Construction of Single-Atom Platinum Catalysts Enabled by CsPbBr[subscript 3] Nanocrystals
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Hu, Huicheng↗
Engineering topics
Chen, Min
Publications and source records attributed to Chen, Min.
4D-STEM of Beam-Sensitive Materials
We report that a scanning electron nanobeam diffraction, or 4D-STEM (four-dimensional scanning transmission electron microscopy), is a flexible and powerful approach to elucidate structure from "soft" materials that are challenging to image in the transmission electron microscope because their structure is easily damaged by the electron beam. In a 4D-STEM experiment, a converged electron beam is scanned across the sample, and a pixelated camera records a diffraction pattern at each scan position. This four-dimensional data set can be mined for various analyses, producing maps of local crystal orientation, structural distortions, crystallinity, or different structural classes. Holding the sample at cryogenic temperatures minimizes diffusion of radicals and the resulting damage and disorder caused by the electron beam. The total fluence of incident electrons can easily be controlled during 4D-STEM experiments by careful use of the beam blanker, steering of the localized electron dose, and by minimizing the fluence in the convergent beam thus minimizing beam damage. This technique can be applied to both organic and inorganic materials that are known to be beam-sensitive; they can be highly crystalline, semicrystalline, mixed phase, or amorphous. One common example is the case for many organic materials that have a π-π stacking of polymer chains or rings on the order of 3.4-4.2 Å separation. If these chains or rings are aligned in some regions, they will produce distinct diffraction spots (as would other crystalline spacings in this range), though they may be weak or diffuse for disordered or weakly scattering materials. We can reconstruct the orientation of the π-π stacking, the degree of π-π stacking in the sample, and the domain size of the aligned regions. This Account summarizes illumination conditions and experimental parameters for 4D-STEM experiments with the goal of producing images of structural features for materials that are beam-sensitive. We will discuss experimental parameters including sample cooling, probe size and shape, fluence, and cameras. 4D-STEM has been applied to a variety of materials, not only as an advanced technique for model systems, but as a technique for the beginning microscopist to answer materials science questions. It is noteworthy that the experimental data acquisition does not require an aberration-corrected TEM but can be produced on a variety of instruments with the right attention to experimental parameters.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Real-Time Investigation of Sn(II) Oxidation in Pb-Free Halide Perovskites by X-ray Absorption and Mössbauer Spectroscopy
Sn(II) halide perovskites are a less toxic alternative to Pb-based materials in perovskite solar cells, but oxidation to Sn(IV) introduces additional degradation pathways. Improving stability requires mechanistic pictures of O 2 - and H 2 O-induced degradation and their synergy. In this work, we demonstrate that X-ray absorption spectroscopy reports the average valency of the bulk material, allowing oxidation kinetics to be measured from minutes to days. Optical and X-ray diffraction studies demonstrate the challenge of isolating oxidative degradation with techniques lacking element specificity and oxidation state sensitivity. Finally, 119Sn Mössbauer spectroscopy is presented as a lab-based technique capable of providing information on valency and speciation throughout oxidation.
14 SOLAR ENERGY↗
Investigating Vegetation Responses to Underground Nuclear Explosions Through Integrated Analyses
Vegetation has the potential to respond to underground nuclear explosions, yet these links have not been fully explored. Given the lack of previously described signatures, the changes in vegetation are possibly subtle. The integration of multiple different data streams is potentially a useful approach to improve signal detection. Here, we investigate whether semi-arid vegetation growth patterns responded to eight legacy underground nuclear tests at the Nevada National Security Site in southern Nevada, USA. We tested for spatial and temporal changes in vegetation cover, tree growth patterns, and tree leaf spectral properties using ground-based measurements, including those from tree-rings and hyperspectral surface vegetation reflectance, as well as space-based measurements of Normalized Difference Vegetation Index (NDVI) from Landsat. Multiple data streams suggest a localized (<1.2 km) spatial pattern whereby tree growth is enhanced closer to the source of the underground test relative to sites further away. We also observed a more regional (>1.2–9 km) pattern whereby tree growth is suppressed coincident with a drought beginning 1 year before the 1989 tests, but continuing in the 5 years following the tests, which is anomalous relative to what is expected based on the response of tree growth to previous droughts. furthermore, quantification of the relative effects of the tests on vegetation remains a challenge due to the coincident drought and the potential for other disturbances to have impacted tree growth at this time, but the integration of these data reveals a more nuanced growth response than any other one data set indicates alone.
