Polymer Electrets and Ferroelectrets

as EAPs: Fundamentals

Ingrid Graz and Axel Mellinger

Contents
1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1
2 A Short History of Electrets . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
3 Polymer Electrets: A Classification . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
3.1 Charge Electrets . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
3.2 Ferroelectrets . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
3.3 Dipole Electrets . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6
4 Charge Stability in Electrets . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
5 Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8

Abstract
Electrets are dielectric materials capable of quasi-permanently storing electric
charges at their surface or in their bulk. This chapter presents a brief history of
electret research, followed by a classification and introduction of the most
important electret materials. The chapter also discusses ferroelectrets and recent
developments in charge stability.

Keywords
Electret • Polymer • Ferroelectret • Dipole • Charge • Stability

I. Graz (*)
Soft Matter Physics, Johannes Kepler University Linz, Linz, Austria
e-mail: Ingrid.graz@jku.at
A. Mellinger
Department of Physics, Central Michigan University, Mount Pleasant, MI, USA
e-mail: axel.mellinger@cmich.edu

# Springer International Publishing Switzerland 2016 1

F. Carpi (ed.), Electromechanically Active Polymers, Polymers and Polymeric
Composites: A Reference Series, DOI 10.1007/978-3-319-31767-0_24-1
2 I. Graz and A. Mellinger

1 Introduction

Electrets are dielectric materials capable of quasi-permanently storing electric

charges at their surface or in their bulk (Sessler 1987). The term “quasi-permanent”
signifies that the characteristic time constants for the decay of the charges are much
longer than the time period over which studies are performed with the electret. The
electret charges are either real excess charges (charge electrets) or result from
oriented dipoles (dipole electrets). Ferroelectrets are a member of the electret family
(charge electrets) based on nonpolar polymers with a porous foam structure with
open or closed cells where the internal surfaces carry positive and negative charges.
The multitude and diversity of electret materials with their different properties,
depending on the charge localization and their internal structure, renders them
very powerful electroactive polymers. In this chapter, we give a short history of
electret research (Sect. 2), followed by a classification and introduction of the most
important electret materials (Sect. 3). Ferroelectrets are discussed in Sect. 3.2.
Section 4 deals with the recent developments in charge stability.

2 A Short History of Electrets

Effects of quasi-permanent charge storage or dipole charge orientation have been

observed since the ancient Greeks. In 1732, electret properties were described by
S. Gray (1732) as a “perpetual attractive power” after generating static electricity of
waxes by contact electrification by cooling of the melts in iron ladles. The term
“electret” was introduced in 1885 by Oliver Heaviside (1885) from a purely theo-
retical point of view as the electrostatic analog to a magnet. In the 1920s, systematic
research was initiated by Mototaro Eguchi in Japan studying carnauba wax and
resins (Eguchi 1925). He exposed molten wax to a strong electric field while
simultaneously cooling and solidifying the samples, and found them to exhibit a
strong negative charge. In the following years, electret research picked up momen-
tum when polymers were identified as promising materials for charge storage
(Gutmann 1948). In the 1960s and early 1970s, poly(tetrafluorethylene) (PTFE)
(Sessler and West 1962) and its copolymers were found to exhibit excellent charge
stability and strong piezo- and pyroelectric effects were demonstrated in poly(vinyl-
idene fluoride) (PVDF) (Kawai 1969; McFee et al. 1972), respectively. A decade
later, amorphous polymer electrets moved into the focus of electret research due to
their large nonlinear optical effects (Singer et al. 1986). In 1986, heterogeneous,
charged cellular polymer electrets with outstanding piezoelectric properties were
introduced as a novel class of electrets (Patent 1986). These materials are called
ferroelectrets to emphasize that they exhibit a spontaneous electric polarization that
can be switched by an external electric field (Bauer et al. 2004). With the advent of
flexible electronics in the new millennium, foil electrets and ferroelectrets found
applications in various types of sensors (Graz et al. 2006; Huang et al. 2007). In
recent years, growing interest in energy harvesting from motion has provided a new
spin to the field (Jean-Mistral et al. 2012; Wang et al. 2013), clearly demonstrating
Polymer Electrets and Ferroelectrets as EAPs: Fundamentals 3

Fig. 1 Schematic view of classification of charge electrets: Homogeneous polymers that carry
excess charges at the surface (a) or within the bulk or volume (b) Heterogeneous charge electrets
consist of a soft and a hard part. The noncentrosymmetry is either due to the sample geometry (c) or
a result of bipolar charging (d)

that there are still unexplored routes for electret research. Novel applications such as
ultraconformable electronics also demand more and more tailored material proper-
ties such as stretchability (Zhang et al. 2014).

