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All sourcesNASA NTRSDOE OSTI
NASA NTRS1987

Large charged drop levitation against gravity

A hybrid electrostatic-acoustic levitator that can levitate and manipulate a large liquid drop in one gravity is presented. To the authors' knowledge, this is the first time such large drops (up to 4 mm in diameter in the case of water) have been levitated against 1-gravity. This makes possible, for the first time, many new experiments both in space and in ground-based laboratories, such as 1)supercooling and superheating, 2) containerless crystal growth from various salt solutions or melts, 3) drop dynamics of oscillating or rotating liquid drops, 4) drop evaporation and Rayleigh bursting, and 5) containerless material processing in space. The digital control system, liquid drop launch process, principles of electrode design, and design of a multipurpose room temperature levitation chamber are described. Preliminary results that demonstrate drop oscillation and rotation, and crystal growth from supersaturated salt solutions are presented.

Rhim, Won-Kyu↗
NASA NTRS2007

Metabolic Heat Regenerated Temperature Swing Adsorption for CO(sub 2) and Heat Removal/Rejection in a Martian PLSS

Two of the fundamental problems facing the development of a Portable Life Support System (PLSS) for use on Mars, are (i) heat rejection (because traditional technologies use sublimation of water, which wastes a scarce resource and contaminates the premises), and (ii) rejection of CO2 in an environment with a ppCO2 of 0.4-0.9 kPa. Patent-pending Metabolic heat regenerated Temperature Swing Adsorption (MTSA) technology is being developed to address both these challenges. The technology utilizes an adsorbent that when cooled with liquid CO2 to near sublimation temperatures (~195K) removes metabolically-produced CO2 in the vent loop. Once fully loaded, the adsorbent is then warmed externally by the vent loop (approx. 300K), rejecting the captured CO2 to Mars ambient. Two beds are used to effect a continuous cycle of CO2 removal/rejection as well as facilitate heat exchange out of the vent loop. Any cryogenic fluid can be used in the application; however, since CO2 is readily available at Mars and can be easily produced and stored on the Martian surface, the solution is rather elegant and less complicated when employing liquid CO2. As some metabolic heat will need to be rejected anyway, finding a practical use for metabolic heat is also an overall benefit to the PLSS. To investigate the feasibility of the technology, a series of experiments was conducted which lead to the selection and partial characterization of an appropriate adsorbent. The adsorbent NaX successfully removed CO2 from a simulated vent loop at the prescribed temperature swing anticipated during PLSS operating conditions on Mars using a cryogenic fluid. Thermal conductivity of the adsorbent was also measured to eventually aid in a demonstrator design of the technology. These results provide no show stoppers to the development of MTSA technology and allow its development to focus on other design challenges as listed in the conclusions.

Iacomini, Christine↗
DOE OSTI2013

Overview of reductants utilized in nuclear fuel reprocessing/recycling

Most of the aqueous processes developed, or under consideration worldwide for the recycling of used nuclear fuel (UNF) utilize the oxido-reduction properties of actinides to separate them from other radionuclides. Generally, after acid dissolution of the UNF, (essentially in nitric acid solution), actinides are separated from the raffinate by liquid-liquid extraction using specific solvents, associated along the process, with a particular reductant that will allow the separation to occur. For example, the industrial PUREX process utilizes hydroxylamine as a plutonium reductant. Hydroxylamine has numerous advantages: not only does it have the proper attributes to reduce Pu(IV) to Pu(III), but it is also a non-metallic chemical that is readily decomposed to innocuous products by heating. However, it has been observed that the presence of high nitric acid concentrations or impurities (such as metal ions) in hydroxylamine solutions increase the likelihood of the initiation of an autocatalytic reaction. Recently there has been some interest in the application of simple hydrophilic hydroxamic ligands such as acetohydroxamic acid (AHA) for the stripping of tetravalent actinides in the UREX process flowsheet. This approach is based on the high coordinating ability of hydroxamic acids with tetravalent actinides (Np and Pu) compared with hexavalent uranium. Thus, the use of AHA offers a route for controlling neptunium and plutonium in the UREX process by complexant based stripping of Np(IV) and Pu(IV) from the TBP solvent phase, while U(VI) ions are not affected by AHA and remain solvated in the TBP phase. In the European GANEX process, AHA is also used to form hydrophilic complexes with actinides and strip them from the organic phase into nitric acid. However, AHA does not decompose completely when treated with nitric acid and hampers nitric acid recycling. In lieu of using AHA in the UREX + process, formohydroxamic acid (FHA), although not commercially available, hold promises as a replacement for AHA. FHA undergoes hydrolysis to formic acid which is volatile, thus allowing the recycling of nitric acid. Unfortunately, FHA powder was not stable in the experiments we ran in our laboratory. In addition, AHA and FHA also decompose to hydroxylamine which may undergo an autocatalytic reaction. Other reductants are available and could be extremely useful for actinides separation. The review presents the current plutonium reductants used in used nuclear fuel reprocessing and will introduce innovative and novel reductants that could become reducers for future research on UNF separation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
NASA NTRS1991