63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗
A Self-Evolution Data Fusion Platform for Large-Scale Water Models
Focal Area: Data acquisition and assimilation enabled by machine learning (ML), artificial intelligence (AI), and advanced methods including experimental/network design/optimization, unsupervised learning (deep learning), leveraging advanced hardware (e.g., edge computing). This development is to enable solving the science questions regarding the human and climatic factors that interact with and drive global water scarcity.
54 ENVIRONMENTAL SCIENCES↗
Potential of hotspot solar‐induced chlorophyll fluorescence for better tracking terrestrial photosynthesis
Abstract Remote sensing of solar‐induced fluorescence (SIF) opens a new window for quantifying a key ecological variable, the terrestrial ecosystem gross primary production (GPP), because of the revealed strong SIF–GPP correlation. However, similar to many other remotely sensed metrics, SIF observations suffer from the sun‐sensor geometry effects, which may have important impacts on the SIF–GPP relationship but remain poorly understood. Here we used remotely sensed SIF, globally distributed tower GPP data, and a mechanistic model to provide a systematic analysis. Our results reveal that leaf physiology, canopy structure, and sun‐sensor geometries all affect the SIF–GPP relationship. In particular, we found that SIF observations in the sun‐tracking hotspot direction can be a better proxy of GPP due to the similar responses of light use efficiency and SIF escaping probability in the hotspot direction to the increasing incoming solar radiation. Such conclusions are supported by a variety of modeling simulations and satellite observations over various plant function types, at different time scales and with satellite observational modes. This study demonstrates the potential and advantage of normalizing SIF observations to the hotspot direction for better global GPP estimations. This study also demonstrates the great potentials of current and future spaceborne sun‐tracking satellite missions for a significant improvement in measuring and monitoring, at a wide range of spatial and temporal scales, the changes in terrestrial ecosystem GPP in response to anticipated changes in the Earth's environmental conditions.
Hao, Dalei↗
Deforestation reshapes land-surface energy-flux partitioning
Land-use and land-cover change significantly modify local land-surface characteristics and water/energy exchanges, which can lead to atmospheric circulation and regional climate changes. In particular, deforestation accounts for a large portion of global land-use changes, which transforms forests into other land cover types, such as croplands and grazing lands. Many previous efforts have focused on observing and modeling land–atmosphere–water/energy fluxes to investigate land–atmosphere coupling induced by deforestation. However, interpreting land–atmosphere–water/energy-flux responses to deforestation is often complicated by the concurrent impacts from shifts in land-surface properties versus background atmospheric forcings. In this study, we used 29 paired FLUXNET sites, to improve understanding of how deforested land surfaces drive changes in surface-energy-flux partitioning. Each paired sites included an intact forested and non-forested site that had similar background climate. We employed transfer entropy, a method based on information theory, to diagnose directional controls between coupling variables, and identify nonlinear cause–effect relationships. Transfer entropy is a powerful tool to detective causal relationships in nonlinear and asynchronous systems. The paired eddy covariance flux measurements showed consistent and strong information flows from vegetation activity (gross primary productivity (GPP)) and physical climate (e.g. shortwave radiation, air temperature) to evaporative fraction (EF) over both non-forested and forested land surfaces. More importantly, the information transfers from radiation, precipitation, and GPP to EF were significantly reduced at non-forested sites, compared to forested sites. We then applied these observationally constrained metrics as benchmarks to evaluate the Energy Exascale Earth System Model (E3SM) land model (ELM). ELM predicted vegetation controls on EF relatively well, but underpredicted climate factors on EF, indicating model deficiencies in describing the relationships between atmospheric state and surface fluxes. Moreover, changes in controls on surface energy flux partitioning due to deforestation were not detected in the model. We highlight the need for benchmarking model simulated surface-energy fluxes and the corresponding causal relationships against those of observations, to improve our understanding of model predictability on how deforestation reshapes land surface energy fluxes.
