Crystallization of nanoparticles induced by precipitation of trace polymeric additives
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99 GENERAL AND MISCELLANEOUS↗
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Structure of the RECK CC domain, an evolutionary anomaly
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99 GENERAL AND MISCELLANEOUS↗
Nanoscale dynamics during self-organized ion beam patterning of Si. II. Kr + bombardment
Understanding the self-organized ion beam nanopatterning of elemental semiconductors, particularly silicon, is of intrinsic scientific and technological interest. This is the second component of a two-part coherent x-ray scattering and x-ray photon correlation spectroscopy (XPCS) investigation of the kinetics and fluctuation dynamics of nanoscale ripple development on silicon during 1 keV Ar + (part I) and Kr + bombardment at 65° polar angle. Here it is found that the ion-enhanced viscous flow relaxation is essentially equal for Kr + -induced patterning as previously found for Ar + patterning despite the difference in ion masses. However, the magnitude of the surface curvature-dependent roughening rate in the early-stage kinetics is larger for Kr + than for Ar + , consistent with expectations that the heavier ion gives an increased mass redistributive contribution to the initial surface instability. As with the Ar + case, fluctuation dynamics in the late stage show a peak in correlation times at the length scale corresponding to the dominant structural feature on the surface—the ripples. Finally, it is shown that speckle motion during the surface evolution can be analyzed to determine spatial inhomogeneities in erosion rate and ripple velocity. This allows the direction and speed of ripple motion to be measured in a real time experiment. In the present case, ripple motion is found to be into the projected direction of the ion source, in contrast to expectations from an existing sputter erosion driven model with parameters derived from binary collision approximation simulations.
36 MATERIALS SCIENCE↗
Sea Level Rise in the CESM Large Ensemble: The Role of Individual Climate Forcings and Consequences for the Coming Decades
The emergence of a spatial pattern in the externally forced response (FR) of dynamic sea level (DSL) during the altimeter era has recently been demonstrated using climate models but our understanding of its initial emergence, drivers, and implications for the future is poor. Here the anthropogenic forcings of the DSL pattern are explored using the Community Earth System Model Large Ensemble (CESM-LE) and Single-Forcing Large Ensemble, a newly available set of simulations where values of individual forcing agents remain fixed at 1920 levels, allowing for an estimation of their effects. Statistically significant contributions to the DSL FR are identified for greenhouse gases (GHGs) and industrial aerosols (AERs), with particularly strong contributions resulting from AERs in the mid-twentieth century and GHGs in the late twentieth and twenty-first century. Secondary, but important, contributions are identified for biomass burning aerosols in the equatorial Atlantic Ocean in the mid-twentieth century, and for stratospheric ozone in the Southern Ocean during the late twentieth century. Key to understanding regional DSL patterns are ocean heat content and salinity anomalies, which are driven by surface heat and freshwater fluxes, ocean dynamics, and the spatial structure of seawater thermal expansivity. Finally, potential implications for the interpretation of DSL during the satellite era and the longer records from tide gauges are suggested as a topic for future research.
54 ENVIRONMENTAL SCIENCES↗
Adjoint-optimized nanoscale light extractor for nitrogen-vacancy centers in diamond
Abstract We designed a nanoscale light extractor (NLE) for the efficient outcoupling and beaming of broadband light emitted by shallow, negatively charged nitrogen-vacancy (NV) centers in bulk diamond. The NLE consists of a patterned silicon layer on diamond and requires no etching of the diamond surface. Our design process is based on adjoint optimization using broadband time-domain simulations and yields structures that are inherently robust to positioning and fabrication errors. Our NLE functions like a transmission antenna for the NV center, enhancing the optical power extracted from an NV center positioned 10 nm below the diamond surface by a factor of more than 35, and beaming the light into a ±30° cone in the far field. This approach to light extraction can be readily adapted to other solid-state color centers.
