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428 records · Page 24

Using Mineralogy of the Bagnold Dune Field in Gale Crater to Interpret Eolian Sediment Sorting on the Martian Surface

The Mars Science Laboratory Curiosity rover landed in Gale crater in August 2012 to characterize modern and ancient surface environments. Curiosity executed a two-phase campaign to study the morphology, activity, physical properties, and chemical and mineralogical composition of the Bagnold Dune Field, an active eolian dune field on the lower slopes of Aeolis Mons (Mount Sharp). Detectable aspects of dune sand mineralogy have been examined from orbit with the visible/short-wave infrared spectrometer CRISMand the thermal-infrared spectrometers THEMIS and TES. CRISM data demonstrate variations in plagioclase, pyroxene, and olivine abundances across the dune field. Curiosity analyzed sediments from two locations in the dune field to evaluate the causes of the mineralogical differences observed from orbit. The Gobabeb sample was collected from Namib Dune, a barchanoidal dune on the upwind margin of the dune field, and the Ogunquit Beach sample was collected from the Mount Desert Island sand patch located downwind from Namib. These samples were sieved to <150 μm and delivered to the CheMin X-ray diffraction instrument for quantitative mineralogical analysis. CRISM-derived mineralogy of the Namib Dune and Mount Desert Island and CheMin-derived mineralogy of the Gobabeb and Ogunquit Beach samples can be used in a value-added manner to interpret grain segregation at the bedform to dune-field scale and evaluate contributions from local sediment sources. Models of CRISM data demonstrate that Mount Desert Island is more enriched in olivine and less enriched in plagioclase than Namib dune, suggesting that fine-grained mafic sediments are preferentially mobilized downwind. Curiosity data indicate olivine also forms a coarse lag on the lee sides of barchanoidal dunes. Minor abundances of hematite, quartz, and anhydrite and small differences in the crystal chemistry of plagioclase and pyroxene derived from CheMin data suggest that sediments from the underlying lacustrine rocks also contribute to the Bagnold sands.

Rampe, E. B.↗

Revealing High-Temperature Reduction Dynamics of High-Entropy Alloy Nanoparticles via In Situ Transmission Electron Microscopy

Understanding the behavior of high-entropy alloy (HEA) materials under hydrogen (H 2 ) environment is of utmost importance for their promising applications in structural materials, catalysis, and energy-related reactions. Herein, the reduction behavior of oxidized FeCoNiCuPt HEA nanoparticles (NPs) in atmospheric pressure H-2 environment was investigated by in situ gas-cell transmission electron microscopy (TEM). The reduction reaction front was maintained at the external surface of the oxide. During reduction, the oxide layer expanded and transformed into porous structures where oxidized Cu was fully reduced to Cu NPs while Fe, Co, and Ni remained in the oxidized form. In situ chemical analysis showed that the expansion of the oxide layer resulted from the outward diffusion flux of all transition metals (Fe, Co, Ni, Cu). Revealing the H-2 reduction behavior of HEA NPs facilitates the development of advanced multicomponent alloys for applications targeting H 2 formation and storage, catalytic hydrogenation, and corrosion removal.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Development of Corrosion Resistant Coatings for Structural Materials for Liquid Fueled Molten Salts Reactors Applications (Final Report)