54 ENVIRONMENTAL SCIENCES↗
Climate change as an incentive for future human migration
Human migration is both motivated and constrained by a multitude of socioeconomic and environmental factors, including climate-related factors. Climatic factors exert an influence on local and regional population density. Here, we examine the implications of future motivation for humans to migrate by analyzing today's relationships between climatic factors and population density, with all other factors held constant. Such “all other factors held constant” analyses are unlikely to make quantitatively accurate predictions, but the order of magnitude and spatial pattern that come out of such an analysis can be useful when considering the influence of climate change on the possible scale and pattern of future incentives to migrate. Our results indicate that, within decades, climate change may provide hundreds of millions of people with additional incentive to migrate, largely from warm tropical and subtropical countries to cooler temperate countries, with India being the country with the greatest number of people with additional incentive to migrate. These climate-driven incentives would be among the broader constellation of incentives that influence migration decisions. Areas with the highest projected population growth rates tend to be areas that are likely to be most adversely affected by climate change.
54 ENVIRONMENTAL SCIENCES↗
DSCOVR/EPIC-derived global hourly and daily downward shortwave and photosynthetically active radiation data at 0.1° × 0.1° resolution
Downward shortwave radiation (SW) and photosynthetically active radiation (PAR) play crucial roles in Earth system dynamics. Spaceborne remote sensing techniques provide a unique means for mapping accurate spatiotemporally continuous SW–PAR, globally. However, any individual polar-orbiting or geostationary satellite cannot satisfy the desired high temporal resolution (sub-daily) and global coverage simultaneously, while integrating and fusing multisource data from complementary satellites/sensors is challenging because of co-registration, intercalibration, near real-time data delivery and the effects of discrepancies in orbital geometry. The Earth Polychromatic Imaging Camera (EPIC) on board the Deep Space Climate Observatory (DSCOVR), launched in February 2015, offers an unprecedented possibility to bridge the gap between high temporal resolution and global coverage and characterize the diurnal cycles of SW–PAR globally. In this study, we adopted a suite of well-validated data-driven machine-learning models to generate the first global land products of SW–PAR, from June 2015 to June 2019, based on DSCOVR/EPIC data. The derived products have high temporal resolution (hourly) and medium spatial resolution (0.1°×0.1°), and they include estimates of the direct and diffuse components of SW–PAR. We used independently widely distributed ground station data from the Baseline Surface Radiation Network (BSRN), the Surface Radiation Budget Network (SURFRAD), NOAA's Global Monitoring Division and the U.S. Department of Energy's Atmospheric System Research (ASR) program to evaluate the performance of our products, and we further analyzed and compared the spatiotemporal characteristics of the derived products with the benchmarking Clouds and the Earth's Radiant Energy System Synoptic (CERES) data. We found both the hourly and daily products to be consistent with ground-based observations (e.g., hourly and daily total SWs have low biases of -3.96 and -0.71 W m -2 and root-mean-square errors (RMSEs) of 103.50 and 35.40 W m -2 , respectively). The developed products capture the complex spatiotemporal patterns well and accurately track substantial diurnal, monthly, and seasonal variations in SW–PAR when compared to CERES data. They provide a reliable and valuable alternative for solar photovoltaic applications worldwide and can be used to improve our understanding of the diurnal and seasonal variabilities of the terrestrial water, carbon and energy fluxes at various spatial scales.
