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At least 1,747 records · Page 97

Accuracy of Kohn–Sham density functional theory for warm- and hot-dense matter equation of state

We study the accuracy of Kohn–Sham density functional theory (DFT) for warm- and hot-dense matter (WDM and HDM). Specifically, considering a wide range of systems, we perform accurate ab initio molecular dynamics simulations with temperature-independent local/semilocal density functionals to determine the equations of state at compression ratios of 3x–7x and temperatures near 1 MK. We find very good agreement with path integral Monte Carlo benchmarks, while having significantly smaller error bars and smoother data, demonstrating the accuracy of DFT for the study of WDM and HDM at such conditions. In addition, using a Δ-machine learned force field scheme, we confirm that the DFT results are insensitive to the choice of exchange-correlation functional, whether local, semilocal, or nonlocal.

Suryanarayana, Phanish (ORCID:0000000151720049)↗

SU-E-J-48: Development of An Abdominal Compression Device for Respiratory Correlated Radiation Therapy

Purpose: The aim of this study is to develop the abdominal compression device which could control pressure level according to the abdominal respiratory motion and evaluate its feasibility. Methods: In this study, we focused on developing the abdominal compression device which could control pressure level at any point of time so the developed device is possible to use a variety of purpose (gating technique or respiratory training system) while maintaining the merit of the existing commercial device. The compression device (air pad form) was designed to be able to compress the front and side of abdomen and the pressure level of the abdomen is controlled by air flow. Pressure level of abdomen (air flow) was determined using correlation data between external abdominal motion and respiratory volume signal measured by spirometer. In order to verify the feasibility of the device, it was necessary to confirm the correlation between the abdominal respiratory motion and respiratory volume signal and cooperation with respiratory training system also checked. Results: In the previous study, we could find that the correlation coefficient ratio between diaphragm and respiratory volume signal measured by spirometer was 0.95. In this study, we confirmed the correlation between the respiratory volume signal and the external abdominal motion measured by belt-transducer (correlation coefficient ratio was 0.92) and used the correlated respiratory volume data as an abdominal pressure level. It was possible to control the pressure level with negligible time delay and respiratory volume data based guiding waveforms could be properly inserted into the respiratory training system. Conclusion: Through this feasibility study, we confirmed the correlation between the respiratory volume signal and the external abdominal motion. Also initial assessment of the device and its compatibility with the respiratory training system were verified. Further study on application in respiratory gated therapy and respiratory training system will be investigated. This work was supported by Radiation Technology R and D program (No. 2013M2A2A7043498)and Basic Atomic Energy Research Institute (BAERI)(No. NRF-2009-0078390) through the National Research Foundation of Korea funded by the Ministry of Science, ICT and Future Planning.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Stress Evolution in Composite Silicon Electrodes during Lithiation/Delithiation

We report real-time average stress measurements on composite silicon electrodes made with two different binders – viz. Carboxymethyl cellulose (CMC) and Polyvinylidene fluoride (PVDF) – during electrochemical lithiation and delithiation. During galvanostatic lithiation at very slow rates, the stress in a CMC-based electrode becomes compressive and increases to 70 MPa, where it reaches a plateau and increases slowly thereafter with capacity. The PVDF-based electrode exhibits similar behavior, although with lower peak compressive stress of about 12 MPa. These initial experiments indicate that the stress evolution in a Si composite electrode depends strongly on the mechanical properties of the binder. Stress data obtained from a series of lithiation/delithiation cycles suggests plasticity induced irreversible shape changes in contacting Si particles, and as a result, the stress response of the system during any given lithiation/delithiation cycle depends on the cycling history of the electrode. While these results constitute the first in situ stress measurements on composite Si electrodes during electrochemical cycling, the diagnostic technique described herein can be used to assess the mechanical response of a composite electrode made with other active material/binder combinations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Leveraging Computational Storage Devices in Campaign Storage [Slides]

Computational storage provides new ways of accelerating data-intensive applications. In-drive data management schemes matter (O_DIRECT, clustered index). Layer violation: “cheating” one filesystem may be possible; cheating multiple layers of filesystems is hard (FS internal load balancing, fail over, compression, concurrency control). The future directions include block-based acceleration to object-based acceleration.

