A new type of core-shell upconversion nanoparticles which can be effectively excited at 795 nm has been designed and synthesized through spatially confined doping of neodymium (Nd(3+)) ions. The use of Nd(3+) ions as sensitizers facilitates the energy transfer and photon upconversion of a series of lanthanide activators (Er(3+), Tm(3+), and Ho(3+)) at a biocompatible excitation wavelength (795 nm) and also significantly minimizes the overheating problem associated with conventional 980 nm excitation. Importantly, the core-shell design enabled high-concentration doping of Nd(3+) (~0 mol %) in the shell layer and thus markedly enhanced the upconversion emission from the activators, providing highly attractive luminescent biomarkers for bioimaging without autofluorescence and concern of overheating.
Due to their layered structure, two-dimensional Ruddlesden-Popper perovskites (RPPs), composed of multiple organic/inorganic quantum wells, can in principle be exfoliated down to few and single layers. These molecularly thin layers are expected to present unique properties with respect to the bulk counterpart, due to increased lattice deformations caused by interface strain. Here, we have synthesized centimetre-sized, pure-phase single-crystal RPP perovskites (CH(CH)NH)(CHNH)PbI (n = 1-4) from which single quantum well layers have been exfoliated. We observed a reversible shift in excitonic energies induced by laser annealing on exfoliated layers encapsulated by hexagonal boron nitride. Moreover, a highly efficient photodetector was fabricated using a molecularly thin n = 4 RPP crystal, showing a photogain of 10 and an internal quantum efficiency of ~34%. Our results suggest that, thanks to their dynamic structure, atomically thin perovskites enable an additional degree of control for the bandgap engineering of these materials.
We demonstrate that the intrinsic properties of monolayer graphene allow it to act as a more effective saturable absorber for mode-locking fiber lasers when compared to multilayer graphene. The absorption of monolayer graphene can be saturated at lower excitation intensity compared to multilayer graphene, graphene with wrinkle-like defects, or functionalized graphene. Monolayer graphene has a remarkably large modulation depth of 65.9%, whereas the modulation depth of multilayer graphene is greatly reduced due to nonsaturable absorption and scattering loss. Picosecond ultrafast laser pulses (1.23 ps) can be generated using monolayer graphene as a saturable absorber. Due to the ultrafast relaxation time, larger modulation depth and lower scattering loss of monolayer graphene, it performs better than multilayer graphene in terms of pulse shaping ability, pulse stability, and output energy.
Molecular rotors have played an important role in recent materials chemistry. Although several studies on functional materials containing molecular rotors have been reported for fluorescence sensing, this concept has yet to be realized in two-dimensional (2D) materials. Here we report the preparation of all-carbon, π-conjugated 2D porous organic nanosheets, named NUS-24, which contain flexible tetraphenylethylene (TPE) units as the molecular rotors. NUS-24 nanosheets exhibit high stability, large lateral size, and ultrathin thickness (2–5 nm). The dynamic TPE rotors exposed on the surface of NUS-24 nanosheets can be restricted in the aggregated state with different water fractions, which is reminiscent of the aggregation-induced emission mechanism, thereby leading to the size-selective turn-on fluorescence by volatile organic compounds. Significantly, the ultrathin 2D nanosheets and its composite membranes show much higher sensitivity and selectivity toward Fe3+ ions and nitro-containing compounds sensing, suggesting their potential applications in explosive detection and environmental monitoring.
Hypochlorous acid (HOCl), as a highly potent oxidant, is well-known as a key "killer" for pathogens in the innate immune system. Recently, mounting evidence indicates that intracellular HOCl plays additional important roles in regulating inflammation and cellular apoptosis. However, the organelle(s) involved in the distribution of HOCl remain unknown, causing difficulty to fully exploit its biological functions in cellular signaling pathways and various diseases. One of the main reasons lies in the lack of effective chemical tools to directly detect HOCl at subcellular levels due to low concentration, strong oxidization, and short lifetime of HOCl. Herein, the first two-photon fluorescent HOCl probe (TP-HOCl 1) and its mitochondria- (MITO-TP) and lysosome- (LYSO-TP) targetable derivatives for imaging mitochondrial and lysosomal HOCl were reported. These probes exhibit fast response (within seconds), good selectivity, and high sensitivity (<20 nM) toward HOCl. In live cell experiments, both probes MITO-TP and LYSO-TP were successfully applied to detect intracellular HOCl in corresponding organelles. In particular, the two-photon imaging of MITO-TP and LYSO-TP in murine model shows that higher amount of HOCl can be detected in both lysosome and mitochondria of macrophage cells during inflammation condition. Thus, these probes could not only help clarify the distribution of subcellular HOCl, but also serve as excellent tools to exploit and elucidate functions of HOCl at subcellular levels.
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