Block copolymer self-assembly derived mesoporous magnetic materials with three-dimensionally (3D) co-continuous gyroid nanostructure.

Magnetic nanomaterials are gaining interest for their many applications in technological areas from information science and computing to next-generation quantum energy materials. While magnetic materials have historically been nanostructured through techniques such as lithography and molecular beam epitaxy, there has recently been growing interest in using soft matter self-assembly. In this work, a triblock terpolymer, poly(isoprene-block-styrene-block-ethylene oxide) (ISO), is used as a structure directing agent for aluminosilicate sol nanoparticles and magnetic material precursors to generate organic-inorganic bulk hybrid films with co-continuous morphology. After thermal processing into mesoporous materials, results from a combination of small angle X-ray scattering (SAXS) and scanning electron microscopy (SEM) are consistent with the double gyroid morphology. Nitrogen sorption measurements reveal a type IV isotherm with H1 hysteresis, and yield a specific surface area of around 200 m2 g-1 and an average pore size of 23 nm. The magnetization of the mesostructured material as a function of applied field shows magnetic hysteresis and coercivity at 300 K and 10 K. Comparison of magnetic measurements between the mesoporous gyroid and an unstructured bulk magnetic material, derived from the identical inorganic precursors, reveals the structured material exhibits a coercivity of 250 Oe, opposed to 148 Oe for the unstructured at 10 K, and presence of remnant magnetic moment not conventionally found in bulk hematite; both of these properties are attributed to the mesostructure. This scalable route to mesoporous magnetic materials with co-continuous morphologies from block copolymer self-assembly may provide a pathway to advanced magnetic nanomaterials with a range of potential applications.

The impact of traffic noise on the capitalization of public walking area: A hedonic analysis of Vienna, Austria.

Traffic noise is a burden at home and outdoors. Economic literature confirms mostly negative effects of traffic noise on house prices, often based on distance between high noise and house location. We extend this literature using rich micro data to examine not only the impact of traffic noise at the house but also provide new results on the impact of traffic noise in public areas surrounding a home. Using Hedonic regression in Vienna, Austria, we confirm that very loud traffic noise (≥65 dB) experienced at the house reduces housing prices and further show that the value of public walking areas near a home, while positive overall, are substantially reduced when exposed to noise. Our findings help to establish spatial patterns in noise capitalization reflecting household exposure and the impact on the capitalized values of public areas in a context where active transportation (e.g. walking, biking) is an important mode of transportation. For policymakers, our findings help quantify and raise important questions as how to address and link the public bad nature of noise pollution to nearby residents.

Overcoming Barriers Associated with Oral Delivery of Differently Sized Fluorescent Core-Shell Silica Nanoparticles.

Oral delivery, while a highly desirable form of nanoparticle-drug administration, is limited by challenges associated with overcoming several biological barriers. Here, the authors study how fluorescent and poly(ethylene glycol)-coated (PEGylated) core-shell silica nanoparticles sized 5 to 50 nm interact with major barriers including intestinal mucus, intestinal epithelium, and stomach acid. From imaging fluorescence correlation spectroscopy studies using quasi-total internal reflection fluorescence microscopy, diffusion of nanoparticles through highly scattering mucus is progressively hindered above a critical hydrodynamic size around 20 nm. By studying Caco-2 cell monolayers mimicking the intestinal epithelia, it is observed that ultrasmall nanoparticles below 10 nm diameter (Cornell prime dots, [C' dots]) show permeabilities correlated with high absorption in humans from primarily enhanced passive passage through tight junctions. Particles above 20 nm diameter exclusively show active transport through cells. After establishing C' dot stability in artificial gastric juice, in vivo oral gavage experiments in mice demonstrate successful passage through the body followed by renal clearance without protein corona formation. Results suggest C' dots as viable candidates for oral administration to patients with a proven pathway towards clinical translation and may generate renewed interest in examining silica as a food additive and its effects on nutrition and health.

Directed Self-Assembly of Diamond Networks in Triblock Terpolymer Films on Patterned Substrates.

