Precisely Patterned Channels in a Vertical Organic Electrochemical Transistor with a Diazirine Photo-Crosslinker.

Organic electrochemical transistors (OECTs) rely on both efficient ionic doping/de-doping process and carrier transport in the mixed ionic-electronic channel under the modulation of gate bias. Moreover, channels that hold photopatterning capability are highly desired to minimize parasitic capacitance and simplify the fabrication process/cost. However, yielding photo-patternable channels with both precise/robust patterning capability and controllable ionic-electronic coupling is still challenging. Herein, double-end trifluoromethyl diazirines (DtFDA) with different chain lengths are introduced in the OECT channel to act as both photo-crosslinker and medium to regulate ionic-electronic transport. Specifically, high-resolution patterns with a minimum line width/gap of 2 µm are realized in p(g2T-T) or Homo-gDPP based channels by introducing DtFDA. Maximum transconductances of 68.6 mS and 81.6 mS, current on/off ratio of 106 and 107 (under a drain voltage of only ±0.1 V), are achieved in p- and n-type vertical OECTs (vOECTs), respectively, along with current densities exceeding 1 kA cm-2 and good cycling stability of more than 100,000 cycles (2000 seconds). This work provides a new and facile strategy for the fabrication of vOECT channels with high resolution and high performance via the introduction of a simple and efficient crosslinker.

Kinetic Resolution Polymerization Enabled Chemical Synthesis of Perfectly Isotactic Polythioesters.

Isotactic polythioesters (PTEs) that are thioester analogs to natural polyhydroxyalkanoates (PHAs) have attracted growing attention due to their distinct properties. However, the development of chemically synthetic methods for preparing isotactic PTEs has long been an intricate endeavour. Herein, we report the successful synthesis of perfectly isotactic PTEs via stereocontrolled ring-opening polymerization. This binaphthalene-salen aluminium (SalBinam-Al) catalyst promoted a robust polymerization of rac-α-substituted-ß-propiothiolactones (rac-BTL and rac-PTL) with highly kinetic resolution, affording perfectly isotactic P(BTL) and P(PTL) with Mn up to 276 kDa. Impressively, the isotactic P(BTL) formed a supramolecular stereocomplex with improved thermal property (Tm=204 °C). Ultimately, this kinetic resolution polymerization enabled the facile isolation of enantiopure (S)-BTL, which could efficiently convert to an important pharmaceutical building block (S)-2-benzyl-3-mercapto-propanoic acid. Isotactic P(PTL) served as a tough and ductile material comparable to the commercialized polyolefins. This synthetic system allowed to access of isotactic PTEs, establishing a powerful platform for the discovery of sustainable plastics.

Ternary Logic Circuit and Neural Network Integration via Small Molecule-Based Antiambipolar Vertical Electrochemical Transistor.

Circuits based on organic electrochemical transistors (OECTs) have great potential in the fields of biosensors and artificial neural computation due to their biocompatibility and neural similarity. However, the integration of OECT-based circuits lags far behind other emerging electronics. Here, ternary inverters based on antiambipolar vertical OECTs (vOECTs) and their integration with the establishment of neural networks are demonstrated. Specifically, by adopting a small molecule (t-gdiPDI) as the channel of vOECT, high antiambipolar performance, with current density of 33.9 ± 2.1 A cm-2 under drain voltage of 0.1 V, peak voltage ≈0 V, low driving voltage < ± 0.6 V, and current on/off ratio > 106, are realized. Consequently, vertically stacked ternary circuits based solely on OECTs are constructed for the first time, showing three distinct logical states and high integration density. By further developing inverter array as the internal fundamental units of ternary weight network hardware circuits for ternary processing and computation, it demonstrates excellent data classification and recognition capabilities. This work demonstrates the possibility of constructing multi-valued logic circuits by OECTs and promotes a new strategy for high-density integration and multivalued computing systems based on organic circuits.