Diffuse Flux Measurements Research Articles

Scalable precision wide-field imaging in radio interferometry – II. AIRI validated on ASKAP data

ABSTRACT Accompanying Part I, this sequel delineates a validation of the recently proposed AI for Regularization in radio-interferometric Imaging (AIRI) algorithm on observations from the Australian Square Kilometre Array Pathfinder (ASKAP). The monochromatic AIRI-ASKAP images showcased in this work are formed using the same parallelized and automated imaging framework described in Part I: ‘uSARA validated on ASKAP data’. Using a Plug-and-Play approach, AIRI differs from uSARA by substituting a trained denoising deep neural network (DNN) for the proximal operator in the regularization step of the forward–backward algorithm during deconvolution. We build a trained shelf of DNN denoisers that target the estimated image dynamic ranges of our selected data. Furthermore, we quantify variations of AIRI reconstructions when selecting the nearest DNN on the shelf versus using a universal DNN with the highest dynamic range, opening the door to a more complete framework that not only delivers image estimation but also quantifies epistemic model uncertainty. We continue our comparative analysis of source structure, diffuse flux measurements, and spectral index maps of selected target sources as imaged by AIRI and the algorithms in Part I – uSARA and WSClean. Overall, we see an improvement over uSARA and WSClean in the reconstruction of diffuse components in AIRI images. The scientific potential delivered by AIRI is evident in further imaging precision, more accurate spectral index maps, and a significant acceleration in deconvolution time, whereby AIRI is four times faster than its subiterative sparsity-based counterpart uSARA.

Technical note: Mobile open dynamic chamber measurement of methane macroseeps in lakes

Abstract. Methane (CH4) seepage (i.e., steady or episodic flow of gaseous hydrocarbons from subsurface reservoirs) has been identified as a significant source of atmospheric CH4. However, radiocarbon data from polar ice cores have recently brought into question the magnitude of fossil CH4 seepage naturally occurring. In northern high latitudes, seepage of subsurface CH4 is impeded by permafrost and glaciers, which are under an increasing risk of thawing and melting in a globally warming world, implying the potential release of large stores of CH4 in the future. Resolution of these important questions requires a better constraint and monitoring of actual emissions from seepage areas. The measurement of these seeps is challenging, particularly in aquatic environments, because they involve large and irregular gas flow rates, unevenly distributed both spatially and temporally. Large macroseeps are particularly difficult to measure due to a lack of lightweight, inexpensive methods that can be deployed in remote Arctic environments. Here, we report the use of a mobile chamber for measuring emissions at the surface of ice-free lakes subject to intense CH4 macroseepage. Tested in a remote Alaskan lake, the method was validated for the measurement of fossil CH4 emissions of up to 1.08 × 104 g CH4 m−2 d−1 (13.0 L m−2 min−1 of 83.4 % CH4 bubbles), which is within the range of global fossil methane seepage and several orders of magnitude above standard ecological emissions from lakes. In addition, this method allows for low diffusive flux measurements. Thus, the mobile chamber approach presented here covers the entire magnitude range of CH4 emissions currently identified, from those standardly observed in lakes to intense macroseeps, with a single apparatus of moderate cost.

Temporal and spatial variations of CO2 diffuse volcanic degassing on Cuicocha Caldera Lake – Ecuador

Cuicocha Caldera is the youngest eruptive center of Cotacachi-Cuicocha Volcanic Complex, located at the north of Ecuador. The caldera contains a lake of 3.95 km2 surface, and a maximum depth of 148 m. Cuicocha Lake is characterized by the presence of CO2 gaseous diffuse emissions, perceptible as bubbling zones. Since 2011, CO2 diffuse flux measurements have been performed in this lake using the accumulation chamber method. The data obtained from twenty surveys were processed by means of the Graphical Statistical Approach and the Sequential Gaussian Simulation. The results reveal that Cuicocha lake has released a total estimated amount of ~400 kt of CO2 in the period between March 2011 and May 2019, with an average rate of 135 t/day. Furthermore, the spatial and temporal analysis of the data made possible the understanding of the processes occurring in the lake: 1) Lake stratification caused by the seasons seem to favor CO2 accumulation in the hipolimnion and its posterior releasing. Minimum total flux values of ~50 t/day have been estimated during “warm” stratified periods and maximum flux values of ~170 t/day have been recorded during “cold” overturn periods. Additionally, at least two anomalous degassing episodes were identified in 2012–2013, seemingly associated to changes in the volcanic activity also detected through seismicity. 2) Cuicocha CO2 degassing seems to be controlled by the existence of diffuse degassing structures at the lake bottom, which correspond to high permeability zones resulting from the intersection between ~NE-SW and ~WNW-ESE oriented structures. We propose a conceptual model to explain the systematic apparition of CO2 anomalies on specific areas of the lake surface.

