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At least 127 records · Page 7

Assessing the impacts of assimilating IASI and MOPITT CO retrievals using CESM-CAM-chem and DART

We report on the results and evaluation with independent measurements from assimilating both MOPITT (Measurements Of Pollution In The Troposphere) and IASI (Infrared Atmospheric Sounding Interferometer) retrieved profiles into the Community Earth System Model (CESM). We used the Data Assimilation Research Testbed ensemble Kalman filter technique, with the full atmospheric chemistry CESM component Community Atmospheric Model with Chemistry. We first discuss the methodology and evaluation of the current data assimilation system with coupled meteorology and chemistry data assimilation. The various capabilities of MOPITT and IASI retrievals are highlighted, with specific attention to instrument vertical sensitivity and coverage and how these impact the analyses. MOPITT and IASI CO retrievals mostly constrain the CO fields close to the main anthropogenic, biogenic, and biomass burning CO sources. In the case of IASI CO assimilation, we also observe constraints on CO far from the sources. During the simulation time period (June and July 2008), CO assimilation of both instruments strongly improves the atmospheric CO state as compared to independent observations, with the higher spatial coverage of IASI providing better results on the global scale. Yet, the enhanced sensitivity of multispectral MOPITT observations to near surface CO over the main source regions provides synergistic effects at regional scales.

54 ENVIRONMENTAL SCIENCES↗

Toward a chemical reanalysis in a coupled chemistry-climate model: An evaluation of MOPITT CO assimilation and its impact on tropospheric composition

Here, we examine in detail a 1 year global reanalysis of carbon monoxide (CO) that is based on joint assimilation of conventional meteorological observations and Measurement of Pollution in The Troposphere (MOPITT) multispectral CO retrievals in the Community Earth System Model (CESM). Our focus is to assess the impact to the chemical system when CO distribution is constrained in a coupled full chemistry-climate model like CESM. To do this, we first evaluate the joint reanalysis (MOPITT Reanalysis) against four sets of independent observations and compare its performance against a reanalysis with no MOPITT assimilation (Control Run). We then investigate the CO burden and chemical response with the aid of tagged sectoral CO tracers. We estimate the total tropospheric CO burden in 2002 (from ensemble mean and spread) to be 371 ± 12% Tg for MOPITT Reanalysis and 291 ± 9% Tg for Control Run. Our multispecies analysis of this difference suggests that (a) direct emissions of CO and hydrocarbons are too low in the inventory used in this study and (b) chemical oxidation, transport, and deposition processes are not accurately and consistently represented in the model. Increases in CO led to net reduction of OH and subsequent longer lifetime of CH 4 (Control Run: 8.7 years versus MOPITT Reanalysis: 9.3 years). Yet at the same time, this increase led to 5-10% enhancement of Northern Hemisphere O 3 and overall photochemical activity via HO x recycling. Such nonlinear effects further complicate the attribution to uncertainties in direct emissions alone. This has implications to chemistry-climate modeling and inversion studies of longer-lived species.

54 ENVIRONMENTAL SCIENCES↗

Visible/near-infrared spectral diversity from in situ observations of the Bagnold Dune Field sands in Gale Crater, Mars

As part of the Bagnold Dune campaign conducted by Mars Science Laboratory rover Curiosity, visible/near–infrared reflectance spectra of dune sands were acquired using Mast Camera (Mastcam) multispectral imaging (445–1013 nm) and Chemistry and Camera (ChemCam) passive point spectroscopy (400–840 nm). By comparing spectra from pristine and rover–disturbed ripple crests and troughs within the dune field, and through analysis of sieved grain size fractions, constraints on mineral segregation from grain sorting could be determined. In general, the dune areas exhibited low relative reflectance, a weak ~530 nm absorption band, an absorption band near 620 nm, and a spectral downturn after ~685 nm consistent with olivine–bearing sands. The finest grain size fractions occurred within ripple troughs and in the subsurface and typically exhibited the strongest ~530 nm bands, highest relative reflectances, and weakest red/near–infrared ratios, consistent with a combination of crystalline and amorphous ferric materials. Coarser–grained samples were the darkest and bluest and exhibited weaker ~530 nm bands, lower relative reflectances, and stronger downturns in the near–infrared, consistent with greater proportions of mafic minerals such as olivine and pyroxene. These grains were typically segregated along ripple crests and among the upper surfaces of grain flows in disturbed sands. Sieved dune sands exhibited progressive decreases in reflectance with increasing grain size, as observed in laboratory spectra of olivine size separates. In conclusion, the continuum of spectral features observed between the coarse– and fine–grained dune sands suggests that mafic grains, ferric materials, and air fall dust mix in variable proportions depending on aeolian activity and grain sorting.

