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At least 127 records · Page 7
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NASA NTRS1981

Diffusion tube

The diffusion tube was designed to operate below about 0.25 percent of water supersaturation. It is simply a long tube lined on the inside with a damp chamois cloth, and heated isothermally to a few degrees centigrade above the incoming air. The diffusion coefficient for water vapor is slightly larger than that for heat, making it possible to supersaturate the airflow. This is the same principle by which transient supersaturations may occur in parallel plate cloud chambers. Only the diffusion of vapor and heat from the walls into the moving air are considered.

Leaitch, R.↗
NASA NTRS1981

Review of isothermal haze chamber performance

The theory of this method of characterizing cloud condensation nuclei (CCN) over the critical supersaturation range of about 0.01% to 0.2% was reviewed, and guidelines for the design and operation of IHC's are given. IHC data are presented and critically analyzed. Two of the four IHC's agree to about 40% over the entire range of critical. a third chamber shows similar agreement with the first two over the lower part of the critical supersaturation range but only a factor of two agreement at higher supersaturation. Some reasons for the discrepancies are given.

Fitzgerald, J. W.↗
NASA NTRS1982

An experimental study of the ice column habit transitions

The influence of supersaturation on column growth of ice crystals forming from atmospheric water vapor was investigated. A high density of crystals was generated on a glass fiber cooled by liquid N2 in a thermal diffusion chamber. Attention was focused on a neighbor-free hollow prism during a stepwise decrease in supersaturation while the crystal temperature was maintained constant. Another experiment involved epitaxial growth of ice crystals on CuS, where nonthickening crystals could only be grown below -7 C. A critical supersaturation was found to be necessary for growth of the basal plane. Beyound the critical value, surface kinetics do not control the growth rate, which is then dominated by the penetration of water molecules through the diffusion field surrounding the crystal.

Cho, N.↗
NASA NTRS1986

Theory of Ostwald ripening in a two-component system

When a two-component system is cooled below the minimum temperature for its stability, it separates into two or more immiscible phases. The initial nucleation produces grains (if solid) or droplets (if liquid) of one of the phases dispersed in the other. The dynamics by which these nuclei proceed toward equilibrium is called Ostwald ripening. The dynamics of growth of the droplets depends upon the following factors: (1) The solubility of the droplet depends upon its radius and the interfacial energy between it and the surrounding (continuous) phase. There is a critical radius determined by the supersaturation in the continuous phase. Droplets with radii smaller than critical dissolve, while droplets with radii larger grow. (2) The droplets concentrate one component and reject the other. The rate at which this occurs is assumed to be determined by the interdiffusion of the two components in the continuous phase. (3) The Ostwald ripening is constrained by conservation of mass; e.g., the amount of materials in the droplet phase plus the remaining supersaturation in the continuous phase must equal the supersaturation available at the start. (4) There is a distribution of droplet sizes associated with a mean droplet radius, which grows continuously with time. This distribution function satisfies a continuity equation, which is solved asymptotically by a similarity transformation method.

Baird, J. K.↗
NASA NTRS1987

Microgravity nucleation and particle coagulation experiments support

A hollow sphere model is developed to predict the range of supersaturation ratio values for refractory metal vapors in a proposed experimental nucleation apparatus. Since the experiments are to be carried out in a microgravity environment, the model neglects the effects of convection and assumes that the only transfer of vapors through an inert gas atmosphere is by conduction and molecular diffusion. A consistent set of physical properties data is assembled for the various candidate metals and inert ambient gases expected to be used in the nucleation experiments. Transient partial pressure profiles are computed for the diffusing refractory species for two possible temperature distributions. The supersaturation ratio values from both candidate temperature profiles are compared with previously obtained experimetnal data on a silver-hydrogen system. The model is used to simulate the diffusion of magnesium vapor through argon and other inert gas atmospheres over ranges of initial and boundary conditions. These results identify different combinations of design and operating parameters which are liekly to produce supersaturation ratio values high enough to induce homogeneous nucleation in the apparatus being designed for the microgravity nucleation experiments.

