Photothermal oxidative dehydrogenation of propane to propylene over Cu/BN catalysts.

Oxidative dehydrogenation of propane (ODHP) is a reaction with significant practical significance. As for the industrial application of ODHP, it is challenging to achieve high activity and high propylene selectivity simultaneously. In this study, to overcome this obstacle, we designed a series of Cu/BN catalysts with unique morphologies for establishing a photothermal ODHP system with high efficiency and selectivity. Characterization and evaluation results revealed that Cu/BN-NS and Cu/BN-NF with enlarged specific surface areas exhibited higher catalytic activities. The localized surface plasmon resonance (LSPR) effect of Cu nanoparticles further enhanced the photothermal catalytic performances of Cu/BN catalysts under visible light irradiation. To the best of our knowledge, it is the first time to establish a BN-based photothermal ODHP catalytic system. This study is expected to pave pathways to realize high activity and propylene selectivity for the practical application of ODHP.

Association between muscle-localized bioelectrical impedance analysis parameters and performance in a multi-set exercise on the isokinetic dynamometer in young women.

This study aimed to verify the relationship between changes in thigh muscle-localized bioelectrical impedance analysis (ML-BIA) parameters and performance in a multiple-set exercise. The sample consisted of 30 female university students (22.1 ± 3.2 years). The ML-BIA parameters, including localized muscle resistance (ML-R), reactance (ML-Xc), and phase angle (ML-AngF), were evaluated using a tetrapolar bioelectric impedance device operating at a frequency of 50 KHz. The multiple sets protocol was performed with an isokinetic dynamometer. For body composition, total and leg lean soft tissue (LST) were evaluated using dual X-ray absortiometry. Student's t-test for paired samples was used to compare the ML-BIA parameters and thigh circumference pre and postexercise. Linear regression analysis was performed to verify the ∆ML-PhA as a predictor of peak torque for the three sets alone while controlling for total and leg LST. There were differences in the ML-R (∆ = 0.02 ± 1.45 Ω; p = 0.001; and E.S = 0.19), ML-Xc (∆ = 2.90 ± 4.12 Ω; p = 0.043; and E.S = 0.36), and thigh circumference (∆ = 0.82 ± 0.60 cm; p < 0.001; and E.S = 0.16) pre- and post-multiple sets. ΔML-PhA was a predictor of performance in the first set (p = 0.002), regardless of total and leg LST. However, the ΔML-PhA lost its explanatory power in the other sets (second and third), and the variables that best explained performance were total and leg LST. The ML-BIA (ML-R and ML-Xc) parameters were sensitive and changed after the multiple sets protocol, and the ΔML-PhA was a predictor of performance in the first set regardless of the total and leg LST.

Enhancing Localized Electron Density over Pd1.4Cu Decorated Oxygen Defective TiO2-x Nanoarray for Electrocatalytic Nitrite Reduction to Ammonia.

Electrocatalytic nitrite (NO2 -) reduction to ammonia (NH3) is a promising method for reducing pollution and aiding industrial production. However, progress is limited by the lack of efficient selective catalysts and ambiguous catalytic mechanisms. This study explores the loading of PdCu alloy onto oxygen defective TiO2-x, resulting in a significant increase in NH3 yield (from 70.6 to 366.4 µmol cm-2 h-1 at -0.6 V vs reversible hydrogen electrode) by modulating localized electron density. In situ and operando studies illustrate that the reduction of NO2 - to NH3 involves gradual deoxygenation and hydrogenation. The process also demonstrated excellent selectivity and stability, with long-term durability in cycling and 50 h stability tests. Density functional theory (DFT) calculations elucidate that the introduction of PdCu alloys further amplified electron density at oxygen vacancies (Ovs). Additionally, the Ti─O bond is strengthened as the d-band center of the Ti 3d rising after PdCu loading, facilitating the adsorption and activation of *NO2. Moreover, the presence of Ovs and PdCu alloy lowers the energy barriers for deoxygenation and hydrogenation, leading to high yield and selectivity of NH3. This insight of controlling localized electron density offers valuable insights for advancing sustainable NH3 synthesis methods.

Nanoflower Microreactor Based Versatile Enhancer for Recognition Cofactor-Dependent Enzyme Biocatalysis toward Saxitoxin Detection.