Interplay of Supersaturation and Solubilization: Lack of Correlation between Concentration-Based Supersaturation Measurements and Membrane Transport Rates in Simulated and Aspirated Human Fluids.

Supersaturating formulations are increasingly being used to improve the absorption of orally administered poorly water-soluble drugs. To better predict outcomes in vivo, we must be able to accurately determine the degree of supersaturation in complex media designed to provide a surrogate for the gastrointestinal environment. Herein, we demonstrate that relying on measurements based on consideration of the total dissolved concentration leads to underestimation of supersaturation and consequently membrane transport rates. Crystalline and amorphous solubilities of two compounds, atazanavir and posaconazole, were evaluated in six different media. Concurrently, diffusive flux measurements were performed in a side-by-side diffusion cell to determine the activity-based supersaturation by evaluating membrane transport rates at the crystalline and amorphous solubilities. Solubility values were found to vary in each medium because of different solubilization capacities. Concentration-based supersaturation ratios were also found to vary for the different media. Activity-based measurements, however, were largely independent of the medium, leading to relatively constant values for the estimated supersaturation. These findings have important consequences for modeling and prediction of supersaturation impact on the absorption rate as well as for better defining the thermodynamic driving force for crystallization in complex media.

Crystallization from Supersaturated Solutions: Role of Lecithin and Composite Simulated Intestinal Fluid.

The overall purpose of this study was to understand the impact of different biorelevant media types on solubility and crystallization from supersaturated solutions of model compounds (atazanavir, ritonavir, tacrolimus and cilnidipine). The first aim was to understand the influence of the lecithin content in FaSSIF. As the human intestinal fluids (HIFs) contain a variety of bile salts in addition to sodium taurocholate (STC), the second aim was to understand the role of these bile salts (in the presence of lecithin) on solubility and crystallization from supersaturated solutions, METHODS: To study the impact of lecithin, media with 3mM STC concentration but varying lecithin concentration were prepared. To test the impact of different bile salts, a new biorelevant medium (Composite-SIF) with a composition simulating that found in the fasted HIF was prepared. The crystalline and amorphous solubility was determined in these media. Diffusive flux measurements were performed to determine the true supersaturation ratio at the amorphous solubility of the compounds in various media. Nucleation induction times from supersaturated solutions were measured at an initial concentration equal to the amorphous solubility (equivalent supersaturation) of the compound in the given medium. It was observed that, with an increase in lecithin content at constant STC concentration (3mM), the amorphous solubility of atazanavir increased and crystallization was accelerated. However, the crystalline solubility remained fairly constant. Solubility values were higher in FaSSIF compared to Composite-SIF. Longer nucleation induction times were observed for atazanavir, ritonavir and tacrolimus in Composite-SIF compared to FaSSIF at equivalent supersaturation ratios. This study shows that variations in the composition of SIF can lead to differences in the solubility and crystallization tendency of drug molecules, both of which are critical when evaluating supersaturating systems.