79 ASTRONOMY AND ASTROPHYSICS↗

Multimodal Imaging of Autofluorescent Sites Reveals Varied Chemical Speciation in SSZ-13 Crystals

In this report a multimodal imaging study of chabazite is used to analyse emissive deposits. A notable difference is seen in the morphology of agglomerated surface deposits and larger subsurface deposits. Comparison of the distribution of organic residue throughout the crystal volume and XRF mapping is demonstrating that a fluorescence-based technique can also be used to indirectly comment on the compositional chemistry of the inorganic framework. A multimodal imaging study of chabazite is used to show the distribution of and discriminate between different emissive deposits arising as a result of the detemplation process. Confocal imaging, 3D fluorescence lifetime imaging, 3D multispectral fluorescence imaging, and Raman mapping are used to show three different types of emissive behaviours each characterised by different spatial distributions, trends in lifetime, spectral signals, and Raman signatures. A notable difference is seen in the morphology of agglomerated surface deposits and larger subsurface deposits, which experience lifetime augmentation due to spatial confinement. The distribution of organic residue throughout the crystal volume is comparable to XRF mapping that shows Si enrichment on the outer edges and higher Al content through the centre, demonstrating that a fluorescence-based technique can also be used to indirectly comment on the compositional chemistry of the inorganic framework.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Possibility of an integrated transmission electron microscope: enabling complex in-situ experiments

Abstract Multimodal in-situ experiments are the wave of the future, as this approach will permit multispectral data collection and analysis during real-time nanoscale observation. In contrast, the evolution of technique development in the electron microscopy field has generally trended toward specialization and subsequent bifurcation into more and more niche instruments, creating a challenge for reintegration and backward compatibility for in-situ experiments on state-of-the-art microscopes. We do not believe this to be a requirement in the field; therefore, we propose an adaptive instrument that is designed to allow nearly simultaneous collection of data from aberration-corrected transmission electron microscopy (TEM), probe-corrected scanning transmission electron microscopy, ultrafast TEM, and dynamic TEM with a flexible in-situ testing chamber, where the entire instrument can be modified as future technologies are developed. The value would be to obtain a holistic understanding of the underlying physics and chemistry of the process-structure–property relationships in materials exposed to controlled extreme environments. Such a tool would permit the ability to explore, in-situ, the active reaction mechanisms in a controlled manner emulating those of real-world applications with nanometer and nanosecond resolution. If such a powerful tool is developed, it has the potential to revolutionize our materials understanding of nanoscale mechanisms and transients. Graphical Abstract

36 MATERIALS SCIENCE↗

Tree-level carbon stock estimations across diverse species using multi-source remote sensing integration

Forests are critical carbon sinks, and remote sensing has been increasingly widely used for forest monitoring and biomass estimations. However, species-specific tree-level studies remain limited. In this study, we demonstrated the feasibility of integrating UAV-based LiDAR with high-resolution optical satellite imagery (0.5 m) to estimate biomass for individual trees across different species. The proposed method accurately estimated biomass for 53 trees (R² = 0.82, rRMSE = 0.44), with species-specific datasets, showing an average 25.2% increase in R² and a 14.8% reduction in rRMSE. A novel vegetation index combining forest structure parameters with vegetation indices (VIs) was developed using high-resolution multispectral satellite data (3 m) to explore its relationship with individual tree biomass. Combining forest structural parameters with VIs further improved estimation accuracy, achieving an R²of 0.89 and an rRMSE of 0.34. Species-specific datasets show an 11.6% increase in R²compared to methods without VIs, and a 22.2% improvement over methods using only VIs. SHapley Additive exPlanations (SHAP) analysis shows that the volume feature played a key role in model performance and remained stable throughout the training process. Altogether, the proposed approach enhances individual tree biomass and carbon sink estimations, showing great potential for large-scale precise forest carbon monitoring using multi-source remote sensing data.