Block copolymers (BCPs) are particularly effective in creating soft nanostructured templates for transferring complex 3D network structures into inorganic materials that are difficult to fabricate by other methods. However, achieving control of the local ordering within these 3D networks over large areas remains a significant obstacle to advancing material properties. Here, we address this challenge by directing the self-assembly of a 3D alternating diamond morphology by solvent vapor annealing of a triblock terpolymer film on a chemically patterned substrate. The hexagonal substrate patterns were designed to match a (111) plane of the diamond lattice. Commensurability between the sparse substrate pattern and the BCP lattice produced a uniformly ordered diamond network within the polymer film, as confirmed by a combination of atomic force microscopy and cross-sectional imaging using focused ion beam scanning electron microscopy. The successful replication of the complex and well-ordered 3D network structure in gold promises to advance optical metamaterials and has potential applications in nanophotonics.

Radiation and Dose-densification of R-CHOP in Aggressive B-cell Lymphoma With Intermediate Prognosis: The UNFOLDER Study.

UNFOLDER (Unfavorable Young Low-Risk Densification of R-Chemo Regimens) is an international phase-3 trial in patients 18-60 years with aggressive B-cell lymphoma and intermediate prognosis defined by age-adjusted International Prognostic Index (aaIPI) of 0 and bulky disease (≥7.5 cm) or aaIPI of 1. In a 2 × 2 factorial design patients were randomized to 6× R-CHOP-14 or 6× R-CHOP-21 (rituximab, cyclophosphamide, doxorubicin, vincristine, and prediso[lo]ne) and to consolidation radiotherapy to extralymphatic and bulky disease or observation. Response was assessed according to the standardized response criteria published in 1999, not including F-18 fluordesoxyglucose positron emission tomography/computed tomography (FDG-PET). Primary endpoint was event-free survival (EFS). A total of 695 of 700 patients were eligible for the intention-to-treat analysis. Totally 467 patients qualified for radiotherapy of whom 305 patients were randomized to receive radiotherapy (R-CHOP-21: 155; R-CHOP-14: 150) and 162 to observation (R-CHOP-21: 81, R-CHOP-14: 81). Two hundred twenty-eight patients not qualifying for radiotherapy were randomized for R-CHOP-14 versus R-CHOP-21. After a median observation of 66 months 3-year EFS was superior in the radiotherapy-arm versus observation-arm (84% versus 68%; P = 0.0012), due to a lower rate of partial responses (PR) (2% versus 11%). PR often triggered additional treatment, mostly radiotherapy. No significant difference was observed in progression-free survival (PFS) (89% versus 81%; P = 0.22) and overall survival (OS) (93% versus 93%; P = 0.51). Comparing R-CHOP-14 and R-CHOP-21 EFS, PFS and OS were not different. Patients randomized to radiotherapy had a superior EFS, largely due to a lower PR rate requiring less additional treatment (NCT00278408, EUDRACT 2005-005218-19).

Intravital imaging of osteocyte integrin dynamics with locally injectable fluorescent nanoparticles.

Osteocytes are the resident mechanosensory cells in bone. They are responsible for skeletal homeostasis and adaptation to mechanical cues. Integrin proteins play a prominent role in osteocyte mechanotransduction, but the details are not well stratified. Intravital imaging with multiphoton microscopy presents an opportunity to study molecular level mechanobiological events in vivo and presents an opportunity to study integrin dynamics in osteocytes. However, fluorescent imaging limitations with respect to excessive optical scattering and low signal to noise ratio caused by mineralized bone matrix make such investigations non-trivial. Here, we demonstrate that ultra-small and bright fluorescent core-shell silica nanoparticles (<7 nm diameter), known as Cornell Prime Dots (C'Dots), are well-suited for the in vivo bone microenvironment and can improve intravital imaging capabilities. We report validation studies for C'Dots as a novel, locally injectable in vivo osteocyte imaging tool for both non-specific cellular uptake and for targeting integrins. The pharmacokinetics of C'Dots reveal distinct sex differences in nanoparticle intracellular dynamics and clearance in osteocytes, which represents a novel topic of study in bone biology. Integrin-targeted C'Dots were used to study osteocyte integrin dynamics. To the best of our knowledge, we report here the first evidence of osteocyte integrin endocytosis and recycling in vivo. Our results provide novel insights in osteocyte biology and will open up new lines of investigation that were previously unavailable in vivo.