Investigating organic carriers' utilization efficiency and bioactivity within organic-inorganic hybrid nanoflowers is critical to constructing sensitive immunosensors. Nevertheless, the sensitivity of immunosensors is interactively regulated by different classes of biomolecules such as antibodies and enzymes. In this work, we introduced a new alkaline phosphatase-antibody-CaHPO4 hybrid nanoflowers (AAHNFs) microreactor based colorimetric immunoprobe. This system integrates a biometric unit (antibody) with a signal amplification element (enzyme) through the biomineralization process. Specifically, the critical factors affecting antibody recognition activity in the formation mechanism of AAHNFs are investigated. The designed AAHNFs retain antibody recognition ability with enhanced protection for encapsulated proteins against high temperature, organic solvents, and long-term storage, facilitating the selective construction of lock structures against antigens. Additionally, a colorimetric immunosensor based on AAHNFs was developed. After ascorbic acid 2-phosphate hydrolysis by alkaline phosphatase (ALP), the generated ascorbic acid decomposes I2 to I-, inducing the localized surface plasmon resonance in the silver nanoplate, which is effectively tuned through shape conversion to develop the sensor. Further, a 3D-printed portable device is fabricated, integrated with a smartphone sensing platform, and applied to the data of collection and analysis. Notably, the immunosensor exhibits improved analytical performance with a 0.1-6.25 ng·mL-1 detection range and a 0.06 ng·mL-1 detection limit for quantitative saxitoxin (STX) analysis. The average recoveries of STX in real samples ranged from 85.9% to 105.9%. This study presents a more in-depth investigation of the recognition element performance, providing insights for improved antibody performance in practical applications.

Dual Plasmons with Bioinspired 3D Network Structure Enabling Ultrahigh Efficient Solar Steam Generation.

Plasmonic nanomaterials such as Au, Ag, and Cu are widely recognized for their strong light-matter interactions, making them promising photothermal materials for solar steam generation. However, their practical use in water evaporation is significantly limited by the trade-off between high costs and poor stability. In this regard, we introduce a novel, nonmetallic dual plasmonic TiN/MoO3-x composite. This composite features a three-dimensional, urchin-like biomimetic structure, with plasmonic TiN nanoparticles embedded within a network of plasmonic MoO3-x nanorods. As a solar absorber, the TiN/MoO3-x composite achieves a high evaporation rate of ∼2.05 kg m-2 h-1 with an energy efficiency up to 106.7% under 1 sun illumination, outperforming the state-of-the-art plasmonic systems. The high photothermal stability and unique dual plasmonic nanostructure of the TiN/MoO3-x composite are demonstrated by advanced in situ laser-heating transmission electron microscopy and photon-induced near-field electron microscopy/electron energy-loss spectroscopy, respectively. This work provides new inspiration for the design of plasmonic materials.

Endpoints and outcomes for localized scleroderma/morphea: a scoping literature review.

BACKGROUND: Current treatment for localized scleroderma (LS) has been shown to halt disease activity, but little is still known about patient experiences with these treatments, nor is there consensus about optimal measurement strategies for future clinical trials. OBJECTIVE: Conduct a scoping review of the literature for the types of outcomes and measures (i.e. clinician-, patient-, and caregiver-reported) utilized in published treatment studies of LS. METHODS: Online databases were searched for articles related to the evaluation of treatment efficacy in LS with a special focus on pediatrics. RESULTS: Of the 168 studies, the most common outcomes used were cutaneous disease activity and damage measured via clinician-reported assessments. The most frequently cited measure was the Localized Scleroderma Cutaneous Assessment Tool (LoSCAT). Few patient-reported outcome measures (PROMs) were used. LIMITATIONS: Some studies only vaguely reported the measures utilized, and the review yielded a low number of clinical trials. CONCLUSION: In addition to evaluating disease activity with clinician-reported measures, the field could obtain critical knowledge on the patient experience by including high-quality PROMs of symptoms and functioning. More clinical trials using a variety of outcomes and measures are necessary to determine the most suitable course of treatment for LS patients.

All-body concept and quantified limits of cooperativity and related effects in homodromic cyclic water clusters from a molecular-wide and electron density-based approach.