Cell separations and the demixing of aqueous two phase polymer solutions in microgravity

Partition in phase separated aqueous polymer solutions is a cell separation procedure thought to be adversely influenced by gravity. In preparation for performing cell partitioning experiments in space, and to provide general information concerning the demixing of immiscible liquids in low gravity, a series of phase separated aqueous polymer solutions have been flown on two shuttle flights. Fluorocarbon oil and water emulsions were also flown on the second flight. The aqueous polymer emulsions, which in one g demix largely by sedimentation and convection due to the density differences between the phases, demixed more slowly than on the ground and the final disposition of the phases was determined by the wetting of the container wall by the phases. The demixing behavior and kinetics were influenced by the phase volume ratio, physical properties of the systems and chamber wall interaction. The average domain size increased linearly with time as the systems demixed.

Brooks, Donald E.↗
DOE OSTI2019

Self–Sorting of 10–µm–Long Single–Walled Carbon Nanotubes in Aqueous Solution

Single-walled carbon nanotubes (SWCNTs) are a class of 1D nanomaterials that exhibit extraordinary electrical and optical properties. However, many of the fundamental studies and practical applications are stymied by sample polydispersity. SWCNTs are synthesized in bulk with broad structural (chirality) and geometrical (length and diameter) distributions; problematically, all known post-synthetic sorting methods rely on ultrasonication, which cuts SWCNTs into short segments (typically <1 μm). Here it is demonstrated that ultralong (>10 μm) SWCNTs can be efficiently separated from the shorter ones through a solution-phase “self-sorting.” It is shown that thin film transistors fabricated from long semiconducting SWCNTs exhibit a carrier mobility as high as ≈90 cm 2 V –1 s –1 , which is ≈10 times higher than the shorter counterparts and well exceeding other known materials such as organic semiconducting polymers (<1 cm 2 V –1 s –1 ), amorphous silicon (≈1 cm 2 V –1 s –1 ), and nanocrystalline silicon (≈50 cm 2 V –1 s –1 ). Mechanistic studies suggest that this self-sorting relies on the equilibrium between isotropic and liquid crystalline SWCNT phases, which is driven by the solution phase behavior above the cloud point of the isotropic phase, and inversely scales with the SWCNT length. Furthermore, this length-dependent self-sorting technique opens a path to attain the long- sought ultralong, electronically pure carbon nanotube materials through scalable solution processing.

36 MATERIALS SCIENCE↗
DOE OSTI2013

Continuous Microreactor-Assisted Solution Deposition for Scalable Production of CdS Films

Solution deposition offers an attractive, low temperature option in the cost effective production of thin film solar cells. Continuous microreactor-assisted solution deposition (MASD) was used to produce nanocrystalline cadmium sulfide (CdS) films on fluorine doped tin oxide (FTO) coated glass substrates with excellent uniformity. We report a novel liquid coating technique using a ceramic rod to efficiently and uniformly apply reactive solution to large substrates (152 mm × 152 mm). This technique represents an inexpensive approach to utilize the MASD on the substrate for uniform growth of CdS films. Nano-crystalline CdS films have been produced from liquid phase at ~90°C, with average thicknesses of 70 nm to 230 nm and with a 5 to 12% thickness variation. The CdS films produced were characterized by UV-Vis spectroscopy, transmission electron microscopy, and X-Ray diffraction to demonstrate their suitability to thin-film solar technology.