42 ENGINEERING↗
Tracking precipitation features and associated large-scale environments over southeastern Texas
Abstract. Deep convection initiated under different large-scale environmental conditions exhibits different precipitation features and interacts with local meteorology and surface properties in distinct ways. Here, we analyze the characteristics and spatiotemporal patterns of different types of convective systems over southeastern Texas using 13 years of high-resolution observations and reanalysis data. We find that mesoscale convective systems (MCSs) contribute significantly to both mean and extreme precipitation in all seasons, while isolated deep convection (IDC) plays a role in intense precipitation during summer and fall. Using self-organizing maps (SOMs), we found that convection can occur under unfavorable conditions without large-scale lifting or moisture convergence. In spring, fall, and winter, front-related large-scale meteorological patterns (LSMPs) characterized by low-level moisture convergence act as primary triggers for convection, while the remaining storms are associated with an anticyclonic pattern and orographic lifting. In summer, IDC events are mainly associated with front-related and anticyclonic LSMPs, while MCSs occur more in front-related LSMPs. We further tracked the life cycle of MCS and IDC events using the Flexible Object Tracker algorithm over southeastern Texas. MCSs frequently initiate west of Houston, traveling eastward for around 8 h to southeastern Texas, while IDC events initiate locally. The average duration of MCSs in southeastern Texas is 6.1 h, approximately 4.1 times the duration of IDC events. Diurnally, the initiation of convection associated with favorable LSMPs peaks at 11:00 UTC, 3 h earlier than that associated with anticyclones.
54 ENVIRONMENTAL SCIENCES↗
Hydration Mechanisms in Nanoparticle Interaction and Surface Energetics
Work on the project advanced molecular level understanding, prediction and control of nanoscale hydration in salt solutions under electric stimuli or ionic patterning. Permeation of nanoporous electrodes at preset voltage underlies the function of ultracapacitors. Transitory regulation of wetting in nanoporous media by electric field spans an array of applications in materials, energy storage, and separation sciences. The physically related modulation of nanoparticle solubility by surface charges can significantly extend the range of the nanomaterial applications, improve processing techniques, and potentially alleviate environmental concerns. Pore/solution equilibria, and activated kinetics of liquid gating by nanoconfined electrolytes are challenging problems at the forefront of experimental and theoretical research. Addressing these problems from a molecular perspective required the development of state-of-the-art simulation algorithms in statistical mechanics to capture complex processes in open systems under electric control. Parallel studies of wetting and dispersibility of polar and ionizing particles aim to uncover predictive relations between electrowetting, chemical functionalization, and geometry of nanomaterial particles. By nonequilibrium dynamic modeling, we elucidated electrolyte flow in nanochanels and associated electrokinetic energy conversion. Research on the program provided training opportunities for the next generation of scientists in computational chemistry. Insights, and methods from the project implicate broad segment of researchers in energy and nanosciences, materials and surface chemistry.
74 ATOMIC AND MOLECULAR PHYSICS↗
Spring Dust in Colorado Plateau: Transport Pathways and Interannual Variability Derived From Two Decades of MERRA‐2 Reanalysis
Spring dust storms in the U.S. Southwest significantly impact environmental and human systems, yet their climatological patterns and driving mechanisms remain poorly understood. Using two decades of MERRA-2 reanalysis data and self-organizing map clustering, we identified four distinct dust transport pathways from surrounding and remote deserts for the top 10% of spring dust events impacting the Colorado Plateau: (a) intense southwesterly near-surface transport where eastward upward transport is blocked by topography, (b) substantial remote transport plus weaker surface emissions, (c) moderate southwesterly transport with stronger upper-level transport, and (d) rare northwesterly pattern linked to the Great Basin sources, which accounts for 38%, 14%, 37%, and 11% of total events, respectively. The frequency and intensity of these events strongly correlate with large-scale climate variability, with increased dust events during La Niña. Our results provide a robust framework for improving seasonal dust forecasts and understanding future dust dynamics under climate change.
