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At least 1,441 records · Page 80

The αs and θs in Rayleigh–Taylor and Richtmyer–Meshkov instabilities

The alphas (α b , α s ) and thetas (θ b , θ s ) are the essential parameters describing the asymptotic growth behavior of the mixing layer driven by Rayleigh–Taylor (RT) and Richtmyer–Meshkov (RM) instabilities at the interface between the fluids. Extensive simulations and experiments have been conducted in the determination of these parameters. The results depend on numerical algorithms, resolutions, and the accuracy of experimental measurements. In this article, we present a unique relationship between the alphas and thetas by applying a simple buoyancy-drag mixing model. Our first main result is that, for the same fluids, these parameters are not independent because they are fundamentally connected by physics principles and they all are functions of the drag coefficients of the fluids. As a consequence, the alphas and thetas are intrinsically coupled. All are functions of any single one of these. Additionally, our second main result is that the RT bubble growth rate (α b ) is determined by the bubble competition process – a merger model – at the edge of the mixing layer. Together, these two main results determine all the alphas and thetas by strictly theoretical reasoning. Applications to both hydro and laser driven experiments at OMEGA are presented.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

A buoyancy–shear–drag–scalar-based turbulence model for power-law acceleration-driven Rayleigh–Taylor, reshocked Richtmyer–Meshkov, and Kelvin–Helmholtz mixing

A previously developed phenomenological turbulence model for Rayleigh–Taylor, reshocked Richtmyer–Meshkov, and Kelvin–Helmholtz instability-induced mixing based on a general buoyancy–shear–drag model [O. Schilling, “A buoyancy–shear–drag-based turbulence model for Rayleigh–Taylor, reshocked Richtmyer–Meshkov, and Kelvin–Helmholtz mixing,” Physica D 402, 132238 (2020)] is extended to include active or passive scalar mixing and power-law acceleration-driven Rayleigh–Taylor mixing. The buoyancy–shear–drag equations are coupled to a scalar variance equation that is used to define the molecular mixing parameter θ m , and when the scalar is active, modifies the Rayleigh–Taylor and Kelvin–Helmholtz mixing layer growth parameters to depend on the asymptotic value of this parameter, θ mol . Here, the scalar variance equation is closed by algebraically or differentially modeling the scalar variance dissipation rate. Nonlinear analytical solutions of the model are obtained in the total and separate bubble and spike mixing layer width formulations with the algebraic scalar variance dissipation rate for each instability, which are then used to calibrate the mechanical and scalar equation coefficients to predict specific values of physical observables and molecular mixing parameters. Surrogate mechanical and scalar turbulent fields can be constructed by multiplying a presumed self-similar spatial profile by appropriate functions of the width and its time derivative, and of the scalar obtained by solving the ordinary differential model equations. The explicit modeling and solution of turbulent transport equations are not required. The bubble and spike mixing layer width and scalar variance equations are then solved numerically for constant-acceleration Rayleigh–Taylor, impulsively reshocked Richtmyer–Meshkov, and Kelvin–Helmholtz mixing, confirming that the prescribed level of molecular mixing is correctly predicted and illustrating the spatiotemporal evolution of the scalar fields.

Buoyancy–drag↗

Two-phase flow measurements and observations in a cooling panel of the reactor cavity cooling system

The analysis of the flow behavior within a cooling panel of a scaled water-cooled reactor cavity cooling system has been performed supported by high-resolution measurements of the void fraction at the risers’ outlet. The results have shown a stable, symmetric distribution of the flow through the risers during subcooled boiling conditions, characterized by small, slow bubbles with average void fraction lower than 0.3 for all risers. As the temperature increased to saturation, flow distribution appeared strongly asymmetrical and unstable, with peaks of void fraction as high as 0.9. Large, faster bubbles were observed during these peaks, immediately followed by flow of subcooled liquid water. Flow stagnation and inversion has also been observed. The high resolution void fraction results, complemented by the measurements of the coolant flow rate and temperatures, not only have further described the behavior of the system under hypothetical accident conditions, but represent a unique set of data to support the validation of system-level codes, and more advanced computational tools.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Achieving superior carbon transfer efficiency and pH control using membrane carbonation with a wide range of CO 2 contents for the coccolithophore Emiliania huxleyi

