Engineering Bright and Mechanosensitive Alkaline-Earth Rare-Earth Upconverting Nanoparticles.

Upconverting nanoparticles (UCNPs) are an emerging platform for mechanical force sensing at the nanometer scale. An outstanding challenge in realizing nanometer-scale mechano-sensitive UCNPs is maintaining a high mechanical force responsivity in conjunction with bright optical emission. This Letter reports mechano-sensing UCNPs based on the lanthanide dopants Yb and Er, which exhibit a strong ratiometric change in emission spectra and bright emission under applied pressure.

Lanthanide-Based Nanosensors: Refining Nanoparticle Responsiveness for Single Particle Imaging of Stimuli.

Lanthanide nanoparticles (LNPs) are promising sensors of chemical, mechanical, and temperature changes; they combine the narrow-spectral emission and long-lived excited states of individual lanthanide ions with the high spatial resolution and controlled energy transfer of nanocrystalline architectures. Despite considerable progress in optimizing LNP brightness and responsiveness for dynamic sensing, detection of stimuli with a spatial resolution approaching that of individual nanoparticles remains an outstanding challenge. Here, we highlight the existing capabilities and outstanding challenges of LNP sensors, en-route to nanometer-scale, single particle sensor resolution.

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

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 (M Ln F MLnF) with a CaF shell. We synthesize 8 alkaline-earth host materials doped with Yb and Tm , with alkaline-earth (M) spanning Ca, Sr, and Ba, MgSr, CaSr, CaBa, SrBa, and CaSrBa.

Extending the Quantum Coherence of a Near-Surface Qubit by Coherently Driving the Paramagnetic Surface Environment.

Surfaces enable useful functionalities for quantum systems, e.g., as interfaces to sensing targets, but often result in surface-induced decoherence where unpaired electron spins are common culprits.

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.

Optically Robust and Biocompatible Mechanosensitive Upconverting Nanoparticles.

Upconverting nanoparticles (UCNPs) are promising tools for background-free imaging and sensing. However, their usefulness for applications depends on their biocompatibility, which we define by their optical performance in biological environments and their toxicity in living organisms. For UCNPs with a ratiometric color response to mechanical stress, consistent emission intensity and color are desired for the particles under nonmechanical stimuli.

Patterned Formation of Highly Coherent Nitrogen-Vacancy Centers Using a Focused Electron Irradiation Technique.

We demonstrate fully three-dimensional and patterned localization of nitrogen-vacancy (NV) centers in diamond with coherence times in excess of 1 ms. Nitrogen δ-doping during chemical vapor deposition diamond growth vertically confines nitrogen to 4 nm while electron irradiation with a transmission electron microscope laterally confines vacancies to less than 450 nm. We characterize the effects of electron energy and dose on NV formation.