Detection of individual molecules is the ultimate goal of any chemical sensor. In the case of gas detection, such resolution has been achieved in advanced nanoscale electronic solid-state sensors, but it has not been possible so far in integrated photonic devices, where the weak light-molecule interaction is typically hidden by noise. Here, we demonstrate a scheme to generate ultrasensitive down-conversion four-wave-mixing (FWM) in a graphene bipolar-junction-transistor heterogeneous D-shaped fiber. In the communication band, the FWM conversion efficiency can change steeply when the graphene Fermi level approaches 0.4 eV. In this condition, we exploit our unique two-step optoelectronic heterodyne detection scheme, and we achieve real-time individual gas molecule detection in vacuum. Such combination of graphene strong nonlinearities, electrical tunability, and all-fiber integration paves the way toward the design of versatile high-performance graphene photonic devices.

Photonic sensors that are able to detect and track biochemical molecules offer powerful tools for information acquisition in applications ranging from environmental analysis to medical diagnosis. The ultimate aim of biochemical sensing is to achieve both quantitative sensitivity and selectivity. As atomically thick films with remarkable optoelectronic tunability, graphene and its derived materials have shown unique potential as a chemically tunable platform for sensing, thus enabling significant performance enhancement, versatile functionalization and flexible device integration. Here, we demonstrate a partially reduced graphene oxide (prGO) inner-coated and fiber-calibrated Fabry-Perot dye resonator for biochemical detection. Versatile functionalization in the prGO film enables the intracavity fluorescent resonance energy transfer (FRET) to be chemically selective in the visible band. Moreover, by measuring the intermode interference via noise canceled beat notes and locked-in heterodyne detection with Hz-level precision, we achieved individual molecule sensitivity for dopamine, nicotine and single-strand DNA detection. This work combines atomic-layer nanoscience and high-resolution optoelectronics, providing a way toward high-performance biochemical sensors and systems.

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Single atomically thick graphene, with unique structural flexibility, surface sensitivity, and effective light-mater interaction, has shown exceptional advances in optoelectronics. It opens a door for diverse functionalized photonic devices, ranging from passive polarizers to active lasers and parametric oscillators. Among them, graphene-fiber biochemical sensors combine the merits of both graphene and fiber structures, demonstrating impressively high performances, such as single-molecule detectability and fast responsibility. These graphene-fiber biochemical sensors can offer tools in various applications, such as gas tracing, chemical analysis, and medical testing. In this paper, we review the emerging graphene-fiber biochemical sensors comprehensively, including the sensing principles, device fabrications, systematic implementations, and advanced applications. Finally, we summarize the state-of-the-art graphene-fiber biochemical sensors and put forward our outlooks on the development in the future.

We demonstrate the steep EO tunability of four-wave-mixing (FWM) in a graphene bipolar-junction-transistor heterogeneous D-shaped fiber (GhDF). This enables the GhDF ultrasensitive to external molecule adsorption/desorption in vacuum, achieving individual gas molecule detections.