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Rational engineering of highly stable and Raman-active nanostructured substrates is still urgently in demand for achieving sensitive and reliable surface-enhanced Raman spectroscopy (SERS) analysis in solution phase. Herein, monodisperse N-doping graphene quantum dots wrapped Au nanoparticles (Au-NGQD NPs) were facilely prepared, and further their applications as substrates in SERS-based detection and cellular imaging have been explored. The as-prepared Au-NGQD NPs exhibit superior long-term stability and biocompatibility, as well as large enhancement capability due to the integration of electromagnetic and chemical enhancements. The practical applicability of the Au-NGQD NPs was verified via the direct SERS tests of several kinds of aromatics in solution phase. Finite-difference time-domain simulations in combination with density functional theory calculation were also successfully used to explain the enhancement mechanism. Furthermore, the Au-NGQD NPs were conjugated with 4-nitrobenzenethiol (4-NBT, as reporter) and 4-mercaptophenylboronic acid (MPBA, as targeting element) to construct the MPBA/4-NBT@Au-NGQD probes, which could specifically recognize glycan-overexpressed cancer cells through SERS imaging on a cell surface. The prepared Au-NGQDs show great potential as superior SERS substrates in solution phase for on-site Raman detection.

The combination of surface-enhanced Raman scattering (SERS) imaging technology with near-infrared (NIR) light-triggered photothermal therapy is of utmost importance to develop novel theranostic platforms. Herein, an aptamer-conjugated Au nanocage/SiO 2 (AuNC/SiO 2 /Apt) core-shell Raman nanoprobe has been rationally designed as the bifunctional theranostic platform to fulfill this task. In this theranostic system, the Raman-labeled Au nanocage (AuNC) was encapsulated into a bioinert shell of SiO 2 , followed by conjugating aptamer AS1411 as the target-recognition moiety. AuNC served as the SERS-active and photothermal substrate due to its large free volume, built-in plasmon effect, and NIR photothermal capacity, while the SiO 2 coating endowed the nanoprobes with good stability and biocompatibility, as well as abundant anchoring sites for surface functionalization. Considering their prominent SERS and photothermal properties, the application potential of the AuNC/SiO 2 /Apt nanoprobes was investigated. The proposed nanoprobes could be applied to targeted detection and SERS imaging of nucleolin-overexpressing cancer cells (MCF-7 cells as the model) from normal cells and also exhibited acceptable photothermal efficacy without systematic toxicity. This theranostic nanoplatform provided a possible opportunity for in situ diagnosis and noninvasive treatment of cancer cells by SERS imaging-guided photothermal therapy.