aerosol transport↗
Understanding the diversity of the West African monsoon system change projected by CORDEX-CORE regional climate models
Understanding real uncertainties in projections is needed to support actions of decision and policy makers. In this study, two state-of-the-art regional climate models with ~ 25 km horizontal resolution forced with three different global climate models are employed to investigate the response of the West African Monsoon (WAM) system under the low (RCP2.6) and high (RCP8.5) emission scenarios. We make a step towards assessing the plausibility of rainfall change (ΔPr) patterns based on the models’ ability to realistically represent the WAM system under the historical period, and by analyzing changes in mechanisms associated with ΔPr patterns. Under global warming, experiments exhibit diverse ΔPr patterns underpinned by different combinations of mechanisms operating simultaneously. A dipole-like surface pressure change between the Sahara Desert and the Guinea Coast appears to be a differentiating factor between experiments featuring homogeneous or increased rainfall over all or a part of the Sahel from those simulating heterogeneous or reduced rainfall over the same domain. This dipole acts by modulating the amount and the extent of deepening of the monsoon flux inland, and hence the latitudinal positioning of the monsoon convective system. This process contributes to moistening the whole or central and eastern Sahel in some experiments while drying the Guinea Coast. The West African Westerly Jet (WAWJ) is responsible for strengthening and moistening the western Sahel under RCP2.6. However, the WAMJ becomes much stronger under RCP8.5 and may have contributed to the drying of the western Sahel by shifting moisture eastwards in addition to the mid-tropospheric moisture divergence through enhanced African Easterly Jet. Furthermore, for experiments expecting wetting (drying) of the Sahel, the strengthening (weakening) of the tropical easterly jet may have contributed to the projected intensification (reduction) of WAM rainfall by favoring uplift (downlift) above 600 hPa. It also emerges that the ΔPr patterns from REMO2015 experiments are likely more plausible than those from RegCM4-v7. The impacts of strong warming on the regional hydrological cycle are further investigated and we found that changes gradually intensify with the level of radiative forcing, highlighting the importance of mitigating warming as recommended by the Paris agreement.
CORDEX-CORE↗
Ni/CeO 2 Nanocatalysts with Optimized CeO 2 Support Morphologies for CH 4 Oxidation
Catalytic oxidation of CH 4 over nonprecious Ni/CeO 2 catalysts has attracted wide attention. Controlling the morphology of a CeO 2 support can enhance the CH 4 oxidation activity without changing the catalyst composition. Here, in this paper, a series of 2 wt % Ni/CeO 2 nanocatalysts with different CeO 2 support morphologies (nanoparticles (P), rods (R), cubes (C)) and synthetic procedures (precipitation, sol-gel (SG)) were evaluated for their CH 4 oxidation performance. The redox properties of CeO 2 supports and corresponding Ni loaded catalysts were characterized by H 2 -temperature-programmed reduction and oxygen storage capacity (OSC) measurements. The relationship among the CeO 2 morphologies, surface areas, redox properties, and CH4 oxidation activity for both CeO 2 supports and Ni/CeO 2 catalysts was established. The findings suggest that CeO 2 -R has a greater amount of surface oxygen vacancies as well as an improved OSC and CH4 oxidation activity compared to CeO 2 -P and CeO 2 -C supports. The same CH 4 oxidation activity pattern was observed for the Ni containing catalysts (Ni/CeO 2 -R > Ni/CeO 2 -P > Ni/CeO 2 -C). Increasing the CeO 2 surface area by using a sol-gel synthesis method (CeO 2 -SG) improved the amount of surface oxygen vacancies and CH 4 oxidation performance of CeO 2 -SG and Ni/CeO 2 -SG compared to CeO 2 -R and Ni/CeO 2 -R, respectively. Finally, all studied Ni/CeO 2 nanocatalysts showed improved hydrothermal stability compared to conventional Pd/Al 2 O 3 .