Lilleleht, L. U.↗
NASA NTRS1989

Growth rate study of canavalin single crystals

The dependence on supersaturation of the growth rate of single crystals of the protein canavalin is studied. In the supersaturation ranges studied, the rate-limiting step for growth is best described by a screw dislocation mechanism associated with interface attachment kinetics. Using a ln-ln plot, the growth-rate data is found to fit a predictive relationship of the form G = 0.012 x the supersaturation to the 6.66, which, together with the solubility curves, allows the growth rate to be estimated under a variety of conditions.

Demattei, R. C.↗
NASA NTRS1993

Mesoscale simulations of the November 25-26 and December 5-6 cirrus cases using the RAMS model

The Regional Atmospheric Modeling System (RAMS), developed at Colorado State University, was used during the First ISCCP (International Satellite Cloud Climatology Project) Regional Experiment (FIRE) 2 (13 Nov. through 6 Dec. 1991) to provide real time forecasts of cirrus clouds. Forecasts were run once a day, initializing with the 0000 UTC dataset provided by NOAA (Forecast Systems Laboratory (FSL) Mesoscale Analysis and Prediction System (MAPS)). In order to obtain better agreement with observations, a second set of simulations were done for the FIRE 2 cases that occurred on 25-26 Nov. and 5-6 Dec. In this set of simulations, a more complex radiation scheme was used, the Chen/Cotton radiation scheme, along with the nucleation of ice occurring at ice supersaturations as opposed to nucleation occurring at water supersaturations that was done in the actual forecast version. The runs using these more complex schemes took longer wall clock time (7-9 hours for the actual forecasts as compared to 12-14 hrs for the runs using the more complex schemes) however, the final results of the simulations were definitely improved upon. Comparisons between these two sets of simulations are given. Now underway are simulations of these cases using a closed analytical solution for the auto-conversion of ice from a pristine ice class (sizes less than about 50 microns in effective diameter) to a snow class (effective diameters on the order of several hundred microns). This solution is employed along with a new scheme for the nucleation of ice crystals due to Meyers et al and Demott et al. The scheme is derived assuming complete gamma distributions for both the pristine and snow classes. The time rate of change of the number concentration and mass mixing-ratio of each distribution is found by calculating either the flux of crystals that grow beyond a certain critical diameter by vapor deposition in an ice supersaturated regime or by calculating the flux of crystals that evaporate to sizes below that same critical effective diameter.

Harrington, J. L.↗
NASA NTRS1995

Nucleation and growth of crystals under cirrus and polar stratospheric cloud conditions

Laboratory studies examine phase changes of hygroscopic substances which occur as aerosol in stratosphere and troposphere (sodium chloride, ammonium sulfate, ammonium bisulfate, nitric acid, sulfuric acid), under controlled conditions, in samples volume 1 to 10(exp -4) ml. Crystallization of salts from supersaturated solutions is examined by slowly evaporating a solution drop on a substrate, under controlled relative humidity, until self nucleation occurs; controlled nucleation of ice in a mm capillary U-tube gives a measured ice crystallization velocity at known supercooling. Two states of crystallization occur for regions where hydrates exist. It is inferred that all of the materials readily exist as supersaturated/supercooled solutions; the degree of metastability appears to be slightly enhanced by inclusion of aircraft produced soot. The crystallization velocity is taken as a measure of viscosity. Results suggest an approach to a glass transition at high molality, supersaturation and/or supercooling within the range of atmospheric interest. It is hypothesized that surface reactions occur more readily on solidified particles - either crystalline or glass, whereas volume reactions are more important on droplets with sufficiently low viscosity and volume diffusivity. Implications are examined for optical properties of such particles in the atmosphere. In a separate experiment, crystal growth was examined in a modified thermal vapor diffusion chamber over the range of cirrus temperature (-30 to -70 C) and under controlled supersaturation and air pressure. The crystals grew at a velocity of 1-2 microns/s, thickness 60-70 micron, in the form of thin column crystals. Design criteria are given for a system to investigate particle growth down to -100 C, (PSC temperatures) where nitric acid particles can be grown under similar control and in the form of hydrate crystals.

