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Theranostic approaches to cancer management offer the possibility of tailoring treatments to individual patients or tumours. However, the development of theranostic nanoparticles optimally suitable for both diagnostic and therapeutic modalities to achieve this is challenging. Here we demonstrate an alternative nanoparticle-free theranostic approach that circumvents many of the difficulties currently hindering clinical translation. Through the use of a multimodal optical probe, we translate the theranostic burden from complex nanoparticles within the body to an external spectroscopic device, thus alleviating many of the constraints imposed on existing theranostic systems. Using this platform, we demonstrate the combination of Raman spectroscopic diagnosis with photodynamic therapy for optical cancer theranostics. Through selection of photosensitisers with suitable optical properties for combination with Raman spectroscopy, we achieve optical theranostics without the need for complex material systems. Sequential delivery of light for real-time Raman spectroscopic diagnosis followed by photosensitiser-specific illumination, enables cancer diagnosis and treatment during a single procedure. We demonstrate the feasibility of this theranostic approach using a panel of clinically-approved photosensitisers using in vitro cell assays across three cancerous cell lines, with in vivo demonstration using subcutaneous xenograft tumour models ongoing. Our results indicate that through careful instrument design, Raman spectroscopic diagnosis can be effectively performed on photosensitiser-containing cells and tissues without impaired diagnostic accuracy or undesired premature photosensitiser activation. Together, these results show that combination of Raman spectroscopy and photodynamic therapy for optical theranostics enables nanoparticle-free cancer detection, diagnosis, and treatment in real-time using a single optical system.
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