Extending the defect tolerance of halide perovskite nanocrystals to hot carrier cooling dynamics.

Defect tolerance is a critical enabling factor for efficient lead-halide perovskite materials, but the current understanding is primarily on band-edge (cold) carriers, with significant debate over whether hot carriers can also exhibit defect tolerance. Here, this important gap in the field is addressed by investigating how intentionally-introduced traps affect hot carrier relaxation in CsPbX nanocrystals (X = Br, I, or mixture). Using femtosecond interband and intraband spectroscopy, along with energy-dependent photoluminescence measurements and kinetic modelling, it is found that hot carriers are not universally defect tolerant in CsPbX, but are strongly correlated to the defect tolerance of cold carriers, requiring shallow traps to be present (as in CsPbI).

Distance-Independent Efficiency of Triplet Energy Transfer from π-Conjugated Organic Ligands to Lanthanide-Doped Nanoparticles.

Lanthanide-doped nanoparticles (LnNPs) possess unique optical properties and are employed in various optoelectronic and bioimaging applications. One fundamental limitation of LnNPs is their low absorption cross-section. This hurdle can be overcome through surface modification with organic chromophores with large absorption cross-sections.

Hybrid Organic-Inorganic Perovskite Superstructures for Ultrapure Green Emissions.

All inorganic CsPbBr superstructures (SSs) have attracted much research interest due to their unique photophysical properties, such as their large emission red-shifts and super-radiant burst emissions. These properties are of particular interest in displays, lasers and photodetectors. Currently, the best-performing perovskite optoelectronic devices incorporate organic cations (methylammonium (MA), formamidinium (FA)), however, hybrid organic-inorganic perovskite SSs have not yet been investigated.

A Dual Sensing Platform for Human Exhaled Breath Enabled by Fe-MIL-101-NH Metal-Organic Frameworks and its Derived Co/Ni/Fe Trimetallic Oxides.

Limited by the insufficient active sites and the interference from breath humidity, designing reliable gas sensing materials with high activity and moisture resistance remains a challenge to analyze human exhaled breath for the translational application of medical diagnostics. Herein, the dual sensing and cooperative diagnosis is achieved by utilizing metal-organic frameworks (MOFs) and its derivative. The Fe-MIL-101-NH serves as the quartz crystal microbalance humidity sensing layer, which exhibits high selectivity and rapid response time (16 s/15 s) to water vapor.

Tunable concentration-dependent upconversion and downconversion luminescence in NaYF: Yb, Er@ NaYF: Yb, Nd core-shell nanocrystals for a dual-mode anti-counterfeiting imaging application.

Lanthanide-doped luminescent nanocrystals display both upconversion luminescence (UCL) and downconversion luminescence (DCL) properties, which offer potential applications in the second near-infrared window (NIR-II) images and biology sensors. Both UCL and DCL are sensitive to concentrations of activators. However, few works reveal the mechanism of concentration-dependent UCL and DCL.

Overcoming Vascular Barriers to Improve the Theranostic Outcomes of Nanomedicines.

Nanotheranostics aims to utilize nanomaterials to prevent, diagnose, and treat diseases to improve the quality of patients' lives. Blood vessels are responsible to deliver nutrients and oxygen to the whole body, eliminate waste, and provide access for patrolling immune cells for healthy tissues. Meanwhile, they can also nourish disease tissues, spread disease factors or cells into other healthy tissues, and deliver nanotheranostic agents to cover all the regions of a disease tissue.

Degradable mesoporous semimetal antimony nanospheres for near-infrared II multimodal theranostics.

Metallic and semimetallic mesoporous frameworks are of great importance owing to their unique properties and broad applications. However, semimetallic mesoporous structures cannot be obtained by the traditional template-mediated strategies due to the inevitable hydrolytic reaction of semimetal compounds. Therefore, it is yet challenging to fabricate mesoporous semimetal nanostructures, not even mention controlling their pore sizes.

Antimony Nanopolyhedrons with Tunable Localized Surface Plasmon Resonances for Highly Effective Photoacoustic-Imaging-Guided Synergistic Photothermal/Immunotherapy.

Antimony (Sb), a typical group VA semimetal, has rarely been studied both experimentally and theoretically in plasmonic photothermal therapy, possibly due to the lack of effective morphology-controllable methods for the preparation of high-quality Sb nanocrystals. In this study, an effective ligand-guided growth strategy to controllably synthesize Sb nanopolyhedrons (Sb NPHs) with ultrahigh photothermal conversion efficiency (PTCE), good photothermal stability, as well as biocompatibility is presented. Furthermore, the modulation effect of different morphologies on localized surface plasmon resonance (LSPR) of Sb NPHs in experimentation is successfully observed.

Near-infrared-II activated inorganic photothermal nanomedicines.

The emergence of near-infrared-II (NIR-II) activated photomedicines has extended the penetration depth for noninvasive theranostics, especially for photothermal nanomedicines. The current early development stage for NIR-II activated photomedicines has focused on creating a greater variety of photothermal agents (PTAs) with superior photothermal conversion ability. However, there is no thorough review for NIR-II inorganic PTAs and most comparisons of the photothermal performances of NIR-II inorganic PTAs are made with NIR-I PTAs.

Artificial Atomic Vacancies Tailor Near-Infrared II Excited Multiplexing Upconversion in Core-Shell Lanthanide Nanoparticles.

