The reactive oxygen species (ROS)-mediated mechanism is the major cause underlying the efficacy of photodynamic therapy (PDT). The PDT procedure is based on the cascade of synergistic effects between light, a photosensitizer (PS) and oxygen, which greatly favors the spatiotemporal control of the treatment. This procedure has also evoked several unresolved challenges at different levels including (i) the limited penetration depth of light, which restricts traditional PDT to superficial tumours; (ii) oxygen reliance does not allow PDT treatment of hypoxic tumours; (iii) light can complicate the phototherapeutic outcomes because of the concurrent heat generation; (iv) specific delivery of PSs to sub-cellular organelles for exerting effective toxicity remains an issue; and (v) side effects from undesirable white-light activation and self-catalysation of traditional PSs. Recent advances in nanotechnology and nanomedicine have provided new opportunities to develop ROS-generating systems through photodynamic or non-photodynamic procedures while tackling the challenges of the current PDT approaches. In this review, we summarize the current status and discuss the possible opportunities for ROS generation for cancer therapy. We hope this review will spur pre-clinical research and clinical practice for ROS-mediated tumour treatments.

Reactive oxygen species generating systems meeting challenges of photodynamic cancer therapy

Photodynamic therapy is a promising treatment method, but its applications are limited by the shallow penetration of visible light. Here, we report a novel X-ray inducible photodynamic therapy (X-PDT) approach that allows PDT to be regulated by X-rays. Upon X-ray irradiation, the integrated nanosystem, comprised of a core of a nanoscintillator and a mesoporous silica coating loaded with photosensitizers, converts X-ray photons to visible photons to activate the photosensitizers and cause efficient tumor shrinkage.

Nanoscintillator-Mediated X-ray Inducible Photodynamic Therapy for In Vivo Cancer Treatment

Current opinion in chemical biology.

X-ray luminescent nanoparticles (NPs), including lanthanide fluorides, have been evaluated for application to deep tissue in vivo molecular imaging using optical tomography. A combination of high material density, higher atomic number and efficient NIR luminescence from compatible lanthanide dopant ions indicates that particles that consist of ALnF4 (A = alkaline, Ln = lanthanide element) may offer a very attractive class of materials for high resolution, deep tissue imaging with X-ray excitation. NaGdF4:Eu3+ NPs produced an X-ray excited luminescence that was among the most efficient of nanomaterials that have been studied thus far. We have systematically studied factors such as (a) the crystal structure that changes the lattice environment of the doped Eu3+ ions within the unit cell; and extrinsic factors such as (b) a gold coating (with attendant biocompatibility) that couples to a plasmonic excitation, and (c) changes in the NPs surface properties via changes in the pH of the suspending medium-all with a significant impact on the X-ray excited luminescence of NaGdF4:Eu3+NPs. The luminescence from an optimally doped hexagonal phase NaGdF4:Eu3+ nanoparticle was 25% more intense compared to that of a cubic structure. We observed evidence of plasmonic reabsorption of midwavelength emission by a gold coating on hexagonal NaGdF4:Eu3+ NPs; fortunately, the NaGdF4:Eu3+ @Au core-shell NPs retained the efficient 5D0→7F4 NIR (692 nm) luminescence. The NaGdF4:Eu3+ NPs exhibited sensitivity to the ambient pH when excited by X-rays, an effect not seen with UV excitation. The sensitivity to the local environment can be understood in terms of the sensitivity of the excitons that are generated by the high energy X-rays (and not by UV photons) to crystal structure and to the surface state of the particles.

/pdf/nagdf4-eu3-nanoparticles-for-enhanced-x-ray-excited-optical-4vx0xpp0ce.pdf

NaGdF4:Eu3+ Nanoparticles for Enhanced X-ray Excited Optical Imaging.

Using X-rays as the irradiation source, a photodynamic therapy process can be initiated in deep tissues. This technology, referred to as X-ray induced PDT, or X-PDT, holds great potential to treat tumors in internal organs. To this end, one question is how to navigate the treatment of tumors with accuracy using external irradiation. Herein we address this issue using a novel LiGa5O8:Cr (LGO:Cr)-based nanoscintillator, which emits persistent, near-infrared X-ray luminescence. This permits deep-tissue optical imaging that can be employed to guide irradiation. Specifically, we encapsulated LGO:Cr nanoparticles and a photosensitizer, 2,3-naphthalocyanine, into mesoporous silica nanoparticles. The nanoparticles were conjugated with cetuximab and systemically injected into H1299 orthotopic non-small cell lung cancer tumor models. The nanoconjugates can efficiently accumulate in tumors in the lungs, confirmed by monitoring the X-ray luminescence from LGO:Cr. Guided by the imaging, external irradiation was applied, leading to efficient tumor suppression while minimally affecting normal tissues. To the best of our knowledge, the present study is the first to demonstrate, with systematically injected nanoparticles, that X-PDT can suppress the growth of deep-seated tumors. The imaging guidance is also new to X-PDT, and is significant to the further transformation of the technology.

