Influence on the Apparent Luminescent Lifetime of Rare-Earth Upconversion Nanoparticles by Quenching the Sensitizer's Excited State for Hypochlorous Acid Detection and Bioimaging.

Lanthanide-ion-doped upconversion materials have been widely used in biological detection, bioimaging, displays, and anticounterfeiting due to their abilities of real-time readings, high spatial resolution, and deep tissue penetration. The typically long fluorescence lifetimes of rare-earth nanoparticles, in the microsecond to millisecond range, make them useful in interference-free lifetime detection imaging. Most detection systems are accompanied by fluorescence resonance energy transfer (FRET), in which the lifetime of the luminescence center can be used as a signal to reveal the degree of FRET. Due to the complex energy level structure and complex energy transfer processes, the apparent lifetimes of upconversion nanoparticles (UCNPs) do not simply equal the decay time of the corresponding energy level, inducing an insignificant lifetime change in the upconversion detection system. In this study, the relationship between the apparent luminescence lifetime of upconversion and the decay rate of each energy level was studied by numerical simulations. It was proved that the apparent lifetime of the emission at 540 nm was mainly affected by the decay rate of Yb3+. We then constructed a nanocomposite with Rh1000 fluorophores loaded onto the surface of UCNPs to quench the sensitizer Yb3+. We found that the lifetime of the emission at 540 nm from Er3+ was affected to a large extent by the number of attached Rh1000 molecules, proving the greater influence on the apparent luminescent lifetime of Er3+ at 540 nm caused by quenching the Yb3+ excited state. The qualitative detection of hypochlorous acid (HClO) in vivo was also achieved using the luminescent lifetime as the signal.

Ln3+-doped nanoparticles with enhanced NIR-II luminescence for lighting up blood vessels in mice.

Probes functioning in the second near-infrared window (1000-1700 nm, NIR-II) exhibit higher resolution and diminished auto-fluorescence compared to those in the traditional NIR region (700-950 nm). Here, we designed and synthesized rare earth ion doped probes with core/shell/shell structures and bright luminescence in the NIR-II region excited at 808 nm. With the doping of Ce3+ ions, the emission intensity of Er3+ at 1530 nm increased 10 times, while the upconversion luminescence decreased to less than 1%. After being modified with polyacrylic acid and polyethylene glycol, the as-obtained water-soluble probe exhibits continuous high-resolution for distinguishing 0.25 mm blood vessels even 10 h after injection. Noteworthily, the imaging of tumors was achieved by injecting the probe, indicating that the designed NIR-II probe has sufficient brightness and the ability to passively target tumor tissue.

Near-Infrared Lanthanide-Doped Nanoparticles for a Low Interference Lateral Flow Immunoassay Test.

The lateral flow immunoassay test (LFT), as a method of a point of care test, is widely used in disease diagnosis, food security, and environment observation due to its portability and testing rapidity. A fluorescence lateral flow immunoassay was developed recently to enhance the sensitivity and accuracy of the LFT. However, for most fluorescence reporters, their emission and excitation wavelengths are located in the ultraviolet or visible region. Serum or whole blood significantly absorbs and scatters light of this region, and this will result in background signal interference. In this study, we replace traditional fluorescence reporters with near-infrared lanthanide-doped nanoparticles (NIR-RENPs) to establish a NIR-LFT platform. Blood and other biological samples scatter and absorb less near-infrared light than visible light, and the autofluorescence of biological samples is rarely located in this region. Therefore, using NIR light as a signal can diminish the interference of background noise and suffer from less signal attenuation. In addition, compared with commonly used NIR organic dye, NIR-RENPs have better stability. It is promising that lateral flow immunoassays based on NIR lanthanide-doped nanoparticles are able to acquire a lower detection limit and better accuracy, and they are more suitable for application in commercial settings.