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Photon avalanche (PA) is a highly nonlinear mode of upconversion that is characterized by 100–1000-fold increase in luminescence intensity upon minute increments of pumping power. The practical realization of numerous possible nano-bio-technology applications utilizing the PA phenomenon will require information on its susceptibility to the material volume and surface. Here, these parameters are investigated via experimental and theoretical PA. The two-color, highly nonlinear PA emission at 475 and 800 nm is clearly observed in bulk single crystal, individual microcrystals, and ensembles of colloidal core and core–shell nanoparticles of LiYF4 host doped with either 3 or 8% of thulium ions. The properties of PA emission, such as PA nonlinearity, PA gain, PA intensity, and luminescence kinetics in these materials show dependence on crystal volume and surface quenching. Theoretical simulations provide understanding of key physical processes that influence PA performance. Moreover, photon avalanche single beam super-resolution imaging is realized for the first time in 3% Tm3+ doped LiYF4 core–shell nanoparticles. The obtained insights and predictions form a solid background for further development and applications of new optimized PA materials.

Avalanche phenomena use steeply nonlinear dynamics to generate disproportionately large responses from small perturbations, and are found in a multitude of events and materials1. Photon avalanching enables technologies such as optical phase-conjugate imaging2, infrared quantum counting3 and efficient upconverted lasing4-6. However, the photon-avalanching mechanism underlying these optical applications has been observed only in bulk materials and aggregates6,7, limiting its utility and impact. Here we report the realization of photon avalanching at room temperature in single nanostructures-small, Tm3+-doped upconverting nanocrystals-and demonstrate their use in super-resolution imaging in near-infrared spectral windows of maximal biological transparency. Avalanching nanoparticles (ANPs) can be pumped by continuous-wave lasers, and exhibit all of the defining features of photon avalanching, including clear excitation-power thresholds, exceptionally long rise time at threshold, and a dominant excited-state absorption that is more than 10,000 times larger than ground-state absorption. Beyond the avalanching threshold, ANP emission scales nonlinearly with the 26th power of the pump intensity, owing to induced positive optical feedback in each nanocrystal. This enables the experimental realization of photon-avalanche single-beam super-resolution imaging7 with sub-70-nanometre spatial resolution, achieved by using only simple scanning confocal microscopy and without any computational analysis. Pairing their steep nonlinearity with existing super-resolution techniques and computational methods8-10, ANPs enable imaging with higher resolution and at excitation intensities about 100 times lower than other probes. The low photon-avalanching threshold and excellent photostability of ANPs also suggest their utility in a diverse array of applications, including sub-wavelength imaging7,11,12 and optical and environmental sensing13-15.

Förster Resonance Energy Transfer (FRET) between donor (D) and acceptor (A) molecules is a phenomenon commonly exploited to study or visualize biological interactions at the molecular level. However, commonly used organic D and A molecules often suffer from photobleaching and spectral bleed-through, and their spectral properties hinder quantitative analysis. Lanthanide-doped upconverting nanoparticles (UCNPs) as alternative D species offer significant improvements in terms of photostability, spectral purity and background-free luminescence detection, but they bring new challenges related to multiple donor ions existing in a single large size UCNP and the need for nanoparticle biofunctionalization. Considering the relatively short Förster distance (typically below 5-7 nm), it becomes a non-trivial task to assure sufficiently strong D-A interaction, which translates directly to the sensitivity of such bio-sensors. In this work we propose a solution to these issues, which employs the photon avalanche (PA) phenomenon in lanthanide-doped materials. Using theoretical modelling, we predict that these PA systems would be highly susceptible to the presence of A and that the estimated sensitivity range extends to distances 2 to 4 times longer (i.e. 10-25 nm) than those typically found in conventional FRET systems. This promises high sensitivity, low background and spectral or temporal biosensing, and provides the basis for a radically novel approach to combine luminescence imaging and self-normalized bio-molecular interaction sensing.

Upconverting FRET assays show complex behavior of luminescence kinetics and spectra for various NPs chemical architectures and excitation schemes.