Current structural alloys, code certified for the MSRs temperature ranges, contain high levels of chromium, making them highly susceptible to molten halide salt corrosion. One potential solution to circumvent the need for code certification of novel alloys, which is expensive and time consuming, is to design claddings that will protect the underlying code certified materials from corrosion damage during operation. In this work, we examined the corrosion of Ni and Cu electroplated, Ni and CuNi weld overlay, Mo-laser clad, and carburized claddings on SS316H for use in molten salt reactor environments. After characterization of the cladded materials (Task 1), static corrosion tests were used to assess corrosion resistance of the claddings in typical molten fluoride salts (Task 2). The corrosion tests were performed in molten FLiNaK at 700°C up to 1000 hours. Pre- and post-corrosion Scanning Electron Microscopy (SEM), energy-dispersive-spectroscopy (EDS), Transmission Electron Microscopy (TEM), X-ray Diffraction (XRD) and glow-discharge-optical-emission-spectroscopy (GDOES) were performed on cladding cross-sections and surfaces to evaluate degradation. The Cu and Ni electroplated samples, as well as the carburized samples, showed excellent corrosion resistance relative to the bare SS316H. To assess high temperature cladding stability, ageing experiments were performed at temperatures up to 900 C in inert atmosphere for the electroplated and carburized samples and a diffusion model was developed to predict long term cladding behavior (Task 3). It was found that the Cu cladding was basically insensitive to the high temperature ageing, except for small secondary phases forming at the interface. On the other hand, the Ni electroplated cladding experienced significant interdiffusion. Nevertheless, the gain in corrosion resistance for a 100μm Ni electroplated cladding is phenomenal, with more than 50% reduction in chromium dissolution from the substrate material for the first 15 years of salt exposure at 700°C. To assess radiation resistance and phase stability, high-temperature 4MeV Ni heavy ion irradiation was performed across the cladding/substrate interface up to 50 displacement-per-atom (DPA) at 500°C and 700°C to assess the phase stability and irradiation behaviors of the electroplated systems (Task 4). The Ni and Cu electroplated systems did not experience void swelling at the contrary to the SS316H substrate due to their nanocrystalline nature. Some level of recrystallization was observed in the cladding, as well as radiation induced segregation and enhanced diffusion. The interface acted as a potent sink for point defects with the presence of a void denuded zone. The mechanical properties of the claddings were assessed using thermal shock, micro-indentation, nano-indentation, and four-point bend testing experiments (Task 5). These experiments were performed on the claddings in as-received, corroded, irradiated, and thermally aged states to determine the effects of typical molten salt reactor environments on cladding integrity. No significant mass loss was observed after repeated thermal shocks. While the electroplated samples softened after high-temperature ageing, irradiation hardening compensate this effect, such that there is little different with the as-received materials. The results of these experiments suggest that the electroplated (copper/nickel) show the greatest promise for application in molten salt reactor development. These claddings prevented any chromium dissolution from occurring during the static corrosion experiments. Additionally, they demonstrated favorable properties for high temperature diffusion, phase stability, interfacial mechanical properties, and irradiation resistance. Weld-overlay cladding are also of great interest and could reach properties similar to the electroplated samples upon optimization (especially with multiple weld passes). The carburized SS316H showed excellent behavior as well, but more work needs to be done to assess their long-term stability. Finally, the Mo-laser clad system was not pursued further due to the manufacturing challenges. It is also worth noting that the Ni cladding systems should behave relatively well in terms of weldability since the Ni-weld overlay microstructure and associated corrosion rate are sound. While the NiCu weld-overlay has even lower corrosion rates than the Ni-weld overlay, more studies on welding of Cu-electroplated systems are necessary since Cu clusters are known to embrittle steels.

36 MATERIALS SCIENCE↗

Effect of Marangoni Convection Generated by Voids on Segregation During Low-G and 1-G Solidification

Solidification experiments, especially microgravity solidification experiments, are often compromised by the evolution of unwanted voids or bubbles in the melt. Although these voids and/or bubbles are highly undesirable, there is currently no effective means of preventing their formation or of eliminating their adverse effects, particularly during microgravity experiments. Marangoni convection caused by these voids can drastically change the transport processes in the melt. Recent microgravity experiments by Matthiesen (1) Andrews (2) and Fripp (3) are perfect examples of how voids and bubbles can affect the outcome of costly space experiments and significantly increase the level of difficulty in interpreting their results. Formation of bubbles have caused problems in microgravity experiments for a long time. Even in the early Skylab mission an unexpectedly large number of bubbles were detected in the four materials processing experiments reported by Papazian and Wilcox (4). They demonstrated that while during ground-based tests bubbles were seen to detach from the interface easily and float to the top of the melt, in low-gravity tests no detachment from the interface occurred and large voids were grown in the crystal. More recently, the lead-tin-telluride crystal growth experiment of Fripp et al.(3) flown aboard the USMP-3 mission has provided very interesting results. The purpose of the study was to investigate the effect of natural convection on the solidification process by growing the samples at different orientations with respect to the gravitational field. Large pores and voids were found in the three solid crystal samples processed in space. Post-growth characterization of the compositional profiles of the cells indicated considerable levels of mixing even in the sample grown in the hot-on-top stable configuration. The mixing was attributed to thermocapillary convection caused by the voids and bubbles which evolved during growth. Since the thermocapillary convection is orientation-independent, diffusion-controlled growth was not possible in any of the samples, even the top-heated one. These results are consistent with recent studies of thermocapillary convection generated by a bubble on a heated surface undertaken by Kassemi and Rashidnia (5-7) where it is numerically and experimentally shown that the thermocapillary flow generated by a bubble in a model fluid (silicone oil) can drastically modify the temperature field through vigorous mixing of the fluid around it, especially under microgravity conditions.