Non-Equilibrium Block Copolymer Self-Assembly Based Porous Membrane Formation Processes Employing Multicomponent Systems.

Porous polymer-derived membranes are useful for applications ranging from filtration and separation technologies to energy storage and conversion. Combining block copolymer (BCP) self-assembly with the industrially scalable, non-equilibrium phase inversion technique (SNIPS) yields membranes comprising periodically ordered top surface structures supported by asymmetric, hierarchical substructures that together overcome performance tradeoffs typically faced by materials derived from equilibrium approaches. This review first reports on recent advances in understanding the top surface structural evolution of a model SNIPS-derived system during standard membrane formation. Subsequently, the application of SNIPS to multicomponent systems is described, enabling pore size modulation, chemical modification, and transformation to non-polymeric materials classes without compromising the structural features that define SNIPS membranes. Perspectives on future directions of both single-component and multicomponent membrane materials are provided. This points to a rich and fertile ground for the study of fundamental as well as applied problems using non-equilibrium-derived asymmetric porous materials with tunable chemistry, composition, and structure.

Ultrasmall Folate Receptor Alpha Targeted Enzymatically Cleavable Silica Nanoparticle Drug Conjugates Augment Penetration and Therapeutic Efficacy in Models of Cancer.

To address the key challenges in the development of next-generation drug delivery systems (DDS) with desired physicochemical properties to overcome limitations regarding safety, in vivo efficacy, and solid tumor penetration, an ultrasmall folate receptor alpha (FRα) targeted silica nanoparticle (C'Dot) drug conjugate (CDC; or folic acid CDC) was developed. A broad array of methods was employed to screen a panel of CDCs and identify a lead folic acid CDC for clinical development. These included comparing the performance against antibody-drug conjugates (ADCs) in three-dimensional tumor spheroid penetration ability, assessing in vitro/ex vivo cytotoxic efficacy, as well as in vivo therapeutic outcome in multiple cell-line-derived and patient-derived xenograft models. An ultrasmall folic acid CDC, EC112002, was identified as the lead candidate out of >500 folic acid CDC formulations evaluated. Systematic studies demonstrated that the lead formulation, EC112002, exhibited highly specific FRα targeting, multivalent binding properties that would mediate the ability to outcompete endogenous folate in vivo, enzymatic responsive payload cleavage, stability in human plasma, rapid in vivo clearance, and minimal normal organ retention organ distribution in non-tumor-bearing mice. When compared with an anti-FRα-DM4 ADC, EC112002 demonstrated deeper penetration into 3D cell-line-derived tumor spheroids and superior specific cytotoxicity in a panel of 3D patient-derived tumor spheroids, as well as enhanced efficacy in cell-line-derived and patient-derived in vivo tumor xenograft models expressing a range of low to high levels of FRα. With the growing interest in developing clinically translatable, safe, and efficacious DDSs, EC112002 has the potential to address some of the critical limitations of the current systemic drug delivery for cancer management.

Addressing Particle Compositional Heterogeneities in Super-Resolution-Enhanced Live-Cell Ratiometric pH Sensing with Ultrasmall Fluorescent Core-Shell Aluminosilicate Nanoparticles.