Effect of sporadic destratification, seasonal overturn, and artificial mixing on CH<sub>4</sub> emissions from a subtropical hydroelectric reservoir

Abstract. Inland waters in general and freshwater reservoirs specifically are recognized as a source of CH4 into the atmosphere. Although the diffusion at the air–water interface is the most studied pathway, its spatial and temporal variations are poorly documented. We measured temperature and O2 and CH4 concentrations every 2 weeks for 3.5 years at nine stations in a subtropical monomictic reservoir which was flooded in 2008 (Nam Theun 2 Reservoir, Lao PDR). Based on these results, we quantified CH4 storage in the water column and diffusive fluxes from June 2009 to December 2012. We compared diffusive emissions with ebullition from Deshmukh et al. (2014) and aerobic methane oxidation and downstream emissions from Deshmukh et al. (2016). In this monomictic reservoir, the seasonal variations of CH4 concentration and storage were highly dependent on the thermal stratification. Hypolimnic CH4 concentration and CH4 storage reached their maximum in the warm dry season (WD) when the reservoir was stratified. Concentration and storage decreased during the warm wet (WW) season and reached its minimum after the reservoir overturned in the cool dry (CD) season. The sharp decreases in CH4 storage were concomitant with extreme diffusive fluxes (up to 200 mmol m−2 d−1). These sporadic emissions occurred mostly in the inflow region in the WW season and during overturn in the CD season in the area of the reservoir that has the highest CH4 storage. Although they corresponded to less than 10 % of the observations, these extreme CH4 emissions (> 5 mmol m−2 d−1) contributed up to 50 % of total annual emissions by diffusion. During the transition between the WD and WW seasons, a new emission hotspot was identified upstream of the water intake where diffusive fluxes peaked at 600 mmol m−2 d−1 in 2010 down to 200 mmol m−2 d−1 in 2012. The hotspot was attributed to the mixing induced by the water intakes (artificial mixing). Emissions from this area contributed 15–25 % to total annual emissions, although they occur in a surface area representative of less than 1 % of the total reservoir surface. We highly recommend measurements of diffusive fluxes around water intakes in order to evaluate whether such results can be generalized.

Assessing Soil Nitrogen Availability using Microdialysis‐Derived Diffusive Flux Measurements

Microdialysis‐based soil sampling offers a potential alternative to traditional soil core extractions that better informs about the availability of nitrogen (N) for plant nutrition. This study compared soil N status, as estimated using 0.5 M K2SO4 and distilled water extractions, with microdialysis‐derived diffusive flux measurements in eight grassland soils up an altitudinal gradient. Soil extracts and microdialysis samples were analyzed for plant‐available N: total free amino acids, NH4+, and NO3−. In terms of the percentage contribution that amino acids, NH4+, and NO3− made to total plant‐available N, the microdialysis‐derived diffusive flux measurements were most similar to distilled water extractions. However, the relative magnitude of the diffusive flux measurements did not always reflect the pool sizes as estimated by the soil extractions, which suggests that the availability of N to plants, via diffusion, may be decoupled from concentration in these soils. The potential and limitations of microdialysis sampling and the implications of the results for soil N management are discussed.

Impact of resuspension of cohesive sediments at the Oyster Grounds (North Sea) on nutrient exchange across the sediment–water interface

Benthic-pelagic exchange processes are recognised as important nutrient sources in coastal areas, however, the relative impact of diffusion, resuspension and other processes such as bioturbation and bioirrigation are still relatively poorly understood. Experimental ship-based data are presented showing the effects of diffusion and resuspension on cohesive sediments at a temperate shelf location in the North Sea. Measurements of diffusive fluxes in both spring (1.76, 0.51, −0.91, 17.6 μmol/m2/h) and late summer (8.53, −0.03, −1.12, 35.0 μmol/m2/h) for nitrate, nitrite, phosphate and dissolved silicon respectively, provided comparisons for measured resuspension fluxes. Increases in diffusive fluxes of nitrate and dissolved silicon to the water column in late summer coincided with decreases in bottom water oxygen concentrations and increases in temperature. Resuspension experiments using a ship board annular flume and intact box core allowed simultaneous measurement of suspended particulate matter, water velocity and sampling of nutrients in the water column during a step wise increase in bed shear velocity. The resuspension of benthic fluff led to small but significant releases of phosphate and nitrate to the water column with chamber concentration increasing from 0.70–0.76 and 1.84–2.22 μmol/L respectively. Resuspension of the sediment bed increased water column concentrations of dissolved silicon by as much as 125% (7.10–15.9 μmol/L) and nitrate and phosphate concentrations by up to 67% (1.84–3.08 μmol/L) and 66% (0.70–1.15 μmol/L) respectively. Mass balance calculations indicate that processes such as microbial activity or adsorption/desorption other than simple release of pore water nutrients must occur during resuspension to account for the increase. This study shows that resuspension is potentially an important pathway for resupplying the water column with nutrients before and during phytoplankton blooms and should therefore be considered along with diffusive fluxes in future ecosystem models.

