Piezoelectric properties and ferroelectric hysteresis effects in uniaxially

stretched nylon-11 fUms

s. C. Mathur, J. I. Scheinbeim, and B. A. Newman
Department of Mechanics and Materials Science. College of Engineering. Rutgers University. New
Brunswick. New Jersey 08903
Oriented nylon-II films [initially quenched (c5 ' form) or slow cooled (a' form) from the melt]
subjected to a series of static positive and negative poling fields were found to show a hysteresislike
behavior of the piezoelectric strain constant d
31
and the piezoelectric stress constant e
31
This
behavior was very similar to that observed in poly(vinylidene fluoride) (PVF
2
) and attributed to
ferroelectric dipole switching, in a previous study. No change in the x-ray diffraction patterns of
the c5'-form films was observed after poling. Changes in the x-ray diffraction patterns of the a'-
form films after poling were consistent with dipole reorientation in the crystalline regions. In both
cases the magnitude of the piezoelectric response of the oriented films was considerably higher
than that of the unoriented films. The melting points of the poled films increased significantly
relative to that of the unpoled films with the same thermal history, which may suggest field-
induced annealing effects.
I. iNTRODUCTiON
Recent investigations I in our laboratory showed that
nylon 11 films can be poled to give films with high piezoelec-
tric activity. The value reported for the piezoelectric strain
constant d
31
1-3 p C/N) of un oriented films was the largest
reported value for any polymer other than poly(vinylidene
fluoride) PVF
2
(-20 P C/N for commercially available ori-
ented films). In more recent studies
2
even higher values
(d
JI
-6 p C/N) have been obtained for nylon 11 films.
Several polymorphic forms have been reported for ny-
lon 11. Fibers drawn from the me1e and solvent cast films
(from a phenoVformic acid solution)4 give the polar a form,
with two strong x-ray reflections (100) and (010) with d spac-
ings at 4.40 and at 3.62 A, respectively. There is also an (001)
reflection with a d spacing at 11.3 A. Melt crystallized mate-
rial shows a similar x-ray pattern to the a form, but with
small systematic differences which will be discussed in a sep-
arate publication. This modification will be termed the a'
form. If melt crystallized nylon 11 films la' form) are heated
above 95C, the two higher angle reflections coalesce to give
a single reflection at 4.16 A.
5
The (00 1) reflection remains at
11.3 A. This modification is termed the c5 form. Quenched
films show an x-ray pattern similar to the c5 form but the
4.16-A reflection is very broad. This modification has been
termed "smectic,>4 but will be referred to here as the c5 ' form.
Finally, a rform{with an x-ray pattern similartothec5 andc5'
forms but with a d spacing at 14.9 A) can be obtained by
casting films from trifiuoroacetic acid solutions.
4
Some of the initial results obtained for nylon 11 showed
puzzling features. Following poling, quenched tilms (c5'
form, with a low degree of crystallinity) s.bowed a higher
piezoelectric response
2
than the melt crystallized films (a'
form with a higher degree of crystallinity). If quenched films
are annealed before poling the piezoelectric response is re-
duced. I However, Scheinbeim
6
measured d
31
at tempera-
tures up to 100 Cand observed thatd
31
increased sharply (to
10 p C/N at 100 0c) at temperatures above the glass transi-
tion temperature T
g
On decreasing temperature to room
temperature, most of the polarization remained (d
31
de-
creased only - 20% relative to its initial value). This behav-
ior is not observed for conventional electrets with polariza-
tion arising from space-charge distributions. Moreover, it
seems unlikely that polarization arises mainly from molecu-
lar dipoles in the amorphous regions (as for example in poly-
vinyl chloride) since this would be lost with the onset of mo-
lecular motion above T
g
In fact, the variation of d
31
with
temperature observed for nylon 11 parallels the behavior of
PVF
2
(T
g
- 50C). No detailed studies have been made
regarding field-induced crystal transitions for nylon 11.
Studies using x-ray diffraction
6
for unpoled quenched nylon-
11 films indicate that there is no phase transition to the a or
a' phases during poling. This suggests the existence of a po-
lar phase in the quenched films and this will be discussed in a
separate pUblication.
