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Sphingosine-1-phosphate (S1P) is a bioactive sphingo-lipid with a broad range of activities coupled to its role in G-protein coupled receptor signalling. Monitoring of both intra and extra cellular levels of this lipid is challenging due to its low abundance and lack of robust affinity assays or sensors. We here report on fluorescent sensory core-shell molecularly imprinted polymer (MIP) particles responsive to near physiologically relevant levels of S1P and the S1P receptor modulator fingolimod phosphate (FP) in spiked human serum samples. Imprinting was achieved using the tetrabutylammonium (TBA) salt of FP or phosphatidic acid (DPPA·Na) as templates in combination with a polymerizable nitrobenzoxadiazole (NBD)-urea monomer with the dual role of capturing the phospho-anion and signalling its presence. The monomers were grafted from ca 300 nm RAFT-modified silica core particles using ethyleneglycol dimethacrylate (EGDMA) as crosslinker resulting in 10-20 nm thick shells displaying selective fluorescence response to the targeted lipids S1P and DPPA in aqueous buffered media. Potential use of the sensory particles for monitoring S1P in serum was demonstrated on spiked serum samples, proving a linear range of 18-60 µM and a detection limit of 5.6 µM, a value in the same range as the plasma concentration of the biomarker.

Our understanding of molecules has stagnated at a single quantum system, with atoms as Newtonian particles and electrons as quantum particles. Here, however, we reveal that both atoms and electrons in a molecule are quantum particles, and their quantum–quantum interactions create a previously unknown, newfangled molecular property—supracence. Molecular supracence is a phenomenon in which the molecule transfers its potential energy from quantum atoms to photo-excited electrons so that the emitted photon has more energy than that of the absorbed one. Importantly, experiments reveal such quantum energy exchanges are independent of temperature. When quantum fluctuation results in absorbing low-energy photons, yet still emitting high-energy photons, supracence occurs. This report, therefore, reveals novel principles governing molecular supracence via experiments that were rationalized by full quantum (FQ) theory. This advancement in understanding predicts the super-spectral resolution of supracence, and molecular imaging confirms such innovative forecasts using closely emitting rhodamine 123 and rhodamine B in living cell imaging of mitochondria and endosomes. [ABSTRACT FROM AUTHOR]

Monitoring multiple molecular probes simultaneously establishes their correlations and reveals the holistic mechanism. Current fluorescence imaging, however, is limited to about four colors because of typically circa 100‐nm spectral width. Herein, we show that molecular supracence imparts superior spectral resolution, resolving eight colors in 300‐nm width, about 37.5‐nm per color. A recently discovered light‐molecule interacting phenomenon, supracence only measures molecular emission above its excitation energy due to entanglement between atomic quantum system and electronic quantum system. As such, supracence takes advantage of sharp spectral edge of a single pathway and excitation specificity to produce narrow bands, whereas fluorescence has to deal with multiple pathways spilling out low‐energy long tail, that causes poor resolution. Thus, supracence enables myriad innovative molecular spectroscopy and microscopic imaging with profound impact broadly. [ABSTRACT FROM AUTHOR]

The currently understood principles about light–molecule interactions are limited, and thus scientific scope beyond current theories is rarely harvested. Herein we demonstrate supracence phenomena, in which the emitted photons have more energy than the absorbed photons. The extra energy comes from couplings of the absorbed and emitted photon to molecular phonons, whose potentials are constantly exchanging with molecular quantum energy and the environment. Thus, supracence is a linear optical process rather than a nonlinear optical process, such as second harmonic generation. Because supracence results in cooled molecular phonons and thus cooled molecules, behavior opposite to that of hot fluorescing emitters is expected. This report reveals certain supracence principles while contrasting fluorescence with supracence in high‐resolution imaging. [ABSTRACT FROM AUTHOR]

Folding–unfolding imparts fluorescence dual color switching, thus a novel concept to switch fluorescence between two distinct colors while avoiding traditional bond rupturing and bond forming in photoswitching. Because folding and unfolding minimize the wear and tear on molecular structures, the new systems have excellent reversibility and fatigue resistance. [ABSTRACT FROM AUTHOR]

The fluorescence brightness of a molecular probe determines whether it can be effectively measured and its water solubility dictates if it can be applied in real-world biological systems. However, molecules brighter than the most efficient fluorescent dyes or particles brighter than quantum dots are hard to come by, especially when they must also be soluble in water. In this report, chromophoric phosphoramidites are used in a solid-state synthesis to construct functional dendrimers. When highly twisted chromophores are chosen and the proper spacers and dendrons are introduced, the resultant dendrimers emit exceptionally bright fluorescence. Chromophores, spacers, and dendrons are stitched together by efficient phosphoramidite reagents, which afford high-yield water-soluble phosphodiester linkages after deprotection. The resulting water-soluble dendrimers are exceptionally bright. [ABSTRACT FROM AUTHOR]

The article offers information on a study concerning fluorescent sensory microparticles which consist of molecularly imprinted polymer (MIP) and silica core. It says that the N-carbobenzyloxy-l-phenylalanine(Cbz-l-Phe or Z-l-Phe, Scheme 1) was used a template and the fluorescent monomer was developed using nitrobenzoxadiazole (NBD) fluorophore. The integration of the MIP on silica microparticles makes the assay response times and the handling of the sensor particles straightforward.

We demonstrate experimentally the Doppler cooling of 40Ca+ ions using the s1/2 → D3/2 electric quadrupole transition, in which the scattering light that is much different from the exciting light makes it possible to collect background-free fluorescence. The idea excluding 397nm excitation has the advantage of high-sensitivity detection and only employs lasers in red and infrared wavelengths, which should be practical for trapped-ion quantum information processing. [ABSTRACT FROM AUTHOR]

Sun-induced chlorophyll fluorescence (SIF) provides a new method for monitoring vegetation photosynthesis from space and has been widely used to estimate gross primary productivity (GPP). However, the ability of SIF obtained from the Orbital Carbon Observatory 2 (OCO-2 SIF) and Global Ozone Monitoring Experiment-2 (GOME-2) to estimate GPP in the cold and arid region of Heihe River Basin remains unclear because previous comparisons were insufficient. Here, we choose maize and alpine meadow to evaluate the performance of SIF obtained by OCO-2 and GOME-2 in GPP estimations. The results of this study show that daily SIF757 had stronger correlations with daily tower GPP than daily SIF771, and the correlation between daily SIF757 and daily tower GPP was stronger than the correlation between 16-d averaged SIF740 and 16-d averaged tower GPP. The 16-d averaged absorbed photosynthetically active radiation (APAR) and reconstructed sun-induced fluorescence (RSIF) had the strongest linear correlations with 16-d averaged tower GPP. GPP_VPM and GPP_RSIF exhibited the best performance in GPP estimation, closely followed by GPP_SIF757, then GPP_SIF771 and GPP_ SIF740. We also found that the robustness of the correlation coefficients of OCO-2 SIF with GOME-2 SIF was highly dependent on the size of their spatial footprint overlaps, indicating that the spatial differences between OCO-2 and GOME-2 footprints contribute to the differences in GPP estimates between OCO-2 and GOME-2. In addition, the differences of viewing zenith angle (VZA), cloud contamination, scale effects, and environmental scalars (Tscalar × Wscalar) can result in differences between OCO-2 SIF and GOME-2 SIF. [ABSTRACT FROM AUTHOR]