Hallett, John↗
NASA NTRS1995

Grain formation around carbon stars. 1: Stationary outflow models

Asymptotic giant branch (AGB) stars are known to be sites of dust formation and undergo significant mass loss. The outflow is believed to be driven by radiation pressure on grains and momentum coupling between the grains and gas. While the physics of shell dynamics and grain formation are closely coupled, most previous models of circumstellar shells have treated the problem separately. Studies of shell dynamics typically assume the existence of grains needed to drive the outflow, while most grain formation models assume a constant veolcity wind in which grains form. Furthermore, models of grain formation have relied primarily on classical nucleation theory instead of using a more realistic approach based on chemical kinetics. To model grain formation in carbon-rich AGB stars, we have coupled the kinetic equations governing small cluster growth to moment equations which determine the growth of large particles. Phenomenological models assuming stationary outflow are presented to demonstrate the differences between the classical nucleation approach and the kinetic equation method. It is found that classical nucleation theory predicts nucleation at a lower supersaturation ratio than is predicted by the kinetic equations, resulting in significant differences in grain properties. Coagulation of clusters larger than monomers is unimportant for grain formation in high mass-loss models but becomes more important to grain growth in low mass-loss situations. The properties of the dust grains are altered considerably if differential drift velocities are ignored in modeling grain formation. The effect of stellar temperature, stellar luminosity, and different outflow velocities are investigated. The models indicate that changing the stellar temperature while keeping the stellar luminosity constant has little effect on the physical parameters of the dust shell formed. Increasing the stellar luminosity while keeping the stellar temperature constant results in large differences in grain properties. For small outflow velocities, grains form at lower supersaturation ratios and close to the stellar photosphere, resulting in larger but fewer grains. The reverse is true when grains form under high outflow velocities, i.e., they form at higher supersaturation ratios, farther from the star, and are much smaller but at larger quantities.

Egan, Michael P.↗
NASA NTRS1996

Solute Nucleation and Growth in Supercritical Fluid Mixtures

This research effort is directed toward two primary scientific objectives: (1) to determine the gravitational effect on the measurement of nucleation and growth rates near a critical point and (2) to investigate the nucleation process in supercritical fluids to aid in the evaluation and development of existing theoretical models and practical applications. A nucleation pulse method will be employed for this investigation using a rapid expansion to a supersaturated state that is maintained for approximately 1 ms followed by a rapid recompression to a less supersaturated state that effectively terminates nucleation while permitting growth to continue. Nucleation, which occurs during the initial supersaturated state, is decoupled from growth by producing rapid pressure changes. Thermodynamic analysis, condensation modeling, apparatus design, and optical diagnostic design necessary for the initiation of a theoretical and experimental investigation of naphthalene nucleation from supercritical CO2 have been completed.

Smedley, Gregory T.↗
NASA NTRS1998

Analysis of Ice Nucleating Aerosol Measurements during SUCCESS: April, May 1996

This section describes our research activities during year three of this effort. In the second year, preliminary archive data sets were submitted to the SUCCESS archive. After additional analyses, final versions were prepared and submitted. These are included on the SUCCESS CD-ROM data editions that were recently released by NASA Ames. Over the range of temperature and supersaturation conditions of our measurements (15 to -40 C, and from ice saturation to approximately 15% water supersaturation), IN concentrations ranged from less than 0.1 to approximately 500 per liter, being generally greater at colder temperatures and higher supersaturations. To estimate the potential of aircraft exhaust as a source of IN, we examined data from six days of the field project when the DC-8 was following closely behind other humidity conditions of our measurements. In April 1997, a microphysical workshop was convened at NCAR to select cases for in depth analyses and to address questions about the consistency of cloud ice crystal measurements (size distributions and mass concentrations) and aerosol size distributions. We attended this meeting and contributed to the discussions. A particular concern was identified in the CN measurements. On the DC-8, CN measurements were obtained by four different investigator groups, using commercially available instrumentation. The DC-8 SUCCESS CN data showed long periods where the measurements were in substantial agreement, but there were also periods with large discrepancies. Several possible factors were identified that could help explain these discrepancies, including minimum detectable particle size, response at reduced pressures, and location of sample inlet on the aircraft.