59 BASIC BIOLOGICAL SCIENCES↗

Elucidate the molecular basis of ampholytic chitosan as a high-performance cryoprotectant to myosin denaturation: The importance of saccharide charges

The uses of charged poly/oligo-saccharides enable the retarding of protein denaturation against various environmental stresses during food storage and manufacturing. However, at subzero temperatures, the molecular basis of such stabilization behaviors, i.e., cryoprotections, remain less explored. Here, in this study, we introduced an ampholytic saccharide, carboxymethyl chitooligosaccharide (CMCO) that effectively inhibited the freezing-induced myosin denaturation. The in-depth cryoprotective mechanism was systematically investigated by using molecular dynamic simulation and multispectral characterizations. Results showed that CMCO may interact with myosin through hydrogen bonding and electrostatic interactions, which caused the expelling of water at protein surfaces and the reduced conformational flexibility of myosin molecules. Due to this water replacement event, both secondary and ternary structures of myosin became freezing-resistant, leading to the inhibited protein aggregations and retained functionalities, such as solubility, Ca 2+ -ATPase activity, and gelling properties. Moreover, cryoprotective behaviors of CMCO were charge-dependent. CMCO with a higher degree of carboxymethyl substitution (DS: 1.2) was inclined to bind and stabilize myosin molecules better than the low-DS (DS: 0.8) one, even though both outperformed other cryoprotective saccharides. Therefore, this investigation not only introducing a high-performance myosin cryoprotectant, but also elaborated the cryoprotective mechanism of ampholytic saccharides.

59 BASIC BIOLOGICAL SCIENCES↗

Bioluminescence Tomography–Guided Radiation Therapy for Preclinical Research

Purpose: In preclinical radiation research, it is challenging to localize soft tissue targets based on cone beam computed tomography (CBCT) guidance. As a more effective method to localize soft tissue targets, we developed an online bioluminescence tomography (BLT) system for small-animal radiation research platform (SARRP). We demonstrated BLT-guided radiation therapy and validated targeting accuracy based on a newly developed reconstruction algorithm. Methods and Materials: The BLT system was designed to dock with the SARRP for image acquisition and to be detached before radiation delivery. A 3-mirror system was devised to reflect the bioluminescence emitted from the subject to a stationary charge-coupled device (CCD) camera. Multispectral BLT and the incomplete variables truncated conjugate gradient method with a permissible region shrinking strategy were used as the optimization scheme to reconstruct bioluminescent source distributions. To validate BLT targeting accuracy, a small cylindrical light source with high CBCT contrast was placed in a phantom and also in the abdomen of a mouse carcass. The center of mass (CoM) of the source was recovered from BLT and used to guide radiation delivery. The accuracy of the BLT-guided targeting was validated with films and compared with the CBCT-guided delivery. In vivo experiments were conducted to demonstrate BLT localization capability for various source geometries. Results: Online BLT was able to recover the CoM of the embedded light source with an average accuracy of 1 mm compared to that with CBCT localization. Differences between BLT- and CBCT-guided irradiation shown on the films were consistent with the source localization revealed in the BLT and CBCT images. In vivo results demonstrated that our BLT system could potentially be applied for multiple targets and tumors. Conclusions: The online BLT/CBCT/SARRP system provides an effective solution for soft tissue targeting, particularly for small, nonpalpable, or orthotopic tumor models.

62 RADIOLOGY AND NUCLEAR MEDICINE↗

Quantifying the influences of spectral resolution on uncertainty in leaf trait estimates through a Bayesian approach to RTM inversion

