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At least 1,207 records · Page 67

Satellite Optical Remote Sensing of Clouds and Aerosols: From Particle Single-Scattering and Gaseous Absorption Through Radiative Transfer to Retrieval Products

Clouds and aerosols are fundamental regulators of Earth’s radiation budget and climate system, influencing both solar and terrestrial radiation through scattering, absorption, and emission processes. Accurate characterization of their physical and radiative properties from space requires a rigorous understanding of particle single-scattering, gaseous absorption, and radiative transfer in the atmosphere, as well as reliable inversion methods. This review synthesizes the physical foundations and algorithmic implementations of satellite-based passive optical remote sensing of clouds and aerosols, spanning the ultraviolet to thermal infrared spectral range. Beginning with electromagnetic scattering theory and state-of-the-art methods for computing single-scattering by nonspherical particles and computationally efficient methods for accounting for atmospheric absorption, we discuss the radiative transfer framework underpinning cloud and aerosol retrievals. The connection between single-scattering and multiple-scattering is rigorously formulated. We then summarize operational and research-grade retrieval techniques, including cloud masking and thermodynamic phase determination, CO₂ slicing for cloud-top pressure, the Nakajima-King shortwave bi-spectral, and infrared split-window approaches for cloud optical thickness and effective particle size, inversion algorithms for determining aerosol properties from multi-spectral and/or multi-angle radiometric and polarimetric measurements, and active-passive sensing synergy. Examples of the global cloud and aerosol climatologies are illustrated using observations from the Moderate Resolution Imaging Spectroradiometer (MODIS) and the Multi-angle Imaging SpectroRadiometer (MISR). Furthermore, the unique strengths of active remote sensing techniques based on spaceborne lidar observations are briefly elaborated in the context of studying ice clouds composed of randomly and horizontally oriented ice crystals, which is a significant challenge for conventional passive remote sensing techniques. By connecting physical theory to practical retrievals, this review highlights both the maturity of current methodologies and the remaining challenges in reducing uncertainties in particle morphology, vertical structure, absorption, and aerosol-cloud interactions. Furthermore, the impact of artificial intelligence (AI) on atmospheric remote sensing is briefly addressed.

Aerosols↗

Mutual separation of Am/Cm/Ln by the use of Novel-Triamide, NTAamide and water-soluble diglycolamide

The new extractant, NTAamide (C8) (N,N,N',N',N'',N''-hexa-octyl-nitriro-tri-acetamide) is a triamide having nitrogen and oxygen atoms in the central frame, then NTAamide (C8) has hybrid performance of complexation to metals by soft and hard donors. It is clear that NTAamide(C8) can extract trivalent An from diluted nitric acid showing small D(Ln), then the separation of An from Ln can be carried out. The separation factor (SF) of Am/Cm by NTAamide(C8) is approximate 1.78-2.08, which is not so high to separate each other. The combination of NTAamide(C8) of extractant and TEDGA (N,N,N',N'-tetraethyl-diglycolamide) as a masking agent shows relatively high SF(Am/Cm) of maximal 6.5. It is obvious that NTAamide(C8) is a promising extractant to achieve the mutual separation among Am/Cm/Ln. The concept of flow-sheet for Am/Cm/Ln separation is designed using NTAamide(C8) and TEDGA. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Mount Logan ice core record of tropical and solar influences on Aleutian Low variability: 500-1998 A.D.