Rogers, D. C.↗
NASA NTRS1997

Characterization of Aircraft Produced Soot and Contrails Near the Tropopause

Participation in the SUCCESS project primarily involved development and deployment of specific instruments for characterizing jet aircraft exhaust emissions as particulates and their subsequent evolution as contrail particles, either liquid or solid, as cirrus. Observations can be conveniently considered in two categories - close or distant from the aircraft. Thus close to the aircraft the exhaust is mixing through the engine turbulence with a much drier and colder environment and developing water/ ice supersaturation along the trail depending on circumstances (near field), whereas distant from the aircraft (far field) the exhaust has cooled essentially to ambient temperature, the turbulence has decayed and any particle growth or evaporation is controlled by the prevailing ambient conditions. Intermediate between these two regions the main aircraft vortices form (one on each side of the aircraft) which tend to inhibit mixing under some conditions, a region extending from a few aircraft lengths to sometimes a hundred times this distance. Our approach to the problem lay in experience gained in characterizing the smoke from hydrocarbon combustion in terms of its cloud forming properties and its potential influence on the radiation properties of the smoke and subsequent cloud from the viewpoint of reduction (absorbtion and scattering ) of solar radiation flux leading to significant global cooling (Hudson et al 1991; Hallett and Hudson 1991). Engine exhaust contains a much smaller proportion of the fuel carbon than is sometimes present in ordinary combustion (less than 0.01% compared with 10%) and influences condensation in quite different ways, to be characterized by the Cloud Condensation Nucleus, CCN - supersaturation spectrum. The transition to ice is to be related to the dilution of solution droplets to freeze by homogeneous nucleation at temperatures somewhat below -40C (Pueschel et al 1998). The subsequent growth of ice particles depends critically on temperature, supersaturation and to some extent pressure, as is demonstrated in an NSF funded project being carried out in parallel with the work reported here. As will be discussed below, nucleation processes themselves and also exhaust impurities also influence the growth of ice particles and may control some aspects of growth of ice in contrails. Instrumentation was designed to give insight into these questions and to be flown on the NASA DC- 8 as a platform. In addition a modest program was undertaken to investigate the properties of laboratory produced smoke produced under controlled conditions from the viewpoint of forming both CCN and CN. The composition of the smoke could inferred from a thermal characterization technique; larger particles were captured by formvar replicator for detailed analysis; ice particles were captured and evaporated in flight on a new instrument, the cloudscope, to give their mass, density and impurity content.

Hallett, John↗
NASA NTRS1999

Step Bunching: Influence of Impurities and Solution Flow

Step bunching results in striations even at relatively early stages of its development and in inclusions of mother liquor at the later stages. Therefore, eliminating step bunching is crucial for high crystal perfection. At least 5 major effects causing and influencing step bunching are known: (1) Basic morphological instability of stepped interfaces. It is caused by concentration gradient in the solution normal to the face and by the redistribution of solute tangentially to the interface which redistribution enhances occasional perturbations in step density due to various types of noise; (2) Aggravation of the above basic instability by solution flowing tangentially to the face in the same directions as the steps or stabilization of equidistant step train if these flows are antiparallel; (3) Enhanced bunching at supersaturation where step velocity v increases with relative supersaturation s much faster than linear. This v(s) dependence is believed to be associated with impurities. The impurities of which adsorption time is comparable with the time needed to deposit one lattice layer may also be responsible for bunching; (4) Very intensive solution flow stabilizes growing interface even at parallel solution and step flows; (5) Macrosteps were observed to nucleate at crystal corners and edges. Numerical simulation, assuming step-step interactions via surface diffusion also show that step bunching may be induced by random step nucleation at the facet edge and by discontinuity in the step density (a ridge) somewhere in the middle of a face. The corresponding bunching patterns produce the ones observed in experiment. The nature of step bunching generated at the corners and edges and by dislocation step sources, as well as the also relative importance and interrelations between mechanisms 1-5 is not clear, both from experimental and theoretical standpoints. Furthermore, several laws controlling the evolution of existing step bunches have been suggested, though unambiguous conclusions are still missing. Addressing these issues is the major goal of the present project. The theory addressing the above problem, experimental methods, several figures which include: (1) the spatial wave numbers at which the system is neutrally stable as a function of growth velocity for linear kinetics and supersaturation for nonlinear kinetics; (2) a schematic of the experiment of lysozyme crystal growing under conditions of natural convection; (3) fluctuations in time, t, of the normal growth rate, R(t), vicinal slope, p(t) and Fourier Spectra of R(t), discussions and conclusions are presented.