Kassemi, M.↗

Interstitial solute segregation at triple junctions: Implications for nanomaterials and a case study of hydrogen in palladium

At very fine grain sizes, grain boundary segregation can deviate from conventional behavior due to triple junction effects. While this issue has been addressed in prior work for substitutional alloys, here we develop a framework that accounts for interstitial sites in the grains, grain boundaries, and triple junctions of model Pd(H) polycrystals. This approach allows computation of interstitial segregation spectra separately at both defect types, which permits an understanding of segregation at all grain sizes via a size-scaling spectral isotherm. Here, the size dependencies of dilute Pd(H) are found to be influenced not only by the triple junction content, but also by grain size–dependent lattice strains; the latter effect is evidenced by size dependencies of individual grain boundary and junction subspectra. The framework proposed here is applicable to interstitial alloys in general and may serve as a basis for interfacial engineering in interstitial nanocrystalline alloys. As an example, we show that using the dilute limit isotherm, hydrogen density can triple in nanocrystalline vis-à-vis microcrystalline Pd due to hydrogen adsorption at intergranular defect sites.

Alloys↗

A Novel Method for Breath Capture Inside a Space Suit

Any non-robotic mission to the Mars surface will need to rely on various life support technologies. The large metabolic generation rate and low tolerance to elevated levels of carbon dioxide (CO2) in the Mars atmosphere make CO2 removal one of the preeminent tasks in this domain. In addition, these same features provide a strong impetus for using regenerable CO2 removal technologies. In the past, many of these regenerable technologies have relied on the low partial pressure CO2 surrounding the vehicle to provide an ultimate sink for removing this gas contaminant, however any Mars mission will have to overcome the presence of the Mars atmosphere. This paper describes the investigation of methods to capture the exhaled CO2 from a suited crewmember before it becomes diluted with the high volumetric air flow present within the space suit. Typical expired air contains CO2 partial pressures in the range of 20-35 mm Hg. This research investigated methods to capture this high partial pressure CO2 prior to its dilution with the low partial pressure CO2 ventilation flow. Specifically the research looked at potential designs for a collection cup for use inside the space suit helmet. This collection cup should not be considered the same as a breathing mask typical of that worn by firefighters, etc. Instead, the collection cup is a non-contact device that makes use of detailed analyses of the ventilation flow environment within the helmet. The research used a detailed Computational Fluid Dynamic (CFD) code called Fluent to provide modeling of the various gas species (CO2, water vapor, O2) as they pass through a helmet. This same model was used to numerically evaluate several different collection cup designs for this same CO2 segregation effort.

Paul, Heather↗

The Role of Marangoni Convection for the FZ-Growth of Silicon

Fluctuations of the electrical resistivity due to inhomogeneous dopant distribution are still a serious problem for the industrial processing yield of doped silicon crystals. In the case of silicon floating-zone growth, the main sources of these inhomogeneities are time- dependent flows in the liquid phase during the growth process. Excluding radio frequency (RF) induced convection, buoyancy and thermocapillary (Marangoni) convection are the two natural reasons for fluid flow. Both originate from temperature/concentration gradients in the melt, buoyancy convection through thermal/concentrational volume expansion, and thermocapillary convection through the temperature/concentration dependence of the surface tension. To improve the properties of grown crystals, knowledge of the strength, the characteristic, and the relation of these two flow mechanisms is essential. By the use of microgravity, the effect and the strength of buoyancy (gravity dependent) and thermocapillary (gravity independent) convection can be separated and clarified. Applying magnetic fields, both convective modes can be influenced: fluid flow can either be damped (static magnetic fields) or overlaid by a regular flow regime (rotating magnetic fields). Two complementary approaches have been pursued: Silicon full zones (experiments on the German sounding rockets TEXUS 7, 12, 22, 29, and 36) with the maximum temperature at half of the zone height and silicon half zones (experiments on the Japanese sounding rockets TR-IA4 and 6) with the maximum temperature at the top of the melt. With the full zone arrangement, the intensity and the frequency of the dopant striations could be determined and the critical Marangoni number could be identified. The half zone configuration is suited to classify the flow pattern and to measure the amplitude and the frequency of temperature fluctuations in the melt by inserting thermocouples or temperature sensors into the melt. All experiments have been carried out in monoellipsoid mirror furnaces. Typical zone geometries are approx. 8 to 14 mm in diameter and height. The crystals grown under microgravity are compared to crystals grown in static axial magnetic fields (B<5 tesla) and in transversal rotating magnetic fields (B<7.5 mT / f=50 Hz). Experimental results are completed by 3D numerical simulations: the obtained temperature and concentration distribution in the melt confirm the damping effect of rotating magnetic fields and explain the change in the radial segregation under static magnetic fields.

