Browse
Submit Data
Databases
API
Help

Dataset Information

0 Views

0 Connections

0 Citations

0 Reanalyses

0 Downloads

Omics score: 0

Confining energy migration in upconversion nanoparticles towards deep ultraviolet lasing.

ABSTRACT: Manipulating particle size is a powerful means of creating unprecedented optical properties in metals and semiconductors. Here we report an insulator system composed of NaYbF4:Tm in which size effect can be harnessed to enhance multiphoton upconversion. Our mechanistic investigations suggest that the phenomenon stems from spatial confinement of energy migration in nanosized structures. We show that confining energy migration constitutes a general and versatile strategy to manipulating multiphoton upconversion, demonstrating an efficient five-photon upconversion emission of Tm(3+) in a stoichiometric Yb lattice without suffering from concentration quenching. The high emission intensity is unambiguously substantiated by realizing room-temperature lasing emission at around 311 nm after 980-nm pumping, recording an optical gain two orders of magnitude larger than that of a conventional Yb/Tm-based system operating at 650 nm. Our findings thus highlight the viability of realizing diode-pumped lasing in deep ultraviolet regime for various practical applications.

SUBMITTER: Chen X

PROVIDER: S-EPMC4729831 | biostudies-other | 2016

REPOSITORIES: biostudies-other

ACCESS DATA

Json Xml

Similar Datasets

Manipulating energy migration within single lanthanide activator for switchable upconversion emissions towards bidirectional photoactivation.

Project description:Reliance on low tissue penetrating UV or visible light limits clinical applicability of phototherapy, necessitating use of deep tissue penetrating near-infrared (NIR) to visible light transducers like upconversion nanoparticles (UCNPs). While typical UCNPs produce multiple simultaneous emissions for unidirectional control of biological processes, programmable control requires orthogonal non-overlapping light emissions. These can be obtained through doping nanocrystals with multiple activator ions. However, this requires tedious synthesis and produces complicated multi-shell nanoparticles with a lack of control over emission profiles due to activator crosstalk. Herein, we explore cross-relaxation (CR), a non-radiative recombination pathway typically perceived as deleterious, to manipulate energy migration within the same lanthanide activator ion (Er3+) towards orthogonal red and green emissions, simply by adjusting excitation wavelength from 980 to 808 nm. These UCNPs allow programmable activation of two synergistic light-gated ion channels VChR1 and Jaws in the same cell to manipulate membrane polarization, demonstrated here for cardiac pacing.

| S-EPMC6764961 | biostudies-literature

Ultralarge anti-Stokes lasing through tandem upconversion.

Project description:Coherent ultraviolet light is important for applications in environmental and life sciences. However, direct ultraviolet lasing is constrained by the fabrication challenge and operation cost. Herein, we present a strategy for the indirect generation of deep-ultraviolet lasing through a tandem upconversion process. A core-shell-shell nanoparticle is developed to achieve deep-ultraviolet emission at 290 nm by excitation in the telecommunication wavelength range at 1550 nm. The ultralarge anti-Stokes shift of 1260 nm (~3.5 eV) stems from a tandem combination of distinct upconversion processes that are integrated into separate layers of the core-shell-shell structure. By incorporating the core-shell-shell nanoparticles as gain media into a toroid microcavity, single-mode lasing at 289.2 nm is realized by pumping at 1550 nm. As various optical components are readily available in the mature telecommunication industry, our findings provide a viable solution for constructing miniaturized short-wavelength lasers that are suitable for device applications.

| S-EPMC8873242 | biostudies-literature

Enhancing multiphoton upconversion through interfacial energy transfer in multilayered nanoparticles.

Project description:Photon upconversion in lanthanide-doped upconversion nanoparticles offers a wide variety of applications including deep-tissue biophotonics. However, the upconversion luminescence and efficiency, especially involving multiple photons, is still limited by the concentration quenching effect. Here, we demonstrate a multilayered core-shell-shell structure for lanthanide doped NaYF4, where Er3+ activators and Yb3+ sensitizers are spatially separated, which can enhance the multiphoton emission from Er3+ by 100-fold compared with the multiphoton emission from canonical core-shell nanocrystals. This difference is due to the excitation energy transfer at the interface between activator core and sensitizer shell being unexpectedly efficient, as revealed by the structural and temperature dependence of the multiphoton upconversion luminescence. Therefore, the concentration quenching is suppressed via alleviation of cross-relaxation between the activator and the sensitizer, resulting in a high quantum yield of up to 6.34% for this layered structure. These findings will enable versatile design of multiphoton upconverting nanoparticles overcoming the conventional limitation.

| S-EPMC7055352 | biostudies-literature

Low threshold lasing emissions from a single upconversion nanocrystal.