/pdf/liga5o8-cr-based-theranostic-nanoparticles-for-imaging-1uk1dfywo8.pdf

LiGa5O8:Cr-based theranostic nanoparticles for imaging-guided X-ray induced photodynamic therapy of deep-seated tumors.

X-rays have been used for non-invasive high-resolution imaging of thick biological specimens since their discovery in 1895. They are widely used for structural imaging of bone, metal implants, and cavities in soft tissue. Recently, a number of new contrast methodologies have emerged which are expanding X-ray's biomedical applications to functional as well as structural imaging. These techniques are promising to dramatically improve our ability to study in situ biochemistry and disease pathology. In this review, we discuss how X-ray absorption, X-ray fluorescence, and X-ray excited optical luminescence can be used for physiological, elemental, and molecular imaging of vasculature, tumors, pharmaceutical distribution, and the surface of implants. Imaging of endogenous elements, exogenous labels, and analytes detected with optical indicators will be discussed.

Advances in functional X-ray imaging techniques and contrast agents

Strain gauges that can provide information with regard to the state of implantable devices are described. The strain gauges can exhibit luminescence that is detectable through living tissue, and the detectable luminescent emission can vary according to the strain applied to the gauge. A change in residual strain of the device can signify a loss of mechanical integrity and/or loosening of the implant, and this can be non-invasively detected either by simple visual detection of the luminescent emission or through examination of the emission with a detector such as a spectrometer or a camera.

/pdf/luminescent-tension-indicating-orthopedic-strain-gauges-for-4le72pwk1r.pdf

Luminescent Tension-Indicating Orthopedic Strain Gauges for Non-Invasive Measurements Through Tissue

/pdf/luminescent-tension-indicating-orthopedic-strain-gauges-for-3g0s6ubqa1.pdf

Luminescent Tension-Indicating Orthopedic Strain Gauges for Non-Invasive Measurements

An orthopaedic screw was designed with an optical tension-indicator to non-invasively quantify screw tension and monitor the load sharing between the bone and the implant. The screw both applies load to the bone, and measures this load by reporting the strain on the screw. The screw contains a colorimetric optical encoder that converts axial strain into colorimetric changes visible through the head of the screw, or luminescent spectral changes that are detected through tissue. Screws were tested under cyclic mechanical loading to mimic in-vivo conditions to verify the sensitivity, repeatability, and reproducibility of the sensor. In the absence to tissue, color was measured using a digital camera as a function of axial load on a stainless steel cannulated (hollow) orthopedic screw, modified by adding a passive colorimetric strain gauge through the central hole. The sensor was able to quantify clinically-relevant bone healing strains. The sensor exhibited good repeatability and reproducibility but also displayed hysteresis due to the internal mechanics of the screw. The strain indicator was also modified for measurement through tissue by replacing the reflective colorimetric sensor with a low-background X-ray excited optical luminescence signal. Luminescent spectra were acquired through 6 mm of chicken breast tissue. Overall, this research shows feasibility for a unique device which quantifies the strain on an orthopedic screw. Future research will involve reducing hysteresis by changing the mechanism of strain transduction in the screw, miniaturizing the luminescent strain gauge, monitoring bending as well as tension, using alternative luminescent spectral rulers based upon near infrared fluorescence or upconversion luminescence, and application to monitoring changes in pretension and load sharing during bone healing.

Development of an optically-based tension-indicating implanted orthopedic screw with a luminescent spectral ruler

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Advances in functional X-ray imaging techniques and contrast agents

Luminescent Tension-Indicating Orthopedic Strain Gauges for Non-Invasive Measurements Through Tissue

Luminescent Tension-Indicating Orthopedic Strain Gauges for Non-Invasive Measurements

Development of an optically-based tension-indicating implanted orthopedic screw with a luminescent spectral ruler