3 Polymer Electrets: A Classification

The short excursion into the history of electret research already shows that there are
numerous different material types and materials with the ability to quasi-
permanently store charges. Depending on the charge carrier type, electrets are
divided into charge electrets and dipole electrets. The following section introduces
both concepts and the most important polymers belonging to each category.

3.1 Charge Electrets

Figure 1 shows a schematic overview of different charge electret types. Homoge-

neous charge electrets based on highly insulating nonpolar or weakly polar and
elastically isotropic polymers with very small dielectric losses exhibit a quasi-
permanent excess charge trapped either at their surface (surface charge electrets)
(Fig. 1a) or within their volume (space charge electrets) (Fig. 1b). Charges trapped
within the bulk can be observed in amorphous or crystalline phases and in semi-
crystalline polymers also at the interfaces between amorphous and crystalline
regions (Maxwell-Wagner effect) (Rollik et al. 1999).
Polytetrafluoroethylene (PTFE) and its copolymers fluoroethylenepropylene
(FEP), perfluoroalkoxy (PFA), and amorphous PTFE, a perfluorinated dioxole
(Teflon ® AF), are the best electret materials for storing negative charges due to the
large electronegativity of the F atom and the highly symmetrical CF2 group with its
small polarizability. They are further capable to retain the charges up to 200  C (Van
4 I. Graz and A. Mellinger

Turnhout 1975). Other widely used nonpolar or weakly polar polymers such as
polyethylene (PE), polypropylene (PP), or poly(ethylene terephthalate) (PET) do not
exhibit comparable electret properties, whereas cyclo-olefines are remarkable
nonfluorinated electrets especially for positive charging with charge stability up to
160  C (Sessler et al. 1997). Low k-dielectric materials are another promising group
of electrets. The silicon-based benzocyclobutene (BCB) and the perfluorinated
cyclobutene (PFCB) show excellent electret properties for both negative and positive
charges with their delocalized electrons (Farona 1996; Kennedy et al. 1995).
Discovered by Jacques Curie and Pierre Curie in 1880 (Curie and Curie 1880),
piezoelectricity describes the strain-induced electrical polarization observed in
noncentrosymmetrical crystals. Being a prerequisite for piezoelectricity, noncentro-
symmetry refers to the lack of an inversion center in the crystal’s unit cell. Out of the
32 point groups (for 230 potential crystal arrangements in 7 axial systems), 21 are
noncentrosymmetrical, and all except one exhibit piezoelectric properties. In order to
render charge electrets piezoelectric, strategies to introduce noncentrosymmetry are
required. In contrast to crystals where symmetry is broken on the atomic scale,
heterogeneous charge electret systems utilize an engineered macroscopically
noncentrosymmetrical charge distribution by combining soft and hard electrets
(Bauer 2006; Qiu 2010). Figure 1c, d schematically shows two electret film assem-
blies consisting of an elastically “soft” and a “hard” charge electret, with charges at
the interface between the two materials. These nonuniform or heterogeneous electret
systems are either built up in layers (of different stiffness) or as a composite where
the matrix and the inclusions have different mechanical properties to obtain elastic
anisotropies. In layered heterogeneous electret systems, piezoelectric-like behavior
results from the geometry: When charges at the interface at the soft and hard layers
are displaced, a change in charges at the surface is induced (Fig. 1c). Figure 1d
shows the foam-like structure of a ferroelectret, another class of heterogeneous space
charge electrets, where the opposite charges located in the soft inclusions within a
harder matrix result in a symmetry breaking, thus exhibiting a very large piezoelec-
tric d33 coefficient. (For more information see Sect. 3.2)

3.2 Ferroelectrets

Heterogeneous voided electrets – now frequently called ferroelectrets – were first

described in the late 1980s (Savolainen et al. 1989), but research did not pick up until
a decade later. They were initially prepared from closed cell polypropylene foams
(Fig. 2a). To render these insulating polymer-systems electroactive, they are exposed
to high electric fields (often exceeding 100 MV/m), which induces microscopic
dielectric barrier discharges within the voids (Lindner et al. 2002; Qiu et al. 2007;
Harris and Mellinger 2014). These microdischarges lead to a charge separation and
the voids’ surfaces become oppositely charged forming macrodipoles (Fig. 2b).
These engineered macrodipoles can be switched in high electric fields similar
to the dipole orientation in ferroelectric materials exhibiting hysteresis loops in
displacement as function of applied electric field (Fig. 2c) (Wegener and Bauer
Polymer Electrets and Ferroelectrets as EAPs: Fundamentals 5

