Electrospun polarity-controlled molecular orientation for synergistic performance of an artifact-free piezoelectric anisotropic sensor.

Anisotropy in mechanical, optical and thermal sensors in a spatial direction has many applications in health care, robotics, aerospace, and tissue engineering. In particular, wearable and implantable sensors respond to stretching and bending strains that probe mechanical energy and track physiological signals. Hence, the development of anisotropic pressure sensors with true piezoelectric (PE) signals is of utmost importance to achieve efficient devices. Herein, a simple and efficient method is developed for high longitudinal and transverse responses, with an approach to isolating a true piezoelectric signal. The electrospun (ES) polarity of oriented dipoles inside flexible fibers gives rise to a high longitudinal/transverse PE response of both lateral and transverse strains. Nanofibers of poly(vinylidene-chlorotrifluoroethylene) copolymers contain poled dipoles, up to 86%, that promote an enhanced PE coefficient of 42 pm V-1 in the case of negative polarity-based electrospinning. It is 40% higher in composition than the commonly adopted positive polarity-biased electrospinning process. We demonstrated the advantage of such a high PE coefficient by the enhanced sensitivity of the longitudinal (VLs = 0.3 V kPa-1, ILs = 0.07 µA kPa-1) as well as transverse (VTs = 1.0 V kPa-1, ITs = 0.8 µA kPa-1) PE response. To counter the ambiguity of high transverse response as compared to longitudinal in electrospun fiber-based devices, a facile method is proposed to isolate the ferroelectret, triboelectric and piezoelectric signals in a fiber-based hybrid device with their independent charge generation mechanisms.

Controlled Molecular Orientation through Intercalation in PVDF Thin Films: Exhibiting Ultralong Retention and Improved Leakage Current.

Ferroelectric switching and retention performance of poly(vinylidene fluoride) (PVDF) thin films improve by the incorporation of unmodified smectite montmorillonite (MMT) clay nanodielectric. In the present study, an intercalated PVDF (clay/PVDF) thin film with edge-on ß-crystallite is fabricated via a heat-controlled spin coating (HCSC) technique. This provides an efficient and simple way to fabricate the edge-on oriented crystallite lamellae with an electroactive ß-phase, facilitating nanoscale ferroelectric switching at a lower voltage compared to the face-on orientation. Here, we demonstrate the polarization retention for periods longer than 20 days (∼480 h, i.e., 1.8 × 106 s), with no degradation in switched nanoscale domains. In addition, by maintaining the relatively high dielectric constant, the incorporation of nanoclay effectively lowers the leakage current by 102 factors. The obtained memory window in the edge-on orientation is 7 V, approximately twice the memory window obtained in the face-on orientation. In short, our findings provide a simple and promising route to fabricate edge-on oriented PVDF thin films, with ultralong retention, high dielectric constant, and improved leakage current.

Hydrogen Bonding-Assisted Complete Ferroelectric ß-Phase Conversion in Poly(vinylidene fluoride) Thin Films: Exhibiting an Excellent Memory Window and Long Retention.

Organic nonvolatile memory with low power consumption is a critical research demand for next-generation memory applications. Ferroelectric switching characteristics of poly(vinylidene fluoride) (PVDF) thin films modified with a trace amount of hydrated Cu salt (CuCl2·2H2O) are explored in the present study. Herein, a Cu salt-mediated PVDF (Cu/PVDF) thin film with preferential edge-on ß-crystallites is fabricated through the orientation-controlled spin coating (OCSC) technique. This work proposes a convenient and effective approach to produce edge-on-oriented electroactive PVDF thin films with a high degree of polar ß-phase, so as to realize the favorable switching under low operating voltages. Herein, chemically modified PVDF is anticipated to form a complex intermediate, which attains its stability by undergoing favorable hydrogen bonding that reorients the C-C structure of PVDF to obtain the ß-conformation. Such information is verified by X-ray photoelectron spectroscopy (XPS). Grazing incidence Fourier transform infrared (GI-FTIR) spectroscopy revealed that the Cu salt incorporated into the PVDF matrix favored the formation of the electroactive ß-phase with edge-on crystallite lamellae. Consequently, the Cu/PVDF thin film demonstrates a good contrast between electric field-assisted written and erased data bits in the piezoresponse force microscopy (PFM) phase image. Furthermore, to obtain the ferroelectric memory window, a metal-ferroelectric-insulator-semiconductor (MFIS) diode with Cu/PVDF as a ferroelectric layer has been fabricated. The capacitance-voltage (C-V) characteristic of the MFIS diode exhibits a memory window of 12 V with a long-term retention behavior (∼longer than 7 days). In a nutshell, we tried to represent a clear understanding of the interfacial interactions of the Cu salt with PVDF, which favor the edge-on formation that results in the promising low-voltage ferroelectric switching and excellent retention response, where any additional electrical poling and/or external stretching is completely possible to be ruled out, thus offering a new prospect for the evolution of devices with long-lasting nonvolatile memories.

Surface Potential Tuned Single Active Material Comprised Triboelectric Nanogenerator for a High Performance Voice Recognition Sensor.

To fabricate a high-performance and ultrasensitive triboelectric nanogenerator (TENG), choice of a combination of different materials of triboelectric series is one of the prime challenging tasks. An effective way to fabricate a TENG with a single material (abbreviated as S-TENG) is proposed, comprising electrospun nylon nanofibers. The surface potential of the nanofibers are tuned by changing the voltage polarity in the electrospinning setup, employed between the needle and collector. The difference in surface potential leads to a different work function that is the key to design S-TENG with a single material only. Further, S-TENG is demonstrated as an ultrahigh sensitive acoustic sensor with mechanoacoustic sensitivity of ≈27 500 mV Pa-1 . Due to high sensitivity in the low-to-middle decibel (60-70 dB) sounds, S-TENG is highly capable in recognizing different voice signals depending on the condition of the vocal cord. This effective voice recognition ability indicates that it has high potential to open an alternative pathway for medical professionals to detect several diseases such as neurological voice disorder, muscle tension dysphonia, vocal cord paralysis, and speech delay/disorder related to laryngeal complications.

Tunable, conductive, self-healing, adhesive and injectable hydrogels for bioelectronics and tissue regeneration applications.

Conductive hydrogels are attracting considerable interest in view of their potential in a wide range of applications that include healthcare and electronics. Such hydrogels are generally incorporated with conductive materials/polymers. Herein, we present a series of conductive hydrogels (Ch-CMC-PDA), prepared with no additional conductive material. The hydrogels were synthesized using a combination of chitosan, cellulose (CMC) and dopamine (DA). The conductivity (0.01-3.4 × 10-3 S cm-1) in these gels is attributed to ionic conductivity. Very few conductive hydrogels are endowed with additional properties like injectability, adhesiveness and self-healing, which would help to widen their scope for applications. While the dynamic Schiff base coupling in our hydrogels facilitated self-healing and injectable properties, polydopamine imparted tissue adhesiveness. The porosity, rheological, mechanical and conductive properties of the hydrogels are regulated by the CMC-dialdehyde-polydopamine (CMC-D-PDA) content. The hydrogel was evaluated in various bioelectronics applications like ECG monitoring and triboelectric nanogenerators (TENG). The ability of the hydrogel to support cell growth and serve as a template for tissue regeneration was confirmed using in vitro and in vivo studies. In summary, the integration of such remarkable features in the ionic-conductive hydrogel would enable its usage in bioelectronics and biomedical applications.