scalable process↗
DOE OSTI2012

Phase behavior of DODAB aqueous solution

Phase behavior of DODAB aqueous solution, prepared without sonication, was studied by adiabatic scanning calorimetry. Measurements revealed four phase transitions with the temperatures 35.2, 39.6, 44.6, and 52.4 Degree-Sign C at heating and one transition at the temperature 40.4 Degree-Sign C at cooling. The first three transitions at heating occur in unilamellar vesicles. The first and third transitions correspond to the subgel-gel and gelliquid phase transitions, corresponding enthalpy jumps are equal to 33 and 49 kJ/mol. The second transition appears after some aging and is similar to gel-ripple phase transition in a DPPC solution, with the enthalpy jump under the transition exceeding 7.4 kJ/mol. The transition occurs in unilamellar vesicles. The transition at the temperature 52.4 Degree-Sign C occurs in another subsystem of the solution, which we believe to be multilamellar vesicles. The enthalpy jump at this transition is equal to 97 kJ/mol, and data analysis suggests that this is a subgel-liquid transition. The phase transition at cooling is the liquid-gel transition in unilamellar vesicles. During the measurements, a slow evolution of the solution occurs, consisting in a change of concentrations of unilamellar and multilamellar vesicles. This transformation mainly occurs at low temperatures.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

Formation mechanism for the nanoscale amorphous interface in pulse-welded Al/Fe bimetallic systems

Pulse or impact welding traditionally has been referred to as “solid-state” welding. By integrating advanced interface characterizations and diffusion calculations, we report that the nanoscale amorphous interface in the pulse-welded Al/Fe bimetallic system is formed by rapid heating and melting of a thin Al layer at the interface, diffusion of iron atoms in the liquid aluminum, and subsequent rapid quenching with diffused iron atoms in solution. This finding challenges the commonly held belief regarding the solid-state nature of the impact-based welding process for dissimilar metals. Elongated ultra-fine grains with high dislocation density and ultra-fine equiaxed grains also are observed in the weld interface vicinity on the steel and aluminum sides, respectively, which further confirms that melting and the subsequent recrystallization occurred on the aluminum side of the interface.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Rapid charging made practical in graphite-based lithium batteries: surface-acoustic wave turbulent electrolyte mixing to overcome diffusion limited charging rates [Final Report]

One of the key limits in rapidly recharging a lithium-ion battery is the depletion of lithium ions within the electrolyte adjacent the anode during charging and long diffusion time to overcome this depletion. It also causes dendrite formation, inefficient use of the lithium, and battery degradation over many charge-discharge cycles. Because the liquid electrolyte remains quiescent and unmixed, this depletion layer’s depth rapidly grows to match the anode-cathode separation distance at even modest charge rates. The solution proposed by PI Prof. James Friend and Co-PI Prof. Ping Liu, both from the University of California, San Diego, is to mix the electrolyte and minimize the Li+ ion concentration gradient during charging. Even in the presence of the separator, the charging rate could then be significantly increased. They propose to accomplish this using surface acoustic wave (SAW)-driven acoustic streaming, a technique employing 10-mW fingernail-sized solid-state devices from the telecommunications industry to drive turbulent mixing to submicron length scales in a manner completely compatible with the typical 20700 and 18650 cells used in electric vehicles. 0.1. Turbulent acoustic streaming mixes the electrolyte during charging—even with separator Our proposed 100-MHz SAW device used to recirculate the electrolyte is compatible with lithium- ion battery electrochemistry, as it is made in our lab of single-crystal lithium niobate. Their solution is straightforward to drive from a DC power source alongside the signal provided during battery charging. The device is only needed during charging and does not consume power dur- ing battery discharge. Uniquely, SAW generates extreme accelerations of over 1 billion meters per second squared in the fluid, driving turbulent mixing from centimeter to submicron length scales, even through the porous separator materials that tend to be used in batteries, all while avoiding interfering with the anode’s solid electrolyte interphase layer that forms during use. By employing novel fluid mechanics, the investigators are proposing a new direction for battery research away from direct use of materials science and electrochemistry. The chemistry agnostic solution may be employed in any battery chemistry that makes use of liquid electrolytes, providing a broader transformative benefit to the battery research community. They are to produce a series of prismatic and 20700-cell sized 2 Ah batteries capable of being charged and discharged at least 500 times without more than 20% loss in battery capacity, and to provide analysis tools useful to the battery research and development community for adopting this approach for other battery chemistries and configurations.

