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All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Dimensionless parameters for cloudy Rayleigh-Bénard convection: Supersaturation, Damköhler, and Nusselt numbers

In steady-state Rayleigh-Bénard convection, heat is transported by turbulent thermal convection from the bottom, hot surface to the top, cold surface, leading to a height-independent sensible heat flux. When water vapor is present and cloud formation occurs, there is also an additional latent heat flux. Heat transport in cloudy Rayleigh-Bénard convection depends on turbulent flow as well as the microphysical state of the clouds: specifically, whether substantial supersaturations exist and whether cloud liquid water is removed through sedimentation/precipitation. In this article we bridge between the Rayleigh-Bénard convection literature and the atmospheric literature. We express the governing equations for cloudy convection in dimensionless form, thereby explicitly identifying the governing parameters relevant to the cloudy case, including Schmidt, Damköhler, supersaturation, and sedimentation numbers. We further connect to the atmospheric literature by obtaining a Nusselt number (dimensionless heat flux) for a cloud-convection system, directly from the conservation equations for temperature and water vapor. This flux has the same form as that identified by Zhang et al. [L. Zhang, K. L. Chong, and K.-Q. Xia, J. Fluid Mech. 874, 1041 (2019)] for convection with water vapor, but is extended to the cloudy case. For equal thermal and water vapor diffusivities, the flux corresponds to the widely used atmospheric quantities equivalent temperature and moist static energy. Using large eddy simulation (LES) of an idealized cloudy Rayleigh-Bénard convection system with fixed boundary conditions, we find that the equivalent heat flux (Nusselt number) is only weakly dependent on the microphysical details of the system, such as liquid water mixing ratio and cloud droplet number concentration. Finally, from the results, we show the vertical profiles of sensible and latent heat fluxes depend on the liquid water content, whereas the equivalent heat flux remains a constant throughout the height of the chamber.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Substantially positive contributions of new particle formation to cloud condensation nuclei under low supersaturation in China based on numerical model improvements

New particle formation (NPF) and subsequent particle growth are important sources of condensation nuclei (CN) and cloud condensation nuclei (CCN). While many observations have shown positive contributions of NPF to CCN at low supersaturation, negative NPF contributions were often simulated in polluted environments. Using the observations in a coastal city of Qingdao, Beijing, and Gucheng in north China, we thoroughly evaluate the simulated number concentrations of CN and CCN using an NPF-explicit parameterization embedded in the WRF-Chem model. For CN, the initial simulation shows large biases of particle number concentrations at 10–40 and 40–100 nm. By adjusting the process of gas–particle partitioning, including the mass accommodation coefficient (MAC) of sulfuric acid, the phase changes in primary organic aerosol emissions, and the condensational amount of nitric acid, the improvement of the particle growth process yields substantially reduced overestimation of CN. Regarding CCN, secondary organic aerosol (SOA) formed from the oxidation of semi-volatile and intermediate-volatility organic compounds (S/IVOCs) is called SI-SOA, the yield of which is an important contributor. At default settings, the SI-SOA yield is too high without considering the differences in precursor oxidation rates. Lowering the SI-SOA yield under linear H 2 SO 4 nucleation scheme results in much-improved CCN simulations compared to observations. On the basis of the bias-corrected model, we find substantially positive contributions of NPF to CCN at low supersaturation (~ 0.2 %) over broad areas of China, primarily due to competing effects of increasing particle hygroscopicity, a result of reductions in SI-SOA amount, surpassing that of particle size decreases. The bias-corrected model is robustly applicable to other schemes, such as the quadratic H 2 SO 4 nucleation scheme, in terms of CN and CCN, though the dependence of CCN on SI-SOA yield is diminished likely due to changes in particle composition. This study highlights potentially much larger NPF contributions to CCN on a regional and even global basis.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1988

Supersaturation of vertically propagating internal gravity waves

The usual assumption that vertically propagating internal gravity waves will cease growing with height once their amplitudes are such as to permit convective instability anywhere within the wave is reexamined. Two factors lead to amplitude limitation: (1) wave clipping associated with convective mixing, and (2) energetic constraints associated with the rate at which the wave can supply energy to the convection. It is found that these two factors limit supersaturation to about 50 percent for waves with short horizontal wavelengths and high relative phase speeds. Usually the degree of supersaturation will be much less. These factors also lead to a gradual, rather than sudden, cessation of wave growth with height.

Lindzen, Richard S.↗
NASA NTRS1990

Crystallization of highly supersaturated solutions - An experimental study

The crystallization of ammonium sulfate solutions under very high supersaturation is investigated. The results imply that high saturation ratios can exist at least to 30 +/- 5 and possibly higher in smaller drops. Under certain atmospheric conditions highly supersaturated drops can persist at even lower temperatures and humidities.