We strongly advocate distinguishing cooperativity from cooperativity-induced effects. From the MOWeD-based approach, the origin of all-body cooperativity is synonymous with physics- and quantum-based processes of electron (e) delocalization throughout water clusters. To this effect, over 10 atom-pairs contribute to the total e-density at a BCP(H,O) between water molecules in a tetramer. Intermolecular all-body e-delocalization, that is, cooperativity, is an energy-minimizing process that fully explains non-additive increase in stability of a water molecule in clusters with an increase in their size. A non-linear change in cooperativity and cooperativity-induced effects, such as (i) structural (e.g., a change in d(O,O)) or topological intra- and intermolecular properties in water clusters (e.g., electron density or potential energy density at bond critical points) is theoretically reproduced by the proposed expression. It predicted the limiting value of delocalized electrons by a H2O molecule in homodromic cyclic clusters to be 1.58e. O-atoms provide the vast majority of electrons that "travel throughout a cluster predominantly on a privileged exchange quantum density highway" (⋅⋅⋅O-H⋅⋅⋅O-H⋅⋅⋅O-H⋅⋅⋅) using Bader's classical bond paths as density bridges linking water molecules. There are, however, additional electron exchange channels that are not seen on molecular graphs as bond paths. A 3D visual representation of the "privileged" and "additional" exchange channels as well as detailed intra- and inter-molecular patterns of e-sharing and (de)localizing is presented. The energy stabilizing contribution made by three O-atoms of neighboring water molecules was found to be large (-597 kcal/mol in cyclic hexamer) and 5 times more significant than that of a classical O-H⋅⋅⋅O intermolecular H-bond.

Acute Localized Exanthematous Pustulosis in a 5-Year-Old Boy With Zosteriform Distrubiton.

Acute localized exanthematous pustulosis (ALEP) is typically a benign drug reaction that occurs shortly after drug intake. We report a five-year-old male who developed a localized, zosteriform pustular rash on his back 10 days after treatment with oseltamivir and ceftriaxone for an upper respiratory tract infection. The lesions, which appeared three days prior to presentation, were mildly itchy and resolved completely without scarring within two days of treatment with topical betamethasone valerate and fusidic acid. No bacterial growth was detected in the pustular culture. This case highlights the rare occurrence of ALEP in a pediatric patient and suggests variations from the EuroSCAR diagnostic criteria, which usually indicate a 72-hour onset post-drug intake, noting instead a 7-14 day onset in atypical cases.To best of our knowledge, This is the first report of ALEP presenting with a zosteriform distribution.

Magnetic Resonance Imaging in the Assessment and Management of Post-injection-Site Morphea.

Morphea, a form of localized scleroderma, can significantly affect individuals by causing skin tightening and discoloration. We describe the case of a 22-year-old woman who presented with progressive skin changes and discomfort in her right gluteal region following a history of an intramuscular injection in the right gluteal region. Clinical examination suggested morphea, prompting us to conduct an MRI to better understand the extent and nature of her condition. The MRI results revealed thickening of the skin layers and signs of inflammation, helping us differentiate between active inflammation and fibrosis. This case illustrates how MRI can provide crucial insights for managing morphea effectively.

Plasma burn-mind the gap.

The programme to design plasma scenarios for the Spherical Tokamak for Energy Production (STEP), a reactor concept aiming at net electricity production, seeks to exploit the inherent advantages of the spherical tokamak (ST) while making conservative assumptions about plasma performance. This approach is motivated by the large gap between present-day STs and future burning plasmas based on this concept. It is concluded that plasma exhaust in such a device is most likely to be manageable in a double null (DN) configuration, and that high core performance is favoured by positive triangularity (PT) plasmas with an elevated central safety factor. Based on a full technical and physics assessment of external heating and current drive (CD) systems, it was decided that the external CD is provided most effectively by microwaves. Operation with active resistive wall mode (RWM) stabilization as well as high elongation is needed for the most compact solution. The gap between existing devices and STEP is most pronounced in the area of core transport, owing to high normalized plasma pressure in the latter which changes qualitatively the nature of the turbulence controlling transport. Plugging this gap will require dedicated experiments, particularly on high-performance STs, and the development of reduced models that faithfully represent turbulent transport at high normalized pressure. Plasma scenarios in STEP will also need to be such that edge localized modes (ELMs) either do not occur or are small enough to be compatible with material lifetime limits. The high current needed for a power plant-relevant plasma leads to the unavoidable generation of high runaway electron beam current during a disruption, where novel mitigation techniques may be needed. This article is part of the theme issue 'Delivering Fusion Energy - The Spherical Tokamak for Energy Production (STEP)'.

Tunable Ag Nanocavity Enhanced Green Electroluminescence from SiNx:O Light-Emitting Diode.