The economic viability of microalgal-derived products relies on rapid CO 2 transfer in a cost-effective manner. Many industrial gas streams contain concentrated CO 2 that, if converted to useful products, would lower greenhouse gas emissions and valorize the wasted CO 2 . Membrane carbonation (MC) uses non-porous hollow-fiber gas-transfer membranes to deliver CO 2 without bubble formation, which makes it possible to achieve a high carbon-transfer efficiency (CTE). However, inert gasses in the industrial streams (e.g., N 2 , O 2 , and H 2 O) can significantly lower the CO 2 -delivery rate. The means to overcome the buildup of inert gases in the membrane lumen is to manage the distal end of the membranes to sweep out inert gases while not wasting significant CO 2 . A MC-venting strategy was evaluated for CO 2 inputs from 5% to 100%. Abiotic tests using a restricted exit flow could achieve >95% CTE abiotic for industrial CO 2 streams. When integrated with semi-continuous cultivation of a marine coccolithophore, Emiliania huxleyi , CO 2 delivery and venting were on-demand based on a pH set points and pH-actuated feed and venting valves. MC using the venting strategy achieved 100% CTE biotic when delivering 100% and 50% CO 2 , which was better than 50% CTE biotic obtained from pH-controlled sparging of 100% CO 2 -sparging. E. huxleyi consistently fixed ~80% of the delivered CO 2 into biomass, and the remaining ~20% to calcite coccoliths. Finally, the compact size of MC modules, stable pH control, and no shear forces from bubble agitation during the CO 2 delivery made MC an ideal match for cultivation of coccolithophores, which are sensitive to shear forces and pH fluctuations.

54 ENVIRONMENTAL SCIENCES↗

Effects of helium cavity size and morphology on the strength of pure titanium

In this study, high-purity α-titanium was implanted with helium to observe cavity morphology – size, number density, and form (i.e., bubbles vs. voids) – effects on materials strength. Increasing implantation temperatures lead to an Arrhenius-type (i.e., exponential) increase in cavity size, a transition from spherical bubbles to faceted voids, and a marked increase in strength (~20–50%). Implanted samples deformed uniformly in contrast to nano-compression of unimplanted or alloyed titanium, but pillars with the largest faceted voids developed a type of bulging localized deformation. Affected voids were repeatedly sheared, becoming rough and shrunken. Dislocation-cavity interactions and the role of helium content within cavities are considered.

36 MATERIALS SCIENCE↗

Reduced order modeling of a fluidized bed particle receiver for concentrating solar power with thermal energy storage

Oxide particles can serve as both the heat transfer and thermal energy storage (TES) media for next-generation concentrating solar power (CSP) plants where high-temperature TES enables dispatchable electricity from efficient power cycles with firing temperatures above 600 °C. Transferring heat to flowing particles at such high temperatures in a MW-scale central tower receiver remains a challenge for the CSP community. For indirect receivers with external walls to contain the particles, maintaining wall temperatures below the limits of structural metal alloys requires high heat transfer coefficients between the wall and the moving particle stream. Bubbling fluidization of downward-flowing particles can sustain high bed-wall heat transfer coefficients (> 1000 W m -2 K -1 ). Using experimentally calibrated correlations for bed-wall heat transfer and vertical particle dispersion, this study implements an axially discretized zonal model of a counterflow fluidized bed receiver to explore how bubbling fluidization may enable indirect cavity particle receivers. High bed-wall heat transfer coefficients support solar fluxes on angled cavity walls > 200 kW m -2 at peak aperture fluxes of 980 kW m -2 while maintaining external wall temperatures < 950 °C. Lateral particle dispersion enables hotter particles near the receiver leading edge to mix with cooler particles further from the leading edge to lower maximum external wall temperatures. Parametric studies identify how mass fluxes, particle dispersion, and solar concentrations impact indirect receiver thermal efficiency and uniformity for a CSP plant. These studies provide a basis for the design of indirect fluidized-bed cavity receivers that can maintain particle outlet temperatures for TES above 750 °C.

