Tip-enhanced Raman spectroscopy (TERS) is capable of probing specific molecular information with high sensitivity, but dual chemical sensing remains a challenge. Another major hindrance to TERS chemical detection in biosamples such as blood is the interference from the strong absorptions of biomolecules. Herein, we report the preparation of an organometallic-conjugated TERS tip. We demonstrate that organometallic chemistry can be perfectly coupled with TERS for dual-molecule sensing. The unique Raman signals generated by the organometallic compound circumvent signal interference from the biomolecules in blood, allowing the rapid analysis of two important molecules (glucose and thiol) in ultralow volume (50 nL) samples. This enabled a correlation between the thiol and glucose levels in the blood of nondiabetic and diabetic patients to be drawn.

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The detection of carbohydrates in human body fluids is critical for disease diagnosis and healthy monitoring. Despite recent advances in glucose sensing, multiplex detection of different carbohydrates within a single assay that is capable of efficiently providing richer health information remains challenging. Herein, we report a versatile surface-enhanced Raman spectroscopy-based platform for the quantitative detection of monosaccharides (glucose, fructose, and galactose) in one test using a displace-and-trap mechanism. Moreover, due to the use of multiple optical interference-free (1800−2200 cm −1 ) signal-independent Raman probes, the detection range of this platform (0.125−7 mg/dL) perfectly covers physiological concentrations, enabling the quantitative detection of glucose and galactose in clinical human saliva samples. This work provides a noninvasive and high-efficiency potential tool for the screening of clinical diabetes and other carbohydrate-related diseases.

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