As the driving source, highly efficient silicon-based light emission is urgently needed for the realization of optoelectronic integrated chips. Here, we report that enhanced green electroluminescence (EL) can be obtained from oxygen-doped silicon nitride (SiNx:O) films based on an ordered and tunable Ag nanocavity array with a high density by nanosphere lithography and laser irradiation. Compared with that of a pure SiNxO device, the green electroluminescence (EL) from the SiNx:O/Ag nanocavity array device can be increased by 7.1-fold. Moreover, the external quantum efficiency of the green electroluminescence (EL) is enhanced 3-fold for SiNx:O/Ag nanocavity arrays with diameters of 300 nm. The analysis of absorption spectra and the FDTD calculation reveal that the localized surface plasmon (LSP) resonance of size-controllable Ag nanocavity arrays and SiNx:O films play a key role in the strong green EL. Our discovery demonstrates that SiNx:O films coupled with tunable Ag nanocavity arrays are promising for silicon-based light-emitting diode devices of the AI period in the future.

Non-empirical peak shape methods based on the physical model of the one trap one recombination center model.

Any experimental Thermoluminescent (TL) glow-peak contains the activation energy information of its corresponding energy level within the band gap in insulating materials. The theory of peak shape methods (PSM) correlates the macroscopic geometrical characteristics of a single TL peak with activation energy of the level responsible for the TL peak by assuming that the area under a TL peak can be approximated by the area of a triangle. In this way the geometrical characteristics becomes the measure of the activation energy. In the present work new PSM expressions are derived, which are not empirical as the existing ones but are based of the physical model of one trap one recombination (OTOR) center. Three cases are considered. (I) Delocalized OTOR for re-trapping probability smaller than the recombination probability. (II) Delocalized OTOR for re-trapping probability greater than recombination probability. (III) Localized transitions OTOR model. The system of differential equations of each case model were solved analytically using the Lambert W function (or equivalently the Wright ω function). Then the resulted analytical expressions of TL intensity as a function of temperature were used to derive new PSM. The new PSM from all cases are formally exactly the same, having, however, strong differentiation in their coefficients. The functionality of the new expressions is tested and its comparison with pre-existing PSM is performed.

Global warming and coastal protected areas: A study on phytoplankton abundance and sea surface temperature in different regions of the Brazilian South Atlantic Coastal Ocean.

In this study, we examined the relationship between sea surface temperature (SST) and phytoplankton abundance in coastal regions of the Brazilian South Atlantic: São Paulo, Paraná, and Santa Catarina, and the Protection Area of Southern right whales (Eubalaena australis) in Santa Catarina (APA), a conservation zone established along 130 km of coastline. Using SST and chlorophyll-a (Chl-a) data from 2002 to 2023, we found significant differences in SST between the regions, with São Paulo having the highest SST, followed by Paraná and Santa Catarina. All locations showed a consistent increase in SST over the years, with North Santa Catarina, APA and São Paulo experiencing the lowest rate of increase. Correlation analyses between SST and Chl-a revealed a stronger inverse relationship in North Santa Catarina and APA, indicating an increased response of Chl-a to SST variations in this region. The presence of protected area appears to play an essential role in reducing the negative impacts of increasing SST. Specifically, while there is a wealth of research on the consequences of global warming on diverse coastal and oceanic areas, heterogeneity among different settings persists and the causes for this necessitating attention. Our findings have implications for both localized scientific approaches and broader climate policies, emphasizing the importance of considering coastal ecosystem resilience to climate change in future conservation and adaptation strategies.

Impact of nanosilver surface electronic distributions on serum protein interaction and hemocompatibility.

Translation of silver-based nanotechnology "from bench to bedside" requires a deep understanding of the molecular aspects of its biological action, which remains controversial at low concentrations and non-spherical morphologies. Here, we present a hemocompatibility approach based on the effect of the distinctive electronic charge distribution in silver nanoparticles (nanosilver) on blood components. On basis of spectroscopic, volumetric, microscopic, dynamic light scattering measurements, pro-coagulant activity tests and cellular inspection we determine that, at extremely low nanosilver concentrations (0.125 - 2.5 µg mL-1) there is a relevant interaction effect on serum albumin and on red blood cells. The explanation has its origin in the surface charge distribution of nanosilver and their electron-mediated energy transfer mechanism. Prism-shaped nanoparticles, with anisotropic charge distributions, act at the surface level generating a compaction of the native protein molecule, while the spherical nanosilver, by exhibiting isotropic surface charge, generates a polar environment comparable to the solvent. Both morphologies induce aggregation at NPs / BSA ≅ 0.044 molar ratio values without altering the coagulation cascade tests, although the spherical-shaped nanosilver has a negative impact on red blood cells. Overall, our results suggest that the electron distributions of nanosilver, even at extremely low concentrations, are a critical factor influencing the molecular structure of blood proteins and red blood cells' membranes. Isotropic forms of nanosilver should be considered with caution, as they are not always the least harmful.