Dold, P.↗

In-service corrosion and grain boundary oxidation in neutron-irradiated 316 stainless steel baffle-former bolts

Reactor core internal components such as baffle-former bolts (BFBs) are subjected to significant mechanical stress, corrosive environment, and neutron irradiation from the reactor core during the plant operation. Over the long operation period, these conditions lead to potential degradation and of the bolts. In this work, characterization was performed on the oxidized surface of stainless steel BFBs harvested from a commercial pressurized water reactor (PWR) after 40 years of operation. The analysis shows that a complex multilayered surface oxide with six identified layers formed that is different from 2-layer structure commonly observed in model experiments. The oxide varies by composition – predominantly Fe, Cr, and Ni, grain size, and phase, and has features resembling both unirradiated and radiation/ corrosion experiments likely due to the low radiation flux compared to ion-irradiation or the test reactor radiation. In addition, grain boundary oxidative attack featured a pathway for Fe and other elements to move from the metal matrix to the outermost oxide. In conclusion, the results help assess PWR lifetime extension, put into context previous experimental studies, and provide input for designing experiments combining radiation and corrosion effects.

Baffle-former bolt↗

Evaluating Transfer and Pumping of Slurries from Pulsed Jet Mixed Vessels

Due to gravity, solids in slurries will settle if density differences between the solids and liquid are positive (i.e., particle has a negative buoyant force) unless rheological properties and flow conditions are adequate to overcome the gravitational effects. The rate of settling depends on the force balance of the particle, which includes the surface forces associated with fluid rheology. Given the same fluid and solid properties, particles that are larger and denser tend to settle faster. When pumping slurry into a vessel at concentrations precluding hindered settling with insufficient mixing, particle and density distributions can result in preferential settling, creating stratification in the solids concentration within the vessel. For vessels with transfer line inlets located in the lower portion of the tank, the stratified solids concentration may be detrimental to the transfer system performance. Elevated concentrations of solids in the slurry entrained at the inlet to the transfer line can result in the effective viscosity or slurry bulk density exceeding the design limits of the pump. These conditions could result in plugging of the transfer line or onset of cavitation of the pumps because of excessive pressure drop. These conditions can be exacerbated with periodic inlet conditions existing at the transfer line inlet. Periodic conditions can result when vessel mixing is intermittent such as with pulsed jet mixers (PJM). The transfer line inlet conditions are impacted by the periodic nature of the PJM operations with respect to suspension of solids and their transport to the inlet of the transfer line. A scaling approach is presented, and corresponding test requirements are developed for assessing the prevention of plugging the pipeline. Line plugging mechanisms are addressed that do not include plugging due to steady-state high-density slurry entering the transfer line and reducing the net positive suction head available (NPSHA) at the pump inlet to below that required for pump operation. Items considered include the transition to reduced relative flow velocities, such that the critical pipe velocity for solids deposition, Ucd, is not maintained, and segregation of heavy solids during the transport. The recommended requirements to prevent plugging include: • Limits for viscosity and density for entrained slurry to prevent the pressure drop in the pipeline from exceeding pump capacity. • Limits for viscosity and density for entrained slurry to prevent the net positive suction head available (NPSHA) from falling below the net positive suction head required (NPSHR) for operating the pump. • Transfer line velocity and flow rate requirements to maintain solids in suspension, while avoiding line plugging that results from deposition of solids within the transfer line. This paper describes the development of the scaling and testing requirements to verify that proposed approaches for transfer and pump out are appropriately developed

periodic flow, mixing, pipeline plugging, scaling,↗

Modeling Functional Organic Chemistry in Arctic Rivers: An Idealized Siberian System