Epitaxial growth of an inert shell around the optical active lanthanide upconversion nanoparticles (UCNPs) is a general strategy to enhance their brightness. Yet, its potential as a tool in multiplexing emission tailoring has rarely been reported. Here, by developing the atomic vacancies into color selectivity actuators, we present an efficient strategy to achieve inert-shell-modulated multiplexing upconversion in 1540 nm activated UCNPs.

Balancing the thickness of sensitizing and inert layers in neodymium-sensitized tetralayer nanoconstructs for optimal ultraviolet upconversion and near-infrared cross-linked hydrogel tissue sealants.

Tuning the configuration of lanthanide-doped upconversion nanoparticles (UCNPs) has been proven to be an effective approach to enhance upconversion (UC) efficiency, especially for neodymium (Nd)-sensitized UCNPs. Rational configuration design can spatially separate activators and sensitizers, achieving the evolution from single core to multilayer structures. However, optimizing multiphoton UC emission via configuration modulation, especially in the ultraviolet range, is yet to be fully investigated.

Upconversion Nanoparticles-Based Multiplex Protein Activation to Neuron Ablation for Locomotion Regulation.

The optogenetic neuron ablation approach enables noninvasive remote decoding of specific neuron function within a complex living organism in high spatiotemporal resolution. However, it suffers from shallow tissue penetration of visible light with low ablation efficiency. This study reports a upconversion nanoparticle (UCNP)-based multiplex proteins activation tool to ablate deep-tissue neurons for locomotion modulation.

Virus-Inspired Deformable Mesoporous Nanocomposites for High Efficiency Drug Delivery.

Mesoporous nanoparticles as a versatile platform for cancer theranostics have been widely used, but their cellular delivery efficiency is still far from satisfactory. Although deformability is emerging as an important parameter influencing cellular uptake enhancement, the facile synthesis of deformable mesoporous nanocomposite with adjustable mechanical property is challenging but meaningful for a deeper understanding of cellular uptake mechanisms and significantly improving cancer therapy. In this work, yolk-shell structured eccentric mesoporous organosilica (YEMO) nanocomposites with adjustable mechanical property are successfully prepared by an organosilane-assisted anisotropic self-assembly approach.

Neodymium-Sensitized Nanoconstructs for Near-Infrared Enabled Photomedicine.

Neodymium (Nd )-sensitized nanoconstructs have gained increasing attention in recent decades due to their unique properties, especially optical properties. The design of various Nd -sensitized nanosystems is expected to contribute to medical and health applications, due to their advantageous properties such as high penetration depth, excellent photostability, non-photobleaching, low cytotoxicity, etc. However, the low conversion efficiency and potential long-term toxicity of Nd -sensitized nanoconstructs are huge obstacles to their clinical translations.

Generating New Cross-Relaxation Pathways by Coating Prussian Blue on NaNdF To Fabricate Enhanced Photothermal Agents.

Cross-relaxation among sensitizers is commonly regarded as deleterious in fluorescent materials, although favorable in photothermal agents. Herein, we coated Prussian blue (PB) on NaNdF nanoparticles to fabricate core-shell nanocomplexes with new cross relaxation pathways between the ladder-like energy levels of Nd ions and continuous energy band of PB. The photothermal conversion efficiency was improved exceptionally and the mechanism of the enhanced photothermal effect was investigated.

An Upconversion Nanoparticle Enables Near Infrared-Optogenetic Manipulation of the Caenorhabditis elegans Motor Circuit.

Near-infrared (NIR) light penetrates tissue deeply, but its application to motor behavior stimulation has been limited by the lack of known genetic NIR light-responsive sensors. We designed and synthesized a Yb/Er/Ca-based lanthanide-doped upconversion nanoparticle (UCNP) that effectively converts 808 nm NIR light to green light emission. This UCNP is compatible with Chrimson, a cation channel activated by green light; as such, it can be used in the optogenetic manipulation of the motor behaviors of Caenorhabditis elegans.

Synergizing Upconversion Nanophotosensitizers with Hyperbaric Oxygen to Remodel the Extracellular Matrix for Enhanced Photodynamic Cancer Therapy.

Photodynamic therapy (PDT) holds great promise as a noninvasive and selective cancer therapeutic treatment in preclinical research and clinical practice; however, it has limited efficacy in the ablation of deep-seated tumor because of hypoxia-associated circumstance and poor penetration of photosensitizers to cancer cells away from the blood vessels. To tackle the obstacles, we propose a therapeutic strategy that synergizes upconversion nanophotosensitizers (UNPSs) with hyperbaric oxygen (HBO) to remodel the extracellular matrix for enhanced photodynamic cancer therapy. The UNPSs are designed to have an Nd-sensitized sandwiched structure, wherein the upconversion core serves as light transducers to transfer energy to the neighboring photosensitizers to produce reactive oxygen species (ROS).

Ultrasmall-Superbright Neodymium-Upconversion Nanoparticles via Energy Migration Manipulation and Lattice Modification: 808 nm-Activated Drug Release.

Nd-sensitized upconversion nanoparticles are among the most promising emerging fluorescent nanotransducers. They are activated by 808 nm irradiation, which features merits such as limited tissue overheating and deeper penetration depth, and hence are attractive for diagnostic and therapeutic applications. Recent studies indicate that ultrasmall nanoparticles (<10 nm) are potentially more suitable for clinical application due to their favorable biodistribution and safety profiles.