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1.
J Phys Chem Lett ; 15(9): 2606-2615, 2024 Mar 07.
Artículo en Inglés | MEDLINE | ID: mdl-38420927

RESUMEN

We investigate the intricate relationship among temperature, pH, and Brownian velocity in a range of differently sized upconversion nanoparticles (UCNPs) dispersed in water. These UCNPs, acting as nanorulers, offer insights into assessing the relative proportion of high-density and low-density liquid in the surrounding hydration water. The study reveals a size-dependent reduction in the onset temperature of liquid-water fluctuations, indicating an augmented presence of high-density liquid domains at the nanoparticle surfaces. The observed upper-temperature threshold is consistent with a hypothetical phase diagram of water, validating the two-state model. Moreover, an increase in pH disrupts the organization of water molecules, similar to external pressure effects, allowing simulation of the effects of temperature and pressure on hydrogen bonding networks. The findings underscore the significance of the surface of suspended nanoparticles for understanding high- to low-density liquid fluctuations and water behavior at charged interfaces.

2.
Chem Mater ; 35(17): 7229-7238, 2023 Sep 12.
Artículo en Inglés | MEDLINE | ID: mdl-37719033

RESUMEN

The unique tunable properties of glasses make them versatile materials for developing numerous state-of-the-art optical technologies. To design new optical glasses with tailored properties, an extensive understanding of the intricate correlation between their chemical composition and physical properties is mandatory. By harnessing this knowledge, the full potential of vitreous matrices can be unlocked, driving advancements in the field of optical sensors. We herein demonstrate the feasibility of using fluoride phosphate glasses co-doped with trivalent praseodymium (Pr3+) and ytterbium (Yb3+) ions for temperature sensing over a broad range of temperatures. These glasses possess high chemical and thermal stability, working as luminescent primary thermometers that rely on the thermally coupled levels of Pr3+ that eliminate the need for recurring calibration procedures. The prepared glasses exhibit a relative thermal sensitivity and uncertainty at a temperature of 1.0% K-1 and 0.5 K, respectively, making them highly competitive with the existing luminescent thermometers. Our findings highlight that Pr3+-containing materials are promising for developing cost-effective and accurate temperature probes, taking advantage of the unique versatility of these vitreous matrices to design the next generation of photonic technologies.

3.
Front Bioeng Biotechnol ; 9: 617328, 2021.
Artículo en Inglés | MEDLINE | ID: mdl-33859978

RESUMEN

Photonic materials featuring simultaneous iridescence and light emission are an attractive alternative for designing novel optical devices. The luminescence study of a new optical material that integrates light emission and iridescence through liquid crystal self-assembly of cellulose nanocrystal-template silica approach is herein presented. These materials containing Rhodamine 6G were obtained as freestanding composite films with a chiral nematic organization. The scanning electron microscopy confirms that the cellulose nanocrystal film structure comprises multi-domain Bragg reflectors and the optical properties of these films can be tuned through changes in the relative content of silica/cellulose nanocrystals. Moreover, the incorporation of the light-emitting compound allows a complementary control of the optical properties. Overall, such findings demonstrated that the photonic structure plays the role of direction-dependent inner-filter, causing selective suppression of the light emitted with angle-dependent detection.

4.
J Phys Chem Lett ; 11(16): 6704-6711, 2020 Aug 20.
Artículo en Inglés | MEDLINE | ID: mdl-32672973

RESUMEN

Liquid water, despite its simple molecular structure, remains one of the most fascinating and complex substances. Most notably, many questions continue to exist regarding the phase transitions and anomalous properties of water, which are subtle to observe experimentally. Here, we report a sharp transition in water at 330 K unveiled through experimental measurements of the instantaneous Brownian velocity of NaYF4:Yb/Er upconversion nanoparticles in water. Our experimental investigations, corroborated by molecular dynamics simulations, elucidate a geometrical phase transition where a low-density liquid (LDL) clusters become percolated below 330 K. Around this critical temperature, we find the sizes of the LDL clusters to be similar to those of the nanoparticles, confirming the role of the upconversion nanoparticle as a powerful ruler for measuring the extensiveness of the LDL hydrogen-bond network and nanometer-scale spatial changes (20-100 nm) in liquids. Additionally, a new order parameter that unequivocally classifies water molecules into two local geometric states is introduced, providing a new tool for understanding and modeling water's many anomalous properties and phase transitions.

5.
Materials (Basel) ; 12(6)2019 Mar 21.
Artículo en Inglés | MEDLINE | ID: mdl-30901813

RESUMEN

Mesoporous silica nanoparticles prepared by organic template-driven synthesis have been successfully explored as carriers of the drug-derivate green luminescent complex of terbium (III) with the nonsteroidal anti-inflammatory drug ketoprofen. The terbium (III) complex was synthesized by reacting ketoprofen sodium salt with terbium (III) chloride, which was further adsorbed onto the surface of mesoporous nanoparticles with a mean particle size of 47 ± 4 nm and pore size of 11 nm. The incorporation of the complex into mesoporous silica nanoparticles was tracked by the decrease in the surface area and pore size of the nanoparticles, and successfully demonstrated by substantial changes in the adsorption isotherms and thermal and vibrational spectroscopy results. The cytotoxicity assay and confocal microscopy have shown that the novel luminescent nanohybrid presents high cell viability and the characteristic terbium (III) emission can be assessed through two-photon excitation, which paves the way for bioimaging applications in nanomedicine.

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