Ferroelectric Properties in Polyamides of m-Xylylenediamine and Dicarboxylic Acids

Murata, Yukinobu; Tsunashima, Kenji; Koizumi, Naokazu; Ogami, Kinji; Hosokawa, Fumihiko; Yokoyama, Kimie

doi:10.1143/jjap.32.l849

Cited by 32 publications

(19 citation statements)

References 12 publications

(16 reference statements)

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“…When the I/T composition is 70/30 mol/mol, Selar is nearly 100% amorphous with a T g around 128 °C. However, amorphous MXDs and Selar nylons (and also alicyclic nylons) have been reported to show ferroelectric switching behavior with broad hysteresis loops. − Although the ferroelectric switching is attributed to the amorphous dipoles in the glassy polymer matrix, its detailed mechanism has not been clearly understood.…”

Section: Introductionmentioning

confidence: 99%

Nature of Ferroelectric Behavior in Main-Chain Dipolar Glass Nylons: Cooperative Segmental Motion Induced by High Poling Electric Field

2018

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Main-chain dipolar glass polymers such as aromatic nylons are promising for high energy density and low loss dielectric applications because of the limited, noncooperative oscillation of highly dipolar amide groups. However, quenched aromatic nylons have been reported to exhibit significant ferroelectric switching upon high field poling. It is desirable to suppress ferroelectric switching for electric energy storage application, and this requires a fundamental understanding of the nature of ferroelectric behavior in dipolar glass nylons. In this work, a nearly 100% amorphous aromatic nylon, Selar, was used to investigate the origin of ferroelectricity in glassy nylons. Using Fourier transform infrared spectroscopy, it was found that hydrogen-bonding strength played an important role in the ferroelectric switching of amide dipoles in the loosely packed glassy matrix. When hydrogen bonding was weak such as in the quenched film, significant ferroelectric switching took place. In contrast, quenched and annealed films did not exhibit any ferroelectric switching. High-voltage broadband dielectric spectroscopy was used to study molecular and segmental motions in Selar. It was observed that the primary contribution to ferroelectric switching came from cooperative segmental motions (i.e., a combination of various sub-T g relaxations, where T g is the glass transition temperature) in the main-chain dipolar glass nylon. This understanding will help us design new aromatic nylons with suppressed segmental motions for high energy density and low loss dielectric applications.

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Section: Introductionmentioning

confidence: 99%

Nature of Ferroelectric Behavior in Main-Chain Dipolar Glass Nylons: Cooperative Segmental Motion Induced by High Poling Electric Field

2018

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“…Thus, the electrical displacement deposited in an area the size of the source electrode, 0.04 cm 2 , is 5±10 nC/cm 2 . This polarization is lower than the remanent polarization, 6 lC/cm 2 , reported by Murata et al, [19] indicating that further improvements to the deposition of the ferroelectric-like insulator are possible, and will further enhance the device performance.…”

Section: Martin Grellmentioning

confidence: 58%

“…Since we cannot determine the actual ªoffº current with the Keithley 2400s, the factor of 200 between the ªonº and ªoffº currents is just the lower limit. Already, compared to our first prototype devices with memory ratios of around 5, a memory ratio of 200 is a big step forward, and the actual theoretical limit is greater than 10 5 (due to MXD6's high remanent polarization of 60 mC/cm 2 , see the literature [19] ). Therefore, further improvement in the future is most definitely achievable.…”

Section: Martin Grellmentioning

confidence: 98%

“…[17,18] In this communication, we present the ªFerrOFETº, an entirely organic memory device. In what results in a huge simplification of the production process, we rely on the discovery by Murata et al [19] of amorphous polymers that exhibit ferroelectric-like properties. Surprisingly, this class of polymers, a cheap, commercially available nylon poly(m-xylylene adipamide) (MXD6) (see Fig.…”

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All‐Organic Permanent Memory Transistor Using an Amorphous, Spin‐Cast Ferroelectric‐like Gate Insulator