Continuous, high-resolution paleoclimate records from the North Pacific region spanning the past 1500 years are rare; and the behavior of the Aleutian Low (ALow) pressure center, the dominant climatological feature in the Gulf of Alaska, remains poorly constrained. Here we present a continuous, 1500 year long, calibrated proxy record for the strength of the wintertime (December–March) ALow from the Mount Logan summit (PR Col; 5200 m asl) ice core soluble sodium time series. We show that ice core sodium concentrations are statistically correlated with North Pacific sea level pressure and zonal wind speed. Our ALow proxy record reveals a weak ALow from circa 900–1300 A.D. and 1575–1675 A.D., and a comparatively stronger ALow from circa 500–900 A.D., 1300–1575 A.D., and 1675 A.D. to present. The Mount Logan ALow proxy record shows strong similarities with tropical paleoclimate proxy records sensitive to the El Niño–Southern Oscillation and is consistent with the hypothesis that the Medieval Climate Anomaly was characterized by more persistent La Niña-like conditions while the Little Ice Age was characterized by at least two intervals of more persistent El Niño-like conditions. The Mount Logan ALow proxy record is significantly (p <0.05) correlated and coherent with solar irradiance proxy records over various time scales, with stronger solar irradiance generally associated with a weaker ALow and La Niña-like tropical conditions. However, a step-like increase in ALow strength during the Dalton solar minimum circa 1820 is associated with enhanced Walker circulation. Furthermore, rising CO 2 forcing or internal variability may be masking the twentieth century rise in solar irradiance.

Meteorology & Atmospheric Sciences↗

Isopycnal mixing by mesoscale eddies significantly impacts oceanic anthropogenic carbon uptake

Abstract Anthropogenic carbon dioxide uptake varies across Earth System Models for reasons that have remained obscure. When varied within a single model, the lateral eddy mixing coefficient A Redi produces a range of uptake similar to the modeled range. The highest uptake, resulting from a simulation with a constant A Redi of 2400 m 2 /s, simulates 15% more historical carbon uptake than a model with A Redi = 400 m 2 /s. A sudden doubling in carbon dioxide produces a 21% range in carbon uptake across the models. Two spatially dependent representations of A Redi produce uptake that lies in the middle of the range of constant values despite predicting very large values in the subtropical gyres. One‐dimensional diffusive models of the type used for integrated assessments can be fit to the simulations, with A Redi accounting for a substantial fraction of the effective vertical diffusion. Such models, however, mask significant regional changes in stratification and biological carbon storage.

Gnanadesikan, Anand↗

Mass Spectrometry-based Assay for High Throughput and High Sensitivity Biomarker Verification

Searching for disease specific biomarkers has become a major undertaking in the biomedical research field as the effective diagnosis, prognosis and treatment of many complex human diseases are largely determined by the availability and the quality of the biomarkers. A successful biomarker as an indicator to a specific biological or pathological process is usually selected from a large group of candidates by a strict verification and validation process. To be clinically useful, the validated biomarkers must be detectable and quantifiable by the selected testing techniques in their related tissues or body fluids. Due to its easy accessibility, protein biomarkers would ideally be identified in blood plasma or serum. However, most disease related protein biomarkers in blood exist at very low concentrations (<1ng/mL) and are “masked” by many none significant species at orders of magnitude higher concentrations. The extreme requirements of measurement sensitivity, dynamic range and specificity make the method development extremely challenging. The current clinical protein biomarker measurement primarily relies on antibody based immunoassays, such as ELISA. Although the technique is sensitive and highly specific, the development of high quality protein antibody is both expensive and time consuming. The limited capability of assay multiplexing also makes the measurement an extremely low throughput one rendering it impractical when hundreds to thousands potential biomarkers need to be quantitatively measured across multiple samples. Mass spectrometry (MS)-based assays have recently shown to be a viable alternative for high throughput and quantitative candidate protein biomarker verification. Among them, the triple quadrupole MS based assay is the most promising one. When it is coupled with liquid chromatography (LC) separation and electrospray ionization (ESI) source, a triple quadrupole mass spectrometer operating in a special selected reaction monitoring (SRM) mode, also known as multiple reaction monitoring (MRM), is capable of quantitatively measuring hundreds of candidate protein biomarkers from a relevant clinical sample in a single analysis. The specificity, reproducibility and sensitivity could be as good as ELISA. Furthermore, SRM MS can also quantify protein isoforms and post-translational modifications, for which traditional antibody-based immunoassays often don’t exist.