The interrogation of metabolic parameters like pH in live-cell experiments using optical super-resolution microscopy (SRM) remains challenging. This is due to a paucity of appropriate metabolic probes enabling live-cell SRM-based sensing. Here we introduce ultrasmall fluorescent core-shell aluminosilicate nanoparticle sensors (FAM-ATTO647N aC' dots) that covalently encapsulate a reference dye (ATTO647N) in the core and a pH-sensing moiety (FAM) in the shell. Only the reference dye exhibits optical blinking enabling live-cell stochastic optical reconstruction microscopy (STORM). Using data from cells incubated for 60 minutes with FAM-ATTO647N aC' dots, pixelated information from total internal reflection fluorescence (TIRF) microscopy-based ratiometric sensing can be combined with that from STORM-based localizations via the blinking reference dye in order to enhance the resolution of ratiometric pH sensor maps beyond the optical diffraction limit. A nearest-neighbor interpolation methodology is developed to quantitatively address particle compositional heterogeneity as determined by separate single-particle fluorescence imaging methods. When combined with STORM-based estimates of the number of particles per vesicle, vesicle size, and vesicular motion as a whole, this analysis provides detailed live-cell spatial and functional information, paving the way to a comprehensive mapping and understanding of the spatiotemporal evolution of nanoparticle processing by cells important, e.g. for applications in nanomedicine.

Innovation in COVID-19 Response: ANNA COVID-19 Surge Support Process and Map.

The COVID-19 pandemic began with uncertainty in how to care for patients and protect staff. The American Nephrology Nurses Association (ANNA) immediately recognized the need to provide its members and others in the nephrology community with as much information as possible. Resources were collected and disseminated in many forms (e.g., publications, webinars, virtual conference sessions). As COVID-19 surges began occurring across the country and staffing reached a crisis level, ANNA collaborated with other organizations to find potential solutions. One solution developed by ANNA was the ANNA COVID-19 Surge Support Process and Map - a process to connect the areas in high need with skilled and available staff. This article describes the ANNA COVID-19 Surge Support Process and Map, which has continued to help address COVID-19 staffing challenges.

Patternable Mesoporous Thin Film Quantum Materials via Block Copolymer Self-Assembly: An Emergent Technology?

Recent developments in quantum materials hold promise for revolutionizing energy and information technologies. The use of soft matter self-assembly, for example, by employing block copolymers (BCPs) as structure directing or templating agents, offers facile pathways toward quantum metamaterials with highly tunable mesostructures via scalable solution processing. Here, we report the preparation of patternable mesoporous niobium carbonitride-type thin film superconductors through spin-coating of a hybrid solution containing an amphiphilic BCP swollen by niobia sol precursors and subsequent thermal processing in combination with photolithography. Spin-coated as-made BCP-niobia hybrid thin films on silicon substrates after optional photolithographic definition are heated in air to produce a porous oxide, and subsequently converted in a multistep process to carbonitrides via treatment with high temperatures in reactive gases including ammonia. Grazing incidence small-angle X-ray scattering suggests the presence of ordered mesostructures in as-made BCP-niobia films without further annealing, consistent with a distorted alternating gyroid morphology that is retained upon thermal treatments. Wide-angle X-ray scattering confirms the synthesis of phase-pure niobium carbonitride nanocrystals with rock-salt lattices within the mesoscale networks. Electrical transport measurements of unpatterned thin films show initial exponential rise in resistivity characteristic of thermal activation in granular systems down to 12.8 K, at which point resistivity drops to zero into a superconducting state. Magnetoresistance measurements determine the superconducting upper critical field to be over 16 T, demonstrating material quality on par with niobium carbonitrides obtained from traditional solid-state synthesis methods. We discuss how such cost-effective and scalable solution-based quantum materials fabrication approaches may be integrated into existing microelectronics processing, promising the emergence of a technology with tremendous academic and industrial potential by combining the capabilities of soft matter self-assembly with quantum materials.

Ultrasmall, Bright, and Photostable Fluorescent Core-Shell Aluminosilicate Nanoparticles for Live-Cell Optical Super-Resolution Microscopy.