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Improving CLM5.0 Biomass and Carbon Exchange Across the Western United States Using a Data Assimilation System
The Western United States is dominated by natural lands that play a critical role for carbon balance, water quality, and timber reserves. This region is also particularly vulnerable to forest mortality from drought, insect attack, and wildfires, thus requiring constant monitoring to assess ecosystem health. Carbon monitoring techniques are challenged by the complex mountainous terrain, thus there is an opportunity for data assimilation systems that combine land surface models and satellite-derived observations to provide improved carbon monitoring. Here, we use the Data Assimilation Research Testbed to adjust the Community Land Model (CLM5.0) with remotely sensed observations of leaf area and above-ground biomass. The adjusted simulation significantly reduced the above-ground biomass and leaf area, leading to a reduction in both photosynthesis and respiration fluxes. The reduction in the carbon fluxes mostly offset, thus both the adjusted and free simulation projected a weak carbon sink to the land. This result differed from a separate observation-constrained model (FLUXCOM) that projected strong carbon uptake to the land. Simulation diagnostics suggested water limitation had an important influence upon the magnitude and spatial pattern of carbon uptake through photosynthesis. We recommend that additional observations important for water cycling (e.g., snow water equivalent, land surface temperature) be included to improve the veracity of the spatial pattern in carbon uptake. Furthermore, the assimilation system should be enhanced to maximize the number of the simulated state variables that are adjusted, especially those related to the recommended observed quantities including water cycling and soil carbon.
54 ENVIRONMENTAL SCIENCES↗
Fabrication of low blaze angle gratings by replication and plasma etch
We suggest a new method of making ultra-low blaze angle gratings for synchrotron application. The method is based on reduction of the blaze angle of a master grating by replication followed by a plasma etch. A master blazed grating with a relatively large blaze angle is fabricated by anisotropic wet etching of a Si single crystal substrate. The surface of the master grating is replicated by a polymer material on top of a quartz substrate by nanoimprinting and then transferred into quartz by a plasma etch. Then a 2nd nanoimprint step is applied to transfer the saw-tooth surface into a resist layer on top of a Si grating substrate. The plasma etch through the patterned resist layer provides transfer of the grooves into the Si substrate and results in reduction of the blaze angle due to the difference in etch rates of the resist and Si. We investigated the impact of the replication process on the groove shape, facet surface roughness, and diffraction efficiency of the fabricated 200 lines/mm low blaze angle grating.
Park, Sooyeon↗
Effects of cation stoichiometry on surface morphology and crystallinity of ZnGeN 2 films grown on GaN by metalorganic chemical vapor deposition
ZnGeN 2 films were grown on GaN-on-sapphire templates via metalorganic chemical vapor deposition. Energy dispersive X-ray spectroscopy was used to estimate the Zn/(Zn+Ge) composition ratio in the films. This ratio decreased with increase in growth temperature but increased with increase in total reactor pressure or Zn/Ge precursor flow rate ratio. Systematic mapping of these key growth parameters has allowed us to identify the growth window to achieve ZnGeN 2 with stoichiometric cation composition. Compositional and statistical analyses performed on data acquired from atom probe tomography provided insight into the local compositional homogeneity. The cations Zn and Ge did not demonstrate segregation or clustering at the sub-nanometer level. Based on X-ray diffraction 2θ-ω scan profiles and transmission electron microscope nano-diffraction patterns, the films with near-stoichiometric cation ratios were single crystalline with planar surfaces, whereas zinc-rich or zinc-poor films were polycrystalline with nonplanar surfaces. The growth direction of the single crystalline ZnGeN 2 films on GaN templates was along the c-axis. Room temperature Raman spectra showed features associated with the phonon density of states, indicating the presence of cation disorder in the lattice. A cathodoluminescence peak associated with transitions involving deep level defects was observed around 640 nm. The intensity of this peak increased by almost 2.5 times as the temperature was reduced to 77 K from room temperature. A similar peak was observed in photoluminescence spectra collected at 80 K.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Regional patterns in hydrologic response, a new three-component metric for hydrograph analysis and implications for ecohydrology, Northwest Volcanic Aquifer Study Area, USA
Spatial patterns of hydrologic response were examined for the Northwest Volcanic Aquifer Study Area (NVASA). The utility of established hydrograph-separation methods for assessing hydrologic response in permeable volcanic terranes was assessed and a new three-component metric for hydrograph analysis was developed. The new metric, which partitions streamflow into subcomponents defined by the timescales of hydrologic response (e.g., fast-runoff, intermediate-interflow and slow-baseflow), was used to gain a fundamental understanding of the regional hydrology, investigate sub-regional differences, influencing factors, and ecohydrological implications. The combined effects of NVASA’s physiography, climate and geology create a strongly coupled surface-groundwater system that produces copious baseflow and limited quantities of runoff and interflow. Patterns of hydrologic response are influenced by the type and rate of precipitation and permeability of the underlying geology. Under variable precipitation conditions the hydrologic response of volcanic terranes with similar permeability and subsurface-storage capacity can be significantly different. From a water management and ecohydrology perspective, understanding regional patterns of hydrologic response and sub-regional differences is fundamental. Results indicate that minimum-flow methods provide the most conservative estimate of baseflow and may be the most robust for filtering out snowmelt bias in baseflow estimates. Baseflow contributes ~75% of the perennial streamflow across the NVASA and represents a critical component of the regional water supply that provides critical cold-water habitat.
