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  1. Abstract

    Microelectronic devices can directly communicate with biology, as electronic information can be transmitted via redox reactions within biological systems. By engineering biology’s native redox networks, we enable electronic interrogation and control of biological systems at several hierarchical levels: proteins, cells, and cell consortia. First, electro-biofabrication facilitates on-device biological component assembly. Then, electrode-actuated redox data transmission and redox-linked synthetic biology allows programming of enzyme activity and closed-loop electrogenetic control of cellular function. Specifically, horseradish peroxidase is assembled onto interdigitated electrodes where electrode-generated hydrogen peroxide controls its activity.E. coli’s stress response regulon,oxyRS, is rewired to enable algorithm-based feedback control of gene expression, including an eCRISPR module that switches cell-cell quorum sensing communication from one autoinducer to another—creating an electronically controlled ‘bilingual’ cell. Then, these disparate redox-guided devices are wirelessly connected, enabling real-time communication and user-based control. We suggest these methodologies will help us to better understand and develop sophisticated control for biology.

     
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  2. Catechol-based materials possess diverse properties that are especially well-suitable for redox-based bioelectronics. Previous top-down, systems-level property measurements have shown that catechol-polysaccharide films ( e.g. , catechol-chitosan films) are redox-active and allow electrons to flow through the catechol/quinone moieties via thermodynamically-constrained redox reactions. Here, we report that catechol-chitosan films are also photothermally responsive and enable near infrared (NIR) radiation to be transduced into heat. When we simultaneously stimulated catechol-chitosan films with NIR and redox inputs, times-series measurements showed that the responses were reversible and largely independent. Fundamentally, these top-down measurements suggest that the flow of energy through catechol-based materials via the redox-based molecular modality and the electromagnetic-based optical modality can be independent. Practically, this work further illustrates the potential of catecholic materials for bridging bio-device communication because it enables communication through both short-range redox modalities and long-range electromagnetic modalities. 
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  3. Abstract

    Reduction–oxidation (redox) reactions provide a distinct modality for biological communication that is fundamentally different from the more‐familiar ion‐based electrical modality. Biology uses these two modalities for communication through different systems (immune versus nervous), and uses different mechanisms to control the flow of the charge carriers: the flow of soluble ions is controlled using structural barriers (i.e., membranes) and gates (e.g., membrane‐spanning protein channels), while the flow of insoluble electrons is controlled using redox‐reaction networks. Here, a simple electrochemical approach to pattern catechols onto a flexible polysaccharide hydrogel is reported and it is demonstrated that the patterned catechol regions serve as nodes for the mediated flow of electrons through redox reactions. Electron flow through this node involves the switching of binary redox states (oxidized and reduced) and this node's redox state can be detected (i.e., “read”) by passively observing its optical absorbance, or actively switching its redox‐state electrochemically. Further, this catechol node can be switched through biological mechanisms, and this enables the fabricated catechol node to be embedded within biochemical redox reaction networks to facilitate the spanning of bio‐electronic communication. Thus, it is envisioned that catechols can emerge as a molecular equivalent to a transistor for miniaturize‐able, deployable and sustainable redox‐linked bioelectronics.

     
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