7
In other preliminary studies, uniaxial-
ly drawn nylon-II quenched films
8
showed higher piezoelec-
tric activity when compared to unoriented films under iden-
tical po1ing conditions. In a recent study of
electric-field-induced changes in the x-ray diffraction pat-
tern
9
of nylon-II films which the authors state to be a mix-
ture of the a and r crystal phases, it was observed that the
crystallites orient in such a way that the dipoles are preferen-
tially aligned in the direction of the poling field. A correla-
tion between the piezoelectric response and the degree of
orientation observed in the x-ray scans was noted.
Most recent investigations of piezoelectric polymers
have centered on explaining and improving the response of
poled poly(vinylidene fluoride) IPVF
2
) films. Although
much work remains to be done with this polymer, including
establishing relationships between electret properties and
crystal morphology and molecular orientation, a general un-
derstanding of the piezoelectric, pyroelectric, and ferroelec-
tric behavior ofPVF
2
has been reached. The idea that PVF
2
electret properties result from the aggregate properties of
polar crystallites with preferred dipole orientation is well
established. It is now known that the piezoelectric coeffi-
cients, d
31
and e31' of poled PVF
2
films are proportional to
the mass fraction of polar crystals present in the films. 10 It is
also known that the application of progressively higher pol-
ing fields results in field-induced phase transitions from non-
2419 J. Appl. Phys. 56 (9), 1 November 1984 0021-8979/84/212419-07$02.40 @ 1984 American Institute of Physics 2419
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polar (or less pol.ar crystal forms) to highly-polar crystal
forms with preferred dipole orientation. II Broadhurst and
co-workers 12 have successfully developed a theoretical mod-
el which relates polymer electret properties to the presence
of these polar crystals with preferred orientation embedded
in an amorphous matrix. Polarization in PVF 2 films can be
caused by field-induced crystal transitions or by ferroelectric
dipole switching. Conventional ac techniques have been
used to observe the hysteresis loopl3 between the electric
displacement and applied electric field for stretched films of
PVF
2
with the form I crystalline phase. Biaxially oriented
PVF
2
films, SUbjected to a sequence of rectangular voltage
steps 14 of successive opposite polarities, produceP-E hyster-
esis loops and switching currents typical of ferroelectrics.
Switching times of several minutes were observed. Tamura
et al.
15
used an electric field of 970 KV /cm (at 50 Hz) and
observed the hysteresis between the field E and the polariza-
tion P at room temperature for uniaxially stretched PVF
2
and reported switching times of the order of 10 msec for
polarization reversal. Infrared transmission 16 techniques
have been used to show the hysteresislike behavior of CF
2
dipoles in the crystalline regions ofbiaxiaHy oriented PVF
2
,
when the field is cycled between positive and negative values.
Biaxially oriented PVF
2
films 17 subjected to a series of static
positive and negative poling fields produce hysteresis curves
for the piezoelectric strain constant d
31
and the piezoelectric
stress constant e
31
showing the ferroelectric characteristics
of phase IV (polar phase II). Such static switching experi-
ments have the advantage that they may take into account
the long time dependence of polarization development. In
addition, since these measurements are not made under
field, they exclude contributions from film conductivity and
from the amorphous regions. X-ray measurements show a
field-induced phase transition from phase II to phase IV. It
was suggested from these x-ray studies, that reversal of po-
larization occurs in two steps: a transformation back to
phase II, fonowed by another transformation to phase IV.
The contribution to the polarization from phase I crystals
also exhibits cyclic behavior and two switching mechanisms
have been proposed: for low fields, 180 flipping, while for
higher fields, 60 ftiping. 18
A study of the piezoelectric and pyroelectric properties
of nylon-II films is instructive because it provides a way of
testing the generality of those concepts put forward to ex-
plain the piezoelectric and pyroelectric properties of PVF 2
films. In order to obtain further information about the ef-
fects of polarization and possible crystal phase transitions in
nylon 11, we studied the poling field dependence of the pie-
zoelectric behavior for uniaxially drawn quenched films (0 '
form). For the second part of the study, static switching ex-
periments were used to determine if nylon 11 shows the same
polarization reversibility as PVF
2
Two types of films were
studied: uniaxially drawn nylon-II quenched films (8' form),
and plasticized, uniaxially drawn nylon-II a' -form films.