Apalutamide for High-Risk Localized Prostate Cancer Following Radical Prostatectomy (Apa-RP).

PURPOSE: Approximately 25% to 50% of patients with high-risk localized prostate cancer experience biochemical recurrence (BCR) within 2 years of radical prostatectomy. The Apa-RP study (NCT04523207) investigated whether adjuvant apalutamide plus androgen deprivation therapy (ADT) in high-risk patients who have undergone radical prostatectomy improved BCR-free survival. MATERIALS AND METHODS: Apa-RP was a multicenter, open-label, single-arm, phase 2 study conducted in community urology practices in the US. High-risk patients who had radical prostatectomy received 12 cycles of apalutamide (240 mg daily; 28-day cycles) plus ADT. The primary end point was BCR-free survival. Secondary end points included testosterone recovery (≥150 ng/dL) and safety. RESULTS: One hundred eight patients were enrolled; median age was 66.0 years (range 46.0-77.0 years). Median preoperative PSA and baseline testosterone were 7.6 ng/mL (range 2.2-62.7 ng/mL) and 340.0 ng/dL (range 43.0-939.0 ng/dL), respectively. The BCR-free rate at 24 months (12 months after completion of planned therapy) was 100% (90% CI 93-100). Serum testosterone recovery rate (≥50 and ≥150 ng/dL) 12 months after treatment completion was 96% (95% CI 88-98) and 77% (95% CI 66-85), respectively. Overall, 107 (99%) patients experienced treatment-emergent adverse events, with 24 (22%) experiencing grade 3 to 4 events. CONCLUSIONS: In Apa-RP, BCR-free survival was 100% with 77% of patients having testosterone recovery (≥150 ng/dL) within 12 months of actual treatment completion and a manageable safety profile. These results provide proof of concept that treatment intensification with 12 cycles of apalutamide plus ADT could become an option for patients with high-risk localized prostate cancer who have undergone radical prostatectomy. TRIAL REGISTRATION: ClinicalTrials.gov Identifier: NCT04523207.

Design of Localized High Concentration Electrolytes for Fast-Charging Lithium-Ion Batteries.

Localized high-concentration electrolytes (LHCEs) have emerged as a promising class of electrolytes to improve the cycle life and energy density of lithium-ion batteries (LIBs). While their application in batteries with lithium-metal anodes is extensively investigated, their behavior in systems with graphite anodes has received less research attention. Herein, the behaviors of four electrolytes in Graphite | LiNiO2 cells are compared. By systematically varying the electrolyte compositions, the impacts of the solvation structure, solvent composition, and salt composition of LHCEs are identified on the rate capability, stability, and propensity for lithium plating in LIB full-cells. It is found that while the solvation structure and solvent composition each play an important role in determining rate capability, the substitution of LiPF6 salt with LiFSI maximizes the rate capability and suppresses irreversible lithium plating. It is now demonstrated via constant-potential cycling, that an appropriately formulated LHCE can, therefore, maintain high reversible capacity and safety under arbitrarily fast charging conditions.

Toward structure and metabolism of glycogen C1-C6 in humans at 7 T by localized 13C MRS using low-power bilevel broadband 1H decoupling.

This work aims to develop and implement a pulse-acquire sequence for three-dimensional (3D) single-voxel localized 13C MRS in humans at 7 T, in conjunction with bilevel broadband 1H decoupling, and to test its feasibility in vitro and in vivo in human calf muscle with emphasis on the detection of glycogen C1-C6. A localization scheme suitable for measuring fast-relaxing 13C signals in humans at 7 T was developed and implemented using the outer volume suppression (OVS) and one-dimensional image selected in vivo spectroscopy (ISIS-1D) schemes, similar to that which was previously reported in humans at 4 T. The 3D 13C localization scheme was followed by uniform 13C adiabatic excitation, all complemented with an option for bilevel broadband 1H decoupling to improve both 13C sensitivity and spectral resolution at 7 T. The performance of the pulse-acquire sequence was investigated in vitro on phantoms and in vivo in the human calf muscle of three healthy volunteers, while measuring glycogen C1-C6. In addition, T1 and T2 of glycogen C1-C6 were measured in vitro at 7 T, as well as T1 of glycogen C1 in vivo. The glycerol C2 and C1,3 lipid resonances were efficiently suppressed in vitro at 7 T using the OVS and ISIS-1D schemes, allowing distinct detection of glycogen C2-C6. While some glycerol remained in calf muscle in vivo, the intense lipid at 130 ppm was efficiently suppressed. The 13C sensitivity and spectral resolution of glycogen C1-C6 in vitro and glycogen C1 in vivo were improved at 7 T using bilevel broadband 1H decoupling. The T1 and T2 of glycogen C1-C6 in vitro at 7 T were consistent compared with those at 8.5 T, while the T1 of glycogen C1 in vivo at 7 T resulted similar to that in vitro. Localized 13C MRS is feasible in human calf muscle in vivo at 7 T, and this will allow further extension of this method for 13C MRS measurements such as in the brain.