97 MATHEMATICS AND COMPUTING↗

FY23 Progress Report on Viscosity and Thermal Conductivity Measurements of Molten Salts

As presented in this report, thermal conductivity and viscosity measurements were performed on key chloride pseudo-binary molten salt systems of relevance to molten salt reactor developers. Thermal conductivity measurements were conducted with a variable gap technique, in which a known heat flux is driven across a molten salt specimen and the temperature difference is measured, allowing calculation of the thermal conductivity. This is achieved by establishing a small gap between the bottom of a cylindrical inner containment, which houses electrical heating elements, and an outer containment, which houses cooling channels; the gap size can be varied by compression of a formed bellows. A new calibration scheme was developed herein, involving a correction factor to the heat flux based on He measurements at various temperatures. Furthermore, the data processing methodology was improved to minimize the impact of radiative heat transfer in the calculation of salt specimen thermal conductivity from the temperature difference measurements. Viscosity measurements were conducted with a rolling ball viscometer, in which a ball rolls some known distance in an angled tubular crucible, and the terminal velocity can be used to calculate the viscosity of the salt. The measurement can be performed in a quartz crucible, with which a standard camera can be used to track the ball, or in a metal crucible, with which x-ray radiography is required to track the ball. A new custom x-ray system was made and dedicated to the rolling ball viscometer to enable high throughput automated measurements with salts which require containment with metal. Both systems have been integrated with a ventilation stack which allows for off-gassing of radioactive material, enabling future measurements with U-bearing salts. The thermal conductivity measurements performed herein were with NaCl-KCl (44 mol% NaCl). This salt system was measured in the previous fiscal year, however the thermal conductivity values obtained were comparatively low, and so the system was remeasured with the aforementioned calibration scheme and improved post-processing techniques. The newly obtained thermal conductivity values for NaCl-KCl (44 mol% NaCl) indicate good agreement with kinetic theory and ab-initio models (within 5–10 %). The viscosity measurements performed herein were with three different compositions of NaCl-KCl: 75, 50, and 25 mol% NaCl; a new calibration scheme was applied to account for variable flow effects in the laminar regime. The results show reasonable agreement with literature (5–20 %, depending on the temperature, composition, and study); however, literature values are likely higher than true values based on pure end-member measurements performed in the comparative studies. The measurements conducted herein do show a trend such that viscosity increases with increasing NaCl concentration, which agrees well with one of two comparative studies. In general, the measurements conducted herein gives confidence in the capability to use these systems to accurately measure thermal conductivity and viscosity of actinide-bearing salts within the next fiscal year.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Containment Chamber Systems Engineering Project

Lawrence Livermore National Laboratory (LLNL) is a leading research laboratory in material properties. The most notable facility at LLNL capable of determining equation of state data for hazardous materials is the National Ignition Facility (NIF). NIF is the most energetic laser in the world and is a very versatile system that allows for a variety of laser configurations and diagnostics. The flexibility that NIF offers makes it an attractive tool for high budget programs researching specific areas of interest. Some programs require many tests to be performed, and although NIF could be an option for performing these tests, the cost and time to perform the tests would not be feasible. Also, many of these tests would underutilize the full capacity of NIF’s lasers, and NIF does not have a dedicated light source suitable for the diagnostic requirement. The needs of these tests do not align with NIF’s capabilities. The physicists are the main stakeholders for the tests, and they require a third-generation light source to meet the desired diagnostic performance. The Dynamic Compression Sector (DCS) within the Advanced Photon Source (APS) at Argonne National Laboratory (ANL) is the facility that will meet necessary laser performance and the X-ray diagnostic performance in order to obtain the desired data. DCS does not have the capability to test hazardous material, and therefore DCS requires a method and hardware for ensuring that no hazardous material is exposed before, during, or after the test. After taking a system engineering evaluation of the need for a solution to perform laser shock experiments on hazardous materials with certain laser and X-ray characteristics, a solution is proposed that meets the requirements of each involved stakeholder. The proposed solution is to contain the targets within sealed vacuum chamber that will meet the protection requirements of each facility. The chamber would be assembled and pumped down at LLNL in facilities that can handle hazardous material. Then, the chamber would be shipped under vacuum to DCS, where the chamber will be inserted into the beam paths. DCS’s laser will enter the sealed chamber and impart a shock into the target of hazardous material while the X-ray will simultaneously image the material. Once each target has been fired, the chamber will be removed from the beam path and shipped to the proper disposal facility.