Stochastic optical reconstruction microscopy (STORM) is an optical super-resolution microscopy (SRM) technique that traditionally requires toxic and non-physiological imaging buffers and setups that are not conducive to live-cell studies. It is observed that ultrasmall (<10 nm) fluorescent core-shell aluminosilicate nanoparticles (aC' dots) covalently encapsulating organic fluorophores enable STORM with a single excitation source and in a regular (non-toxic) imaging buffer. It is shown that fourfold coordinated aluminum is responsible for dye blinking, likely via photoinduced redox processes. It is demonstrated that this phenomenon is observed across different dye families leading to probes brighter and more photostable than the parent free dyes. Functionalization of aC' dots with antibodies allows targeted fixed cell STORM imaging. Finally, aC' dots enable live-cell STORM imaging providing quantitative measures of the size of intracellular vesicles and the number of particles per vesicle. The results suggest the emergence of a powerful ultrasmall, bright, and photostable optical SRM particle platform with characteristics relevant to clinical translation for the quantitative assessment of cellular structures and processes from live-cell imaging.

Fluorescent Silica Nanoparticles to Label Metastatic Tumor Cells in Mineralized Bone Microenvironments.

During breast cancer bone metastasis, tumor cells interact with bone microenvironment components including inorganic minerals. Bone mineralization is a dynamic process and varies spatiotemporally as a function of cancer-promoting conditions such as age and diet. The functional relationship between skeletal dissemination of tumor cells and bone mineralization, however, is unclear. Standard histological analysis of bone metastasis frequently relies on prior demineralization of bone, while methods that maintain mineral are often harsh and damage fluorophores commonly used to label tumor cells. Here, fluorescent silica nanoparticles (SNPs) are introduced as a robust and versatile labeling strategy to analyze tumor cells within mineralized bone. SNP uptake and labeling efficiency of MDA-MB-231 breast cancer cells is characterized with cryo-scanning electron microscopy and different tissue processing methods. Using a 3D in vitro model of marrow-containing, mineralized bone as well as an in vivo model of bone metastasis, SNPs are demonstrated to allow visualization of labeled tumor cells in mineralized bone using various imaging modalities including widefield, confocal, and light sheet microscopy. This work suggests that SNPs are valuable tools to analyze tumor cells within mineralized bone using a broad range of bone processing and imaging techniques with the potential to increase the understanding of bone metastasis.

Block Copolymer Self-Assembly-Directed and Transient Laser Heating-Enabled Nanostructures toward Phononic and Photonic Quantum Materials.

Three-dimensional (3D) periodic ordering of silicon (Si), an inorganic semiconductor, on the mesoscale was achieved by combining block copolymer (BCP) self-assembly (SA) based mesoporous alternating gyroidal network formation with nonequilibrium transient laser heating. 3D continuous and periodically ordered alternating gyroidal mesoporous carbon thin-film networks were prepared from spin coating, SA under solvent vapor annealing (SVA), and thermal processing of mixtures of a triblock terpolymer with resorcinol resols. The resulting mesoporous thin films, acting as structure-directing templates, were backfilled with amorphous silicon (a-Si). Nanosecond excimer laser heating led to transient Si melts conformally filling the template pores and subsequent Si crystallization. The ordered mesostructure of the organic polymer-derived templates was kept intact, despite being thermally unstable at the high temperatures around the Si melting point (MP), leading to high pattern transfer fidelity. As evidenced by a combination of grazing incidence small-angle X-ray scattering (GISAXS) and scanning electron microscopy (SEM), after template removal, the crystalline Si (c-Si) inherited the inverse network topology of the 3D mesoporous thin-film templates, but with reduced F222 space group symmetry (D2 point group symmetry) from compression of the cubic alternating gyroid lattice. Structures with this reduced symmetry have been proposed as photonic and phononic materials exhibiting topologically protected Weyl points, adding to the emerging field of BCP SA-directed quantum materials promising advanced physics and materials properties.

Changes in lower limb biomechanics when following floor-projected foot placement visual cues for gait rehabilitation.