Fig. 2 Scanning electron microscope image showing a PP foam ferroelectret cross-section

(a) (courtesy of Mika Pajannen, VTT, Finland) and schematic depiction of engineered macrodipoles
within the voids of the ferroelectret (b) and hysteresis loop exhibited when switching of the
macrodipoles orientation (c) (After Bauer et al. 2004)

Fig. 3 Schematic view of the classification of dipole electrets: Amorphous dipole electrets (a) must
contain preferentially oriented molecular dipoles that are either located as guest charges in the
polymer (i), attached to the side (ii), or located in the main chain (iii). Semicrystalline dipole
electrets (b) exhibit both oriented molecular dipoles and Maxwell-Wagner compensation charges at
the interfaces to the crystalline regions
6 I. Graz and A. Mellinger

2005; Qiu et al. 2013). Their ferroelectric-like properties (Sessler and Hillenbrand
1999; Neugschwandtner et al. 2001), especially their very strong piezoelectric effect,
with d33 coefficients up to 1000 pC/N (Zhang et al. 2006) by far exceeding those of
piezoelectric ceramics such as BaTiO3, makes them very promising materials for
various applications such as pressure sensors, radiation dosimeters, or ultrasound
transducers. With their low acoustical impedance enabling very good coupling to air,
these novel ferroic materials are highly suitable for microphones and loudspeakers.
In recent years, the family of ferroelectrets has been extended from foam systems
to engineered voided structures featuring materials such as PTFE and FEP. These
novel heterogeneous space charge systems are characterized by their extremely high
piezoelectric coefficients (Zhang et al. 2006) along with improved charge stability to
temperatures above 120 C (Hu and von Seggern 2006; Zhang et al. 2007) as well as
mechanical compliance enabling new applications (Zhang et al. 2014). For more
details see Sect. 4.

3.3 Dipole Electrets

In contrast to charge electrets with their stored real charges, dipole electrets are
characterized by a preferential orientation of their molecular dipoles. Here amor-
phous and semicrystalline dipole electrets are distinguished. Amorphous dipole
electrets are characterized by a quasi-permanent dipole polarization in the amor-
phous phases (Fig. 3a), whereas semicrystalline ones show a permanent dipole
orientation in the crystalline phases and additionally contain Maxwell-Wagner
compensation charges at the interfaces between amorphous and crystalline regions
for stabilizing the polarization (Fig. 3b) (Mopsik and Broadhurst 1975; Broadhurst
et al. 1978; Sessler et al. 1992).

3.3.1 Amorphous Dipole Electrets

Amorphous dipole electrets exhibit preferentially oriented molecular or microscopic
dipoles (Mopsik and Broadhurst 1975), where the orientation is achieved by means
of poling. All electrets need to be charged, poled, or both, requiring large electric
fields applied to the electret material. For more details see the chapter on ▶ Polymer
Electrets and Ferroelectrets as EAPs: Materials of this book. The incorporation of
molecular dipoles in amorphous polymers is based on different concepts illustrated
in Fig. 3a. In the most simple approach (termed a guest-host system), a nonpolar
polymer host is doped with molecular dipoles (3a i) (Singer 1986). Alternatively,
polymers can carry dipoles attached to their side chains (Fig. 3a ii) or separated by
spacer groups in the main chain (Fig. 3a iii) (Stockmayer 1967; Riande and Saiz
1992). Only a few amorphous dipole electrets show piezoelectric and pyroelectric
responses. Amongst them are nonlinear optical polymers with very large dipole
moments. Here the chromophores form the molecular dipoles with acceptor-donor
groups linked by delocalized π-electrons. Typically, chromophores are very stable at
high temperatures and light intensities. An example for a nonlinear guest-host
polymer is a poly(methylmethacrylate) (PMMA) based network forming polymer
Polymer Electrets and Ferroelectrets as EAPs: Fundamentals 7

with dissolved chromophore, Disperse Red 1, side groups (Singer et al. 1986). More
details on nonlinear optical polymers can be found elsewhere (Bauer-Gogonea and
Bauer 2001). Another interesting amorphous dipole electret with a large dipole
moment in its repeat unit is vinylidenecyanide vinylacetate copolymer (P(VDCN-
VAc) (Norwood et al. 1992) or poly(styrenemaleic anhydride)/Disperse Red 1 P
(S-MA)DR1) side chain polymer (Ahlheim and Lehr 1994).