25 ENERGY STORAGE↗
DOE OSTI2014

Composition Driven, Statistical Review of Cast Stone Screening Matrix Results

Recent studies in support of Cast Stone development for the Hanford Site were designed to screen the effects of mix components on properties and performance of the waste form. Dry blend components, including portland cement, blast furnace slag, and Class F fly ash, sourced from both southeastern and northwestern suppliers, were included in the screening matrix. Multiple decontaminated salt solutions (simulated) were combined with the dry blend components at various liquid to solid ratios following a statistically designed matrix of compositions. Properties of the resulting mixes and performance of the cured materials were then measured and related to the dry blend components and salt solutions that were used for each mix. At the conclusion of the screening matrix work, SRNL felt that additional insight into the study might be obtained by relating the properties and performance of the materials to the composition of each Cast Stone mix, as opposed to just the dry blend – salt solution combination. This memorandum provides the results of a statistically driven review of the screening matrix data as a function of the composition of each mix. It is meant to augment the results obtained by reviewing the screening matrix data as a function of the dry blend and salt solution combination.

Edwards, T. B.↗
DOE OSTI2021

Kinetics of solid–liquid interface motion in molecular dynamics and phase-field models: crystallization of chromium and silicon

The results of molecular dynamics (MD) simulations of the crystallization process in one-component materials and solid solution alloys reveal a complex temperature dependence of the velocity of the crystal–liquid interface featuring an increase up to a maximum at 10–30% undercooling below the equilibrium melting temperature followed by a gradual decrease of the velocity at deeper levels of undercooling. At the qualitative level, such non-monotonous behaviour of the crystallization front velocity is consistent with the diffusion-controlled crystallization process described by the Wilson–Frenkel model, where the almost linear increase of the interface velocity in the vicinity of melting temperature is defined by the growth of the thermodynamic driving force for the phase transformation, while the decrease in atomic mobility with further increase of the undercooling drives the velocity through the maximum and into a gradual decrease at lower temperatures. At the quantitative level, however, the diffusional model fails to describe the results of MD simulations in the whole range of temperatures with a single set of parameters for some of the model materials. The limited ability of the existing theoretical models to adequately describe the MD results is illustrated in the present work for two materials, chromium and silicon. It is also demonstrated that the MD results can be well described by the solution following from the hodograph equation, previously found from the kinetic phase-field model (kinetic PFM) in the sharp interface limit. The ability of the hodograph equation to describe the predictions of MD simulation in the whole range of temperatures is related to the introduction of slow (phase field) and fast (gradient flow) variables into the original kinetic PFM from which the hodograph equation is obtained. The slow phase-field variable is responsible for the description of data at small undercoolings and the fast gradient flow variable accounts for local non-equilibrium effects at high undercoolings. The introduction of these two types of variables makes the solution of the hodograph equation sufficiently flexible for a reliable description of all nonlinearities of the kinetic curves predicted in MD simulations of Cr and Si. This article is part of the theme issue ‘Transport phenomena in complex systems (part 1)’.

Science & Technology - Other Topics↗
DOE OSTI2020

Solidification of REDC Organics and Airborne Release Fraction Measurements

The Radiochemical Engineering Development Center (REDC) generates various liquid organic wastes from processing irradiated targets to recover heavy elements. In the past, these organics were discharged to the Oak Ridge National Laboratory (ORNL) liquid low-level waste (LLLW) system, along with the aqueous waste. Because of a reduction in aqueous LLLW from other ORNL generators and an increase in the radionuclide concentration, particularly 238 Pu, in the organic waste stream, the organics can no longer be discharged to the LLLW system. The plan is to solidify the liquid organic waste for disposal as solid debris waste. The documented safety analysis for REDC uses an airborne release fraction of 5 x 10 -4 with a respirable fraction of 0.2 for plutonium and other actinides from packaged solid debris waste during a fire scenario, for an overall airborne release fraction/respirable fraction of 10 -4 . Solidifying the organic liquids, either by using PM-199 Organoclay ® or by grouting, would produce solid waste forms with no free liquid, which should qualify for disposal at the Waste Isolation Pilot Plant. The use of Organoclay would be much simpler to implement inside a hot cell. Granular Organoclay can be added to the organic waste solutions until there is a dry layer on top of the liquid and then allowed to cure for a few hours. Grouting the liquids would require using multiple ingredients and mixing steps. Both methods produced waste forms that trapped cerium, as a surrogate for plutonium, inside the waste, with airborne release fractions during fire scenario tests of well below the 10 -4 limit.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2024