Environmental Molecular Sciences Laboratory↗

Discovering Hidden Material Properties of MgCl 2 at Atomic Resolution with Structured Temporal Electron Illumination of Picosecond Time Resolution

Abstract A combination of atomic resolution phase contrast electron microscopy and pulsed electron beams reveals pristine properties of MgCl 2 at 1.7 Å resolution that were previously masked by air and beam damage. Both the inter‐ and intra‐layer bonding in pristine MgCl 2 are weak, which leads to uncommonly large local orientation variations that characterize this Ziegler–Natta catalyst support. By delivering electrons with 1–10 ps pulses and ≈160 ps delay times, phonons induced by the electron irradiation in the material are allowed to dissipate before the subsequent delivery of the next electron packet, thus mitigating phonon accumulations. As a result, the total electron dose can be extended by a factor of 80–100 to study genuine material properties at atomic resolution without causing object alterations, which is more effective than reducing the sample temperature. In conditions of minimal damage, beam currents approach femtoamperes with dose rates around 1 eÅ −2 s −1 . Generally, the utilization of pulsed electron beams is introduced herein to access genuine material properties while minimizing beam damage.

Kisielowski, Christian↗

Orbital Angular Momentum from Self‐Assembled Concentric Nanoparticle Rings

Abstract Ring‐shaped nanostructures can focus, filter, and manipulate electromagnetic waves, but are challenging to incorporate into devices using standard nanofabrication techniques. Directed self‐assembly (DSA) of block copolymers (BCPs) on lithographically patterned templates has successfully been used to fabricate concentric rings and spirals as etching masks. However, this method is limited by BCP phase behavior and material selection. Here, a straightforward approach to generate ring‐shaped nanoparticle assemblies in thin films of supramolecular nanocomposites is demonstrated. DSA is used to guide the formation of concentric rings with radii spanning 150–1150 nm and ring widths spanning 30–60 nm. When plasmonic nanoparticles are used, ring nanodevice arrays can be fabricated in one step, and the completed devices produce high‐quality orbital angular momentum (OAM). Nanocomposite DSA simplifies and streamlines nanofabrication by producing metal structures without etching or deposition steps; it also introduces interparticle coupling as a new design axis. Detailed analysis of the nanoparticle ring assemblies confirms that the supramolecular system self‐regulates the spatial distribution of its components, and thus exhibits a degree of flexibility absent in DSA of BCPs alone, where structures are determined by polymer‐pattern incommensurability. The present studies also provide guidelines for developing self‐regulating DSA as an alternative to incommensurability‐driven methods.

Vargo, Emma↗

Encapsulating High–Temperature Superconducting Twisted van der Waals Heterostructures Blocks Detrimental Effects of Disorder

High-temperature cuprate superconductors based van der Waals (vdW) heterostructures hold high technological promise. One of the obstacles hindering their progress is the detrimental effect of disorder on the properties of the vdW-devices-based Josephson junctions (JJs). Here, a new method of fabricating twisted vdW heterostructures made of Bi 2 Sr 2 CuCa 2 O 8+δ , crucially improving the JJ characteristics and pushing them up to those of the intrinsic JJs in bulk samples, is reported. The method combines cryogenic stacking using a solvent-free stencil mask technique and covering the interface by insulating hexagonal boron nitride crystals. Despite the high-vacuum condition down to 10 –6 mbar in the evaporation chamber, the interface appears to be protected from water molecules during the in situ metal deposition only when fully encapsulated. Comparing the current-voltage curves of encapsulated and unencapsulated interfaces, it is revealed that the encapsulated interfaces' characteristics are crucially improved, so that the corresponding JJs demonstrate high critical currents and sharpness of the superconducting transition comparable to those of the intrinsic JJs. Finally, it is shown that the encapsulated heterostructures are more stable over time.