Chernov, A. A.↗
NASA NTRS2000

Is it Possible to have the Similar Unit Cell in Crystals of Different form from the same Macromolecule? (A Case Study of Ribosome Crystals)

Three different types of ribosome crystals were grown by the vapor diffusion technique in hanging drops as described in (1,2). The ribosome is a large asymmetric RNA-protein complex (2.3 million Da), which is protein syntheses machinery of the cell. In this poster we would like to discuss the features of ribosome crystallization. Ribosomes were purified from the thermophilic bacteria Thermus thermophilus by centrifugation (3). Three types of crystals (needle, flat tetragonal and tetragonal-like pyramid) can be grown from the same solution; furthermore, in the same drop using 10-15% 2-methyl-2,4- pentanediol as a precipitant. The crystals appeared in 5-48 hours. The crystals were stable and can co-exist in solution over long period of time. The kinetics of appearance of different crystal forms was different: first the needle crystals were grown, then the tetragonal, and finally the tetragonal pyramids. Later studies of the process of ribosome crystal growth depending on supersaturation showed that low supersaturation results in the appearance of tetragonal plates or tetragonal-like pyramids. An electron microscopy study, together with computer modeling, has shown that crystals of different forms have a high probability of having the same unit cell parameters. According to these experiments the following conclusion can be dranvn: the level of supersaturation of the macromolecule in a crystallizing solution is one of the major factors for forming three-dimensional crystals convenient for X-rays diffraction analysis. From the same macromolecule solution, crystals of different forms can be grown at approximately the same conditions by varying the concentration of macromolecule in the solution. Ion-macromolecule and water-macromolecule interactions, apparently, play the main role in the formation of the unit cell of the crystals.

Karpova, E. A.↗
NASA NTRS2001

Cloud Microphysics Budget in the Tropical Deep Convective Regime

Cloud microphysics budgets in the tropical deep convective regime are analyzed based on a 2-D cloud resolving simulation. The model is forced by the large-scale vertical velocity and zonal wind and large-scale horizontal advections derived from TOGA COARE for a 20-day period. The role of cloud microphysics is first examined by analyzing mass-weighted mean heat budget and column-integrated moisture budget. Hourly budgets show that local changes of mass-weighted mean temperature and column-integrated moisture are mainly determined by the residuals between vertical thermal advection and latent heat of condensation and between vertical moisture advection and condensation respectively. Thus, atmospheric thermodynamics depends on how cloud microphysical processes are parameterized. Cloud microphysics budgets are then analyzed for raining conditions. For cloud-vapor exchange between cloud system and its embedded environment, rainfall and evaporation of raindrop are compensated by the condensation and deposition of supersaturated vapor. Inside the cloud system, the condensation of supersaturated vapor balances conversion from cloud water to raindrop, snow, and graupel through collection and accretion processes. The deposition of supersaturated vapor balances conversion from cloud ice to snow through conversion and riming processes. The conversion and riming of cloud ice and the accretion of cloud water balance conversion from snow to graupel through accretion process. Finally, the collection of cloud water and the melting of graupel increase raindrop to compensate the loss of raindrop due to rainfall and the evaporation of raindrop.

Li, Xiao-Fan↗
NASA NTRS2002

Surface Processes of Faceted Growth

Atomic force microscopy and high precision optical interferometry allow to analyze the processes that are in the core of our present understanding of faceted crystal growth. Some of these processes will be reviewed. Recent experiments suggest that the Gibbs-Thomson Law (GTL) may not be applicable to the weakly fluctuating strongly polygonized steps, with low kink density. Propagation rate of a straight short step segment changes with the segment length much steeper than predicted by GTL. If the step fluctuations are still well developed, the typical transition length may be determined just by the radius of rounded comers of the polygonized step. If fluctuations do not have enough time to develop, the kinetic effects may be essential. Indeed, 'communications' between comers of a short straight step segment may occur and, thus, the GTL may be implemented only via kink exchange. E.g., dissolutions of this short segment at macroscopic equilibrium occurs as follows: The kinks are split from one comer as a result of fluctuations, and annihilate with kinks of the opposite sign generated by another comer. Similarly, an exchange via chain of kinks on a rough step is the mechanism to implement the GT Law. If there is a supersaturation with respect to a large crystal, the kinks not only diffuse along the step, but move back the generating comers. This 'wind' prevents communication between the comers and places upper limit supersaturation only below which GTL is applicable. Steps replace kinks in the 3D case, though, of course, another dimensionality brings about another physics. Another specific problem to think about is if fluctuations are always fast enough to provide enough kinks for linear dependence of step rate on supersaturation. Increasing azimuthal polygonization of growth hillocks is a sign of insufficient fluctuation rate. Morphological stability of vicinal faces is usually considered on the basis of mutually parallel steps. Azimuthal anisotropy and interlacing of step bunches inducing the well known bunch splitting is another challenge. Among other challenging problems are: existence of surface diffusion on the crystal/so1ution interface, step interaction in solutions, achievement of step flow modes from liquids, impurity effects. New phenomena essential in biomacromolecular crystallization is another interesting area.