42 ENGINEERING↗

Long-Range Ordered Amorphous Atomic Chains as Building Blocks of a Superconducting Quasi-One-Dimensional Crystal

Crystalline and amorphous structures are two of the most common solid-state phases. Crystals having orientational and periodic translation symmetries are usually both short-range and long-range ordered, while amorphous materials have no long-range order. Short-range ordered but long-range disordered materials are generally categorized into amorphous phases. In contrast to the extensively studied crystalline and amorphous phases, the combination of short-range disordered and long-range ordered structures at the atomic level is extremely rare and so far has only been reported for solvated fullerenes under compression. Here, a report on the creation and investigation of a superconducting quasi-1D material with long-range ordered amorphous building blocks is presented. Using a diamond anvil cell, monocrystalline (TaSe4)(2)I is compressed and a system is created where the TaSe(4)atomic chains are in amorphous state without breaking the orientational and periodic translation symmetries of the chain lattice. Strikingly, along with the amorphization of the atomic chains, the insulating (TaSe4)(2)I becomes a superconductor. The data provide critical insight into a new phase of solid-state materials. The findings demonstrate a first ever case where superconductivity is hosted by a lattice with periodic but amorphous constituent atomic chains.

combination of crystalline and amorphous structure↗

Experimental characterization of energetic material dynamics for multiphase blast simulation.

Currently there is a substantial lack of data for interactions of shock waves with particle fields having volume fractions residing between the dilute and granular regimes, which creates one of the largest sources of uncertainty in the simulation of energetic material detonation. To close this gap, a novel Multiphase Shock Tube has been constructed to drive a planar shock wave into a dense gas-solid field of particles. A nearly spatially isotropic field of particles is generated in the test section by a gravity-fed method that results in a spanwise curtain of spherical 100-micron particles having a volume fraction of about 19%. Interactions with incident shock Mach numbers of 1.66, 1.92, and 2.02 were achieved. High-speed schlieren imaging simultaneous with high-frequency wall pressure measurements are used to reveal the complex wave structure associated with the interaction. Following incident shock impingement, transmitted and reflected shocks are observed, which lead to differences in particle drag across the streamwise dimension of the curtain. Shortly thereafter, the particle field begins to propagate downstream and spread. For all three Mach numbers tested, the energy and momentum fluxes in the induced flow far downstream are reduced about 30-40% by the presence of the particle field. X-Ray diagnostics have been developed to penetrate the opacity of the flow, revealing the concentrations throughout the particle field as it expands and spreads downstream with time. Furthermore, an X-Ray particle tracking velocimetry diagnostic has been demonstrated to be feasible for this flow, which can be used to follow the trajectory of tracer particles seeded into the curtain. Additional experiments on single spherical particles accelerated behind an incident shock wave have shown that elevated particle drag coefficients can be attributed to increased compressibility rather than flow unsteadiness, clarifying confusing results from the historical database of shock tube experiments. The development of the Multiphase Shock Tube and associated diagnostic capabilities offers experimental capability to a previously inaccessible regime, which can provide unprecedented data concerning particle dynamics of dense gas-solid flows.

36 MATERIALS SCIENCE↗

Kalman-filtered compressive sensing for high resolution estimation of anthropogenic greenhouse gas emissions from sparse measurements.

The estimation of fossil-fuel CO2 emissions (ffCO2) from limited ground-based and satellite measurements of CO2 concentrations will form a key component of the monitoring of treaties aimed at the abatement of greenhouse gas emissions. The limited nature of the measured data leads to a severely-underdetermined estimation problem. If the estimation is performed at fine spatial resolutions, it can also be computationally expensive. In order to enable such estimations, advances are needed in the spatial representation of ffCO2 emissions, scalable inversion algorithms and the identification of observables to measure. To that end, we investigate parsimonious spatial parameterizations of ffCO2 emissions which can be used in atmospheric inversions. We devise and test three random field models, based on wavelets, Gaussian kernels and covariance structures derived from easily-observed proxies of human activity. In doing so, we constructed a novel inversion algorithm, based on compressive sensing and sparse reconstruction, to perform the estimation. We also address scalable ensemble Kalman filters as an inversion mechanism and quantify the impact of Gaussian assumptions inherent in them. We find that the assumption does not impact the estimates of mean ffCO2 source strengths appreciably, but a comparison with Markov chain Monte Carlo estimates show significant differences in the variance of the source strengths. Finally, we study if the very different spatial natures of biogenic and ffCO2 emissions can be used to estimate them, in a disaggregated fashion, solely from CO2 concentration measurements, without extra information from products of incomplete combustion e.g., CO. We find that this is possible during the winter months, though the errors can be as large as 50%.