Greenhouse gas emissions from reservoirs of the western United States

Six reservoirs located in the Western United States (F. D. Roosevelt, Dworshak, Wallula, Shasta, Oroville, and New Melones) were sampled in order to estimate their greenhouse gas (GHG) emissions. Two types of fluxes were assessed: (1) diffusive fluxes of methane (CH4) and carbon dioxide (CO2) at the air/water interface and (2) degassing fluxes of CH4 and CO2 from water passing through the turbine spillways. Diffusive flux measurements indicated that the surface of the reservoirs were a source of CH4 during the sampling period (from +3.2 to +9.5 mg CH4 m−2 d−1). Oroville (+1026 mg CO2 m−2 d−1) and Shasta (+1247 mg CO2 m−2 d−1) surfaces were also sources of CO2. In contrast, the surface of all the other reservoirs constituted sinks for CO2 (from −349 to −1195 mg CO2 m−2 d−1). Degassing fluxes ranged from +0.003 to +0.815 t CH4 d−1, and from +16 to +324 t CO2 d−1. Daily GHG budgets ranged from +0.146 to +2.228 t CH4 d−1, and from −15 to +224 t CO2 d−1. Degassing fluxes represented an important term of these budgets. A significant correlation was observed between the magnitude of CO2 diffusive fluxes and the water pH (R2 = 0.81; p < 0.0001). All other correlations between GHG diffusive fluxes and independent variables tested were weak and/or not significant. Finally, while attempting to resolve the spatial variability in diffusive fluxes, we were able to cluster reservoirs neither according to geological nor ecological criteria.

Reanalysis ofVoyagerUltraviolet Spectrometer Limits to the Extreme‐Ultraviolet and Far‐Ultraviolet Diffuse Astronomical Flux

We reexamine Voyager Ultraviolet Spectrometer (UVS) data used to establish upper limits to the 500-900 A and 900-1100 A cosmic diffuse background. The measurement of diffuse flux with the Voyager UVS data requires complex corrections for noise sources which are far larger than the astronomical signal. In the analyses carried out to date, the upper limits obtained on the diffuse background show statistical anomalies which indicate that substantial systematic errors are present. We detail these anomalies and identify specific problems with the analyses. We derive statistically robust 2 σ upper limits for continuum flux of 570 photons s-1 cm-2 sr-1 A-1 and for the 1000 A diffuse line flux of 11,790 photons s-1 cm-2 sr-1. The true limits may be substantially higher because of unknown systematic uncertainties. The new statistical limits alone are insufficient to support previous conclusions based on the Voyager data, including work on the character of interstellar dust and estimates of the diffuse extragalactic far-UV background as absorbed by intergalactic dust.

Characterizing soil fertility by ion diffusive flux measurements

The general acceptance of diffusion as a rate-limiting step in transferring ions to plant roots was considered in characterizing soil fertility. Soil ion diffusive flux measurements to an exchange resin were measured with two soil: resin cells, one with untreated soil, the other with the same soil fertilized with P, K, and Cl. The P, K, and Cl that diffused to the resin of each cell was extracted and determined. Using only these measurements and some simplifying assumptions of diffusion theory, calculations were made of the soil's P and K solution concentration, adsorbed concentration, a capacity factor, transmission factor, and quantity of fertilizer needed to attain any desired flux. Excellent to fair correlations existed between these calculated values and traditionally measured chemical quantities. Plant uptake of P and K was generally well correlated with diffusive flux measurements as well as traditional chemical measurements.