Antibody–antigen (Ab–Ag) recognition is the primary event at the basis of many biosensing platforms. In label-free biosensors, these events occurring at solid–liquid interfaces are complex and often difficult to control technologically across the smallest length scales down to the molecular scale. Here a molecular-scale technique, such as single-molecule force spectroscopy, is performed across areas of a real electrode functionalized for the immunodetection of an inflammatory cytokine, viz. interleukin-4 (IL4). The statistical analysis of force–distance curves allows us to quantify the probability, the characteristic length scales, the adhesion energy, and the time scales of specific recognition. These results enable us to rationalize the response of an electrolyte-gated organic field-effect transistor (EGOFET) operated as an IL4 immunosensor. Two different strategies for the immobilization of IL4 antibodies on the Au gate electrode have been compared: antibodies are bound to (i) a smooth film of His-tagged protein G (PG)/Au; (ii) a 6-aminohexanethiol (HSC₆NH₂) self-assembled monolayer on Au through glutaraldehyde. The most sensitive EGOFET (concentration minimum detection level down to 5 nM of IL4) is obtained with the first functionalization strategy. This result is correlated to the highest probability (30%) of specific binding events detected by force spectroscopy on Ab/PG/Au electrodes, compared to 10% probability on electrodes with the second functionalization. Specifically, this demonstrates that Ab/PG/Au yields the largest areal density of oriented antibodies available for recognition. More in general, this work shows that specific recognition events in multiscale biosensors can be assessed, quantified, and optimized by means of a nanoscale technique.

Graphene is regarded as the ultimate material for future flexible, high‐performance, and wearable electronics. Herein, a novel, robust, all‐green, highly reliable (yield ≥ 99%), and upscalable technology is reported for wearable applications comprising reduced graphene oxide (rGO) as the electroactive component in liquid‐gated transistors (LGTs). rGO is a formidable material for future flexible and wearable applications due to its easy processability, excellent surface reactivity, and large‐area coverage. A novel protocol is established toward the high‐yield fabrication of flexible rGO LGTs combining high robustness (>1.5 h of continuous operation) with state‐of‐the‐art performances, being similar to those of their rigid counterparts operated under liquid gating, including field‐effect mobility of ≈10⁻¹ cm² V⁻¹ s⁻¹ and transconductance of ≈25 µS. Permeable membranes have been proven crucial to operate flexible LGTs under mechanical stress with reduced amounts of solution (<20 µL). Our rGO LGTs are operated in artificial sweat exploiting two different layouts based on lateral‐flow paper fluidics. These approaches pave the road toward future real‐time tracking of perspiration via a simple and cost‐effective approach. The reported findings contribute to the robust and scalable production of novel graphene‐based flexible devices, whose features fulfill the requirements of wearable electronics.

Chemical sensing is a strategic field of science and technology ultimately aiming at improving the quality of our lives and the sustainability of our Planet. Sensors bear a direct societal impact on well-being, which includes the quality and composition of the air we breathe, the water we drink, and the food we eat. Pristine low-dimensional materials are widely exploited as highly sensitive elements in chemical sensors, although they suffer from lack of intrinsic selectivity towards specific analytes. Here, we showcase the most recent strategies on the use of (supra)molecular interactions to harness the selectivity of suitably functionalized 0D, 1D, and 2D low-dimensional materials for chemical sensing. We discuss how the design and selection of receptors via machine learning and artificial intelligence hold a disruptive potential in chemical sensing, where selectivity is achieved by the design and high-throughput screening of large libraries of molecules exhibiting a set of affinity parameters that dictates the analyte specificity. We also discuss the importance of achieving selectivity along with other relevant characteristics in chemical sensing, such as high sensitivity, response speed, and reversibility, as milestones for true practical applications. Finally, for each distinct class of low-dimensional material, we present the most suitable functionalization strategies for their incorporation into efficient transducers for chemical sensing.