BACKGROUND: Lately, the projection of foot placement visual cues onto the floor has been considered for use in gait rehabilitation. While promising, this approach needs further basic assessment to ensure proper uses. RESEARCH QUESTION: Does following floor-projected foot placement visual cues of one's natural walking pattern induce gait mechanics changes immediately or after a practice period? METHODS: Gait mechanics data from fifteen healthy individuals (7 female, 25.4 ±â€¯5.0 years, 21.5 ±â€¯1.68 kg/m2) was collected during normal walking without visual cues, and during two testing phases (immediate and after 45-60 min of practice) of walking with floor-projected visual cues depicting their normal spatial parameters. Magnitudes and variabilities of spatial gait parameters and sagittal plane lower limb kinematics and kinetics were compared between the three testing phases using repeated measures ANOVA and post-hoc paired t-tests. RESULTS: Compared to normal walking without foot placement visual cues, there was a statistically significant (p < 0.05) increase in stride length (maximum change of 0.01 ±â€¯0.01 m), stance phase knee flexion (2.0 ±â€¯2.5°), and swing phase hip flexion (1.2 ±â€¯1.3°) in both immediate and post-practice testing phases, along with an increase in terminal stance hip (0.28 ±â€¯0.38 %BW*Ht) and knee (0.25 ±â€¯0.25 %BW*Ht) flexion moments in the immediate testing phase. All of these changes between testing phases were smaller than their corresponding normal gait smallest real differences (SRD). With the addition of visual cues, variability was statistically significantly decreased in spatial parameters and increased in knee flexion angle at heel strike and knee flexion moment in terminal stance. SIGNIFICANCE: While biomechanical changes were observed, their magnitudes were small enough to suggest that floor-projected visual cues can be used in gait retraining without introducing unintended gait changes. Furthermore, the results suggested that lengthy practice periods are not necessary. The validity of these observations will, however, need to be confirmed in cases of severe impairments.

Ultrasmall PEGylated and Targeted Core-Shell Silica Nanoparticles Carrying Methylene Blue Photosensitizer.

Photodynamic therapy (PDT) presents an alternative noninvasive therapeutic modality for the treatment of cancer and other diseases. PDT relies on cytotoxic singlet oxygen (reactive oxygen species or ROS) that is locally generated through energy transfer between a photosensitizer (PS) and molecularly dissolved triplet oxygen. While a number of nanoparticle-based PS vehicles have been described, because of their beneficial and proven biodistribution and pharmacokinetic profiles, ultrasmall nanoparticles with diameters below 10 nm are particularly promising. Here, we investigate two different particle designs deviating from ultrasmall poly(ethylene glycol)-coated (PEGylated) fluorescent core-shell silica nanoparticles referred to as Cornell prime dots (C' dots) by replacing the fluorescent dye with a photosensitizer (psC' dots), here the methylene blue (MB) derivate MB2. In the first approach (design 1), MB2 is encapsulated into the matrix of the silica core, while in the second approach (design 2), MB2 is grafted onto the silica core surface in between chains of the sterically stabilizing poly(ethylene glycol) (PEG) corona. We compare both cases with regard to their singlet oxygen quantum yields, ΦΔ, with the effective ΦΔeff per particle reaching 111 ± 3 and 161 ± 5% for designs 1 and 2, respectively, substantially exceeding single MB2 molecule performance. Encapsulation significantly improves PS photostability, while surface conjugation diminishes it, relative to free MB2. Finally, we show that both particle designs allow functionalization with a targeting peptide, cyclo(Arg-Gly-Asp-D-Tyr-Cys) [c(RGDyC)]. Results suggest that psC' dots are a promising targeted platform for PDT applications, e.g. in oncology, that may combine colloidal stability, efficient renal clearance limiting off-target accumulation, targeted delivery to sites of disease, and effective ROS generation maximizing therapeutic efficacy.

Dye Encapsulation in Fluorescent Core-Shell Silica Nanoparticles as Probed by Fluorescence Correlation Spectroscopy.