The remote monitoring of plant canopies is critically needed for understanding of terrestrial ecosystem mechanics and biodiversity as well as capturing the short- to long-term responses of vegetation to disturbance and climate change. A variety of orbital, sub-orbital, and field instruments have been used to retrieve optical spectral signals and to study different vegetation properties such as plant biochemistry, nutrient cycling, physiology, water status, and stress. Radiative transfer models (RTMs) provide a mechanistic link between vegetation properties and observed spectral features, and RTM spectral inversion is a useful framework for estimating these properties from spectral data. However, existing approaches to RTM spectral inversion are typically limited by the inability to characterize uncertainty in parameter estimates. Here, we introduce a Bayesian algorithm for the spectral inversion of the PROSPECT 5 leaf RTM that is distinct from past approaches in two important ways: First, the algorithm only uses reflectance and does not require transmittance observations, which have been plagued by a variety of measurement and equipment challenges. Second, the output is not a point estimate for each parameter but rather the joint probability distribution that includes estimates of parameter uncertainties and covariance structure. We validated our inversion approach using a database of leaf spectra together with measurements of equivalent water thickness (EWT) and leaf dry mass per unit area (LMA). The parameters estimated by our inversion were able to accurately reproduce the observed reflectance (RMSE VIS = 0.0063, RMSE NIR-SWIR = 0.0098) and transmittance (RMSE VIS = 0.0404, RMSE NIR-SWIR = 0.0551) for both broadleaved and conifer species. Inversion estimates of EWT and LMA for broadleaved species agreed well with direct measurements (CV EWT = 18.8%, CV LMA = 24.5%), while estimates for conifer species were less accurate (CV EWT = 53.2%, CV LMA = 63.3%). To examine the influence of spectral resolution on parameter uncertainty, we simulated leaf reflectance as observed by ten common remote sensing platforms with varying spectral configurations and performed a Bayesian inversion on the resulting spectra. We found that full-range hyperspectral platforms were able to retrieve all parameters accurately and precisely, while the parameter estimates of multispectral platforms were much less precise and prone to bias at high and low values. We also observed that variations in the width and location of spectral bands influenced the shape of the covariance structure of parameter estimates. Lastly, our Bayesian spectral inversion provides a powerful and versatile framework for future RTM development and single- and multi-instrumental remote sensing of vegetation.

54 ENVIRONMENTAL SCIENCES↗

NASA's surface biology and geology designated observable: A perspective on surface imaging algorithms

The 2017-2027 National Academies' Decadal Survey, Thriving on Our Changing Planet, recommended Surface Biology and Geology (SBG) as a "Designated Targeted Observable" (DO). The SBG DO is based on the need for capabilities to acquire global, high spatial resolution, visible to shortwave infrared (VSWIR; 380 - 2500 nm; ~30 m pixel resolution) hyperspectral (imaging spectroscopy) and multispectral midwave and thermal infrared (MWIR: 3-5 µm; TIR: 8-12 µm; ~60 m pixel resolution) measurements with sub-monthly temporal revisits over terrestrial, freshwater, and coastal marine habitats. To address the various mission design needs, an SBG Algorithms Working Group of multidisciplinary researchers has been formed to review and evaluate the algorithms applicable to the SBG DO across a wide range of Earth science disciplines, including terrestrial and aquatic ecology, atmospheric science, geology, and hydrology. Here, we summarize current state-of-the-practice VSWIR and TIR algorithms that use airborne or orbital spectral imaging observations to address the SBG DO priorities identified by the Decadal Survey: (i) terrestrial vegetation physiology, functional traits, and health; (ii) inland and coastal aquatic ecosystems physiology, functional traits, and health; (iii) snow and ice accumulation, melting, and albedo; (iv) active surface composition (eruptions, landslides, evolving landscapes, hazard risks); (v) effects of changing land use on surface energy, water, momentum, and carbon fluxes; and (vi) managing agriculture, natural habitats, water use/quality, and urban development. We review existing algorithms in the following categories: snow/ice, aquatic environments, geology, and terrestrial vegetation, and summarize the community-state-of-practice in each category. Finally, this effort synthesizes the findings of more than 130 scientists.

54 ENVIRONMENTAL SCIENCES↗

Using soil library hyperspectral reflectance and machine learning to predict soil organic carbon: Assessing potential of airborne and spaceborne optical soil sensing