The reasons for plasticization in the latter case was to be able
to stretch the films at lower temperatures and to increase
their piezoelectric activity. X-ray diffraction and differential
scanning calorimetry were used to study the crystalline re-
gions after various poling histories.
2420 J. Appl. Phys., Vol. 56. No.9, 1 November 1984
II. EXPERIMENT
Nylon-II films were made in two different forms. Melt
pressing at 205-210 C followed by slow cooling gave the a'
form. The quenched films were obtained by melt pressing the
nylon-II powder in the same temperature range and then
quenching the molten films into ice water. In both cases, the
nylon-II powder was pressed between aluminum foil at 3000
psi. The quenched films were then uniaxially stretched to a
draw ratio of2.5: I in an Instron at 23 C at an extension rate
of 0.05 in./min. X-ray photographs showed that the 0' form
with the chain direction in the direction of draw resulted.
The a' films were very difficult to stretch at temperatures
below 120 DC, so we decided to plasticize these films before
stretching. The films were plasticized by immersing in 2-
Ethyl 1,3 Hexanediol at 75C for! h. The content ofpl.asti-
cizer was found to be 11.6% by weight. These films were
then uniaxially stretched to a draw ratio of 2.4: I at 50 C at
the same extension rate as before. X-ray photographs
showed that the a' form with chain direction in the direction
of draw resulted.
Rectangular samples were cut from the stretched films,
keeping the longer dimension parallel to the draw direction.
Electrodes were coated on the samples using silver paint.
Poling was carried out using a conventional two-terminal
method with the sample placed between two copper elec-
trodes. An automatic voltage ramper raised the voltage
across the sample to the desired level at a constant rate. After
reaching the desired field, the temperature was raised to the
poling temperature. On completion of poling, the tempera-
ture was lowered with the field on. The quenched films were
poled at 75 C for 30 min. Because of excessive breakdown at
75 C, the a' samples were poled at 50 C for the same length
oftime. All samples were poled in a vacuum of - 10-
5
Torr.
Uniaxially stretched quenched films were subjected to pol-
ing fields up to 900 kV /cm. The piezoelectric strain constant
d
P
iezoelectric stress constant e
31
, dielectric constant, and
31'
modulus were measured in a Toyo-Seiki Piezotron at 3 Hz.
To study the hysteresis effects, films were taken in static
steps up to poling fields of 300 kV Icm and then the poling
field direction was reversed. Two cycles were completed
with fields up to 350 kV /cm in each direction. The same
sample was used for all fields. During the measurements of
d e dielectric constants and modul.us performed after
31' 31'
each static poling step, the hard silver-paint electrodes were
removed and soft silver epoxy was used for the electrodes.
The a' films were also poled for two cycles, with fields up to
350 kV /crn in each direction of poling.
Flat-film x-ray patterns and wide-angle diffraction
scans were taken at different stages of poling. Differential
scanning calorimetry studies were made using a Perkin-
Elmer DSC I-B and a heating rate of 10 C/min.
iii. RESULTS
A. Electrical measurements
Figures l(a) and l(b) show the results for uniaxially
stretched nylon-II quenched films. The values for both d
31
and e31 increase with increasing poling fields. The value for
d
31
(3.47 P C/N) is -25% greater than that observed for
Mathur, Scheinbeim, and Newman 2420
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10<)
-
"e
600
-0
e
-
..
.. 40()
e
NYLON l1("EL T PAEaaED , QUENCHED)
DRAWN: 2.':1, 2S-C. 0.0"".1.111.
POLINQ: "/0, SOMln.
NYLON 1 HMeL 'T PRES8ED .. QUENCHED)
OR AWN: 2.&:1. 211':, O.OlSln./min.
1 SeC. 30rnln.
e
e

e

o
10()
POLING FIELD H,W lem)
(b)
FIG. \. (a) Piezoelectric strain constant d
31
vs poling fields for uniaxially
stretched nylon-II (quenched) films; poled at 75 C for 30 min. (b) Piezoelec-
tric stress constant e
31
vs poling fields for uniaxially stretched nylon-II
(quenched) films, poled at 75 C for 30 min.
2421 J. Appl. Phys., Vol. 56, No.9, 1 November 1984
unoriented films in previous studies I under identical poling
conditions (500 kV fcm; 75 0q while the value for e
31
(5.47
mCfm
2
) is - 85% greater than that for the unoriented films.