Synthetic advances in the formation of ultrasmall (<10 nm) fluorescent poly(ethylene glycol)-coated (PEGylated) core-shell silica nanoparticles (SNPs), enabling improved particle size and surface chemical property control have led to successful clinical translation of SNPs as diagnostic probes in oncology. Despite the success of such probes, details of the dye incorporation and resulting silica architecture are still poorly understood. Here, we employ afterpulse-corrected fluorescence correlation spectroscopy (FCS) to monitor fast fluorescence fluctuations (lag times <10-5 s) of the negatively charged cyanine dye Cy5 as a probe to study such details for dye encapsulation in 5 nm silica cores of PEGylated core-shell SNPs (C dots). Upon deposition of additional silica shells over the silica core we find that the amplitude of photo-induced cis-trans isomerization decreases, suggesting that the Cy5 dyes are located near or on the surface of the original SNP cores. In combination with time correlated fluorescence decay measurements we deduce radiative and non-radiative rates of the Cy5 dye in these particles. Results demonstrate that FCS is a well-suited tool to investigate aspects of the photophysics of fluorescent nanoparticles, and that conformational changes of cyanine dyes like Cy5 are excellent indicators for the local dye environment within ultrasmall SNPs.

Quantitative Comparison of Dye and Ultrasmall Fluorescent Silica Core-Shell Nanoparticle Probes for Optical Super-Resolution Imaging of Model Block Copolymer Thin Film Surfaces.

In recent years, high-resolution optical imaging in the far field has provided opportunities for alternative approaches to nanocharacterization traditionally dominated by electron and scanning probe microscopies. Here, we report the optical super-resolution imaging of model block copolymer (BCP) thin film surface nanostructures through stochastic optical reconstruction microscopy (STORM). We compare a set of surface-functionalized fluorescent core-shell silica nanoparticles encapsulating two different organic dyes, Cy3 and Cy5, with the corresponding free dyes in STORM. Using various click-type chemistries, these probes are covalently attached to the surface of specific blocks of BCP thin films, enabling selective block labeling and optical visualization. We demonstrate that the enhanced brightness of these particle probes offers distinct advantages over conventional dye labeling, outperforming one of the best STORM dyes available (Cy5).

Amorphous Quantum Nanomaterials.

In quantum materials, macroscopic behavior is governed in nontrivial ways by quantum phenomena. This is usually achieved by exquisite control over atomic positions in crystalline solids. Here, it is demonstrated that the use of disordered glassy materials provides unique opportunities to tailor quantum material properties. By borrowing ideas from single-molecule spectroscopy, single delocalized π-electron dye systems are isolated in relatively rigid ultrasmall (<10 nm diameter) amorphous silica nanoparticles. It is demonstrated that chemically tuning the local amorphous silica environment around the dye over a range of compositions enables exquisite control over dye quantum behavior, leading to efficient probes for photodynamic therapy (PDT) and stochastic optical reconstruction microscopy (STORM). The results suggest that efficient fine-tuning of light-induced quantum behavior mediated via effects like spin-orbit coupling can be effectively achieved by systematically varying averaged local environments in glassy amorphous materials as opposed to tailoring well-defined neighboring atomic lattice positions in crystalline solids. The resulting nanoprobes exhibit features proven to enable clinical translation.

High-birefringence direct UV-written waveguides for use as heralded single-photon sources at telecommunication wavelengths.

Direct UV-written waveguides are fabricated in silica-on-silicon with birefringence of (4.9 ± 0.2) × 10-4, much greater than previously reported in this platform. We show that these waveguides are suitable for the generation of heralded single photons at telecommunication wavelengths by spontaneous four-wave mixing. A pulsed pump field at 1060 nm generates pairs of photons in highly detuned, spectrally uncorrelated modes near 1550 nm and 800 nm. Waveguide-to-fiber coupling efficiencies of 78-91 % are achieved for all fields. Waveguide birefringence is controlled through dopant concentration of GeCl4 and BCl3 using the flame hydrolysis deposition process. The technology provides a route towards the scalability of silica-on-silicon integrated components for photonic quantum experiments.