Ray, Jaideep↗

Multi-Frame X-Ray Imaging Using a Streak Camera with a Patterned Photocathode, LAO-008-16, Year 1 of 2

Presentation describes development of a new time-resolved x-ray imaging system based on compressed ultrafast photography (CUP) to achieve multi-frame imaging for energies in the 1–10 keV range with a frame rate between 1 to 10 frames per nanosecond depending on the sweep time. A patterned gold photocathode was constructed for use with an existing Kentech x-ray streak camera. Significant work in reconstruction algorithms was performed to enable reconstructions of data that are much less sparse. These algorithms were tested with optical streak camera CUP data acquired at Livermore Operations.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Low-compressibility and hard material carbon nitride imide C{sub 2}N{sub 2}(NH): First principles calculations

First principles calculations are performed to investigate the structural, mechanical, and electronic properties of C{sub 2}N{sub 2}(NH). Our calculated lattice parameters are in good agreement with the experimental data and previous theoretical values. Orthorhombic C{sub 2}N{sub 2}(NH) phase is found to be mechanically stable at an ambient pressure. Based on the calculated bulk modulus and shear modulus of polycrystalline aggregate, C{sub 2}N{sub 2}(NH) can be regarded as a potential candidate of ultra-incompressible and hard material. Furthermore, the elastic anisotropy and Debye temperatures are also discussed by investigating the elastic constants and moduli. Density of states and electronic localization function analysis show that the strong C-N covalent bond in CN{sub 4} tetrahedron is the main driving force for the high bulk and shear moduli as well as small Poisson's ratio of C{sub 2}N{sub 2}(NH). -- Graphical abstract: Contours of electronic localization function (ELF) of C{sub 2}N{sub 2}(NH) on the: (0 0 1) plane (a), (1 0 0) plane (b), an ELF of Si{sub 2}N{sub 2}(NH) on the: (0 0 1) plane (c) and (1 0 0) plane (d). Display Omitted Research highlights: The structural, mechanical, and electronic properties of C{sub 2}N{sub 2}(NH) have been studied. C{sub 2}N{sub 2}(NH) is a potential low compressible and hard material. Both C{sub 2}N{sub 2}(NH) and Si{sub 2}N{sub 2}(NH) are found to have insulating feature with large band gaps. The strong covalent C-N bonding in CN{sub 4} tetrahedrons play a key role in the incompressibility and hardness of C{sub 2}N{sub 2}(NH). The chemical bonding in these two solids is a complex mixture of covalent and ionic characters.

36 MATERIALS SCIENCE↗

SEPARATION OF THE RIBBON FROM GLOBALLY DISTRIBUTED ENERGETIC NEUTRAL ATOM FLUX USING THE FIRST FIVE YEARS OF IBEX OBSERVATIONS

The Interstellar Boundary Explorer (IBEX) observes the IBEX ribbon, which stretches across much of the sky observed in energetic neutral atoms (ENAs). The ribbon covers a narrow (∼20°-50°) region that is believed to be roughly perpendicular to the interstellar magnetic field. Superimposed on the IBEX ribbon is the globally distributed flux that is controlled by the processes and properties of the heliosheath. This is a second study that utilizes a previously developed technique to separate ENA emissions in the ribbon from the globally distributed flux. A transparency mask is applied over the ribbon and regions of high emissions. We then solve for the globally distributed flux using an interpolation scheme. Previously, ribbon separation techniques were applied to the first year of IBEX-Hi data at and above 0.71 keV. Here we extend the separation analysis down to 0.2 keV and to five years of IBEX data enabling first maps of the ribbon and the globally distributed flux across the full sky of ENA emissions. Our analysis shows the broadening of the ribbon peak at energies below 0.71 keV and demonstrates the apparent deformation of the ribbon in the nose and heliotail. We show global asymmetries of the heliosheath, including both deflection of the heliotail and differing widths of the lobes, in context of the direction, draping, and compression of the heliospheric magnetic field. We discuss implications of the ribbon maps for the wide array of concepts that attempt to explain the ribbon's origin. Thus, we present the five-year separation of the IBEX ribbon from the globally distributed flux in preparation for a formal IBEX data release of ribbon and globally distributed flux maps to the heliophysics community.