The values tend to reach a plateau at fields of 800 k V f cm
under the given poling conditions. The highest value for d
31
obtained was 4.2 p C/N and that for e
31
was 7.2 rnCfm
2
at a
poling field of 900 kV fcrn. The samples could not be poled at
higher fields without breakdown occurring. The frequency
of dielectric breakdown increased rapidly at fields above 600
k V fern. The modulus of all the samples was also measured in
the Piezotron and the ratio of e
31
fd
31
= modulus, matched
within experimental error. The modulus of all samples after
poling at various fields remained constant. The dielectric
constant remained essentially constant following different
poling fields up to fields of 700 kV fern and then showed a
slight increasing trend with applied field.
Figure 2 shows the hysteresis loop for d
31
for uniaxially
stretched nylon-II quenched films. During the first cycle,
the sample was initially subjected to poling fields of 100, 200,
and 300 kV fcm and the value of d
31
increased as observed
previously. Then, the sample was subjected to poling fields in
the reverse direction: - 100, - 200, - 300, and - 350
kV fern. The value of d
31
went through zero at a field of
- 180 kV fern. At a poling field of - 350 kV fern, the value
of d
31
was - 1.33 p C/N. When the sample was again sub-
jected to forward poling fields, the value of d
31
went through
zero again at a field of 180 k V fern. The second cycle of re-
versed and forward poling produced similar paths within
Z

0
I

a

'" '0
_1,Or
,
-2.0\
I
-3,Or FIRST CYCLE
seCOND CYClE
- 400 300 -200 -100 a 100 200 300 400
POLING FIELD (KV/em)
FIG. 2. Hysteresis loop of d
31
for uniaxially stretched nylon-II (quenched)
films.
Mathur, Scheinbeim, and Newman 2421
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experimental error. Figure 3 shows the hysteresis loop for
the piezoelectric stress constant e
3l
The behavior is essential-
ly similar in trend to that of the piezoelectric strain constant.
Figures 4 and 5 show the hysteresis loop for d
3l
ande3l'
respectively, for plasticized, uniaxially stretched nylon-II
(a') films. When the sample was first subjected to a series of
forward poling fields, the values of d
3l
and e
3l
increased
sharply. At a poling field of 350 kV fcm, d
31
was 2.75 p C/N
and e
3l
was 1.7 mCfm2. On subsequent reversed poling, d
3l
became zero at a field of - 250 kV fern. At - 350 kV fcm,
d
3l
was - 1.5 p C/N and e
3l
was - 1.08 mC/m
2
When the
poling direction is switched back to the positive direction,
the value again goes through zero but at a field of 180 kV f
cm, the value obtained for the quenched films. Similar be-
havior is observed during the second cycle; however, the val-
ues of d
3l
and e
3l
are much lower at the end of the second
cycle;d
3
! was 0.95 p C/N ande
3
! was 0.64 mC/m
2
Since the
same sample has been subjected to all the poling fields at
50 C, we might be observing an annealing effect resulting in
increased crystal perfection making poling more difficult
and leading to a lowering of the values for d
3
! and e
31
.
B. X-ray measurements
X-ray diffraction scans for unpoled (with the same ther-
mal history as the poled sample) and poled (650 kV /cm;
75 C; 30 min) uniaxially stretched nylon-II quenched films
in reflection and transmission modes showed no difference
in the x-ray diffraction patterns. Flat-film x-ray patterns for
these films (poled and unpoled) in the transmision mode (x-
-2.0
-3.0'
x FmST CYCLE
IECO .. D CYCLE
-400 -300 -200 -100 0 100 200 300 400
POLING FIELD (KV fCrA)
FIG. 3. Hysteresis loop of e
31
for uniaxially stretched nylon-II (quenched)
films.
2422 J. Appl. Phys., Vol. 56, No.9, 1 November 1984
Z
0
!!;
-...
"
3.0
2.0
1.0
0
-1.0 -
-2.0 X FIfII8T CYCLE
SECOND CYCLE
-400 -300 -200 -100 0 100 200 300 400
POLING FIELD (KVfcm)
FIG. 4. Hysteresis loop of d
31
for uniaxially stretched, plasticized nylon-II
(a') films.