Queen, Brian↗
NASA NTRS1953

Supersaturation in the spontaneous formation of nuclei in water vapor

According to experience, a certain supersaturation is required for condensation of water vapor in the homogeneous phase; that is, for inception of the condensation, at a prescribed temperature, the water vapor partial pressure must lie above the saturation pressure. The condensation starts on so-called condensation nuclei. Solid or liquid suspended particles may serve as nuclei; these particles may either a priori be present in the gas phase (dust, soot), or may spontaneously be formed from the vapor molecules to be condensed themselves. Only the second case will be considered. Gas ions which facilitate the spontaneous formation of nuclei may be present or absent. The supersaturations necessary for spontaneous nucleus formation are in general considerable higher than those in the presence of suspended particles.

CONDENSATION↗
NASA NTRS1995

Supersaturated Electrolyte Solutions: Theory and Experiment

Highly supersaturated electrolyte solutions can be prepared and studied employing an electrodynamic levitator trap (ELT) technique. The ELT technique involves containerless suspension of a microdroplet thus eliminating dust, dirt, and container walls which normally cause heterogeneous nucleation. This allows very high supersaturations to be achieved. A theoretical study of the experimental results obtained for the water activity in microdroplets of various electrolyte solutions is based on the development of the Cahn-Hilliard formalism for electrolyte solutions. In the approach suggested the metastable state for electrolyte solutions is described in terms of the conserved order parameter omega(r,t) associated with fluctuations of the mean solute concentration n(sub 0). Parameters of the corresponding Ginzburg-Landau free energy functional which defines the dynamics of metastable state relaxation are determined and expressed through the experimentally measured quantities. A correspondence of 96-99 % between theory and experiment for all solutions studied was achieved and allowed the determination of an analytical expression for the spinodal concentration n(sub spin), and its calculation for various electrolyte solutions at 298 K. The assumption that subcritical solute clusters consist of the electrically neutral Bjerrum pairs has allowed both analytical and numerical investigation of the number-size N(sub c) of nucleation monomers (aggregates of the Bjerrum pairs) which are elementary units of the solute critical clusters. This has also allowed estimations for the surface tension Alpha, and equilibrium bulk energy Beta per solute molecule in the nucleation monomers. The dependence of these properties on the temperature T and on the solute concentration n(sub 0) through the entire metastable zone (from saturation concentration n(sub sat) to spinodal n(sub spin) is examined. It has been demonstrated that there are the following asymptotics: N(sub c), = I at spinodal concentration and N(sub c) = infinity at saturation.

Izmailov, Alexander F.↗
NASA NTRS1996

Thermodynamic Studies of Levitated Microdroplets of Highly Supersaturated Electrolyte Solutions

Highly supersaturated electrolyte solutions are studied by employing an electrodynamic levitator trap (ELT) technique. The ELT technique involves containerless suspension of a microdroplet thus eliminating dust, dirt, and container walls which normally cause heterogeneous nucleation. This allows very high supersaturations to be achieved. A theoretical study of the experimental results obtained for the water activity in microdroplets of various electrolyte solutions is based on the development of the Cahn-Hilliard formalism for electrolyte solutions. A correspondence of 96-99% between the theory and experiment for the all solutions studied was achieved and allowed the determination of an analytical expression for the spinodal concentration n(sub spin) and its calculation for various electrolyte solutions at 298 K.

Myerson, Allan S.↗
NASA NTRS1996

Gravity Induced Formation of Concentration Gradients in Supersaturated Binary Solutions

Experimental and theoretical studies of the formation of solute concentration gradient in supersaturated binary solutions in a gravitational field were carried out. The formation of solute concentration gradient was associated with the gravity induced redistribution of subcritical solute clusters. The birth-death process of the new solute-rich phase domains (subcritical solute clusters) was described in terms of the time-dependent Ginzburg Landau model developed for metastable state relaxation in binary (solute + solvent) non-critical solutions in the presence of a gravitational field. A new mathematical Ansatz was developed for solution of the model equations. This Ansatz has allowed to approach for the first time the following important problems: (1) Microstructure of solute distribution inside of the subcritical solute clusters. The analytical results obtained demonstrate that solute inside of the subcritical solute clusters is heterogeneously distributed with a spatially periodic structure. (2) Macrostructure of the solute subcritical clusters distribution in a gravitational field. The subcritical solute clusters are found to be distributed heterogeneously in a gravitational field. This heterogeneity, which is due to the heterogeneous birth-death process of the subcritical solute clusters in a gravitational field, initiates a noticeable solute concentration gradient in vertical columns of supersaturated binary solutions. An analysis and comparison of theoretical results and experimental data related to the solute concentration gradient formation in a gravitational field are presented. It is also demonstrated that the critical radius of solute clusters (radius of nucleation) and induction time are gravity-dependent.