Soil organic carbon (SOC) is a key variable to determine soil functioning, ecosystem services, and global carbon cycles. Spectroscopy, particularly optical hyperspectral reflectance coupled with machine learning, can provide rapid, efficient, and cost-effective quantification of SOC. However, how to exploit soil hyperspectral reflectance to predict SOC concentration, and the potential performance of airborne and satellite data for predicting surface SOC at large scales remain relatively underknown. Here, this study utilized a continental-scale soil laboratory spectral library (37,540 full-pedon 350–2500 nm reflectance spectra with SOC concentration of 0–780 g·kg –1 across the US) to thoroughly evaluate seven machine learning algorithms including Partial-Least Squares Regression (PLSR), Random Forest (RF), K-Nearest Neighbors (KNN), Ridge, Artificial Neural Networks (ANN), Convolutional Neural Networks (CNN), and Long Short-Term Memory (LSTM) along with four preprocessed spectra, i.e. original, vector normalization, continuum removal, and first-order derivative, to quantify SOC concentration. Furthermore, by using the coupled soil-vegetation-atmosphere radiative transfer model, we simulated twelve airborne and spaceborne hyper/multi-spectral remote sensing data from surface bare soil laboratory spectra to evaluate their potential for estimating SOC concentration of surface bare soils. Results show that LSTM achieved best predictive performance of quantifying SOC concentration for the whole data sets (R 2 = 0.96, RMSE = 30.81 g·kg –1 ), mineral soils (SOC ≤ 120 g·kg –1 , R 2 = 0.71, RMSE = 10.60 g·kg –1 ), and organic soils (SOC > 120 g·kg –1 , R 2 = 0.78, RMSE = 62.31 g·kg –1 ). Spectral data preprocessing, particularly the first-order derivative, improved the performance of PLSR, RF, Ridge, KNN, and ANN, but not LSTM or CNN. We found that the SOC models of mineral and organic soils should be distinguished given their distinct spectral signatures. Finally, we identified that the shortwave infrared is vital for airborne and spaceborne hyperspectral sensors to monitor surface SOC. This study highlights the high accuracy of LSTM with hyperspectral/multispectral data to mitigate a certain level of noise (soil moisture <0.4 m 3 ·m –3 , green leaf area < 0.3 m 2 ·m –2 , plant residue <0.4 m 2 ·m –2 ) for quantifying surface SOC concentration. Forthcoming satellite hyperspectral missions like Surface Biology and Geology (SBG) have a high potential for future global soil carbon monitoring, while high-resolution satellite multispectral fusion data can be an alternative.

54 ENVIRONMENTAL SCIENCES↗

Airborne hyperspectral imaging of cover crops through radiative transfer process-guided machine learning

Cover cropping between cash crop growing seasons is a multifunctional conservation practice. Timely and accurate monitoring of cover crop traits, notably aboveground biomass and nutrient content, is beneficial to agricultural stakeholders to improve management and understand outcomes. Currently, there is a scarcity of spatially and temporally resolved information for assessing cover crop growth. Remote sensing has a high potential to fill this need, but conventional empirical regression operated with coarse-resolution multispectral data has large uncertainties. Therefore, this study utilized airborne hyperspectral imaging techniques and developed new process-guided machine learning approaches (PGML) for cover crop monitoring. Specifically, we deployed an airborne hyperspectral system covering visible to shortwave-infrared wavelengths (400–2400 nm) to acquire high spatial (0.5 m) and spectral (3–5 nm) resolution reflectance over 23 cover crop fields across Central Illinois in March and April of 2021. Airborne hyperspectral surface reflectance with high spectral and spatial resolution can be well matched with field data to quantify cover crop traits. Furthermore, the PGML models were pre-trained by synthetic data from soil-vegetation radiative transfer modeling (one million records), and then fine-tuned with field data of cover crop biomass and nutrient content. Results show that airborne hyperspectral data with PGML can achieve high accuracy to predict cover crop aboveground biomass (R 2 = 0.72, relative RMSE = 15.16%) and nitrogen content (R 2 = 0.69, relative RMSE = 16.59%) through leave-one-field-out cross-validation. Unlike the pure data-driven approach (e.g., partial least-squares regression), PGML incorporated radiative transfer knowledge and obtained higher predictive performance with fewer field data. Meanwhile, with field data for model fine-tuning, PGML predicted biomass more accurately than the inversion of radiative transfer models. Here we also found that the red edge has a high contribution in quantifying aboveground biomass and nitrogen content, followed by green and shortwave spectra. This study demonstrated the first attempt of utilizing hyperspectral remote sensing to accurately quantify cover crop traits. We highlight the strength of PGML in exploiting sensing data to quantify ecosystem variables to advance agroecosystem monitoring for sustainable agricultural management.