54 ENVIRONMENTAL SCIENCES↗
Curvature-controlled geometrical lensing behavior in self-propelled colloidal particle systems
In many biological systems, the curvature of the surfaces cells live on influences their collective properties. Curvature should likewise influence the behavior of active colloidal particles. We show using molecular simulation of self-propelled active particles on surfaces of Gaussian curvature (both positive and negative) how curvature sign and magnitude can alter the system's collective behavior. Curvature acts as a geometrical lens and shifts the critical density of motility-induced phase separation (MIPS) to lower values for positive curvature and higher values for negative curvature, which we explain theoretically by the nature of parallel lines in spherical and hyperbolic space. Curvature also fluidizes dense MIPS clusters due to the emergence of defect patterns disrupting the crystalline order inside the clusters. Using our findings, we engineer three confining surfaces that strategically combine regions of different curvature to produce a host of novel dynamical behaviors, including cyclic MIPS on spherocylinders, directionally biased cyclic MIPS on spherocones, and position dependent cluster fluctuations on metaballs.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Evaluation of E3SM land model snow simulations over the western United States
Abstract. Seasonal snow has crucial impacts on climate, ecosystems, and humans, but it is vulnerable to global warming. The land component (ELM) of the Energy Exascale Earth System Model (E3SM) mechanistically simulates snow processes from accumulation, canopy interception, compaction, and snow aging to melt. Although high-quality field measurements, remote sensing snow products, and data assimilation products with high spatio-temporal resolution are available, there has been no systematic evaluation of the snow properties and phenology in ELM. This study comprehensively evaluates ELM snow simulations over the western United States at 0.125∘ resolution during 2001–2019 using the Snow Telemetry (SNOTEL) in situ networks, MODIS remote sensing products (i.e., MCD43 surface albedo product), the spatially and temporally complete (STC) snow-covered area and grain size (MODSCAG) and MODIS dust and radiative forcing in snow (MODDRFS) products (STC-MODSCAG/STC-MODDRFS), and the snow property inversion from remote sensing (SPIReS) product and two data assimilation products of snow water equivalent and snow depth – i.e., University of Arizona (UA) and SNOw Data Assimilation System (SNODAS). Overall the ELM simulations are consistent with the benchmarking datasets and reproduce the spatio-temporal patterns, interannual variability, and elevation gradients for different snow properties including snow cover fraction (fsno), surface albedo (αsur) over snow cover regions, snow water equivalent (SWE), and snow depth (Dsno). However, there are large biases of fsno with dense forest cover and αsur in the Rocky Mountains and Sierra Nevada in winter, compared to the MODIS products. There are large discrepancies of snow albedo, snow grain size, and light-absorbing particle-induced snow albedo reduction between ELM and the MODIS products, attributed to uncertainties in the aerosol forcing data, snow aging processes in ELM, and remote sensing retrievals. Against UA and SNODAS, ELM has a mean bias of −20.7 mm (−35.9 %) and −20.4 mm (−35.5 %), respectively, for spring, and −13.8 mm (−27.8 %) and −10.2 mm (−22.2 %), respectively, for winter. ELM shows a relatively high correlation with SNOTEL SWE, with mean correlation coefficients of 0.69 but negative mean biases of −122.7 mm. Compared to the snow phenology of STC-MODSCAG and SPIReS, ELM shows delayed snow accumulation onset dates by 17.3 and 12.4 d, earlier snow end dates by 35.5 and 26.8 d, and shorter snow durations by 52.9 and 39.5 d, respectively. This study underscores the need for diagnosing model biases and improving ELM representations of snow properties and snow phenology in mountainous areas for more credible simulation and future projection of mountain snowpack.
