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The versatile nature of organic conjugated materials renders their flawless integration into a diverse family of optoelectronic devices with light-harvesting, photodetection, or light-emitting capabilities. Classes of materials that offer the possibilities of two or more distinct optoelectronic functions are particularly attractive as they enable smart applications while providing the benefits of the ease of fabrication using low-cost processes. Here, we develop a novel, multi-purpose conjugated small molecule by combining boron-azadipyrromethene (aza-BODIPY) as electron acceptor with triphenylamine (TPA) as end-capping donor units. The implemented donor–acceptor–donor (D–A–D) configuration, in the form of TPA-azaBODIPY-TPA, preserves ideal charge transfer characteristics with appropriate excitation energy levels, with the additional ability to be used as either a charge transporting interlayer or light-sensing semiconducting layer in optoelectronic devices. To demonstrate its versatility, we first show that TPA-azaBODIPY-TPA can act as an excellent hole transport layer in methylammonium lead triiodide (MAPbI3)-based perovskite solar cells with measured power conversion efficiencies exceeding 17%, outperforming control solar cells with PEDOT:PSS by nearly 60%. Furthermore, the optical bandgap of 1.49 eV is shown to provide significant photodetection in the wavelength range of up to 800 nm where TPA-azaBODIPY-TPA functions as donor in near-infrared organic photodetectors (OPDs) composed of fullerene derivatives. Overall, the established versatility of TPA-azaBODIPY-TPA, combined with its robust thermal stability as well as excellent solubility and processability, provides a new guide for developing highly efficient multi-purpose electronic materials for the next-generation of smart optoelectronic devices. (Figure presented.).

Biofilms are part of the natural lifecycle of bacteria and are known to cause chronic infections that are difficult to treat. Most antibiotics are developed and tested against bacteria in the planktonic state and are ineffective against bacterial biofilms. The oxazolidinones, including the last resort drug linezolid, are one of the main classes of synthetic antibiotics progressed to clinical use in the last 50 years. They have a unique mechanism of action and only develop low levels of resistance in the clinical setting. With the aim of providing insight into strategies to design more potent antibiotic compounds with activity against bacterial biofilms, we review the biofilm activity of clinically approved oxazolidinones and report on structural modifications to oxazolidinones and their delivery systems which lead to enhanced anti-biofilm activity.

Organic based redox active materials and coatings are increasingly being investigated as solutions for more efficient energy devices, catalysts, sensors, and biomedical technologies. Their advantage is negating the necessity for expensive and unsustainable rare earth metals seen in other redox active materials. Challenges to their wide-spread usage remain, including versatility of coatings on a wide range of substrates, and creating smart devices that can respond to environmental stimuli. A new light responsive radical releasing redox coating has been developed, that can be rapidly and stably applied to a diverse range of substrates including silicon dioxide, plastics, and microparticles. These coatings rapidly cleave upon irradiation with UV-A light to release stable nitroxides from the surface coating. These coatings are developed into microparticle sensors for radical oxygen species, which are able to detect the generation of free radicals in a model system for particulate matter pollution. These new responsive organic redox coatings also offer future potential to function as switchable organic electrodes, and biomedical surface coatings to prevent biofouling and reduce inflammation.

Organic electrochemical transistors (OECTs) are presently a focus of intense research and hold great potential in expanding the horizons of the bioelectronics industry. The notable characteristics of OECTs, including their electrolyte-gating, which offers intimate interfacing with biological environments, and aqueous stability, make them particularly suitable to be operated within a living organism (in vivo). Unlike the existing in vivo bioelectronic devices, mostly based on rigid metal electrodes, OECTs form a soft mechanical contact with the biological milieu and ensure a high signal-to-noise ratio because of their powerful amplification capability. Such features make OECTs particularly desirable for a wide range of in vivo applications, including electrophysiological recordings, neuron stimulation, and neurotransmitter detection, and regulation of plant processes in vivo. In this review, a systematic compilation of the in vivo applications is presented that are addressed by the OECT technology. First, the operating mechanisms, and the device design and materials design principles of OECTs are examined, and then multiple examples are provided from the literature while identifying the unique device properties that enable the application progress. Finally, one critically looks at the future of the OECT technology for in vivo bioelectronic applications.

An alternative synthetic route towards the widely employed electroactive poly(TEMPO methacrylate) (PTMA) via a thermally robust methoxyamine-protecting group is demonstrated herein. Protection of the radical moiety of hydroxy-TEMPO with a methyl functionality and subsequent esterification with methacrylic anhydride allows the high-yielding formation of the novel monomer methyl-TEMPO methacrylate (MTMA). The polymerization of MTMA to poly(MTMA) (PMTMA) is investigated via free radical polymerization and reversible addition–fragmentation chain-transfer polymerization (RAFT), a reversible-deactivation radical polymerization technique. Cleavage of the temperature-stable methoxyamine functionality by oxidative treatment of PMTMA with meta-chloroperbenzoic acid (mCPBA) releases the electroactive PTMA. The redox activity of PTMA was confirmed by cyclic voltammetry in lithium-ion coin cells.

Treatment of biofilm-related Staphylococcus aureus infections represents an important medical challenge worldwide, as biofilms, even those involving drug-susceptible S. aureus strains, are highly refractory to conventional antibiotic therapy. Nitroxides were recently shown to induce the dispersal of Gram-negative biofilms in vitro, but their action against Gram-positive bacterial biofilms remains unknown. Here, we demonstrate that the biofilm dispersal activity of nitroxides extends to S. aureus, a clinically important Gram-positive pathogen. Coadministration of the nitroxide CTEMPO (4-carboxy-2,2,6,6-tetramethylpiperidin-1-yloxyl) with ciprofloxacin significantly improved the biofilm eradication activity of the antibiotic against S. aureus. Moreover, covalently linking the nitroxide to the antibiotic moiety further reduced the ciprofloxacin minimal biofilm eradication concentration. Microscopy analysis revealed that fluorescent nitroxide-antibiotic hybrids could penetrate S. aureus biofilms and enter cells localized at the surface and base of the biofilm structure. No toxicity to human cells was observed for the nitroxide CTEMPO or the nitroxide-antibiotic hybrids. Taken together, our results show that nitroxides can mediate the dispersal of Gram-positive biofilms and that dual-acting biofilm eradication antibiotics may provide broad-spectrum therapies for the treatment of biofilm-related infections.