79 ASTRONOMY AND ASTROPHYSICS↗

Heat release analysis for rapid compression machines: Challenges and opportunities

Heat release analysis (HRA) is commonly used in combustion studies to derive understandings of chemical and physical processes in situations where direct measurement is not practical. In internal combustion engines, it is typically based on crank-angle resolved pressure diagnostics. However, it has not been applied extensively to rapid compression machine datasets. There are various challenges associated with rigorous application of HRA, including a reasonable accounting of physical processes that occur during the test period, such as heat loss. Limitations associated with transducer robustness and data acquisition system fidelity also exist. On the other hand, there is potential to extract a wealth of information from pressure-time histories via HRA, such as quantifying the evolution and trends of preliminary exothermicity, e.g., low- and intermediate-temperature heat release, across a range of thermodynamic conditions; detecting the existence of non-uniform ignition phenomena during a test; and providing additional targets for the evaluation and improvement of chemical kinetic models. Finally, this work discusses such opportunities, and some approaches towards resolving various challenges.

42 ENGINEERING↗

Detection of Synchrophasor False Data Injection Attack using Feature Interactive Network

The synchrophasor data recorded by Phasor Measurement Units (PMUs) plays an increasingly critical role in the regulation and situational awareness of power systems. However, the widely installed PMUs are vulnerable to multiple malicious attacks from cyber hackers during data transmission and storage. To address this problem, a Modified Ensemble Empirical Mode Decomposition (MEEMD) is proposed first to extract the intrinsic mode functions of each Synchrophasor Data Attacks (SDA). The frequency-based adaptive screening criterion embedded in MEEMD is used to eliminate the false intrinsic mode functions. Next, a Multivariate Convolutional Neural Network (MCNN) is proposed to identify multiple SDA by utilizing the extracted intrinsic mode functions and original SDA as input vectors. A fusion block as the main structure of MCNN is also leveraged to increase the diversity of features and compress the model parameters. Integrating MEEMD and MCNN, a framework with automatic feature extraction and multi-source information fusion capability, referred to as Feature Interactive Network (FIN), is proposed to detect multiple SDA. Based on the proposed FIN framework, six types of SDA are explored for the first time using actual synchrophasor data in FNET/Grideye that was collected from different locations in the U.S. Eastern Interconnection. Finally, a large quantity of experiments with different attack strengths are used to evaluate the adaptability and classification performance of the proposed FIN.

24 POWER TRANSMISSION AND DISTRIBUTION↗

PART 1- techno-economic analysis of a grid scale Ground-Level Integrated Diverse Energy Storage (GLIDES) technology

In this paper, a techno-economic model / cost reduction analysis of a low-cost, dispatchable / scalable, efficient Ground-Level Integrated Diverse Energy Storage (GLIDES) system is analyzed, along with a review of existing state-of-the-art energy storage technologies. The introduced technology, GLIDES, which was invented at the Oak Ridge National Laboratory (ORNL), stores energy by compression and expansion of air using water as a liquid piston inside high-pressure reservoirs. GLIDES is introduced by combining Pumped Hydroelectric Storage (PHS) and Compressed Air Energy Storage (CAES) technologies. Here, by replacing inefficient gas compressor and turbine with higher efficiency liquid turbomachines for liquid-piston compression/expansion, GLIDES achieves higher roundtrip efficiency than other gas compression-based energy storage technologies and is a scalable energy storage system. For cost reduction purposes, various pressure reservoirs including steel vessels, carbon fiber vessels, pipe segments, and underground pressure reservoirs are analyzed in this paper. Based on the analyzed data using the models discussed in this paper, energy storage costs as low as ~$14/kWh and ~346/kWh (roundtrip efficiency (RTE) ~80%) can be achieved for a grid-scale GLIDES using depleted oil/gas reservoirs and high-pressure pipe segments respectively.