3.3.2 Semicrystalline Dipole Electrets

In semicrystalline dipole electrets, polar crystallites are present in addition to the
polar amorphous phase (Fig. 2b). In the technically most interesting semicrystalline
dipole electrets such as polyvinylidene fluoride (PVDF) and its copolymers with
trifluoroethylene (P(VDF-TrFE)) (Lovinger 1983) or hexafluoropropylene
(P(VDF-HFP)), odd Nylons 7 and 11, polyureas, polyurethanes (PU), and some
liquid crystalline polymers, the crystallites are ferroelectric (Vasudevan et al. 1979;
Hattori et al. 1996). The terpolymer poly(vinylidene-fluoride–trifluoroethylene–-
chlorotrifluoroethylene) (P(VDF-TrFE-CTFE)) has been shown to have relaxor
ferroelectric properties as the CTFE group destabilizes the long-range order of the
ferroelectric phase (Xu et al. 2001).

4 Charge Stability in Electrets

The key property of charge electrets is the extremely long lifetime of the surface or
bulk charge. From measurements at elevated temperature, room temperature life-
times in the range of 103 to 2.6  105 years have been extrapolated (Xia and
Gerhard-Multhaupt 1999; Xia et al. 2003). A commonly held view is that these
charges are held in “traps” with an energy depth of at least 1 eV, since charges in
shallower traps (trap depth <<1 eV) have a high thermal activation rate. Małecki
suggested a rate equation model (Małecki 1999), where carrier annihilation at the
electrode and by free, implanted charges causes a transition from a short-term,
exponential decay – resulting from ohmic conductivity – to a long-term linear
decay over thousands of years. This model requires the presence of deep traps to
minimize thermal activation of charge carriers.
Meunier et al. calculated trap energies resulting from impurities that are com-
monly present in the type of polyethylene used for cable insulation (Meunier
et al. 2001) and found charge carrier densities of up to 1017 cm 3 with lifetimes of
30,000 years. Some of the impurities have been identified through their lumines-
cence spectra (Teyssedre et al. 2001).
The “traditional” tool to investigate charge stability and energetic trap depths is
the thermally stimulated discharge method (Van Turnhout 1999). However, this
technique is limited to trap depths below 1.5 eV, since the high temperatures required
to free charges from deeper traps lead to thermal decomposition of the material under
investigation. In recent years, photostimulated discharge (PSD) spectroscopy
(Brodribb et al. 1975), a technique where charge carriers are excited out of their
traps by absorption of monochromatic visible or UV radiation, has provided some
8 I. Graz and A. Mellinger

experimental evidence for the existence of “deep” traps (Mellinger et al. 2004; Yue
et al. 2013). A significant case of state-selective detrapping was found in cellular
polypropylene, a well-known ferroelectret (Mellinger et al. 2003). The material
exhibits three PSD current maxima at 276, 223, and 198 nm, which can be (at least
partially) selectively bleached by irradiation at the respective wavelengths. During
UV irradiation, the piezoelectric activity of the ferroelectret was monitored in situ
using dielectric resonance spectroscopy. No change in its d33 coefficient was found
during irradiation at 276 and 223 nm, whereas irradiation below 210 nm resulted in a
gradual reduction of d33. As the piezoelectric properties are caused by charges
trapped on the inner surfaces of the voids, this observation directly links these
charges to the 6.2 eV traps corresponding to the 198 nm maximum in the PSD
spectrum. This experimental proof of charges in deep traps, responsible for the
astonishing stability of electrets, allows a deeper understanding and enables new
directions of electret research.

5 Conclusion

Electrets and ferroelectrets are a class of EAPs comprising a variety of very different
materials such as amorphous, semicrystalline, closed- or open cell foams, or hetero-
geneous layered polymers, waxes, and elastomers. This plethora of polymer electrets
exhibits along with its main ability to store charges a range of electroactive proper-
ties such as piezo- and pyroelectricity or switchable polarization. Novel heteroge-
neous systems with improved charge retention at elevated temperatures and the
understanding of charge trapping mechanisms are key foci of ongoing research.
With this growing knowledge and novel evolutions of materials, the number of
potential applications in pressure/temperature sensors, microphones, or energy
harvesting is increasing, paving a bright future for electrets.

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