Multicomponent Simultaneous Identification Network (MSINet): An Advanced Deep Learning Model for Boosting Multiplex SERS Detection in Untreated Real Samples.

Surface-enhanced Raman spectroscopy (SERS) represents unique advantages for on-site analysis due to its high sensitivity, high specificity, and applicability to gaseous, liquid, and solid samples. However, the complex and unknown components in matrices, as well as competitive adsorptions between targets, will cause signal fluctuation and spectral overlap, which make it challenging to detect multiple targets in untreated real samples. Herein, we designed a deep learning model named the multicomponent simultaneous identification network (MSINet) for analyzing the SERS spectra of untreated samples and output qualitative and content evaluation results of multiple inside targets. The hierarchical feature extraction and multiple feature integration made MSINet robust to signal fluctuations and spectral overlaps while requiring only a small amount of training to quantify target contents in any samples due to its threshold judgment rule. Using the MSINet-assisted SERS detection scheme, the presence and content levels of multiple UV absorbers in seawater, food additives in ready-to-drink cocktails, and biomarkers in human serum could all be determined with ≥0.90 accuracy when facing testing databases. But in contrast, the accuracy in evaluating the target contents in the above untreated samples by the standard curve method was as low as 0.05. The powerful ability to process spectral data, an easy-to-use graphical user interface, and "zero" extra cost make MSINet a universal tool to assist arbitrary SERS sensors in performing high-throughput detection of real samples, leading to great potential in on-site analysis.