[Moderately hypofractionated dose escalation radiotherapy for localized prostate cancer, ESHYPRO: Results of a retrospective single-centre series evaluating safety and efficacy]. / Escalade de dose en radiothérapie modérément hypofractionnée pour les cancers de la prostate localisés, ESHYPRO : résultats d'une série monocentrique rétrospective évaluant la toxicité et l'efficacité.

PURPOSE: Prostate cancer is the most frequent cancer among men and radiotherapy hypofractionation regimens have become standard treatments for the localized stages, but the absence of increased risk of acute and late genitourinary or gastrointestinal toxicity of the dose escalation still must be demonstrated. MATERIAL AND METHODS: The study population included all patients with localized prostatic adenocarcinoma treated at the institut Curie from February 2016 to March 2018 by external radiation delivered by a linear accelerator using an image-guided conformal intensity modulation technique at a total dose of 75Gy in 30 fractions of 2.5Gy in the planning target volume that included the prostate and the proximal seminal vesicles, and could be paired with a prophylactic lymph node radiotherapy at 46Gy in 23 fractions with simultaneous integrated boost. RESULTS: A total of 166 patients were included. Among them, 68.6% were unfavourable intermediate or (very) high risk. The median age and follow-up were 71.4years and 3.96years. One hundred and forty-nine patients received prophylactic lymph node radiotherapy (89.8%). One hundred and thirty-one patients received hormonotherapy (78.9%). Genito-urinary toxicity events of grades 2 or above during radiotherapy, at 6months, 1year and 5years were respectively 36.7%, 8.8%, 3.1% and 4.7%. Two patients had late grade 4 toxicity at 5years (1.6%). Grade 2 gastrointestinal toxicity events during radiotherapy, 6months, 1year and 5years were respectively 15.1%, 1.9%, 14.6% and 9.3%. Of these, eight patients had grade 3 toxicity (6.2%). There was no grade 4 toxicity. Analyses did not reveal any predictive factor for toxicity. The 5-year overall, progression-free, and specific survival rates were respectively 82.4%, 85.7%, and 93.3%. Serum prostate specific antigen concentration and cardiovascular risk factors were found to be predictive factors of deterioration in overall survival (P=0.0028 for both). CONCLUSION: External radiotherapy for localized prostatic cancer with our moderately hypofractionated dose escalation regimen is well tolerated. In the absence of increased late toxicity, the analysis of the modes of long-term relapses will be interesting to determine the benefit of this dose escalation on local and distant relapses.

Distribution of Single-Particle Resonances Determines the Plasmonic Response of Disordered Nanoparticle Ensembles.

Understanding how colloidal soft materials interact with light is crucial to the rational design of optical metamaterials. Electromagnetic simulations are computationally expensive and have primarily been limited to model systems described by a small number of particles-dimers, small clusters, and small periodic unit cells of superlattices. In this work we study the optical properties of bulk, disordered materials comprising a large number of plasmonic colloidal nanoparticles using Brownian dynamics simulations and the mutual polarization method. We investigate the far-field and near-field optical properties of both colloidal fluids and gels, which require thousands of nanoparticles to describe statistically. We show that these disordered materials exhibit a distribution of particle-level plasmonic resonance frequencies that determines their ensemble optical response. Nanoparticles with similar resonant frequencies form anisotropic and oriented clusters embedded within the otherwise isotropic and disordered microstructures. These collectively resonating morphologies can be tuned with the frequency and polarization of incident light. Knowledge of particle resonant distributions may help to interpret and compare the optical responses of different colloidal structures, correlate and predict optical properties, and rationally design soft materials for applications harnessing light.