In Vivo Detection of Gold−Imidazole Self-Assembly Complexes: NIR-SERS Signal Reporters

Abstract

Here we report in vitro and in vivo detection of self-assembled Au-imidazole by using near-infrared surface-enhanced Raman scattering (NIR-SERS). In vivo, the Au-imidazole structures were administered into tumor-bearing mice and detected noninvasively. The self-assembled Au-imidazole complexes were generated by the adsorption of imidazole molecules onto Au nanoparticles (NP) and were then characterized as aqueous suspensions by using NIR-SERS, angle-dependent light scattering with fractal dimension analysis, and visible extinction spectroscopy. The structure and optical activity was sensitive to imidazole concentration and Au NP size. Specifically, the Au-imidazole assemblies formed at lower imidazole concentrations had the lowest fractal dimension (D(f) = 1.2) and the largest Raman enhancement factors for the dominant NIR-SERS feature, a ring-breathing vibrational mode at 954 cm(-1). Changes in elastic scattering intensity, fractal dimension, and surface plasmon absorption were observed with increasing imidazole concentration. The Raman enhancement factor was also found to range between 10(6) and 10(9) with different primary Au nanoparticle sizes. For the higher enhancement factor systems, NIR-SERS detection of Au-imidazole was performed with data acquisitions time of only 5 s. The largest enhancement was observed for the 954-cm(-1) feature at an imidazole concentration of 1.9 microM when coupled to 54-nm-diameter Au NPs (the largest NP tested). Finally, we show the first demonstration of in vivo, noninvasive, and real-time SERS detection.