2004

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Organic field-effect transistors (OFETs) are one of the current hot topics in the materials science and materials chemistry field.[1±3] Of similar performance, but cheaper than amorphous silicon, [4] OFETs are aimed at disposable, mobile, flexible low-duty applications. Memory elements for OFET applications, such as display driver logic [5,6] or radio frequency identification (RFID) tags are, [7,8] however, limited: capacitor elements for active matrix display logic are volatile and refreshment is current-intensive. First attempts at non-volatile organic memories involve electrets [9] and capacitors integrated in the gate electrode (ªfloating gatesº).[10] These transistor memories, however, have to be charged at high voltages for seconds, and the memory is not truly permanent (timescale: minutes). Inorganic permanent single transistor memories using ferroelectrics [11±15] overcome this for high-quality inorganic electronics, but are not suitable for OFETs due to poor performance of organic semiconductors on them, [16] cost, and incompatibility with flexible substrates, an important advantage of organic transistors. [17,18] In this communication, we present the ªFerrOFETº, an entirely organic memory device. In what results in a huge simplification of the production process, we rely on the discovery by Murata et al. [19] of amorphous polymers that exhibit ferroelectric-like properties. Surprisingly, this class of polymers, a cheap, commercially available nylon poly(m-xylylene adipamide) (MXD6) (see Fig. 1a, with n = 4), is ferroelectric-like in its amorphous state, not in its crystalline state.[20] Ferroelectric-like means that the displacement versus electric field (D±E) hysteresis exhibits the same shape as typical ferroelectric materials but, as an amorphous material, it does not exhibit the thermodynamic phase or crystalline structure associated with ferroelectricity. The polymer does not exhibit a Curie temperature, above which the remanent polarization ceases; instead ferroelectric-like behavior is only observed up COMMUNICATIONS

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“…However, to fully achieve this goal, equally cheap and versatile memories will have to be developed for products such as radio-frequency identification devices (RFIDs) and disposable circuitry. This property was first seen in MXD6 by Murata et al [9]. Here, we present a prototype device for such memory applications, an organic single transistor permanent memory device, which we call the 'FerrOFET' [7,8].…”

Section: Introductionmentioning

confidence: 99%

All-organic single-transistor permanent memory device

et al. 2004

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We present an all-organic permanent memory transistor using an amorphous spin-cast gate insulator. This gate insulator exhibits a remanent polarisation in its amorphous state, a unique property, which is best described as "ferroelectric-like". The memory transistor thus built perform extremely well, even when compared to inorganic ferroelectric memory transistors; the memory "on" to memory "off" current ratio is close to 3x10 4 , while time-dependent studies show retention times of 14 hours and more. INTRODUCTION:Organic electronics have received substantial research and development attention from academia [1,2] and industry [3,4] during the last two decades. Therein, organic field-effect transistors (OFETs) show great potential for applications in flexible, mobile, and ultra-low-cost electronics. However, to fully achieve this goal, equally cheap and versatile memories will have to be developed for products such as radio-frequency identification devices (RFIDs) and disposable circuitry. Owing to the applications of these transistors, current organic memory solutions are unsuitable as they are either based on capacitors, usually volatile and power intensive, or necessitate very high voltages for the writing process, with retention times of less than three hours [5,6]. Here, we present a prototype device for such memory applications, an organic single transistor permanent memory device, which we call the 'FerrOFET' [7,8]. This memory device is a single transistor memory that is built around a polymeric gate insulator with ferroelectric-like properties in the amorphous phase: poly-m-xylylene adipamide (MXD6), a cheap, commercially available nylon. Ferroelectric-like here means that the displacement versus electric field (D-E) hysteresis exhibits a remanent polarisation without the thermodynamic phase or crystallinity. This property was first seen in MXD6 by Murata et al [9]. The appearance of this polarization hysteresis in the amorphous phase, a very unique characteristic, is most probably due to hydrogen bond alignment, as it decreases with increasing crystallinity, reducing the freedom of the hydrogen bonds [10]. The 'FerrOFET' is most closely related to inorganic ferroelectric FETs (FEFETs) that use a crystalline, inorganic ferroelectric material together with an inorganic semiconductor. The ferroelectric material has to be annealed at very high temperatures, and due to incompatible lattice constants, an intermediate insulating layer has to be employed. While very high memory ratios and retention times can be achieved [11], most FEFETs perform at the levels of the 'FerrOFET' or even exhibit much smaller memory ratios [12,13]. There have been efforts to move FEFETs towards the use for organic electronics circuitry, either by using an evaporated small molecule like sexithiophene [14] or pentacene [15] on an inorganic ferroelectric, or an organic semiconductor on the well-known organic ferroelectric material polyvinylidene fluoride (PVDF) or one of its copolymers [16]. To the best of our knowledge, the

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Ferroelectric Properties in Polyamides of m-Xylylenediamine and Dicarboxylic Acids

Cited by 32 publications

References 12 publications

Nature of Ferroelectric Behavior in Main-Chain Dipolar Glass Nylons: Cooperative Segmental Motion Induced by High Poling Electric Field

Nature of Ferroelectric Behavior in Main-Chain Dipolar Glass Nylons: Cooperative Segmental Motion Induced by High Poling Electric Field

All‐Organic Permanent Memory Transistor Using an Amorphous, Spin‐Cast Ferroelectric‐like Gate Insulator

All-organic single-transistor permanent memory device

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