Rivers of the Arctic will become ever more important for the global climate, since they carry a majority of continental dissolved organic carbon flux into the rapidly changing polar ocean. Aqueous organics comprise a wide array of functional groups, several of which are likely to impact coastal and open water biophysical properties. Light attenuation, interfacial films, aerosol formation, gas release and momentum exchange can all be cited. We performed Lagrangian kinetic modeling for the evolution of riverine organic chemistry as the molecules in question make their way from the highlands to Arctic outlets. Classes as diverse as the proteins, sugars, lipids, re-condensates, humics, bio-tracers and small volatiles are all included. Our reduced framework constitutes an idealized northward flow driving a major hydrological discharge rate and primarily representing the Russian Lena. Mountainous, high solute and tundra sources are all simulated, and they meet up at several points between soil and delta process reactors. Turnover rates are parameterized beginning with extrapolated coastal values imposed along a limited tributary network, with connections between different terrestrial sub-ecologies. Temporal variation of our total dissolved matter most closely resembles the observations when we focus on the restricted removal and low initial carbon loads, suggesting relatively slow transformation along the water course. Thus, channel combinations and mixing must play a dominant role. Nevertheless, microbial and photochemical losses help determine the final concentrations for most species. Chemical evolution is distinct for the various functionalities, with special contributions from pre- and post-reactivity in soil and delta waters. Several functions are combined linearly to represent the collective chromophoric dissolved matter, characterized here by its absorption. Tributaries carry the signature of lignin phenols to segregate tundra versus taiga sources, and special attention is paid to the early then marine behaviors of low molecular weight volatiles. Heteropolycondensates comprise the largest percentage of reactive carbon in our simulations due to recombination/accumulation, and they tend to be preeminent at the mouth. Outlet concentrations of individual structures such as amino acids and absorbers lie above threshold values for biophysical influence, on the monolayer and light attenuation. The extent of coastal spreading is examined through targeted regional box modeling, relying on salinity and color for calibration. In some cases, plumes reach the scale of peripheral arctic seas, and amplification is expected during upcoming decades. Conclusions are mapped from the Lena to other boreal discharges, and future research questions are outlined regarding the bonding type versus mass release as permafrost degrades. Dynamic aqueous organic coupling is recommended for polar system models, from headwaters to coastal diluent.

54 ENVIRONMENTAL SCIENCES↗

Exploring structural transitions at grain boundaries in Nb using a generalized embedded atom interatomic potential

The advancement in experimental techniques, like the atom probe tomography and high resolution electron microscopy, is fueling interest in studying structural transformations of grain boundaries in metal and alloys to uncover correlations between mechanical properties and solute or impurity segregation to grain boundaries. Atomistic modeling is an important tool that can pinpoint the intricate dynamics of grain boundary phase transitions, but the lack of accurate interatomic potentials needed to simulate the complex dynamics of grain boundary structural transitions and identify different metastable phases has been the bottleneck. To this end, we use niobium as a model body centered cubic (BCC) metal and develop an interatomic potential to study grain boundary phase transitions. The potential for Nb is based on a generalization of the embedded atomic method potential and has sufficient flexibility to learn complex energy landscapes using a small set of training structures. We systematically test and validate the using data from ab initio density functional theory calculations and experiments. Using this potential, we calculate energies of multiple symmetric-tilt grain boundaries spanning a wide range of misorientation angles. Additionally, we explore different metastable structures of the Σ 27(552) [$1\overline{1}0$] grain boundary and use molecular dynamic simulations to study the coexistence of metastable phases and grain boundary transitions at finite temperature.

36 MATERIALS SCIENCE↗

Atomic motifs govern the decoration of grain boundaries by interstitial solutes

Abstract Grain boundaries, the two-dimensional defects between differently oriented crystals, tend to preferentially attract solutes for segregation. Solute segregation has a significant effect on the mechanical and transport properties of materials. At the atomic level, however, the interplay of structure and composition of grain boundaries remains elusive, especially with respect to light interstitial solutes like B and C. Here, we use Fe alloyed with B and C to exploit the strong interdependence of interface structure and chemistry via charge-density imaging and atom probe tomography methods. Direct imaging and quantifying of light interstitial solutes at grain boundaries provide insight into decoration tendencies governed by atomic motifs. We find that even a change in the inclination of the grain boundary plane with identical misorientation impacts grain boundary composition and atomic arrangement. Thus, it is the smallest structural hierarchical level, the atomic motifs, that controls the most important chemical properties of the grain boundaries. This insight not only closes a missing link between the structure and chemical composition of such defects but also enables the targeted design and passivation of the chemical state of grain boundaries to free them from their role as entry gates for corrosion, hydrogen embrittlement, or mechanical failure.