Chernov, A.↗
NASA NTRS2003

Step Bunch Evolution on Vicinal Faces of KDP

For in-situ studies of the formation and evolution of step patterns in solution growth, we have assembled an experimental setup based on Michelson interferometry with the growing crystal surface as one of the reflective surfaces. The device allows data collection over a relatively large area (approximately 4 sq. mm) in situ and in real time during growth. The depth resolution is improved over traditional interferometry using phase-shifted images combining by a suitable algorithm. We achieve a depth resolution of approximately 50 Angstroms. Lateral resolution, dependent on the degree of magnification, is around 0.3 to 5 microns. The crystal chosen as a model in this work is potassium dihydrogen phosphate (KDP), the optically non-linear material widely used in frequency doubling applications. Kinetics of KDP crystallization is well studied so that KDP can serve as a benchmark for our investigations. We present quantitative results on the onset, initial stages and development of instabilities in moving step trains on vicinal crystal surfaces at varying supersaturation, flow rate, and flow direction. The kinetics data suggest that at low supersaturations, step bunching is caused by impurity retardation of the steps, while at higher supersaturations, we link the non-linearity during growth to interdependence of the velocity and density of the steps evidenced in independent experiments. The behavior on the surface is very dynamic, small bunches both merge and split from larger bunches as they travel across the facet. We present evidence that despite these dynamics, under steady conditions there exists a limiting value to step bunch height. This height is reached at distances between 600 and 1000 microns from the step source. In our experiments, we observed the retention of this step bunch height limit up to the path of 1500 microns.

Booth, N. A.↗
NASA NTRS2003

Crystallization Physics in Biomacromolecular Systems

The crystals are built of molecules of protein, nucleic acid and their complexes, like viruses, approx. 5x10(exp 3)+ 3x10(exp 6) Da in weight and 2 + 20 nm in effective diameter. This size strongly exceeds action range of molecular forces and makes a big difference with inorganic crystals. Intermolecular contacts form patches on the biomacromolecular surface. Each patch may occupy only a small percent of the whole surface and vary from polymorph to polymorph of the same protein. Thus, under different conditions (pH, solution chemistry, temperature, any area on the macromolecular surface may form a contact. The crystal Young moduli, E approx. equals 0.1 + 0.5 GPa are more than 10 times lower than that of inorganics and the biomolecules themselves. Water within biocrystals (30-70%) is unable to flow unless typical deformation time is longer than approx. 10(exp -5)s. This explains the discrepancy between light scattering and static measurements of E. Nucleation and Growth requires typically concentrations exceeding the equilibrium ones up to 100 times - because of the new size scale results in 10 - 10(exp 3) times lower kinetic coefficients than that needed for inorganic solution growth. All phenomena observed in the latter occur with protein crystallization and are even better studied by AFM. Crystals are typically facetted. Among unexpected findings of general significance are - net molecular exchange flux at kinks is much lower than that expected from supersaturation, steps with low (< approx. 10(exp -2)) kink density at steps follow Gibbs-Thomson law only at very low supersaturations, step segment growth rate may be independent of step energy. Crystal perfection is a must of biocrystallization to achieve the major goal to find 3-D atomic structure of biomacromolecules by x-ray diffraction. Poor diffraction resolution (> 3Angstrom) makes crystallization a bottleneck for structural biology. All defects typical of small molecule crystals are found in biocrystals, but the defects responsible for poor resolution are not identified. Conformational changes are one of them. Biocrystallization in microgravity reportedly results in 20% cases of better crystals. The mechanism of how lack of convection can do this is still not clear. Lower supersaturation, self-purification &om preferentially trapped homologous impurities and step bunching are viable hypotheses.

Chernov, A. A.↗