Organic electrochemical transistors (OECTs) are devices with broad potential in bioelectronic sensing, circuits, and neuromorphic hardware. Their unique properties arise from the use of organic mixed ionic/electronic conductors (OMIECs) as the active channel. Typical OMIECs are linear polymers, where defined and controlled microstructure/morphology, and reliable characterization of transport and charging can be elusive. Semiconducting two‐dimensional polymers (2DPs) present a new avenue in OMIEC materials development, enabling electronic transport along with precise control of well‐defined channels ideal for ion transport/intercalation. To this end, a recently reported 2DP, TIIP, is synthesized and patterned at 10 µm resolution as the channel of a transistor. The TIIP films demonstrate textured microstructure and show semiconducting properties with accessible oxidation states. Operating in an aqueous electrolyte, the 2DP‐OECT exhibits a device‐scale hole mobility of 0.05 cm2 V–1 s–1 and a µC* figure of merit of 1.75 F cm–1 V–1 s–1. 2DP OMIECs thus offer new synthetic degrees of freedom to control OECT performance and may enable additional opportunities such as ion selectivity or improved stability through reduced morphological modulation during device operation.

Molecular electronic spin qubits are promising candidates for quantum information science applications because they can be reliably produced and engineered via chemical design. Embedding electronic spin qubits within two-dimensional polymers (2DPs) offers the possibility to systematically engineer inter-qubit interactions while maintaining long coherence times, both of which are prerequisites to their technological utility. Here, we introduce electronic spin qubits into a diamagnetic 2DP by n-doping naphthalene diimide subunits with varying amounts of CoCp 2 and analyze their spin densities by quantitative electronic paramagnetic resonance spectroscopy. Low spin densities (e.g., 6.0 × 10 12 spins mm −3 ) enable lengthy spin−lattice (T 1 ) and spin−spin relaxation (T 2 ) times across a range of temperatures, ranging from T 1 values of 164 ms at 10 K to 30.2 μs at 296 K and T 2 values of 2.36 μs at 10 K to 0.49 μs at 296 K for the lowest spin density sample examined. Higher spin densities and temperatures were both found to diminish T 1 times, which we attribute to detrimental cross-relaxation from spin− spin dipolar interactions and spin−phonon coupling, respectively. Higher spin densities decreased T 2 times and modulated the T 2 temperature dependence. We attribute these differences to the competition between hyperfine and dipolar interactions for electron spin decoherence, with the dominant interaction transitioning from the former to the latter as spin density and temperature increase. Overall, this investigation demonstrates that dispersing electronic spin qubits within layered 2DPs enables chemical control of their inter-qubit interactions and spin decoherence times.

This review explores recent progress in the use of chiral metal–organic frameworks (MOFs) as platforms for circularly polarised luminescence (CPL), chiroptical switching, and second-order nonlinear optics (NLO).

Conventional adsorbents for CO2 capture typically utilize swings in temperature and/or pressure to adsorb and desorb CO2. These mechanisms can be energy-intensive, which has inspired further research on alternative capture mechanisms such as electro-swing CO2 capture. For this, metal–organic frameworks (MOFs) have been suggested as a potential adsorbent owing to their stability, ultrahigh surface areas, and ability to facilitate redox reactions. However, MOFs have not yet been utilized for the electrochemical capture of CO2. In this work, we demonstrate the facile synthesis of a redox-active MOF-based adsorbent for the electrochemical capture of CO2, and we employ spectroelectrochemistry to understand the adsorbent’s interaction with CO2. This represents an advancement toward the scalable production of electro-swing adsorbents and signals that MOFs can be successfully employed for this process.