Particle detection through the quantum counter concept in YAG:Er3+^{3+}

We report about a novel scheme for particle detection based on the infrared quantum counter concept. Its operation consists of a two-step excitation process of a four level system, that can be realized in rare earth-doped crystals when a cw pump laser is tuned to the transition from the second to the fourth level. The incident particle raises the atoms of the active material into a low lying, metastable energy state, triggering the absorption of the pump laser to a higher level. Following a rapid non-radiative decay to a fluorescent level, an optical signal is observed with a conventional detectors. In order to demonstrate the feasibility of such a scheme, we have investigated the emission from the fluorescent level $^4$S$_{3/2}$ (540 nm band) in an Er$^{3+}$-doped YAG crystal pumped by a tunable titanium sapphire laser when it is irradiated with 60 keV electrons delivered by an electron gun. We have obtained a clear signature this excitation increases the $^{4}I_{13/2}$ metastable level population that can efficiently be exploited to generate a detectable optical signal

A 25 micron-thin microscope for imaging upconverting nanoparticles with NIR-I and NIR-II illumination.

Rationale: Intraoperative visualization in small surgical cavities and hard-to-access areas are essential requirements for modern, minimally invasive surgeries and demand significant miniaturization. However, current optical imagers require multiple hard-to-miniaturize components including lenses, filters and optical fibers. These components restrict both the form-factor and maneuverability of these imagers, and imagers largely remain stand-alone devices with centimeter-scale dimensions. Methods: We have engineered INSITE (Immunotargeted Nanoparticle Single-Chip Imaging Technology), which integrates the unique optical properties of lanthanide-based alloyed upconverting nanoparticles (aUCNPs) with the time-resolved imaging of a 25-micron thin CMOS-based (complementary metal oxide semiconductor) imager. We have synthesized core/shell aUCNPs of different compositions and imaged their visible emission with INSITE under either NIR-I and NIR-II photoexcitation. We characterized aUCNP imaging with INSITE across both varying aUCNP composition and 980 nm and 1550 nm excitation wavelengths. To demonstrate clinical experimental validity, we also conducted an intratumoral injection into LNCaP prostate tumors in a male nude mouse that was subsequently excised and imaged with INSITE. Results: Under the low illumination fluences compatible with live animal imaging, we measure aUCNP radiative lifetimes of 600 μs - 1.3 ms, which provides strong signal for time-resolved INSITE imaging. Core/shell NaEr0.6Yb0.4F4 aUCNPs show the highest INSITE signal when illuminated at either 980 nm or 1550 nm, with signal from NIR-I excitation about an order of magnitude brighter than from NIR-II excitation. The 55 μm spatial resolution achievable with this approach is demonstrated through imaging of aUCNPs in PDMS (polydimethylsiloxane) micro-wells, showing resolution of micrometer-scale targets with single-pixel precision. INSITE imaging of intratumoral NaEr0.8Yb0.2F4 aUCNPs shows a signal-to-background ratio of 9, limited only by photodiode dark current and electronic noise. Conclusion: This work demonstrates INSITE imaging of aUCNPs in tumors, achieving an imaging platform that is thinned to just a 25 μm-thin, planar form-factor, with both NIR-I and NIR-II excitation. Based on a highly paralleled array structure INSITE is scalable, enabling direct coupling with a wide array of surgical and robotic tools for seamless integration with tissue actuation, resection or ablation

The route toward a diode-pumped 1-W erbium 3-µm fiber laser

A rate-equation analysis of the erbium 3-um ZBLAN fiber laser is performed. The computer calculation includes the longitudinal spatial resolution of the host material. It considers ground-state bleaching, excited-state absorption (ESA), interionic processes, lifetime quenching by co-doping, and stimulated emission at 2.7 um and 850 nm. State-of-the-art technology including double-clad diode pumping is assumed in the calculation. Pump ESA is identified as the major problem of this laser. With high Er3+ concentration, suitable Pr3+ co-doping, and low pump density, ESA is avoided and a diode-pumped erbium 3-um ZBLAN laser is predicted which is capable of emitting a transversely single-mode output power of 1.0 W when pumped with 7-W incident power at 800 nm. The corresponding output intensity which is relevant for surgical applications will be in the range of 1.8 MW/cm2. Compared to Ti:sapphire-pumped cascade-lasing regimes, the proposed approach represents a strong decrease of the requirements on mirror coatings, cavity alignment, and especially pump intensity. Of the possible drawbacks investigated in the simulation, only insufficient lifetime quenching is found to have a significant influence on laser performance

Sub-20 nm Core-Shell-Shell Nanoparticles for Bright Upconversion and Enhanced Förster Resonant Energy Transfer.

Upconverting nanoparticles provide valuable benefits as optical probes for bioimaging and Förster resonant energy transfer (FRET) due to their high signal-to-noise ratio, photostability, and biocompatibility; yet, making nanoparticles small yields a significant decay in brightness due to increased surface quenching. Approaches to improve the brightness of UCNPs exist but often require increased nanoparticle size. Here we present a unique core-shell-shell nanoparticle architecture for small (sub-20 nm), bright upconversion with several key features: (1) maximal sensitizer concentration in the core for high near-infrared absorption, (2) efficient energy transfer between core and interior shell for strong emission, and (3) emitter localization near the nanoparticle surface for efficient FRET. This architecture consists of β-NaYbF4 (core) @NaY0.8-xErxGd0.2F4 (interior shell) @NaY0.8Gd0.2F4 (exterior shell), where sensitizer and emitter ions are partitioned into core and interior shell, respectively. Emitter concentration is varied (x = 1, 2, 5, 10, 20, 50, and 80%) to investigate influence on single particle brightness, upconversion quantum yield, decay lifetimes, and FRET coupling. We compare these seven samples with the field-standard core-shell architecture of β-NaY0.58Gd0.2Yb0.2Er0.02F4 (core) @NaY0.8Gd0.2F4 (shell), with sensitizer and emitter ions codoped in the core. At a single particle level, the core-shell-shell design was up to 2-fold brighter than the standard core-shell design. Further, by coupling a fluorescent dye to the surface of the two different architectures, we demonstrated up to 8-fold improved emission enhancement with the core-shell-shell compared to the core-shell design. We show how, given proper consideration for emitter concentration, we can design a unique nanoparticle architecture to yield comparable or improved brightness and FRET coupling within a small volume

Axion dark matter detection by laser induced fluorescence in rare-earth doped materials

open11openBraggio, Caterina; Carugno, Giovanni; Chiossi, Federico; Lieto, Alberto Di; Guarise, Marco; Maddaloni, Pasquale; Ortolan, Antonello; Ruoso, Giuseppe; Santamaria, Luigi; Tasseva, Jordanka; Tonelli, MauroBraggio, Caterina; Carugno, Giovanni; Chiossi, Federico; Lieto, Alberto Di; Guarise, Marco; Maddaloni, Pasquale; Ortolan, Antonello; Ruoso, Giuseppe; Santamaria, Luigi; Tasseva, Jordanka; Tonelli, Maur