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This perspective offers insights from discussions conducted during the Telluride Science meeting on organic mixed ionic and electronic conductors, outlining the challenges associated with understanding the behavior of this intriguing materials class.

 

The commercially available polyelectrolyte complex poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) is ubiquitous in organic and hybrid electronics. As such, it has often been used as a benchmark material for fundamental studies and the development of new electronic devices. Yet, most studies on PEDOT:PSS have focused on its electronic conductivity in dry environments, with less consideration given to its ion transport, coupled ionic-electronic transport, and charge storage properties in aqueous environments. These properties are essential for applications in bioelectronics (sensors, actuators), charge storage devices, and electrochromic displays. Importantly, past studies on mixed ionic-electronic transport in PEDOT:PSS neglected to consider how the molecular structure of PSS affects mixed ionic-electronic transport. Herein, we therefore investigated the effect of the molecular weight and size distribution of PSS on the electronic properties and morphology of PEDOT:PSS both in dry and aqueous environments, and overall performance in organic electrochemical transistors (OECTs). Using reversible addition–fragmentation chain transfer (RAFT) polymerization with two different chain transfer agents, six PSS samples with monomodal, narrow ( Đ = 1.1) and broad ( Đ = 1.7) size distributions and varying molecular weights were synthesized and used as matrices for PEDOT. We found that using higher molecular weight of PSS ( M n = 145 kg mol −1 ) and broad dispersity led to OECTs with the highest transconductance (up to 16 mS) and [ μC *] values (∼140 F cm −1 V −1 s −1 ) in PEDOT:PSS, despite having a lower volumetric capacitance ( C * = 35 ± 4 F cm −3 ). The differences were best explained by studying the microstructure of the films by atomic force microscopy (AFM). We found that heterogeneities in the PEDOT:PSS films (interconnected and large PEDOT- and PSS-rich domains) obtained from high molecular weight and high dispersity PSS led to higher charge mobility ( μ OECT ∼ 4 cm 2 V −1 s −1 ) and hence transconductance. These studies highlight the importance of considering molecular weight and size distribution in organic mixed ionic-electronic conductor, and could pave the way to designing high performance organic electronics for biological interfaces. 

Haptic devices are in general more adept at mimicking the bulk properties of materials than they are at mimicking the surface properties. Herein, a haptic glove is described which is capable of producing sensations reminiscent of three types of near‐surface properties: hardness, temperature, and roughness. To accomplish this mixed mode of stimulation, three types of haptic actuators are combined: vibrotactile motors, thermoelectric devices, and electrotactile electrodes made from a stretchable conductive polymer synthesized in the laboratory. This polymer consists of a stretchable polyanion which serves as a scaffold for the polymerization of poly(3,4‐ethylenedioxythiophene). The scaffold is synthesized using controlled radical polymerization to afford material of low dispersity, relatively high conductivity, and low impedance relative to metals. The glove is equipped with flex sensors to make it possible to control a robotic hand and a hand in virtual reality (VR). In psychophysical experiments, human participants are able to discern combinations of electrotactile, vibrotactile, and thermal stimulation in VR. Participants trained to associate these sensations with roughness, hardness, and temperature have an overall accuracy of 98%, whereas untrained participants have an accuracy of 85%. Sensations can similarly be conveyed using a robotic hand equipped with sensors for pressure and temperature.