54 ENVIRONMENTAL SCIENCES↗
Photoluminescence Dynamics Defined by Exciton Trapping Potential of Coupled Defect States in DNA-Functionalized Carbon Nanotubes
Chemical reactions between semiconducting single-wall carbon nanotubes (SWCNTs) and single-stranded DNA (ssDNA) achieve spatially patterned covalent functionalization sites and create coupled fluorescent quantum defects on the nanotube surface, tailoring SWCNT photophysics for applications such as single-photon emitters in quantum information technologies. The evaluation of relaxation dynamics of photoluminescence (PL) from those coupled quantum defects is essential for understanding the nanotube electronic structure and beneficial to the design of quantum light emitters. Here, we measured the PL decay for ssDNA-functionalized SWCNTs as a function of the guanine content of the ssDNA oligo that dictates the red-shifting of their PL emission peaks relative to the band-edge exciton. We then correlate the observed dependence of PL decay dynamics on energy red-shifts to the exciton potential energy landscape, which is modeled using first-principles approaches based upon the morphology of ssDNA-altered SWCNTs obtained by atomic force microscopy (AFM) imaging. In this work, our simulations illustrate that the multiple guanine defects introduced within a single ssDNA strand strongly interact to create a deep exciton trapping well, acting as a single hybrid trap. The emission decay from the distinctive trapping potential landscape is found to be biexponential for ssDNA-modified SWCNTs. We attributed the fast time component of the biexponential PL decay to the redistribution of exciton population among the lowest energy bright states and a manifold of dark states emerging from the coupling of multiple guanine defects. The long lifetime component in the biexponential decay, on the other hand, is attributed to the redistribution of exciton population among different exciton trapping sites that arise from the binding of multiple ssDNA strands along the nanotube axis. AFM measurements indicate that those trapping sites are separated on average by ~8 nm along the nanotube axis.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Data from "A Bayesian Record Linkage Approach to Applications in Tree Demography Using Overlapping LiDAR Scans"
Processed LiDAR data and environmental covariates from 2015 and 2019 LiDAR scans in the Vicinity of Snodgrass Mountain (Western Colorado, USA), in a geographic subset used in primary analysis for the research paper.This package contains LiDAR-derived canopy height maps for 2015 and 2019, crown polygons derived from the height maps using a segmentation algorithm, and environmental covariates supporting the model of forest growth. Source datasets include August 2015 and August 2019 discrete-return LiDAR point clouds collected by Quantum Geospatial for terrain mapping purposes on behalf of the Colorado Hazard Mapping Program and the Colorado Water Conservation Board. Both datasets adhere to the USGS QL2 quality standard. The point cloud data were processed using the R package lidR to generate a canopy height model representing maximum vegetation height above the ground surface, using a pit-free algorithm.This dataset was compiled to assess how spatial patterns of tree growth in montane and subalpine forests are influenced by water and energy availability. Understanding these growth patterns can provide insight into forest dynamics in the Southern Rocky Mountains under changing climatic conditions.This dataset contains .tif, .csv, and .txt files. This dataset additionally includes a file-level metadata (flmd.csv) file that lists each file contained in the dataset with associated metadata; and a data dictionary (dd.csv) file that contains column/row headers used throughout the files along with a definition, units, and data type.
54 ENVIRONMENTAL SCIENCES↗