A Sequential Dual‐Lock Strategy for Photoactivatable Chemiluminescent Probes Enabling Bright Duplex Optical Imaging

Abstract

Chemiluminescence (CL)‐based technologies have revolutionized in vivo monitoring of biomolecules. However, significant technical hurdles have limited the achievement of trigger‐controlled, bright, and enriched CL signal. Herein, a dual‐lock strategy uses sequence‐dependent triggers for bright optical imaging with real‐time fluorescent signal and ultra‐sensitive CL signal. These probes can obtain an analyte‐triggered accumulation of stable pre‐chemiluminophore with aggregation‐induced emission (AIE), and then the pre‐chemiluminophore exhibits a rapid photooxidation process (1,2‐dioxetane generation) by TICT‐based free‐radical addition, thereby achieving an enrichment and bright CL signal. The dual‐lock strategy expands the in vivo toolbox for highly accurate analysis and has for the first time allowed access to accurately sense and trace biomolecules with high‐resolution, dual‐mode of chemo‐fluoro‐luminescence, and three‐dimensional (3D) imaging in living animals.

Near-Infrared Fluorescence MOF Nanoprobe for Adenosine Triphosphate-Guided Imaging in Colitis

“…Various methods have been developed for ATP sensing in recent years such as colorimetry, electrochemical sensing, and electrochemiluminescence. − Although these methods have their own characteristics and advantages, the deficiency in real-time in situ detection in vivo still exists. Relatively, fluorescence detection has more preponderance in vivo because of its simplicity, high sensitivity, and direct viewing. − To date, several fluorescence probes based on various materials have been explored for successful ATP sensing. Unfortunately, there are still some limitations.…”

Near‐InfraredFluorescent Nanoprobe for Detecting Hydrogen Peroxide in Inflammation and Ischemic Kidney Injury

“…Fluorescence detection technique is one of the effective and convenient imaging tools to identify the target biomarkers in bio‐system. [ 11‐20 ] Compared to other methods, fluorescence technique shows higher sensitivity, simple operation process and non‐destructive imaging capability. [ 21‐24 ] To date, various fluorescent probes especially those with long‐wavelength emission have been synthesized for H 2 O 2 detection, as summarized in Table S1.…”

Amplification of Activated Near-Infrared Afterglow Luminescence by Introducing Twisted Molecular Geometry for Understanding Neutrophil-Involved Diseases

“…In recent years, great research interest has focused on the technology and materials of afterglow luminescent imaging. ,, As compared to the widely used fluorescence imaging, afterglow imaging does not require real-time external light excitation, therefore leading to negligible autofluorescence, higher sensitivity, and deeper imaging depth. , To date, two categories of afterglow agents have been developed: (1) inorganic afterglow materials containing rare-earth metal such as europium and praseodymium and 2) organic afterglow materials including semiconducting polymer (e.g., poly­[2-methoxy-5-(2-ethylhexyloxy)-1,4-phenylenevinylene])-based and small molecule (e.g., Schaap’s dioxetane)-based ones. − Nevertheless, the inorganic and organic afterglow materials capable of responding to the disease biomarkers/microenvironments selectively remain limited . Among versatile afterglow agents, Schaap’s dioxetane-based agents in particular the ones developed by Shabat and co-workers exhibit distinctive merits including facile synthesis and modification, bright afterglow luminescence in water, and convenience to build activatable afterglow probes. ,,− A number of activatable afterglow probes based on Schaap’s dioxetane by caging the phenol group with specific responsive moieties have been developed to visualize the targets such as cathepsins, hydrogen peroxide (H 2 O 2 ), and formaldehyde. ,, Recently, significant efforts have been contributed to red shift the Schaap’s dioxetane-based afterglow luminescence in a physiological environment, such as conjugation with conventional near-infrared (NIR) fluorophores, changing the substituent in the phenol core, and nanoparticle formulation. ,, Despite these exciting pioneer studies, there is still room left to improve the luminescent brightness and afterglow time in NIR region (>650 nm) for advanced in vivo applications.…”