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Ultrasensitive trace-detection of toxic and carcinogenic polycyclic aromatic hydrocarbons (PAHs) can ceaselessly propel the environmental surveillance in aqueous ecosystems. Due to the intrinsic nonadsorptive feature of PAHs, the promising technique of surface-enhanced Raman scattering (SERS) spectroscopy has been restricted to diverse functional ligands-based surface modifications of nano-substrates. However, it is not suitable for practical ultralow liquid analysis. Herein, we propose an extraordinary strategy to boost liquid-near infrared (NIR)-SERS activity of plasmonic Au/Ag nano-urchins (NUs) by introducing extra 808 nm laser-triggered an additional strong electromagnetic enhancement into routine 785 nm laser-Raman system. The synergistic double laser-excited NIR-SERS of colloidal Au/Ag NUs enables the Raman signals of crystal violet to be significantly enhanced, approaching a maximum of ∼34-fold increase than that of traditional bare 785 nm laser-excitation. More importantly, the improved liquid-NIR-SERS enables the  in-situ  detection limit of pyrene molecules in lake water to be achieved at ∼10 −9  M, which is already better than many previous SERS results based on the complicated functionalized nano-substrates. The established double laser-boosted NIR-SERS can also be easily extended to the simultaneous trace-detection of three PAHs-contaminated mixtures, supporting well distinguishable capability. Undoubtedly, the present work opens a new versatile and innovative avenue for ultrasensitive NIR-SERS monitoring of nonadsorptive toxic pollutants in wastewater.

Synergistic double laser beam-boosted liquid-NIR-SERS for ultralow detection of non-adsorptive polycyclic aromatic hydrocarbons in lake water