14 SOLAR ENERGY↗

A phase-field model of quasi-brittle fracture for pressurized cracks: Application to UO 2 high-burnup microstructure fragmentation

Here, in this paper, we present a phase-field model of quasi-brittle fracture with pressurized cracks, with dedicated applications for polycrystalline materials. The model is formulated as a minimization problem within the variational framework. The external work done by pressure on the crack surfaces is included in the objective function. Several careful modeling choices lead to a regularization-length-independent critical strength. The model is constructed to give a softening response with an underlying linear traction-separation law. The pressure-dependent softening response and the regularization of the prescribed pressure are demonstrated with a (quasi) one-dimensional numerical analysis. In a two-dimensional numerical analysis under plane strain assumptions, the critical stress corresponding to crack propagation (as predicted by our quasi-brittle fracture model) is compared with linear elastic fracture mechanics (LEFM) analytical solutions. Our model is further utilized to simulate fission-gas-induced fragmentation of the UO 2 high-burnup structure (HBS). Simulation results show that pressurized bubbles can cause crack nucleation and propagation, and that the bubble size and the surrounding external pressure affect the critical pressure corresponding to crack nucleation. Simulations of a partial HBS at different recrystallization stages show that different grain structures (due to recrystallization) also influence crack paths and fragmentation morphology.

36 MATERIALS SCIENCE↗

Atomic resolution scanning transmission electron microscopy at liquid helium temperatures for quantum materials

Fundamental quantum phenomena in condensed matter, ranging from correlated electron systems to quantum information processors, manifest their emergent characteristics and behaviors predominantly at low temperatures. This necessitates the use of liquid helium (LHe) cooling for experimental observation. Atomic resolution scanning transmission electron microscopy combined with LHe cooling (cryo-STEM) provides a powerful characterization technique to probe local atomic structural modulations and their coupling with charge, spin and orbital degrees-of-freedom in quantum materials. However, achieving atomic resolution in cryo-STEM is exceptionally challenging, primarily due to sample drifts arising from temperature changes and noises associated with LHe bubbling, turbulent gas flow, etc. In this work, we demonstrate atomic resolution cryo-STEM imaging at LHe temperatures using a commercial side-entry LHe cooling holder. Firstly, we examine STEM imaging performance as a function of He gas flow rate, identifying two primary noise sources: He-gas pulsing and He-gas bubbling. Secondly, we propose two strategies to achieve low noise conditions for atomic resolution STEM imaging: either by temporarily suppressing He gas flow rate using the needle valve or by acquiring images during the natural warming process. Lastly, we show the applications of image acquisition methods and image processing techniques in investigating structural phase transitions in Cr 2 Ge 2 Te 6 , CuIr 2 S 4 , and CrCl 3 . In conclusion, our findings represent an advance in the field of atomic resolution electron microscopy imaging for quantum materials and devices at LHe temperatures, which can be applied to other commercial side-entry LHe cooling TEM holders.

36 MATERIALS SCIENCE↗

Imaging Charged Exciton Localization in van der Waals WSe 2 /MoSe 2 Heterobilayers

Exciton localization in transition-metal dichalcogenide monolayers is behind a variety of interesting phenomena and applications, including broad-spectrum solar cells and singlephoton emissions. Strain fields at the periphery of topographically distinct features such as nanoscopic bubbles were recently associated with localized charge-neutral excitons. Here, we use tip-enhanced photoluminescence (PL) to visualize excitons in WSe 2 /MoSe 2 heterobilayers (HBL). We find strong optical emission from charged excitons, particularly positively charged trions, in HBL supported by interlayer charge transfer. Our results reveal strong trion confinement, with a localization length scale comparable to the trion size, at the apex region inside individual nanoscopic bubbles. Nano-PL mapping also shows sub-10 nm spatial variations in the localized trion emission spectra, which stem from atomic-scale potential energy fluctuations. These findings demonstrate the possibility of confining charged exciton complexes that are electrically tunable, opening up further opportunities to probe many-body exciton physics, and to explore additional possible sites for strong exciton localization that can lead to quantum emissions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Raman Shifts in Two-Dimensional van der Waals Magnets Reveal Magnetic Texture Evolution

Two-dimensional (2D) van der Waals magnets comprise rich physics that can be exploited for spintronic applications. We investigate the interplay between spin-phonon coupling and spin textures in a 2D van der Waals magnet by combining magneto-Raman spectroscopy with cryogenic Lorentz transmission electron microscopy. Here we find that when stable skyrmion bubbles are formed in the 2D magnet, a field-dependent Raman shift can be observed, and this shift is absent for the 2D magnet prepared in its ferromagnetic state. Correlating these observations with numerical simulations that take into account field-dependent magnetic textures and spin--phonon coupling in the 2D magnet, we associate the Raman shift to field-induced modulations of the skyrmion bubbles and derive the existence of inhomogeneity in the skyrmion textures over the film thickness.