54 ENVIRONMENTAL SCIENCES↗
Multi-scale integration of satellite remote sensing improves characterization of dry-season green-up in an Amazon tropical evergreen forest
In tropical forests, leaf phenology-particularly the pronounced dry-season green-up-strongly regulates biogeochemical cycles of carbon and water fluxes. However, uncertainties remain in the understanding of tropical forest leaf phenology at different spatial scales. Phenocams accurately characterize leaf phenology at the crown and ecosystem scales but are limited to a few sites and time spans of a few years. Time-series satellite observations might fill this gap, but the commonly used satellites (e.g. MODIS, Landsat and Sentinel-2) have resolutions too coarse to characterize single crowns. To resolve this observational challenge, we used the PlanetScope constellation with a 3m resolution and near daily nadir-view coverage. We first developed a rigorous method to cross-calibrate PlanetScope surface reflectance using daily BRDF-adjusted MODIS as the reference. We then used linear spectral unmixing of calibrated PlanetScope to obtain dry-season change in the fractional cover of green vegetation (GV) and non-photosynthetic vegetation (NPV) at the PlanetScope pixel level. We used the Central Amazon Tapajos National Forest k67 site, as all necessary data (from field to phenocam and satellite observations) was available. For this proof of concept, we chose a set of 22 dates of PlanetScope measurements in 2018 and 16 in 2019, all from the six drier months of the year to provide the highest possible cloud-free temporal resolution. Our results show that MODIS-calibrated dry-season PlanetScope data (1) accurately assessed seasonal changes in ecosystem-scale and crown-scale spectral reflectance; (2) detected an increase in ecosystem-scale GV fraction (and a decrease in NPV fraction) from June to November of both years, consistent with local phenocam observations with R 2 around 0.8; and (3) monitored large seasonal trend variability in crown-scale NPV fraction. Finally, our results highlight the potential of integrating multi-scale satellite observations to extend fine-scale leaf phenology monitoring beyond the spatial limits of phenocams.
54 ENVIRONMENTAL SCIENCES↗
Global land use for 2015-2100 at 0.05° resolution under diverse socioeconomic and climate scenarios
Global future land use (LU) is an important input for Earth system models for projecting Earth system dynamics and is critical for many modeling studies on future global change. Here we generated a new global gridded LU dataset using the Global Change Analysis Model (GCAM) and a land use spatial downscaling model, named Demeter, under the five Shared Socioeconomic Pathways (SSPs) and four Representative Concentration Pathways (RCPs) scenarios. Compared to existing similar datasets, the presented dataset has a higher spatial resolution (0.05°×0.05°) and spreads under a more comprehensive set of SSP-RCP scenarios (in total 15 scenarios), and considers uncertainties from the forcing climates. We compared our dataset with the Land Use Harmonization version 2 (LUH2) dataset and found our results are in general spatially consistent with LUH2. The presented dataset will be useful for global Earth system modeling studies, especially for the analysis of the impacts of land use and land cover change and socioeconomics, as well as the characterizing the uncertainties associated with these impacts.
54 ENVIRONMENTAL SCIENCES↗
Highly safe and cyclable Li-metal batteries with vinylethylene carbonate electrolyte
Not Available
Zhang, Qiankui↗
Exploring the Use of DSCOVR/EPIC Satellite Observations to Monitor Vegetation Phenology
Vegetation phenology plays a pivotal role in regulating several ecological processes and has profound impacts on global carbon exchange. Large-scale vegetation phenology monitoring mostly relies on Low-Earth-Orbit satellite observations with low temporal resolutions, leaving gaps in data that are important for monitoring seasonal vegetation phenology. High temporal resolution satellite observations have the potential to fill this gap by frequently collecting observations on a global scale, making it easier to study change over time. This study explored the potential of using the Earth Polychromatic Imaging Camera (EPIC) onboard the Deep Space Climate Observatory (DSCOVR) satellite, which captures images of the entire sunlit face of the Earth at a temporal resolution of once every 1–2 h, to observe vegetation phenology cycles in North America. We assessed the strengths and shortcomings of EPIC-based phenology information in comparison with the Moderate-resolution Imaging Spectroradiometer (MODIS), Enhanced Thematic Mapper (ETM+) onboard Landsat 7, and PhenoCam ground-based observations across six different plant functional types. Our results indicated that EPIC could capture and characterize seasonal changes of vegetation across different plant functional types and is particularly consistent in the estimated growing season length. Our results also provided new insights into the complementary features and benefits of the four datasets, which is valuable for improving our understanding of the complex response of vegetation to global climate variability and other disturbances and the impact of phenology changes on ecosystem productivity and global carbon exchange.
Weber, Maridee A.↗
First-Principles Simulations of X-ray Transient Absorption for Probing Attosecond Electron Dynamics
Not Available
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