60 APPLIED LIFE SCIENCES↗

Dynamic and accurate assessment of acetaminophen-induced hepatotoxicity by integrated photoacoustic imaging and mechanistic biomarkers in vivo

The prediction and understanding of acetaminophen (APAP)-induced liver injury (APAP-ILI) and the response to therapeutic interventions is complex. This is due in part to sensitivity and specificity limitations of currently used assessment techniques. Here we sought to determine the utility of integrating translational non-invasive photoacoustic imaging of liver function with mechanistic circulating biomarkers of hepatotoxicity with histological assessment to facilitate the more accurate and precise characterization of APAP-ILI and the efficacy of therapeutic intervention. Perturbation of liver function and cellular viability was assessed in C57BL/6J male mice by Indocyanine green (ICG) clearance (Multispectral Optoacoustic Tomography (MSOT)) and by measurement of mechanistic (miR-122, HMGB1) and established (ALT, bilirubin) circulating biomarkers in response to the acetaminophen and its treatment with acetylcysteine (NAC) in vivo. We utilised a 60% partial hepatectomy model as a situation of defined hepatic functional mass loss to compared acetaminophen-induced changes to. Integration of these mechanistic markers correlated with histological features of APAP hepatotoxicity in a time-dependent manner. They accurately reflected the onset and recovery from hepatotoxicity compared to traditional biomarkers and also reported the efficacy of NAC with high sensitivity. ICG clearance kinetics correlated with histological scores for acute liver damage for APAP (i.e. 3 h timepoint; r = 0.90, P < 0.0001) and elevations in both of the mechanistic biomarkers, miR-122 (e.g. 6 h timepoint; r = 0.70, P = 0.005) and HMGB1 (e.g. 6 h timepoint; r = 0.56, P = 0.04). For the first time we report the utility of this non-invasive longitudinal imaging approach to provide direct visualisation of the liver function coupled with mechanistic biomarkers, in the same animal, allowing the investigation of the toxicological and pharmacological aspects of APAP-ILI and hepatic regeneration. - Highlights: • Imaging and circulating biomarker “tool box” proposed for liver injury and repair. • Liver function monitored in real time during acetaminophen hepatotoxicity. • Approach based on ICG clearance measured by MSOT. • ICG kinetics correlates with established methods for liver injury detection. • Approach can be used for prediction of response to therapeutic interventions.

60 APPLIED LIFE SCIENCES↗

Comparing land surface temperature and mean radiant temperature for urban heat mapping in Philadelphia

Many cities are experiencing more frequent extreme heat during hot summers. With the rise of global temperature, the thermal comfort in urban areas become even worse. Quantitative information of the spatial distributions of urban heat has become increasingly important for resilience and adaptation to climate change in cities. This study compares satellite-derived land surface temperature (LST) and urban microclimate modeling-based mean radiant temperature (Tmrt) for mapping the urban heat distributions in Philadelphia, Pennsylvania, USA. Here, the LST was estimated based on Landsat 8 thermal imagery with a spatial resolution of around 100 m, while the Tmrt was simulated based on high resolution LiDAR and national aerial imagery program multispectral aerial imageries with a spatial resolution of 1 m. Result shows that both LST and Tmrt show a similar general pattern of the urban heat across the study area, while the Tmrt presents much more details of the heat variations street by street and neighborhood by neighborhood. The LST tends to have a stronger relationship with the Tmrt on building roofs, which are usually not the place for human activities. This studyprovides evidence for choosing more appropriate metrics in urban heat-related studies.

54 ENVIRONMENTAL SCIENCES↗

Electrochemical Structure of the Plasma–Liquid Interface

Nonthermal atmospheric pressure plasma in contact with a liquid yields a variety of energetic photons, ions, and electrons, which can be transported into the plasma–liquid interface (PLI). Similar to the electrochemical interface formed between a solid electrode and electrolyte in conventional electrochemical systems, the charge-transfer process across the PLI is able to promote reduction–oxidation (redox) reactions. However, in the case of free plasma jets in contact with liquids, the absence of solid electrodes obscures the spatial locations of the electrochemical half-reactions. Herein, we present a spatial electrochemical measurement technique used to characterize an aqueous solution in contact with an atmospheric pressure plasma jet. The technique is based on measuring the potential difference between two identical Ag/AgCl electrochemical electrodes positioned at different locations within the solution. More specifically, electrochemical maps were made by measuring the potential of one electrochemical electrode positioned at different locations near the PLI with respect to the other electrochemical electrode positioned far away from the PLI in the bulk solution. Regions in the map with negative and positive potential differences between these electrochemical electrodes were used to identify the electrodeless cathode and anode, respectively. Here, visualization of the spatial distribution of molecular colorimetric redox indicators by multispectral imaging revealed that reduction was occurring near the plasma jet centerline while oxidation was occurring further away in solution, which constitutes an independent confirmation of the electrochemical maps.