Izmailov, Alexander F.↗
NASA NTRS1997

Liquid-Liquid Phase Separation in Supersaturated Lysozyme Solutions and Associated Precipitate Formation/Crystallization

Using cloud point determinations, the phase boundaries (binodals) for metastable liquid-liquid (L-L) separation in supersaturated hen egg white lysozyme solutions with 3%, 5%, and 7% (wlv) NaCl at pH= 4.5 and protein concentrations c between 40 and 400 mg/ml were determined. The critical temperature for the binodal increased approximately linearly with salt concentration. The coexisting liquid phases both remained supersaturated but differed widely in protein concentration. No salt repartitioning was observed between the initial and the two separated liquid phases. After the L-L separation, due to the presence of the high protein concentration phase, crystallization occurred much more rapidly than in the initial solution. At high initial protein concentrations, a metastable gel phase formed at temperatures above the liquid binodal. Both crystal nucleation and gel formation were accelerated in samples that had been cycled through the binodal. Solutions in the gel and L-L regions yielded various types of precipitates. Based on theoretical considerations, previous observations with other proteins, and our experimental results with lysozyme, a generic phase diagram for globular proteins is put forth. A limited region in the (T,c) plane favorable for the growth of protein single crystals is delineated.

Muschol, Martin↗
NASA NTRS1997

Gaseous abundances and methane supersaturation in Titan's troposphere

Various properties of Titan's troposphere are inferred from an analysis of Voyager I infrared spectrometer (IRIS) data between 200 and 600/ cm. Two homogeneous spectral averages acquired at widely separated emission angles are chosen for the analysis. Both data sets are associated with northern low latitudes very close to that of the radio science ingress occultation point. Solutions require simultaneous nonlinear least-squares fits to the two IRIS data sets, coupled with iteration of the radio occultation refractivity data. Values and associated 1-sigma uncertainties of several parameters are inferred from our analysis. These include mole fractions for molecular hydrogen (approx. 0.0011), argon (small), and methane near the surface ( approx. 0.057). Solutions are also obtained for the hydrogen parafraction (close to equilibrium, with considerable uncertainty), air temperature near the surface ( approx. 93 K), surface surface temperature discontinuity (approx. 1 K), and maximum degree of methane supersaturation in the upper troposphere (approx. 1.5). Actual values for the above-mentioned parameters depend on the amount of ethane cloud near the tropopause. There is no evidence for methane clouds in the upper troposphere, nor is their presence compatible with large degrees of supersaturation. A wave number dependence for the stratospheric haze opacity is inferred similar to that found for a polymeric residue created in laboratory discharge experiments. This haze appears to be uniformly distributed with latitude between altitudes of 40 and 160 km, provided those nighttime data at southern high latitudes that are discounted.

Samuelson, Robert E.↗
NASA NTRS2000

Lidar Measurements of Relative Humidity and Ice Supersaturation in the Upper Troposphere

We compute upper tropospheric relative humidity profiles using water vapor profiles measured by an airborne DIAL and a ground-based Raman lidar. LASE water vapor and MTP temperature profiles acquired from the NASA DC-8 aircraft during the recent Pacific Exploratory Mission Tropics B (PEM Tropics B) field mission in the tropical Pacific and the SAGE-III Ozone Loss and Validation Experiment (SOLVE) in the Arctic as well as water vapor profiles derived from the ground-based DOE ARM Southern Great Plains (SGP) CART Raman lidar are used. Comparisons of the lidar water vapor measurements with available in situ measurements show reasonable agreement for water vapor mixing ratios above 0.05 g/kg. Relative humidity frequency distributions computed using LASE data indicate that ice supersaturation occurred about 5-11% of the time when temperatures were below -35 C. While a higher frequency of ice supersaturation was observed during SOLVE, higher peak values of relative humidity were observed during PEM Tropics B. The relative humidity fields associated with cirrus clouds are also examined.

Ferrare, Richard A.↗
NASA NTRS2013

Can Supersaturation Affect Protein Crystal Quality?

In quiescent environments (microgravity, capillary tubes, gels) formation of a depletion zone is to be expected, due either to limited sedimentation, density driven convection or a combination of both. The formation of a depletion zone can: Modify solution supersaturation near crystal; Give rise to impurity partitioning. It is conjectured that both supersaturation and impurity partitioning affect protein crystal quality and size. Further detailed investigations on various proteins are needed to assess above hypothesis.