-1,0
eeco",o CYCLE
-400 -300 -200 -100 0 100 200 300 400
POLING FIELD (KVfcm)
FIG. 5. Hysteresis loop of e31 for uniaxially stretched, plasticized nylon II
(a') films.
Mathur, Scheinbeim, and Newman 2422
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ray beam normal to the plane of the film and to the c axis) and
in the edge-reflection mode (x-ray beam parrallel to the plane
of the film and perpendicular to the c axis) also showed no
significant change in the x-ray pattern with poling for the
quenched films. Figures 6 and 7 show the x-ray diffraction
scans for unpoled and poled films in reflection and transmis-
sion modes, respectively of, the uniaxial stretched a
'
films
through two complete cycles of poling of the hysteresis ex-
periment. The unpoled sample had the same thermal history
as the poled sample. The intensity ofthe (010) reflection has
decreased signilicantly compared to that of the (100) reflec-
tion for the poled sample in reflection mode (Fig. 6). The
complementary (reverse) effect is seen in the scan taken in
transmission mode (Fig. 7). This would be expected if the
dipoles align perpendicular to the film during poling. In a
recent study9 for nylon-II (a) films, similar x-ray changes
were observed after poling and were related to the reorienta-
tion of crystallites (under the effect of poling fields) so that
the dipoles align in the direction of the applied field. Figure 8
shows the flat-film x-ray pattern of these samples in trans-
mission mode and Fig. 9 show the flat-film pattern in the
edge reflection mode.
C. DSC measurements
Figure 10 shows DSC endotherms for the uniaxially
stretched quenched films. Equal weights of each sample
were used. The peak melting point shows an increasing trend
with higher poling fields. The melting peak for the unpoled
sample is 192.5 C, while for the sample poled at 800kV /cm,
it has increased to 194C. The increase may be attributed to
the fact that annealing is occurring under high poling fields.
Figure 11 shows the DSC melting endotherms for the
uniaxially stretched, plasticized nylon-Ii (a
'
) films. For the
unpoled sample (thermal history the same as for the poled
sample) the melting peak occurs at 187.5 C, while for the
poled sample (at the end of the hysteresis cycles) the peak is
at 190 C. Premelting is indicated by the slope in the base line
observed before the melting endotherm of the poled sample.
I - - - ' ~ , ... ,-, , ..
< same .a poled)
_ Pol.d {end of hysteresl. cyc'es'
Last PoUng Field: 350 KY'/em
(100)
32 28 24
28
c-axis
18 12
_ ... _--_ ..... ----,
NYlon-l11..'
Plasticized
Drawn: 2,4: 1
FIG. 6. X-ray diffraction scans (reflection mode) for unpoled and poled,
uniaxially stretched, plasticized nylon-II (a') films.
2423 J. Appl. Phys . Vol. 56. No.9. 1 November 1984
r---------------....
------Unpoled (fhermal history
same as poled)
- Poled (end of hyst$resis cycles)
32 2. 2' 20
28
16
--_ ... - - .. --..........,
13'
.vC-aJCls
'2
Nylon-11 #C,:
Plasticized
Drawn: 2.4: 1
FIG. 7. X-ray diffraction scans (transmission mode) for unpoled and poled.
uniaxially stretched. plasticized nylon-II (a') films.
FIG. 8. Flat-film x-ray patterns for unpoled and poled, uniaxially stretched.
plasticized nylon-II (a') films; x-ray beam normal to the plane of the film
and perpendicular to the c axis.
Mathur. Scheinbeim, and Newman 2423
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FIG. 9. Flat-film x-ray patterns for unpoled and poled. uniaxially, plasti-
cized nylon-II (a') films; x-ray beam parallel to the plane of the rum and
perpendicular to c axis.
IV. DISCUSSION AND CONCLUSIONS
The present study shows that the piezoelectric proper-
ties of nylon-II films show similar behavior to the piezoelec-
tric properties of PVF
2
films in several important ways.
(1) The quenched films show appreciably higher piezoe-
lectric activity in the oriented fonn as compared. to the unor-
iented fonn studied earIier.