2D van der Waals magnet↗

Elastic Properties of Plasma-Exposed Tungsten Predicted by Molecular-Dynamics Simulations

We report results of systematic molecular-dynamics computations of the elastic properties of single-crystalline tungsten containing structural defects, voids and overpressurized He nanobubbles, related to plasma exposure of tungsten serving as a plasma- facing component (PFC) in nuclear fusion devices. Our computations reveal that the empty voids are centers of dilatation resulting in development of tensile stress in the tungsten matrix, whereas He-filled voids (nanobubbles) introduce compressive stress in the plasma-exposed tungsten. We find that the dependence of the elastic moduli of plasma-exposed tungsten, namely, the bulk, Young, and shear modulus, on its void fraction follows a universal exponential scaling relation. We also find that the elastic moduli of plasma-exposed tungsten soften substantially as a function of He content in the tungsten matrix, following an exponential scaling relation; this He-induced exponential softening is in addition to the softening caused in the matrix with increasing temperature. A systematic characterization of the dependence of the elastic moduli on the He bubble size reveals that He bubble growth affects significantly both the bulk modulus and the Poisson ratio of plasma-exposed tungsten, while its effect on the Young and shear moduli of the plasma-exposed material is weak. Our findings contribute directly to the development of a structure-properties database that is required for the predictive modeling of the dynamical response of PFCs in nuclear fusion devices.

36 MATERIALS SCIENCE↗

3D Printed Nickel–Molybdenum-Based Electrocatalysts for Hydrogen Evolution at Low Overpotentials in a Flow-Through Configuration

Three-dimensional (3D) printed, hierarchically porous nickel molybdenum (NiMo) electrocatalysts were synthesized and evaluated in a flow-through configuration for the hydrogen evolution reaction (HER) in 1.0 M KOH(aq) in a simple electrochemical H-cell. 3D NiMo electrodes possess hierarchically porous structures because of the resol-based aerogel precursor, which generates superporous carbon aerogel as a catalyst support. Relative to a traditional planar electrode configuration, the flow-through configuration allowed efficient removal of the hydrogen bubbles from the catalyst surface, especially at high operating current densities, and significantly decreased the overpotentials required for HER. An analytical model that accounted for the electrokinetics of HER as well as the mass transport with or without the flow-through configuration was developed to quantitatively evaluate voltage losses associated with kinetic overpotentials and ohmic resistance due to bubble formation in the porous electrodes. Furthermore, the chemical composition, electrochemical surface area (ECSA), and roughness factor (RF) were also systematically studied to assess the electrocatalytic performance of the 3D printed, hierarchically porous NiMo electrodes. An ECSA of 25163 cm2 was obtained with the highly porous structures, and an average overpotential of 45 mV at 10 mA cm–2 was achieved over 24 h by using the flow-through configuration. The flow-through configuration evaluated in the simple H-cell achieved high electrochemical accessible surface areas for electrochemical reactions and provided useful information for adaption of the porous electrodes in flow cells.

08 HYDROGEN↗

Interfacial Chemistry Involved in Selective Separation of NMC/LMO and LCO/LMO Binary Cathode Materials by Froth Flotation Using Oleic Acid