36 MATERIALS SCIENCE↗

Day 640 infrared line and continuum measurements: Dust formation in SN 1987A

We have measured day 640-645 line and continuum spectra of (Ni II) 6.6 micrometer (Ne II) 12.8 micrometer (line emission was not detected), and (Fe II) 17.9 and 26.0 micrometer from SN 1987A. The high velocity feature at v(sub HVF) approximately 3900 km/sec found in both of our day 410 (Fe II) spectra is again detected in the day 640 (Ni II) spectrum, although the signal-to-noise of the day 640 (Fe II) spectra is insufficient to show this feature. The continuum fluxes provide clear evidence for the formation of dust between day 410 and day 640 and are best fitted by a graybody spectrum with a temperature of 342 +/- 17 K at day 640 and a surface area corresponding to a minimum dust velocity v(sub dust) = 1910 +/- 170 km/sec. Optically thin dust emissivity laws proportional to lambda(exp -1) or lambda(exp -2) are inconsistent with the data. Either the dust grains are large (radius a much greater than 4 micrometer and radiate like individual blackbodies, or else they are located in clumps optically thick in the 6-26 micrometer range. The (Ni II) 6.6 micrometer line flux yields a minimum Ni(+) mass of 5.8 +/- 1.6 x 10(exp -4) solar mass and a Ni/Fe abundance ratio of 0.06 +/- 0.02, equal to the solar value. The ratio of the two (Fe II) line profiles implies a gas temperature 2600 +/- 700 K, a drop of 1800 +/- 800 K from our day 410 measurement. The (Fe II) 26.0 micrometer line flux has decreased by a factor of 2 and the day 640 (Ni II) profile is blueshifted by -440 +/- 270 km/sec, relative to observations before day 500. We show that the decrease in the (Fe II) flux and the blueshift are not produced by a decrease in electron scattering optical depth, electron density, or temperature, but rather are probably due to obscuration by the same dust which produces the infrared continuum. This supports the interpretation that the dust spectrum is produced by optically thick clumps. We discuss possible explanations for the discrepancy between the mass of Fe(+) detected and the total iron mass required to power the light curve. The decrease in the (Fe II) fluxes relative to the decrease required to account for the blueshifts of optical lines from non-iron-group elements and the similarity between v(sub dust) and the Ni(+) expansion velocity imply a spatial association between the dust clumps and the iron-group elements. In addition, the larger blueshift observed for the near and far-infrared, heavy metal transitions relative to non-iron-group lines suggests that the iron-group elements are somewhat segregated from lighter elements such as the Mg(sup 0) and O(sup 0) responsible for shorter wavelength lines. We speculate that FeS may be an important constituent of the dust. A comparison of our line profiles with radiative transfer models shows that while power law and exponential density distributions yield reasonable fits to the data, polytrope distributions provided significantly worse agreement. The best fits require a substantial fraction of the iron to be undetectable, and are consistent with maximum expansion velocities of v(sub max) approximately 3000 km/sec.

Colgan, Sean W. J.↗

Dynamical Signatures of Thermotoga maritima Maltose-Binding Proteins Affected by Ligand Binding

Functional segregation among protein isoforms depends on the interplay of their overall structures and the molecular dynamics of these structures. Thermotoga maritima maltose-binding protein (tmMBP) isoforms show size-dependent differential binding of maltose and malto-oligomers while maintaining remarkable fold conservation. This differential behavior needs detailed characterization in native-like aqueous conditions to understand the effects of protein dynamics on ligand binding and recognition. Small-angle neutron scattering (SANS), neutron spin echo (NSE) spectroscopy, and dynamic light scattering (DLS) were used in conjunction with previously published computational molecular dynamics (MD) simulations to understand the dynamic behavior of tmMBPs experimentally. SANS provided information on the overall structure of the molecules, while NSE was used to determine the dynamics in the nanosecond time scale. Both tmMBP2 and tmMBP3 have a bidomain architecture linked with a flexible hinge, with the binding pocket sitting in the cleft between the two domains. tmMBP2 and tmMBP3 showed different solution dynamics, with the translational and rotational components dominating the dynamics of both systems, resulting in a clear differentiation of their diffusion pattern. A faster dynamics component was also observed and was attributed to segmental dynamics. Differences observed between the ligand-free (apo) and ligand-bound (holo) states of the two proteins are attributed to conformational entropy. Our results highlight the intricacies of how structure and dynamics can together shape binding to a repertoire of substrates in structurally similar proteins.

Diffusion↗