Development of imageable photothermal theranostics has attracted considerable attention for imaging guided photothermal therapy (PTT) with high tumor ablation accuracy. In this study, we strategically constructed a near-infrared (NIR) cyanine dye by introducing a rigid cyclohexenyl ring to the heptamethine chain to obtain a heptamethine dye CySCOOH with high fluorescence intensity and good stability. By covalent conjugation of CySCOOH onto human serum albumin (HSA), the as-prepared HSA@CySCOOH nanoplatform is highly efficient for NIR fluorescence/photoacoustic/thermal multimodality imaging and photothermal tumor ablation. The theranostic capability of HSA@CySCOOH was systematically evaluated both in vitro and in vivo. Most intriguingly, complete tumor elimination was achieved by intravenous injection of HSA@CySCOOH (CySCOOH, 1 mg/kg; 808 nm, 1.0 W/cm2 for 5 min) on 4T1 tumor-bearing mice, with no weight loss, noticeable toxicity, or tumor recurrence being observed. This as-prepared protein-based nanotheranostics exhibits high water dispersibility, no off target cytotoxicity, good biodegradability and biocompatibility, thus facilitating its clinical translation for cancer photothermal theranostics.

The imaging of sentinel lymph nodes (SLNs), the first defense against primary tumor metastasis, has been considered as an important strategy for noninvasive tracking tumor metastasis in clinics. In this study, we developed an imaging contrast system based on fluorescent dye-loaded mesoporous silica nanoparticles (MSNPs) that integrate near-infrared (NIR) fluorescent and photoacoustic (PA) imaging modalities for efficient SLN mapping. By balancing the ratio of dye and nanoparticles for simultaneous optimization of dual-modality imaging (NIR and PA), the dye encapsulated MSNP platform was set up to generate both a moderate NIR emission and PA signals simultaneously. Moreover, the underlying mechanisms of the relevance between optical and PA properties were discovered. Subsequently, dual-modality imaging was achieved to visualize tumor draining SLNs up to 2 weeks in a 4T1 tumor metastatic model. Obvious differences in uptake rate and contrast between metastatic and normal SLNs were observed both in vivo and ex vivo. Based on all these imaging data, it was demonstrated that the dye-loaded MSNPs allow detection of regional lymph nodes in vivo with time-domain NIR fluorescent and PA imaging methods efficiently.

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Photoacoustic imaging (PA) has emerged as a novel and noninvasive imaging modality owing to its high spatial resolution and high soft tissue contrast. Herein, we loaded a near-infrared (NIR) fluorescence dye (CySCOOH) onto the surface of PEGylated graphene oxide (GO) via π-π stacking to increase the NIR absorbance of GO. The PA imaging proved that PEGylated GO-CysCOOH (GO-PEG-CysCOOH) significantly enhances the PA signal in the tumor site compared with free GO-PEG. We then utilized the strong optical absorbance of GO-PEG-CySCOOH in the NIR region for in vivo photothermal therapy, achieving efficient tumor ablation after intravenous injection of GO-PEG-CySCOOH and low-power laser irradiation on the tumor. Our results indicate that this graphene-based nanocomposite can be developed as a promising contrast agent for PA imaging and a thermal agent for imaging guided photothermal therapy.