The variability in cathode compositions within recycled lithium-ion battery (LIB) feedstocks poses a significant challenge to efficient downstream refining processes. This study demonstrates the feasibility of using froth flotation with oleic acid as a collector to selectively separate lithium nickel-manganese-cobalt oxide (NMC) and lithium cobalt oxide (LCO) from lithium manganese oxide (LMO) materials. Laboratory-scale flotation tests achieved an 80% separation efficiency in a single stage, producing a froth product with >90% purity of NMC/LCO at approximately 90% yield. Concurrently, the LMO materials were enriched in the sink product with ∼90% purity and ∼90% yield. This approach was further validated using recycled cathode materials, confirming its applicability to realistic feedstocks. The underlying mechanism governing the selective separation of NMC/LCO from LMO was investigated using ζ-potential measurements, contact angle measurements, bubble-particle attachment experiments, and X-ray photoelectron spectroscopy (XPS) analysis. Both contact angle and bubble-particle attachment results confirmed that oleic acid adsorption rendered NMC and LCO surfaces hydrophobic, thereby enhancing flotation recovery. At pH 5, oleic acid adsorbed preferentially onto NMC and LCO surfaces via electrostatic interactions, while exhibiting minimal adsorption on LMO surfaces. However, separation efficiency deteriorated at higher pH, which was attributed to the co-flotation of LMO materials caused by oleate chemisorption on MnOH + species. This work establishes froth flotation as a viable cathode/cathode separation strategy, providing a low-cost, scalable pathway to preconcentrate and enrich nickel-rich and cobalt-rich cathode active materials from incompatible cathode chemistries for direct recycling or hydrometallurgical processing. Furthermore, this study reveals, for the first time, the mechanism of oleate adsorption on the surface of different cathode materials.

PH↗

Genesis and Propagation of Fractal Structures During Photoelectrochemical Etching of n-Silicon

The genesis, propagation, and dimensions of fractal-etch patterns that form anodically on front- or back-illuminated n-Si(100) photoelectrodes in contact with 11.9 M NH 4 F (aqueous) have been investigated during either a linear potential sweep or a constant potential hold ( E = +6.0 V versus Ag/AgCl). Optical images collected in situ during electrochemical experiments reflected the location and underlying mechanism of initiation and propagation of the structures on the surface. X-ray photoelectron spectroscopic (XPS) data collected for samples emersed from the electrolyte at varied times provided detailed information about the chemistry of the surface during fractal etching. The fractal structure was strongly influenced by the orientation of the crystalline Si sample. Furthermore, the etch patterns were initially generated at points along the circumference of bubbles that formed upon immersion of n-Si(100) samples in the electrolyte, most likely due to the electrochemical and electronic isolation of areas beneath bubbles. XPS data showed the presence of a tensile-stressed silicon surface throughout the etching process as well as the presence of SiO x F y on the surface. The two-dimensional fractal dimension, D f,2D , of the patterns increased with etching time to a maximum observed value of D f,2D = 1.82. Promotion of fractal etching near etch masks that electrochemically and electronically isolated areas of the photoelectrode surface enabled the selective placement of highly branched structures at desired locations on an electrode surface.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Exceptional Mineral Scaling Resistance from the Surface Gas Layer: Impacts of Surface Wetting Properties and the Gas Layer Charging Mechanism

Mineral scaling is a phenomenon that occurs on submerged surfaces in contact with saline solutions. In membrane desalination, heat exchangers, and marine structures, mineral scaling reduces process efficiency and eventually leads to process failure. Therefore, achieving long-term scaling resistance is beneficial to enhancing process performance and reducing operating and maintenance costs. While evidence shows that superhydrophobic surfaces may reduce mineral scaling kinetics, prolonged scaling resistance is limited due to the finite stability of the entrained gas layer present in a Cassie–Baxter wetting state. Additionally, superhydrophobic surfaces are not always feasible for all applications, but strategies for long-term scaling resistance with smooth or even hydrophilic surfaces are often overlooked. In this study, we elucidate the role of interfacial nanobubbles on the scaling kinetics of submerged surfaces of varied wetting properties, including those that do not entrain a gas layer. We show that both solution conditions and surface wetting properties that promote interfacial bubble formation enhances scaling resistance. In the absence of interfacial bubbles, scaling kinetics decrease as surface energy decreases, while the presence of bulk nanobubbles enhances the scaling resistance of the surface with any wetting property. The findings in this study allude to scaling mitigation strategies that are enabled by solution and surface properties that promote the formation and stability of interfacial gas layers and provide insights to surface and process design for greater scaling resistance.

calcite↗

Adsorption Hysteresis Under Control: Tuning Host–Guest Interactions via a Genetic Algorithm