Electrochemical Control for Corrosion in Molten Chlorides During CSP Plant Operation

The Liquid Pathway of the Concentrating Solar Power Generation 3 (CSP Gen3) program proposed low-cost molten chloride salt for energy storage. However, online corrosion control was identified as a remining major risk of the Liquid Pathway approach. This project addressed that risk. Electrochemical solutions for corrosion mitigation during CSP plant operation were investigated and their feasibility and scalability were evaluated. The leading cause of corrosion in molten chloride salt systems was identified as corrosive impurities that form within the salt upon exposure to trace amounts of air and moisture. Leveraging electrochemistry, reduction/oxidation reactions can be employed to remove these corrosive impurities. In Phase 1 of this project, a bench-scale batch electrochemical reactor was designed, fabricated, and used to assess the kinetics and thermodynamics of electrochemical salt purification. In Phase 2, a laboratory-scale flow reactor was designed, fabricated, and used to assess the efficacy of the electrochemical method under flowing conditions. Results show that under proposed operating conditions for the Liquid Pathway Gen3 Pilot Plant, the electrochemical method is significantly more effective at removing impurities than alternative chemical and thermal methods, and that the electrochemical method produces less harmful byproducts. A key advance made in the course of this project was the development of a 2-electrode method for electrochemical purification that is more scalable than previously developed 3 electrode methods. This novel method is based on Magnesium (Mg) electrowinning. A provisional patent based on this invention has been submitted (USPTO Application No. 63/480,355). Additional key advances made during this project include assessment of the effect of dissimilar alloys on corrosion, kinetic and thermodynamic evaluation of thermolysis reactions of impurities within the molten salt, characterization of byproducts of purification reactions, and generation of IP focused on isolating value-added products using molten salt-based electrochemistry that could be deployed to valorize the process (USPTO Application No. 63/478,806). Ultimately, this project represented a step toward feasibility of Liquid Pathway Gen3 CSP. The method developed under this project could significantly reduce capital expenses and operating costs and increase plant profitability by enabling use of less expensive alloys, decreasing maintenance, and increasing plant longevity. Key focus areas for follow-on work have been identified as 1) evaluation of the efficacy of the electrochemical method under turbulent conditions in a larger flow system, such as the FASTR loop, 2) development of methods for removal of purification byproducts, 3) modeling pilot and industrial scale performance of electrochemical salt purification during plant operation and 4) further assessment of the effect of impurities on salt vapor phase.

14 SOLAR ENERGY↗
DOE OSTI2018

Spontaneous Reshaping and Splitting of AgCl Nanocrystals under Electron Beam Illumination

Abstract AgCl is photosensitive and thus often used as micromotors. However, the dynamics of individual AgCl nanoparticle motion in liquids upon illumination remains elusive. Here, using liquid cell transmission electron microscope (TEM), AgCl nanocrystals reshaping and splitting spontaneously in an aqueous solution under electron beam illumination are observed. It is found that the AgCl nanocrystals are negatively charged in the liquid environment, where the charge induces a repulsive Coulomb force that reshapes and stretches those nanocrystals. Upon extensive stretching, the AgCl nanocrystal splits into small nanocrystals and each nanocrystal retracts back into cuboid shapes due to the cohesive surface. This analysis shows that each nanocrystal maintains a single crystal rocksalt structure during splitting. The splitting of AgCl nanocrystals is analogous to the electrified liquid droplets or other reported the Coulomb fission phenomenon, but with distinctive structural properties. Revealing of the dynamic behavior of AgCl nanocrystals opens the opportunity to explore their potential applications as actuators for nanodevices.