Most free-living bacteria can attach to surfaces and aggregate to grow into multicellular communities encased in extracellular polymeric substances called biofilms. Biofilms are recalcitrant to antibiotic therapy and a major cause of persistent and recurrent infections by clinically important pathogens worldwide (e.g., Pseudomonas aeruginosa, Escherichia coli, and Staphylococcus aureus). Currently, most biofilm remediation strategies involve the development of biofilm-inhibition agents, aimed at preventing the early stages of biofilm formation, or biofilm-dispersal agents, aimed at disrupting the biofilm cell community. While both strategies offer some clinical promise, neither represents a direct treatment and eradication strategy for established biofilms. Consequently, the discovery and development of biofilm eradication agents as comprehensive, stand-alone biofilm treatment options has become a fundamental area of research. Here we review our current understanding of biofilm antibiotic tolerance mechanisms and provide an overview of biofilm remediation strategies, focusing primarily on the most promising biofilm eradication agents and approaches. Many of these offer exciting prospects for the future of biofilm therapeutics for a large number of infections that are currently refractory to conventional antibiotics.

Bacterial biofilm formation on medical devices is a threat to healthcare systems worldwide as bacteria within a biofilm are more resistant to standard antimicrobial therapies. Herein, we introduce a nitroxide-based antibiofilm coating strategy, which is specifically designed to prevent biofilm formation of Gram-negative pathogens such as Pseudomonas aeruginosa. Nitroxide-decorated hydroxyapatite surfaces were readily prepared in an aqueous dip-coating procedure using a nitroxide-functionalized catecholamine as a polymerizable coating agent. Additional spatial control over the polymer surface deposition on titanium was gained by applying a photolithographic coating setup. All nitroxide-coated surfaces exhibited excellent antibiofilm properties toward PA14 surface colonization as biofilm formation was completely suppressed. Importantly, the surrounding adhesive polymer matrix did not interfere with the nitroxide-characteristic antibiofilm properties. The herein introduced platform technology represents a bioinspired and versatile coating approach, offering a safe and prophylactic avenue to combat biofilm contamination on a variety of surfaces.

Recent advances in helium ion microscopy (HIM) have enabled the use of fine-focused He+ beams to image and shape materials at the nanoscale. In addition to traditional ion milling, the beam can also be used to induce reactions, such as cross-linking, in films of organic molecules. Here, we compare the use of focused ion and electron beams to fabricate spatially-defined cross-linked features in nanometre-thick films of tetracene. Ion and electron beam treatments were performed using the focussed energetic beams in a HIM and a scanning electron microscope, respectively. The patterned samples were analysed by optical microscopy, HIM, atomic force microscopy and nanoindentation. For samples fabricated using both energetic beams, the total deposited particle dose could be used to modify the optical properties, thickness and hardness of the dosed regions. X-ray photoelectron spectroscopy revealed that the dosed regions exhibited a higher sp3 content, consistent with crosslinking; rinsing in solvent showed that the patterned regions were insoluble and could be isolated by removing the unmodified film through dissolution. These molecular nanopatterns demonstrate the promise for ultrahigh resolution chemical lithography, and for fabrication of nanocomponents with tailored physical properties.

Fluorescent probes are widely used for imaging and measuring dynamic processes in living cells. Fluorescent antibiotics are valuable tools for examining antibiotic-bacterial interactions, antimicrobial resistance and elucidating antibiotic modes of action. Profluorescent nitroxides are ‘switch on’ fluorescent probes used to visualize and monitor intracellular free radical and redox processes in biological systems. Here, we have combined the inherent fluorescent and antimicrobial properties of the fluoroquinolone core structure with the fluorescence suppression capabilities of a nitroxide to produce the first example of a profluorescent fluoroquinolone-nitroxide probe. Fluoroquinolone-nitroxide (FN) 14 exhibited significant suppression of fluorescence (36-fold), which could be restored via radical trapping (fluoroquinolone-methoxyamine 17) or reduction to the corresponding hydroxylamine 20. Importantly, FN 14 was able to enter both Gram-positive and Gram-negative bacterial cells, emitted a measurable fluorescence signal upon cell entry (switch on), and retained antibacterial activity. In conclusion, profluorescent nitroxide antibiotics offer a new powerful tool for visualizing antibiotic-bacterial interactions and researching intracellular chemical processes.

This work demonstrates a new pathway to the direct on-surface fabrication of surface coatings by showing that application of a plasma can lead to dehalogenative coupling of small aromatic molecules at a catalytic surface. Specifically, we show that a room temperature, atmospheric pressure plasma can be used to fabricate a coating through a surface-confined dehalogenation reaction. Plasma treatments were performed using a dielectric barrier discharge (DBD) technique under pure nitrogen with a variety of power levels and durations. Samples were analysed by optical and helium ion microscopy (HIM), X-ray photoelectron spectroscopy (XPS), optical profilometry, and contact angle measurement. By varying the plasma parameters we could control the chemistry, morphology and roughness of the film. Surface wettability also varied with the plasma parameters, with high-dose plasmas leading to a hydrophobic surface with water contact angles up to 130°.