Mesoporous adsorbent materials offer a large volumetric capacity; however, cyclic adsorption/desorption processes in these systems often suffer from hysteresis and may require a significant pressure swing to access this capacity. To mitigate hysteresis, a proposed strategy is to include nucleation sites on the walls of the mesoporous material to facilitate droplet and bubble formation, lowering the free energy barriers to the respective phase transitions. It is unclear, however, what combination of adsorbate− adsorbent interactions and spatial patterning would be beneficial for a given application, considering that improvements to some sorption properties may come at the expense of other attributes. To understand these interconnected observables, we examine two model systems, planar-slit and cylindrical pores with tunable interaction sites, using GPU-accelerated transition matrix Monte Carlo simulations. The simulations provide a free energy map of the pressure−adsorption space in a matter of minutes, which we use to track adsorption isotherm characteristics as a function of adsorbent properties. We then leverage the rapid acquisition of simulation data to construct a genetic algorithm to iteratively modify interaction sites of the slit-pore wall to minimize the hysteresis of this system without sacrificing uptake. We find that the adsorption branch of the isotherm is easily modulated via the average host−guest interaction strength, but desorption is only adjustable if there is a suitable bubble nucleation site. Within the context of a slit-pore system, we identify relative interaction strengths and patch sizes required to gain control over both branches of the hysteresis loop.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Field-Coupled Water Splitting with Metal-Free Donor–Acceptor Covalent Organic-Framework Junctions

Advancing metal-free electrocatalysts for hydrogen and oxygen evolution reactions (HER/OER) across acidic and alkaline media requires coordinated control of intermediate binding thermodynamics, interfacial charge delivery, and near-electrode transport dynamics. Here, we design amide-linked benzene–triazine covalent organic frameworks (BTA/TzTA-Hz COFs) and integrate them with carbon nanotubes (CNTs) to form COF–CNT junctions that establish a built-in interfacial electric field. Density functional theory (DFT) and electrostatic potential maps indicate complementary active motifs, with benzene-proximal fragments associated with HER and triazine-proximal motifs associated with OER. CNT integration shifts the contact-potential difference by ≈0.20 V, while operando electrochemical impedance spectroscopy suggests partially separable high-frequency junction-charging and lower-frequency Faradaic/transport responses. A 300 mT static magnetic field lowers the HER and OER overpotentials by tens of millivolts. Under anodic bias, the effective interfacial charging capacitance increases, and Mott–Schottky analysis shows an apparent ∼0.15 V flat-band shift with an essentially unchanged slope. Together, these observations are consistent with field-perturbed interfacial charging and altered bias partitioning. Field-dependent impedance and bubble imaging are consistent with magnetohydrodynamic convection that promotes bubble detachment and near-electrode mass transport for both half-reactions, and they reveal an OER-specific high-frequency perturbation under anodic bias. Under field, the heterostructure reaches an OER onset overpotential of ∼261 mV and requires an overpotential of 366 mV at 10 mA cm –2 in alkaline electrolyte. These results illustrate how reticular-framework chemistry, junction engineering, and both built-in and applied fields can program reactivity through interfacial electrostatics and near-electrode transport in organic-framework electrocatalysts.

Garcia-Enriquez, Lissette [Univ. of Texas at El Pa↗

How Does LCL Height Influence Deep Convective Updraft Width?

Previous studies have hypothesized that the width of deep convection should positively scale with lifting condensation level (LCL) height. To evaluate this hypothesis, we analyzed idealized large-eddy simulations with varying LCL heights and initial warm bubble widths in unsheared environments with comparable convective available potential energy. For a given initial warm bubble width, simulations with higher LCLs result in wider, deeper, and stronger cloudy updrafts compared to simulations with lower LCLs. Rising dry thermals in higher LCL simulations experience longer residence times within the sub-cloud layer, and consequently entrain more conditionally unstable air and grow wider before reaching the LCL. The resulting cloudy updrafts are wider, deeper, and have faster vertical velocities because of a reduction in entrainment-driven dilution of buoyancy, relative to lower LCL simulations. These results confirm the hypothesized positive relationship between LCL height and deep convective updraft width, and provide a physical explanation for this relationship.

58 GEOSCIENCES↗