Project description:Cross-relaxation among neighboring emitters normally causes self-quenching and limits the brightness of luminescence. However, in nanomaterials, cross-relaxation could be well-controlled and employed for increasing the luminescence efficiency at specific wavelengths. Here we report that cross-relaxation can modulate both the brightness of single upconversion nanoparticles and the threshold to reach population inversion, and both are critical factors in producing the ultra-low threshold lasing emissions in a micro cavity laser. By homogenously coating a 5-μm cavity with a single layer of nanoparticles, we demonstrate that doping Tm3+ ions at 2% can facilitate the electron accumulation at the intermediate state of 3H4 level and efficiently decrease the lasing threshold by more than one order of magnitude. As a result, we demonstrate up-converted lasing emissions with an ultralow threshold of continuous-wave excitation of ~150 W/cm2 achieved at room temperature. A single nanoparticle can lase with a full width at half-maximum as narrow as ~0.45 nm.

| S-EPMC7708641 | biostudies-literature

Precisely Tailoring Upconversion Dynamics via Energy Migration in Core-Shell Nanostructures.

Project description:Upconversion emission dynamics have long been believed to be determined by the activator and its interaction with neighboring sensitizers. Herein this assumption is, however, shown to be invalid for nanostructures. We demonstrate that excitation energy migration greatly affects upconversion emission dynamics. "Dopant ions' spatial separation" nanostructures are designed as model systems and the intimate link between the random nature of energy migration and upconversion emission time behavior is unraveled by theoretical modelling and confirmed spectroscopically. Based on this new fundamental insight, we have successfully realized fine control of upconversion emission time behavior (either rise or decay process) by tuning the energy migration paths in various specifically designed nanostructures. This result is significant for applications of this type of materials in super resolution spectroscopy, high-density data storage, anti-counterfeiting, and biological imaging.

| S-EPMC5887923 | biostudies-literature

Dye Sensitization for Ultraviolet Upconversion Enhancement.

Project description:Upconversion nanocrystals that converted near-infrared radiation into emission in the ultraviolet spectral region offer many exciting opportunities for drug release, photocatalysis, photodynamic therapy, and solid-state lasing. However, a key challenge is the development of lanthanide-doped nanocrystals with efficient ultraviolet emission, due to low conversion efficiency. Here, we develop a dye-sensitized, heterogeneous core-multishelled lanthanide nanoparticle for ultraviolet upconversion enhancement. We systematically study the main influencing factors on ultraviolet upconversion emission, including dye concentration, excitation wavelength, and dye-sensitizer distance. Interestingly, our experimental results demonstrate a largely promoted multiphoton upconversion. The underlying mechanism and detailed energy transfer pathway are illustrated. These findings offer insights into future developments of highly ultraviolet-emissive nanohybrids and provide more opportunities for applications in photo-catalysis, biomedicine, and environmental science.

| S-EPMC8623389 | biostudies-literature

Triplet energy migration-based photon upconversion by amphiphilic molecular assemblies in aerated water.

Project description:A molecular self-assembly approach is developed to resolve an outstanding issue in triplet energy migration-based photon upconversion (TEM-UC), that is, air-stable TEM-UC in water. Amphiphilic cationic acceptor (emitter) molecules self-assemble in water via hydrophobic and hydrogen bonding interactions, with which anionic donor (sensitizer) molecules are integrated through electrostatic interactions. Triplet energy is quantitatively transferred from the excited donor to the acceptor, which is followed by effective triplet energy migration among the pre-organized acceptors. It leads to TTA and concomitant UC emission in water. The dense acceptor chromophore arrays with extended hydrogen bonding networks show efficient barrier properties against molecular oxygen, as demonstrated by the stable UC emission even in air-saturated water.

| S-EPMC6020542 | biostudies-literature

Higher-Order Multiphoton Absorption Upconversion Lasing Based on ZnO/ZnMgO Multiple Quantum Wells.

