further, the model was
able to predict a range for the crack-percolating factor of silver thin films on kapton, where 1.1 < < 2.1.
Finally, a potential application in the form of a strain-protection switch is presented in the form of silver
flake ink printed on PDMS. The inkjet printed conductor on PDMS demonstrated both loss of continuity
at < 0.005 and the ability to recover its initial resistance upon returning to L0 during cyclic strain. As
such, it could have the potential as a crucial interconnection switch that disables sensitive device
components from functioning during strain and reconnects such components when the system is no longer
under strain.
Acknowledgements
The work was conducted at the C. S. Draper Laboratory and received funding from the laboratory. We
would like to acknowledge the meaningful contributions of Brian Smith, Joseph Louis, Joseph Ricker,
Peter Standley, Abigail Spencer, and Peter Lewis, without whom the project would not have been able to
reach this point.
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