We present two-dimensional Mg(OH)2 sheets and their vertical heterojunctions with CVD-MoS2 for the first time as flexible 2D insulators with anomalous lattice vibration and chemical and physical properties. New hydrothermal crystal growth technique enabled isolation of environmentally stable monolayer Mg(OH)2 sheets. Raman spectroscopy and vibrational calculations reveal that the lattice vibrations of Mg(OH)2 have fundamentally different signature peaks and dimensionality effects compared to other 2D material systems known to date. Sub-wavelength electron energy-loss spectroscopy measurements and theoretical calculations show that Mg(OH)2 is a 6 eV direct-gap insulator in 2D, and its optical band gap displays strong band renormalization effects from monolayer to bulk, marking the first experimental confirmation of confinement effects in 2D insulators. Interestingly, 2D-Mg(OH)2 sheets possess rather strong surface polarization (charge) effects which is in contrast to electrically neutral h-BN materials. Using 2D-Mg(OH)2 sheets together with CVD-MoS2 in the vertical stacking shows that a strong change transfer occurs from n-doped CVD-MoS2 sheets to Mg(OH)2, naturally depleting the semiconductor, pushing towards intrinsic doping limit and enhancing overall optical performance of 2D semiconductors. Results not only establish unusual confinement effects in 2D-Mg(OH)2, but also offer novel 2D-insulating material with unique physical, vibrational, and chemical properties for potential applications in flexible optoelectronics.
A data set of observed daily precipitation, maximum and minimum temperature, gridded to a 1/16° (~6 km) resolution, is described that spans the entire country of Mexico, the conterminous U.S. (CONUS), and regions of Canada south of 53° N for the period 1950-2013. The dataset improves previous products in spatial extent, orographic precipitation adjustment over Mexico and parts of Canada, and reduction of transboundary discontinuities. The impacts of adjusting gridded precipitation for orographic effects are quantified by scaling precipitation to an elevation-aware 1981-2010 precipitation climatology in Mexico and Canada. Differences are evaluated in terms of total precipitation as well as by hydrologic quantities simulated with a land surface model. Overall, orographic correction impacts total precipitation by up to 50% in mountainous regions outside CONUS. Hydrologic fluxes show sensitivities of similar magnitude, with discharge more sensitive than evapotranspiration and soil moisture. Because of the consistent gridding methodology, the current product reduces transboundary discontinuities as compared with a commonly used reanalysis product, making it suitable for estimating large-scale hydrometeorologic phenomena.
Earth-abundant sustainable inorganic thin-film solar cells, independent of precious elements, pivot on a marginal material phase space targeting specific compounds. Advanced materials characterization efforts are necessary to expose the roles of microstructure, chemistry, and interfaces. Herein, the earth-abundant solar cell device, Cu2ZnSnS(4-x)Sex, is reported, which shows a high abundance of secondary phases compared to similarly grown Cu2ZnSnSe4.
Wetlands are the world's largest natural source of methane, a powerful greenhouse gas. The strong sensitivity of methane emissions to environmental factors such as soil temperature and moisture has led to concerns about potential positive feedbacks to climate change. This risk is particularly relevant at high latitudes, which have experienced pronounced warming and where thawing permafrost could potentially liberate large amounts of labile carbon over the next 100 years. However, global models disagree as to the magnitude and spatial distribution of emissions, due to uncertainties in wetland area and emissions per unit area and a scarcity of in situ observations. Recent intensive field campaigns across the West Siberian Lowland (WSL) make this an ideal region over which to assess the performance of large-scale process-based wetland models in a high-latitude environment. Here we present the results of a follow-up to the Wetland and Wetland CH4 Intercomparison of Models Project (WETCHIMP), focused on the West Siberian Lowland (WETCHIMP-WSL). We assessed 21 models and 5 inversions over this domain in terms of total CH4 emissions, simulated wetland areas, and CH4 fluxes per unit wetland area and compared these results to an intensive in situ CH4 flux data set, several wetland maps, and two satellite surface water products. We found that (a) despite the large scatter of individual estimates, 12-year mean estimates of annual total emissions over the WSL from forward models (5.34 ± 0.54 Tg CH4 yr-1), inversions (6.06 ± 1.22 Tg CH4 yr-1), and in situ observations (3.91 ± 1.29 Tg CH4 yr-1) largely agreed; (b) forward models using surface water products alone to estimate wetland areas suffered from severe biases in CH4 emissions; (c) the interannual time series of models that lacked either soil thermal physics appropriate to the high latitudes or realistic emissions from unsaturated peatlands tended to be dominated by a single environmental driver (inundation or air temperature), unlike those of inversions and more sophisticated forward models; (d) differences in biogeochemical schemes across models had relatively smaller influence over performance; and (e) multiyear or multidecade observational records are crucial for evaluating models' responses to long-term climate change.
Climate factors including soil temperature and moisture, incident solar radiation, and atmospheric carbon dioxide concentration are important environmental controls on methane (CH4) emissions from northern wetlands. We investigated the spatiotemporal distributions of the influence of these factors on northern high-latitude wetland CH4 emissions using an enhanced version of the Variable Infiltration Capacity (VIC) land surface model. We simulated CH4 emissions from wetlands across the pan-Arctic domain over the period 1948–2006, yielding annual average emissions of 36.1 ± 6.7 Tg CH4 yr-1 for the period 1997–2006. We characterized historical sensitivities of CH4 emissions to air temperature, precipitation, incident long- and shortwave radiation, and atmospheric [CO2] as a function of average summer air temperature and precipitation. Emissions from relatively warm and dry wetlands in the southern (permafrost-free) portion of the domain were positively correlated with precipitation and negatively correlated with air temperature, while emissions from wetter and colder wetlands further north (permafrost) were positively correlated with air temperature. Over the entire period 1948–2006, our reconstructed CH4 emissions increased by 20 %, the majority of which can be attributed to an increasing trend in summer air temperature. We estimated future emissions in response to 21st century warming as predicted by CMIP5 (Coupled Model Intercomparison Project Phase 5) model projections to result in end-of-century CH4 emissions 38–53 % higher than our reconstructed 1997–2006 emissions, accompanied by the northward migration of warmer and drier than optimal conditions for CH4 emissions, implying a reduced role for temperature in driving future increases in emissions.