2D materials↗

Thermal Disorder‐Induced Strain and Carrier Localization Activate Reverse Halide Segregation

The reversal of halide ions is studied under various conditions. However, the underlying mechanism of heat-induced reversal remains unclear. This work finds that dynamic disorder-induced localization of self-trapped polarons and thermal disorder-induced strain (TDIS) can be co-acting drivers of reverse segregation. Localization of polarons results in an order of magnitude decrease in excess carrier density (polaron population), causing a reduced impact of the light-induced strain (LIS – responsible for segregation) on the perovskite framework. Meanwhile, exposing the lattice to TDIS exceeding the LIS can eliminate the photoexcitation-induced strain gradient, as thermal fluctuations of the lattice can mask the LIS strain. Under continuous 0.1 W cm -2 illumination (upon segregation), the strain disorder is estimated to be 0.14%, while at 80 °C under dark conditions, the strain is 0.23%. However, in situ heating of the segregated film to 80 °C under continuous illumination (upon reversal) increases the total strain disorder to 0.25%, where TDIS is likely to have a dominant contribution. Therefore, the contribution of entropy to the system's free energy is likely to dominate, respectively. Various temperature-dependent in situ measurements and simulations further support the results. These findings highlight the importance of strain homogenization for designing stable perovskites under real-world operating conditions.

36 MATERIALS SCIENCE↗

Manufacturing Over Many Scales: High Fidelity Macroscale Coverage of Nanoporous Metal Arrays via Lift-Off-Free Nanofabrication

A low-cost, high-throughput, lift-off-free nanolithographic method is developed for creating hexagonal arrays of sub-30-nm-sized pores on a metal film, achieving uniform coverage over an entire wafer of 10 cm in diameter. Additionally, spherical nanodomains of poly(methyl methacrylate) are demonstrated to be well-controlled and self-aligned within a polystyrene matrix layer on a metal thin film without any intermediary coating. After removal of PMMA, the porous PS thin film acts as an etch mask for defining nanoscale pores in the metal underlayer by Ar ion beam milling, resulting in wafer-scale patterning with great fidelity.

36 MATERIALS SCIENCE↗

Electrical Transport Anisotropy Controlled by Oxygen Vacancy Concentration in (111) LaAlO 3 /SrTiO 3 Interface Structures

The two dimensional conducting gas that forms at the interface between the two insulators LaAlO 3 (LAO) and SrTiO 3 (STO)1, 2 has garnered a lot of attention due to wide variety of physical phenomena that it exhibits, including strong spin–orbit coupling,3, 4 superconductivity,5-8 magnetism,7-12 and localization effects,13 among others. From the earliest studies,1 it has been well established that the conditions during film growth or the post-growth treatment of samples can have a substantial effect on the properties of the interface. In particular, the amount of oxygen vacancies introduced during growth or through post-growth treatment can change the conductance of the LAO/STO interface by orders of magnitude.2, 13-17 Experiments on bulk STO18 samples and STO films19 indicate that the enhanced conduction induced by oxygen vacancies is associated with defect states introduced in the band gap of the STO at the interface, adding donor levels close to the STO conduction band edge, and acceptor levels near the valence band.18, 19 All of these earlier studies were performed on samples grown in the (001) crystal orientation. Here we report studies of the effects of various post-growth treatments on the transport properties of (111) oriented LAO/STO interface structures, which have been shown to exhibit a strong anisotropy of their properties along different crystal directions.20 As with the (001) samples, we find that the presence of oxygen vacancies increases the conductance of the interface, but at the same time also substantially decreases the anisotropy. This suggests that the defect states introduced by oxygen vacancies contribute isotropically to charge transport, partially masking the strongly anisotropic contribution of the intrinsic bands. In addition, our work shows that one can reversibly tune the transport properties of LAO/STO interface samples by applying appropriate post-growth treatment.