25 ENERGY STORAGE↗

FeCoSiBNbCu bulk metallic glass with large compressive deformability studied by time-resolved synchrotron X-ray diffraction

By adding 0.5 at. % Cu to the strong but brittle [(Fe{sub 0.5}Co{sub 0.5}){sub 0.75}Si{sub 0.05}B{sub 0.20}]{sub 96}Nb{sub 4} bulk metallic glass, fully amorphous rods with diameters up to 2 mm were obtained. The monolithic samples with 1 mm diameter revealed a fracture strain of 3.80% and a maximum stress of 4143 MPa upon compression, together with a slight work-hardening behavior. SEM micrographs of fractured samples did neither reveal any shear bands on the lateral surface nor the typical vein patterns which characterize ductile fracture. However, some layers appear to have flowed and this phenomenon took place before the brittle final fracture. An estimate of the temperature rise ΔT in the shear plane gives 1039 K, which is large enough to melt a layer of 120 nm. The overall performance and the macroscopic plastic strain depend on the interaction between cleavage-like and viscous flow-like features. Mechanical tests performed in-situ under synchrotron radiation allowed the calculation of the strain tensor components, using the reciprocal-space data and analyzing the shift of the first (the main) and the second broad peak positions in the X-ray diffraction patterns. The results revealed that each atomic shell may have a different stiffness, which may explain the macroscopic compressive plastic deformation. Also, there were no signs of (nano) crystallization induced by the applied stress, but the samples preserve a monolithic amorphous structure until catastrophic failure occurs.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Testing of Crystalline Silicotitanate to Support Tank-Side Cesium Removal System Operations - 20458

The direct feed of waste from the Hanford tank farms to the Low-Activity Waste Facility at the Hanford Waste Treatment and Immobilization Plant requires an intermediate treatment step that prepares the waste for vitrification. Washington River Protection Solutions (WRPS) selected a near-tank treatment system known as the Tank-Side Cesium Removal (TSCR) system to perform the required intermediate treatment functions. The approach in the TSCR system is to filter waste supernatant with a sintered metal dead-end filter and then use a series of ion exchange columns to remove cesium; this system has several similarities to the Tank Closure Cesium Removal system that has been deployed on the Savannah River Site. The ion exchange media proposed for use is crystalline silicotitanate (CST), which is a non-elutable media with a high affinity for cesium. Because the media is non-elutable, loaded columns will be blown down with compressed air, moved into interim storage, and replaced with new columns when cesium capacity is reached. The assumed extent and rate of drying that could be achieved in the TSCR column geometry lacked confirmation by experimental data. In addition, once the columns are loaded with cesium, they generate flammable gases (primarily hydrogen) via radiolysis acting on any resident liquids, i.e., moisture, remaining in the media bed. An assessment of available information on CST concluded that gas generation data that bounds expected operational conditions were needed to support the TSCR system safety basis and planned operations. Working with WRPS, Pacific Northwest National Laboratory (PNNL) designed and conducted testing with CST media to address the need for (a) representative in-column drying data, and (b) bounding flammable gas generation data. Drying testing was performed using a full-height column with a diameter of approximately 2 inches with injected air at temperatures of 18 deg. C and 30 deg. C. Gas generation testing was conducted in an engineered bunker that allowed simultaneous irradiation of up to eight samples at a time. These two experimental approaches used at PNNL for the CST testing are summarized and the major outcomes are presented. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Laboratory Strategies for Hydrate Formation in Fine‐Grained Sediments

Abstract Fine‐grained sediments limit hydrate nucleation, shift the phase boundary, and hinder gas supply. Laboratory experiments in this study explore different strategies to overcome these challenges, including the use of a more soluble guest molecule rather than methane, grain‐scale gas‐storage within porous diatoms, ice‐to‐hydrate transformation to grow lenses at predefined locations, forced gas injection into water saturated sediments, and long‐term guest molecule transport. Tomographic images and thermal and pressure data provide rich information on hydrate formation and morphology. Results show that hydrate formation is inherently displacive in fine‐grained sediments; lenses are thicker and closer to each other in compressible, high specific surface area sediments subjected to low effective stress. Temperature and pressure trajectories follow a shifted phase boundary that is consistent with capillary effects. Exo‐pore growth results in freshly formed hydrate with a striped and porous structure; this open structure becomes an effective pathway for gas transport to the growing hydrate front. Ice‐to‐hydrate transformation goes through a liquid stage at premelt temperatures; then, capillarity and cryogenic suction compete, and some water becomes imbibed into the sediment faster than hydrate reformation. The geometry of hydrate lenses and the internal hydrate structure continue evolving long after the exothermal response to hydrate formation has completely decayed. Multiple time‐dependent processes occur during hydrate formation, including gas, water and heat transport, sediment compressibility, reaction rate, and the stochastic nucleation process. Hydrate formation strategies conceived for this study highlight the inherent difficulties in emulating hydrate formation in fine‐grained sediments within the relatively short time scale available for laboratory experiments.

Lei, L.↗