Project description:In the progress of nonlinear optics, multiphoton absorption (MPA) upconversion lasing enables many vital applications in bioimaging, three-dimensional optical data storage, and photodynamic therapy. Here, efficient four-photon absorption upconversion lasing from the ZnO/ZnMgO multiple quantum wells (MQWs) at room temperature is realized. Moreover, the MPA upconversion lasing and third-harmonic generation peak generated in the MQWs under the excitation of a femtosecond (fs) laser pulse were observed concurrently, and the essential differences between each other were studied comprehensively. Compared with the ZnO film, the upconversion lasing peak of the ZnO/ZnMgO MQWs exhibits a clear blue shift. In addition, the four-photon absorption upconversion photoluminescence (PL) intensity was enhanced in the MQWs/Au nanoparticles (NPs) by the metal-localized surface plasmons (LSPs). The work paves the way for short-wavelength lasers by taking advantage of the high stability and large exciton binding energy of the MQWs' structures.

| S-EPMC9457886 | biostudies-literature

Bright Infrared-to-Ultraviolet/Visible Upconversion in Small Alkaline Earth-Based Nanoparticles with Biocompatible CaF<sub>2</sub> Shells.

Project description:Upconverting nanoparticles (UCNPs) are promising candidates for photon-driven reactions, including light-triggered drug delivery, photodynamic therapy, and photocatalysis. Herein, we investigate the NIR-to-UV/visible emission of sub-15 nm alkaline-earth rare-earth fluoride UCNPs (M1-x Lnx F2+x, MLnF) with a CaF2 shell. We synthesize 8 alkaline-earth host materials doped with Yb3+ and Tm3+ , with alkaline-earth (M) spanning Ca, Sr, and Ba, MgSr, CaSr, CaBa, SrBa, and CaSrBa. We explore UCNP composition, size, and lanthanide doping-dependent emission, focusing on upconversion quantum yield (UCQY) and UV emission. UCQY values of 2.46 % at 250 W cm-2 are achieved with 14.5 nm SrLuF@CaF2 particles, with 7.3 % of total emission in the UV. In 10.9 nm SrYbF:1 %Tm3+ @CaF2 particles, UV emission increased to 9.9 % with UCQY at 1.14 %. We demonstrate dye degradation under NIR illumination using SrYbF:1 %Tm3+ @CaF2 , highlighting the efficiency of these UCNPs and their ability to trigger photoprocesses.

| S-EPMC8281583 | biostudies-literature

Enhancement of single upconversion nanoparticle imaging by topologically segregated core-shell structure with inward energy migration

Project description:Manipulating topological arrangement is a powerful tool for tuning energy migration in natural photosynthetic proteins and artificial polymers. Here, we report an inorganic optical nanosystem composed of NaErF4 and NaYbF4, in which topological arrangement enhanced upconversion luminescence. Three architectures are designed for considerations pertaining to energy migration and energy transfer within nanoparticles: outside-in, inside-out, and local energy transfer. The outside-in architecture produces the maximum upconversion luminescence, around 6-times brighter than that of the inside-out at the single-particle level. Monte Carlo simulation suggests a topology-dependent energy migration favoring the upconversion luminescence of outside-in structure. The optimized outside-in structure shows more than an order of magnitude enhancement of upconversion brightness compared to the conventional core-shell structure at the single-particle level and is used for long-term single-particle tracking in living cells. Our findings enable rational nanoprobe engineering for single-molecule imaging and also reveal counter-intuitive relationships between upconversion nanoparticle structure and optical properties. Manipulating topological arrangement is a powerful tool for tuning the energy migration in molecular systems and inorganic materials. Here, authors synthesize NaErF4 and NaYbF4 upconversion nanoparticles with different architectures and demonstrate topology-dependent enhancement of upconversion luminescence, with up to an order of magnitude increase in brightness compared to conventional core-shell architectures.

| S-EPMC9546905 | biostudies-literature

OmicsDI is part of the ELIXIR infrastructure

OmicsDI is an Elixir interoperability service. Learn more ›

Tweets

OmicsDI Databases

PRIDE
PeptideAtlas
MassIVE
JPOST Repository
Physiome Model Repository

EGA
EVA
ENA
LINCS
PAXDB
Cell Collective

MetaboLights
Metabolomics Workbench
MetabolomeExpress
GNPS
BioModels
FAIRDOMHub

ArrayExpress
dbGaP
ExpressionAtlas
GEO
NODE

Information

Databases
Help
API
Contact us
Code on GitHub
Terms of use
Submit Data