36 MATERIALS SCIENCE↗

Janus Membranes via Diffusion-Controlled Atomic Layer Deposition

The first use of atomic layer deposition (ALD) to produce Janus membranes is reported, with an example system consisting of a compositional gradient ranging from hydrophilic Al 2 O 3 on one face to hydrophobic poly(propylene) on the opposite face. Alternating pulses of trimethyl aluminum and water vapor lead to the growth of covalently bonded Al 2 O 3 conforming to the membrane pore surfaces. Precise control of ALD parameters significantly affects the surface wetting of the modified membrane face and the depth of Al 2 O 3 infiltration into the porosity. This depth control derives from slow precursor diffusion through the 200 nm membrane pores compared to much faster ALD surface reactions. For a given precursor exposure and purge time, increasing the number of ALD cycles decreases the water contact angle at the modified surface from hydrophobic to hydrophilic, until the water droplet is completely imbibed by the membrane. To demonstrate the utility of these Janus membranes, a hydrophilic/superaerophobic Janus treatment is shown to greatly reduce the size of air bubbles generated through the membrane, enabling faster mixing. This technique represents the first application of vapor-deposited covalently bonded metal oxides to form Janus membranes. Further opportunities are afforded by the ability to laterally pattern Al 2 O 3 across the membrane surface via physical masking.

36 MATERIALS SCIENCE↗

Dual‐Scale Nanostructures via Evaporative Assembly

Abstract Dual‐scale hierarchical structures with regular microscale patterns and varying degree of nanoscale crystalline order are synthesized on physically and chemically homogeneous substrates by evaporative self‐assembly with a suspension of DNA‐functionalized nanoparticles (NPs) with a charged core shell. For a certain NP concentration range, periodic concentric rings in a stripe‐like micropattern are produced over macroscale surface areas by an NP monolayer with hexagonal lattice structure at the nanoscale. The stripe width, spacing, and nanoparticle ordering can be controlled by varying the NP concentration. The results indicate that the interplay between “stick‐slip” motion of the droplet contact line and coulombic and steric NP interactions control the formation of the observed structures. A simple analytical model is proposed to account for the experimental observations and guide the future design of different nanostructure morphologies. This work demonstrates a simple cost‐effective mask‐free method for fabricating large‐area nanostructured 2D materials and metasurfaces for applications ranging from energy conversion/storage to optoelectronics and nanophotonics.

Srivastava, Sunita↗

Evaporative Assembly: Dual-Scale Nanostructures via Evaporative Assembly (Adv. Mater. Interfaces 7/2020)

In article number 1901954, Sunita Srivastava, Surita R. Bhatia, and co-workers demonstrate that evaporative assembly of functionalized nanoparticles can yield striking dual-scale hierarchical structures. Regular microscale stripes of nanoparticle monolayers with hexagonal nanoscale order are obtained on physically and chemically homogeneous substrates through evaporation of a suspension of DNAfunctionalized nanoparticles with a charged shell. The stripe width, spacing and nanoparticle ordering can be controlled by varying nanoparticle concentration and can be described by a simple analytical model. The results indicate that the interplay between “stick-slip” motion of the droplet contact line and Coulombic and steric nanoparticle interactions control the formation of the observed structures. Finally, this work demonstrates a simple cost-effective mask-free method for fabricating nanostructured 2D materials and metasurfaces for applications ranging from energy conversion/storage to optoelectronics and nanophotonics.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

An Aerosol Jet Printed Resistance Temperature Detector‐Micro Hotplate with Temperature Coefficient of Resistance Stabilized by Electrical Sintering

