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Chemiluminescence resonance energy transfer–based nanoparticles for quantum yield–enhanced cancer phototheranostics.

ABSTRACT: Chemiluminescence (CL) has recently gained attention for CL resonance energy transfer (CRET)–mediated photodynamic therapy of cancer. However, the short duration of the CL signal and low quantum yield of the photosensitizer have limited its translational applications. Here, we report CRET-based nanoparticles (CRET-NPs) to achieve quantum yield–enhanced cancer phototheranostics by reinterpreting the hidden nature of CRET. Owing to reactive oxygen species (ROS)–responsive CO2 generation, CRET-NPs were capable of generating a strong and long-lasting photoacoustic signal in the tumor tissue via thermal expansion–induced vaporization. In addition, the CRET phenomenon of the NPs enhanced ROS quantum yield of photosensitizer through both electron transfer for an oxygen-independent type I photochemical reaction and self-illumination for an oxygen-dependent type II photochemical reaction. Consequently, owing to their high ROS quantum yield, CRET-NPs effectively inhibited tumor growth with complete tumor growth inhibition in 60% of cases, even with a single treatment.

SUBMITTER: Jeon J

PROVIDER: S-EPMC7314564 | biostudies-literature | 2020 May

REPOSITORIES: biostudies-literature

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Project description:DNAzymes have emerged as an important class of sensors for a wide variety of metal ions, with florescence DNAzyme sensors as the most widely used in different sensing and imaging applications because of their fast response time, high signal intensity, and high sensitivity. However, the requirements of an external excitation light source and its associated power increase the cost and size of the fluorometer, making it difficult to be used for portable detections. To overcome these limitations, we report herein a DNAzyme sensor that relies on chemiluminescence resonance energy transfer (CRET) without the need for external light. The sensor is constructed by combining the functional motifs from both Pb2+-dependent 8-17 DNAzyme conjugated to fluorescein (FAM) and hemin/G-quadruplex that mimics horseradish peroxidase to catalyze the oxidation of luminol by H2O2 to yield chemiluminescence. In the absence of Pb2+, the hybridization between the enzyme and substrate strands bring the FAM and hemin/G-quadruplex in close proximity, resulting in CRET. The presence of Pb2+ ions can drive the cleavage on the substrate strand, resulting in a sharp decrease in the melting temperature of hybridization and thus separation of the FAM from hemin/G-quadruplex. The liberated CRET pair causes a ratiometric increase in the donor's fluorescent signal and a decrease in the acceptor signal. Using this method, Pb2+ ions have been measured rapidly (<15 min) with a low limit of detection at 5 nM. By removing the requirement of exogenous light excitation, we have demonstrated a simple and portable detection using a smartphone, making the DNAzyme-CRET system suitable for field tests of lake water. Since DNAzymes selective for other metal ions or targets, such as bacteria, can be obtained using in vitro selection, the method reported here opens a new avenue for rapid, portable, and ratiometric detection of many targets in environmental monitoring, food safety, and medical diagnostics.

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Chemiluminescence resonance energy transfer–based nanoparticles for quantum yield–enhanced cancer phototheranostics.

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