Lanthanide-doped heterostructured nanocomposites were developed by using cation exchange method and successfully applied toward advanced optical anti-counterfeiting and information storage

Luminescence thermometers exhibiting ratiometric response in their emission spectrum are widely investigated but to obtain two‐dimensional measurements, either the emission spectrum must be slowly scanned over the area of interest or the emission decomposed using two separate detector arrays with spectral filters. Here, the authors propose to exploit instead an excitation‐spectrum based ratiometric response. In AVO4 (A = Lu, Y, Gd, La) nanocrystals doped with Eu3+, the 1 E(1 T 1)→ 1 B 2(1 T 2) absorption band is thermally enhanced with respect to the 1 A 2(1 T 1)→ 1 B 2(1 T 2) of the V5+ ion. When observing the Eu3+ emission as a result of (VO4)3− to Eu3+ charge transfer, the ratio of intensities recorded upon two different excitation wavelengths is temperature dependent. This response is exploited for transient 2‐dimensional temperature imaging using two ultraviolet light emitting diodes (LEDs) for excitation, which are subsequently pulsed, while recording the emission on a single camera. As a demonstration, a YVO4:Eu3+ coated metal plate is subjected to localised heating by a flame. Thanks to the efficient excitation and signal collection, an accuracy of 0.6 °C and a precision of 1.5 °C are achieved at a resolution of 160 μm and a repetition rate of 2.5 Hz, all with peak LED powers below 1 mW and a single low‐frame‐rate camera.

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Photon avalanche (PA) is an anti-Stokes process in which lanthanide-doped materials can emit upconverted luminescence in a highly non-linear manner. PA was recently demonstrated in thulium (III)-doped NaYF4 colloidal nanoparticles at room temperature, with reported nonlinearities (power factors) exceeding 30. Importantly, good rate-equations model agreement with experimental data was achieved, which enabled the derivation of the rates of energy transfer processes, providing a foundation for further developments and optimization of similar materials and their new applications. In order to apply PA to, for example, luminescent (nano)thermometry, we need to have a better understanding of the susceptibility of photon avalanche phenomenon to temperature variation. For this purpose, we study how the temperature and energy-gap-dependent multiphonon relaxation and inter-ionic energy transfer processes affect the photon avalanche behavior. As a result of these simulations, high susceptibility to temperature changes with relative sensitivity over 40 %⋅K−1 above 400 K (up to 15 %⋅K−1at room temperature) was noted. Moreover, by knocking-out the temperature dependences of the individual processes involved in the PA, we found the temperature dependence of the multiphonon relaxation of the intermediate F34 state to the ground state to be the primary one responsible for the simulated temperature dependence of PA emission. This process is observed to be more significant than temperature dependencies of energy looping and phonon assisted ground state non-resonant absorption. Although there are challenges with a single band technique, these results still show the great potential, especially when used ratiometrically with different excitation wavelengths.

Vitamin K, especially its K2 form, is considered to be a protective factor against developing vascular changes and bone lesions that are common complications in kidney transplant (KTx) recipients. There is a growing number of studies showing that KTx patients are at risk of vitamin K deficiency. The aim of this study was to evaluate the intake of vitamin K1 and K2 in the diet of patients in the late period after KTx. During a routine visit at one outpatient transplantation clinic in Central Europe, a diet survey questionnaire was filled in by 151 clinically stable KTx recipients and compared with medical history, anthropometric measurements and laboratory tests. Mean vitamin K1 intake was 120.9 ± 49 μg/day and vitamin K2 (MK, menaquinone) intake 28.69 ± 11.36 μg/day, including: MK-4: 25.9 ± 9.9 μg/day; MK-5: 0.1 ± 0.2 μg/day; MK-6: 0.2 ± 0.4 μg/day; MK-7: 0.2 ± 0.23 μg/day; MK-8: 1 ± 1.9 μg/day; MK-9: 0.9 ± 2.3 μg/day; and MK-10: 0.2 ± 0.5 μg/day. Our study showed that KTx recipients’ diets contained adequate amounts of vitamin K1, whereas the intake of vitamin K2 seemed insufficient.

Abstract Lanthanide-doped upconversion nanoparticles (UCNPs) are capable of converting near-infra-red excitation into visible and ultraviolet emission. Their unique optical properties have advanced a broad range of applications, such as fluorescent microscopy, deep-tissue bioimaging, nanomedicine, optogenetics, security labelling and volumetric display. However, the constraint of concentration quenching on upconversion luminescence has hampered the nanoscience community to develop bright UCNPs with a large number of dopants. This review surveys recent advances in developing highly doped UCNPs, highlights the strategies that bypass the concentration quenching effect, and discusses new optical properties as well as emerging applications enabled by these nanoparticles.

For more than two centuries, Muslims have been retelling different stories about the origin of their call to prayer. While the converging details of these narratives offer a glimpse of Muslim cultural memory and its preservation, the diverging elements reflect different mechanisms that facilitate the adaption of this cultural memory to new contexts and concerns. Based on the work of Jan Assmann, the present study explores how Muslims conserved and adapted their cultural memory to keep their common identity and expand their diversity following distinctive religious, political, or personal forms of belongings. The narratives concerned with the origin of the Islamic call to prayer and preserved in various written text collections offer a fertile ground to analyze how this part of Muslim cultural memory became the vehicle of a permanent but adaptable Muslim identity.