Abstract Aerosol jet printing (AJP) is an emerging direct write tool enabling rapid prototyping and fabrication of electronics components. AJP provides faster and less expensive production of devices with feature sizes of >10 microns compared to traditional MEMS processes. Herein, the fabrication of a resistance temperature detector‐micro hotplate (RTD‐µHP) is reported using AJP printed silver. AJP eliminates sophisticated MEMS processes such as masking, alignment, and etching. The compatibility of the AJP process with a broad range of materials is demonstrated by printing highly resolved lines on rigid and flexible substrates. Optimal thermal sintering conditions of AJP printed silver (Ag) lines are found by in situ resistance measurements. To stabilize the temperature coefficient of resistance (TCR) of the RTD‐µHP at high operating current levels, electrical sintering is performed on the RTD‐µHPs. Electrical sintering improves the conductivity of fully thermally sintered Ag RTD‐µHPs by 32% and provides a burn‐in mechanism for stabilizing the TCR. The TCR of the RTD‐µHPs after electrical sintering is 3.80 × 10 −3 at 22 °C, close to the value for bulk Ag. The performance of the RTD‐µHPs is tested using a reference thermocouple. The RTD‐µHPs show reliable and repeatable heating and temperature sensing up to 70 °C in air.

Sui, Yongkun↗

Molecular Layer Deposited Aluminum‐Based Hybrid Resist for High‐Resolution Nanolithography and Direct Ultra‐High Aspect Ratio Pattern Transfer

Inorganic-containing hybrid photoresists are critical for next-generation extreme ultraviolet (EUV) lithography and angstrom-era semiconductor miniaturization. However, associated conventional solution processing struggles to achieve ultrathin, uniform films with high conformality and compositional control, limiting overall patterning performance. Here, this study reports the systematic lithographic patterning characterization of an Al-based hybrid resist synthesized via vapor-phase molecular layer deposition (MLD), using the trimethylaluminum (TMA) metal precursor and the hydroquinone (HQ) aromatic organic linker. The resist supports both sub-20 nm high-resolution nanolithography and virtually infinite silicon plasma etch selectivity. Lithographic performance studied using electron beam lithography (EBL) as a proxy for EUV shows that, under an optimized process adopting post-exposure bake, the resist achieves the best resolution of 15.4 nm linewidth under stringent 1:1 line-space high-density patterning—limited only by the minimum beam size of the EBL system. The resist also shows wide dose latitude and balanced performance in resolution, roughness, and sensitivity. The infinite silicon etch selectivity, stemming from spontaneous aluminum oxyfluoride passivation layer formation, enables fabrication of micrometer-tall, 40 nm-wide silicon nanofin structures using only a ≈30 nm-thick resist layer, without no hard mask. These results highlight the potential of MLD-based hybrid resists for developing next-generation resist materials for micro/nanoelectronics manufacturing.

36 MATERIALS SCIENCE↗

Designing Magnetic Anisotropy through Strain Doping

Abstract The coupling between a material's lattice and its underlying spin state links structural deformation to magnetic properties; however, traditional strain engineering does not allow the continuous, post‐synthesis control of lattice symmetry needed to fully utilize this fundamental coupling in device design. Uniaxial lattice expansion induced by post‐synthesis low energy helium ion implantation is shown to provide a means of bypassing these limitations. Magnetocrystalline energy calculations can be used a priori to estimate the predictive design of a material's preferred magnetic spin orientation. The efficacy of this approach is experimentally confirmed in a spinel CoFe 2 O 4 model system where the epitaxial film's magnetic easy axis is continuously manipulated between the out‐of‐plane (oop) and in‐plane (ip) directions as lattice tetragonality moves from ip to oop with increasing strain doping. Macroscopically gradual and microscopically abrupt changes to preferential spin orientation are demonstrated by combining ion irradiation with simple beam masking and lithographic procedures. The ability to design magnetic spin orientations across multiple length scales in a single crystal wafer using only crystal symmetry considerations provides a clear path toward the rational design of spin transfer, magnetoelectric, and skyrmion‐based applications where magnetocrystalline energy must be dictated across multiple length scales.

36 MATERIALS SCIENCE↗