Absorption↗

3D Volumetric Structural Hierarchy Induced by Colloidal Polymerization of a Quantum-Dot Ionic Liquid Monomer Conjugate

Hierarchically structured emissive quantum dot (CdS/CdSe) poly(ionic liquid) composites are synthesized through colloidal polymerization within a lyotropic liquid crystal, yielding a solvent-responsive nanoparticle (NP) composite possessing four ordered structural motifs. The composite is prepared by coassembling an amphiphilic ionic liquid (IL) monomer, 3-decyl-1-vinylimidazolium chloride, [C 10 VIm + ][Cl - ], and IL monomer, 3-(10-mercaptodecyl)-1-vinylimidazolium bromide surface-functionalized quantum dots, QD-[SC 10 VIm + ][Br - ], in 30 wt % water. Photo (UV)-initiated free radical polymerization serves to form a colloidal copolymer that collimates pairs of QDs within the core of large cylinders (average diameter = 21 nm and length = 422 nm), as evidenced by ultrasmall-angle X-ray scattering (USAXS). As revealed by continuous wave terahertz multispectral reconstructive 3-D imaging, the subsurface structure along the cylinder axis undergoes dynamic rearrangement between 2D hexagonal and cubic packing. The polymerized ionic liquid sheath surrounding the QDs is composed of concentric hexagonally perforated lamellae (HPL) with an interlamellar repeat distance of 3 nm, as determined by small-angle X-ray scattering (SAXS). The encapsulated QDs retain crystallinity (TEM and WAXS) and emission characteristics (photoluminescence spectroscopy, lambda(EM) = 638 nm). Phenomenological time-dependent Ginzburg-Landau calculations verify the mesoscale cylinders arise from the topological constraints imposed by the in-plane perforations of the polymerized ionic liquid as it wraps around the hard (unmalleable) spherical QDs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Designing an Observing System to Study the Surface Biology and Geology (SBG) of the Earth in the 2020s

Abstract Observations of planet Earth from space are a critical resource for science and society. Satellite measurements represent very large investments and United States (US) agencies organize their effort to maximize the return on that investment. The US National Research Council conducts a survey of Earth science and applications to prioritize observations for the coming decade. The most recent survey prioritized a visible to shortwave infrared imaging spectrometer and a multispectral thermal infrared imager to meet a range of needs for studying Surface Biology and Geology (SBG). SBG will be the premier integrated observatory for observing the emerging impacts of climate change by characterizing the diversity of plant life and resolving chemical and physiological signatures. It will address wildfire risk, behavior, and recovery as well as responses to hazards such as oil spills, toxic minerals in minelands, harmful algal blooms, landslides, and other geological hazards. The SBG team analyzed needed instrument characteristics (spatial, temporal, and spectral resolutions, measurement uncertainty) and assessed the cost, mass, power, volume, and risk of different architectures. We present an overview of the Research and Applications trade‐study analysis of algorithms, calibration and validation needs, and societal applications with specifics of substudies detailed in other articles in this special collection. We provide a value framework to converge from hundreds down to three candidate architectures recommended for development. The analysis identified valuable opportunities for international collaboration to increase the revisit frequency, adding value for all partners, leading to a clear measurement strategy for an observing system architecture.

54 ENVIRONMENTAL SCIENCES↗

Plasmonic photoconductive terahertz focal-plane array with pixel super-resolution

Abstract Imaging systems operating in the terahertz part of the electromagnetic spectrum are attractive due to their ability to penetrate many opaque materials and provide unique spectral signatures of various chemicals. However, the use of terahertz imagers in real-world applications has been limited by the slow speed, large size, high cost and complexity of present systems, largely due to the lack of suitable terahertz focal-plane array detectors. Here we report a terahertz focal-plane array that can directly provide the spatial amplitude and phase distributions, along with the ultrafast temporal and spectral information of an imaged object. It consists of a two-dimensional array of ~0.3 million plasmonic photoconductive nanoantennas optimized to rapidly detect broadband terahertz radiation with a high signal-to-noise ratio. We utilized the multispectral nature of the amplitude and phase data captured by these plasmonic nanoantennas to image different objects, including super-resolved etched patterns in a silicon substrate and defects in battery electrodes. By eliminating the need for raster scanning and spatial terahertz modulation, our terahertz focal-plane array offers more than a 1,000-fold increase in the imaging speed compared with the state of the art and potentially suits a broad range of applications in industrial inspection, security screening and medical diagnosis, among others.

Optics↗