Tian, Xuezeng↗
NASA NTRSDate not supplied

Development of thermostable carbonic anhydrases using structure-guided recombination for use in CO2 removal systems on spacecraft

Carbon capture and storage has been a research area of great interest in recent years asa method for mitigation of CO2emissions, due to the effects of climate change. The development of technologies for the efficient capture of CO2are also of great interest for human spaceflight applications. One of the most promising technologies in this area is CO2 scrubbing using liquid amines, unfortunately, liquid amines with low heats of desorption tend to have slow CO2binding kinetics. One potential solution to this problem is to use the enzyme carbonic anhydrase (CA) to enhance the kinetics of CO2binding to liquid amines, allowing the overall process to be more energy efficient. Interest in using carbonic anhydrase as a biocatalyst has led to a number of efforts to improve the thermostability and solvent tolerance of several distinct carbonic anhydrase enzymes. In the work described here, we screened through a diverse set of natural carbonic anhydrases to identify candidates for protein engineering aimed at increased stability and activity in various liquid amines. We then used SCHEMA structure-guided recombination to develop a set of chimeric carbonic anhydrases with high thermostability and activity. These chimeras were used as the starting points for further protein engineering work targeting activity in liquid amine systems. Our ultimate goal is to test the engineered enzymes in a liquid amine system for cabin air revitalization on ISS or other spacecraft.

Life Support↗
DOE OSTI2021

Crowded electrolytes containing redoxmers in different states of charge: Solution structure, properties, and fundamental limits on energy density

Nonaqueous redox flow batteries use liquid electrolytes containing redox-active organic molecules (redoxmers) as their energy storage medium. To maximize energy density, the redoxmer concentration needs to be maximized while maintaining low viscosity and high ionic conductivity. During charge, a redoxmer molecule pairs with an ion in the electrolyte while another ion migrates across the membrane to maintain electric neutrality. In a crowded electrolyte, this reconstitution changes physical and chemical properties of the solution. To explore these behaviors, a phenothiazine redoxmer fully miscible with acetonitrile was used, and electrochemical charge was mimicked by chemical oxidation. The solutions were examined using small-angle X-ray scattering, nuclear magnetic resonance, and conductometry and modeled using classical molecular dynamics. Overall, our study indicates that physical and structural properties of redoxmer solutions in both states of charge make it exceedingly difficult to increase the redoxmer concentrations over 2 M at any temperature without compromising dynamic properties of such solutions. The cause for this limitation is proximity to a gel-like regime in which fluidity, diffusivity, and ionic conductivity exponentially decrease with increasing concentration. This tendency is compounded by non-Arrhenius behavior of the electrolyte: a small increase in the concentration outruns gains in fluidity and conductivity at a higher temperature. Thus the properties of crowded electrolytes generally make it impossible to operate when gel-like behavior sets in. Pushing the redoxmer concentration to 2.5-3 M might be possible for small redoxmer molecules, but it would require the use of ionic liquid electrolytes at 340-360 K. (C) 2021 Elsevier B.V. All rights reserved.

25 ENERGY STORAGE↗
DOE OSTI2015

Do protein crystals nucleate within dense liquid clusters?

The evolution of protein-rich clusters and nucleating crystals were characterized by dynamic light scattering (DLS), confocal depolarized dynamic light scattering (cDDLS) and depolarized oblique illumination dark-field microscopy. Newly nucleated crystals within protein-rich clusters were detected directly. These observations indicate that the protein-rich clusters are locations for crystal nucleation. Protein-dense liquid clusters are regions of high protein concentration that have been observed in solutions of several proteins. The typical cluster size varies from several tens to several hundreds of nanometres and their volume fraction remains below 10{sup −3} of the solution. According to the two-step mechanism of nucleation, the protein-rich clusters serve as locations for and precursors to the nucleation of protein crystals. While the two-step mechanism explained several unusual features of protein crystal nucleation kinetics, a direct observation of its validity for protein crystals has been lacking. Here, two independent observations of crystal nucleation with the proteins lysozyme and glucose isomerase are discussed. Firstly, the evolutions of the protein-rich clusters and nucleating crystals were characterized simultaneously by dynamic light scattering (DLS) and confocal depolarized dynamic light scattering (cDDLS), respectively. It is demonstrated that protein crystals appear following a significant delay after cluster formation. The cDDLS correlation functions follow a Gaussian decay, indicative of nondiffusive motion. A possible explanation is that the crystals are contained inside large clusters and are driven by the elasticity of the cluster surface. Secondly, depolarized oblique illumination dark-field microscopy reveals the evolution from liquid clusters without crystals to newly nucleated crystals contained in the clusters to grown crystals freely diffusing in the solution. Collectively, the observations indicate that the protein-rich clusters in lysozyme and glucose isomerase solutions are locations for crystal nucleation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