1
Under identical poling condi-
tions, the value of d
31
was found to be 25% higher and e
31
- 85% higher for the uniaxially stretched films compared to
the unoriented films. In the case of drawn PVF
2
films, the
increase is much greater because in addition to the orienta-
tion of chains in the draw direction a conversion from the
nonpolar (phase II) to polar (phase I) crystal forms takes
place on drawing. No such crystal transition occurred on
drawing the quenched nylon-Ii films. The results should be
compared to the increase in piezoelectric activity of the ori-
ented phase I PVF
2
films over the unol'iented phase I films
observed by Scheinbeim and Chung. 18 Here, the increase in
the hydrostatic piezoelectric coefficient d
h
and the pyroelec-
tric coefficient P
y
of films with a draw ratio - 2.5 over the
unoriented phase I films is -90% and -100%, respective-
ly, which compares with the observed increase - 85% for e
31
2424 J. Appl. Phys., Vol. 56, No.9, 1 November 1984

a:
w
::r:
l-
e
o
z
w
,
,
NVlon- 11
Drawn: 2.4: 1


-------- I'
170 180 190
I'
I : UNPOLED
" I,
" , ,
I I
, :
"
"
':
I I
r'
':
,
I,
, I
200 210
TEMPERATURE C
FIG. 10. DSC endotherms for unpoled and poled. uniaxially stretched ny-
lon-II (quenched) films.
::!:
a:
w
::r:
l-
e
o
z
w
Nylon- 1 1 .i:
Plasticized
Drawn: 2.4:1
-----Unpoled (thermal history same as poled)
--Poled (end of hysteresis cycles)
Last Poling Field: 350 KV/cm
170
,
... --" ."
180
.'
, ,
190
TEMPERATURE (OC)
200
FIG. 11. DSC endotherms for unpoled and poled. uniaxially stretched,
plasticized nylon-II (a') films.
Mathur. Scheinbeim, and Newman 2424
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for nylon 11. Since the increase in modulus with draw ratio
differs in the two cases exact comparisons cannot be made.
No field-induced crystal transitions were observed for nylon
11; neither are such transitions observed for phase I PVF
2

For the case of PVF 2. the increase in piezoelectric and pyro-
electric activity of oriented films over unoriented films (with
the same crystal form) is readily understood in terms of the
crystal dipole orientation and chain orientation with respect
to the applied field. Both the 180 switching and 60 switch-
ing mechanisms proposed are more effective for chains per-
pendicular to the field direction. Our results are also quite
consistent with such an explanation. For nylon 11, the in-
crease in piezoelectric response with higher poling fields,
until some saturation appears also parallels the behavior of
PVF2
(2) For the plasticized a' -form films no field-induced
crystal phase transition occurred on poling. However, the
crystallites appear to reorient in a way consistent with crys-
tal dipole alignment in the field direction. In a previous
study9 a similar reorientation was observed for unoriented
films.
(3) The static switching experiments demonstrate that
both the quenched (0' form) and a'-form nylon-II rums
show a reversible polarization with hysteresis behavior of the
piezoelectric strain and stress constants. This behavior par-
alleled the behavior of phase IV PVF
2
films
l9
and is quite
consistent with an explanation in terms of crystal ferroelec-
tric switching.
(4) The DSC studies showed that for both the quenched
films and the a' -form films that an increase in melting point
occurred following the application of high poling fields rela-
tive to unpoled films with the same thermal history. This
2425 J. Appl. Phys., Vol. 56, No.9, 1 November 1984
suggests that the high applied fields can complement the
annealing process taking place at the elevated temperature
and leading to an increase in crystal perfection.
ACKNOWLEDGMENT
This work was supported in part by the Office of Naval
Research.
lB. A. Newman, P. Chen, K. D. Pae, and 1. I. Scheinbeim, J. Appl. Phys.
51,516111980).
2A. Sen, S. C. Mathur, B. A. Newman, and J. I. Scheinbeim (unpublished).
3W. P. Slichter, J. Polym. Sci. 36, 259 (1959).
"T. Sasaki, Polym. Lett. 3, 557 (1965).
5B. A. Newman, T. P. Sham, and K. D. Pae, J. Appl. Phys. 48,4092 (1977).
6J. I. Scheinbeim, J. Appl. Phys. 52, 5939 (1981).
7B. A. Newman, J. I. Scheinbeim, and K. Kim (unpublished).
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