Gorti, Sridhar↗
NASA NTRS2013

Can Solution Supersaturation Affect Protein Crystal Quality?

The formation of large protein crystals of "high quality" is considered a characteristic manifestation of microgravity. The physical processes that predict the formation of large, high quality protein crystals in the microgravity environment of space are considered rooted in the existence of a "depletion zone" in the vicinity of crystal. Namely, it is considered reasonable that crystal quality suffers in earth-grown crystals as a result of the incorporation of large aggregates, micro-crystals and/or large molecular weight "impurities", processes which are aided by density driven convective flow or mixing at the crystal-liquid interface. Sedimentation and density driven convection produce unfavorable solution conditions in the vicinity of the crystal surface, which promotes rapid crystal growth to the detriment of crystal size and quality. In this effort, we shall further present the hypothesis that the solution supersaturatoin at the crystal surface determines the growth mechanism, or mode, by which protein crystals grow. It is further hypothesized that protein crystal quality is affected by the mechanism or mode of crystal growth. Hence the formation of a depletion zone in microgravity environment is beneficial due to inhibition of impurity incorporatoin as well as preventing a kinetic roughening transition. It should be noted that for many proteins the magnitude of neither protein crystal growth rates nor solution supersaturation are predictors of a kinetic roughening transition. That is, the kinetic roughening transition supersaturation must be dtermined for each individual protein.

Gorti, Sridhar↗
NASA NTRS2016

An Assessment of the Radiative Effects of Ice Supersaturation Based on in Situ Observations

We use aircraft observations combined with the reanalysis data to investigate the radiative effects of ice supersaturation (ISS). Our results show that although the excess water vapor over ice saturation itself has relatively small radiative effects, mistaking it as ice crystals in climate models would lead to considerable impacts: on average, +2.49 W/m(exp 2) change in the top of the atmosphere (TOA) radiation, -2.7 W/m(exp 2) change in surface radiation, and 1.47 K/d change in heating rates. The radiative effects of ISS generally increase with the magnitudes of supersaturation. However, there is a strong dependence on the preexisting ice water path, which can even change the sign of the TOA radiative effect. It is therefore important to consider coexistence between ISS and ice clouds and to validate their relationship in the parameterizations of ISS in climate models.

Tan, Xiaoxiao↗
NASA NTRSDate not supplied

Bluntness and Supersaturation Effects on the Second Mode Instability in Mach 10 Flow

An experimental campaign was conducted on a 7-degree half-angle cone in the NASA Langley Research Center 31-Inch Mach 10 Tunnel to investigate the impact of nosetip radius and freestream supersaturation on the development of the second mode instability. The model was instrumented with surface-mounted Kulite® and PCB® pressure transducers and thermocouples. Power spectral density plots demonstrate the anticipated trends of the second mode instability weakening and shifting to lower frequencies with increased bluntness. Heat transfer measurements suggest laminar flow over the bulk of the model for most testing conditions, with evidence of transition by the cone base for the sharpest nosetip (R = 0.15 mm) at the higher unit Reynolds numbers. The dynamic surface pressure and heat transfer measurements show that reducing the temperature of the freestream to a supersaturated state has a significant stabilizing effect on the model boundary layer. The surface measurements are observed to be highly dependent on the level of clustering in the freestream. Significant changes in surface pressure spectra due to total temperature reduction are first noted below T0= 948 K, while more substantial fluctuation reductions are found below T0= 810 K.

Hypersonics↗
DOE OSTI2021

Labile Fe(III) supersaturation controls nucleation and properties of product phases from Fe(II)-catalyzed ferrihydrite transformation

We report Fe(II)-catalyzed ferrihydrite (Fh) transformation to more crystalline iron (oxyhydr)oxide phases is a widely occurring geochemical process which has been extensively studied as a function of Fe(II)/Fh ratios at fixed Fh loadings. However, recent isolation of an intermediate Fe(III) species resulting from Fe(II)-Fh contact that facilitates transformation by dissolution/reprecipitation suggests that the kinetics and properties of product phases will instead depend mostly on its rate of accumulation to a critical concentration, consistent with principles in the classical nucleation theory (CNT). This suggests a dependence both on the loading of Fe(II) on the surface, which controls the rate of labile Fe(III) formation, as well as the available volume of solution, which also impacts how fast it can achieve its critical concentration to nucleate product phases. To specifically examine the latter effect, here we studied transformation of 15 mg Fh in 1 mM FeSO 4 solutions at pH 7.2 in batch suspensions of 30 mL, 150 mL, and 450 mL volumes. Time-dependent concentrations of aqueous Fe(II), surface-associated Fe(II), and resulting labile Fe(III) were monitored along with bulk solids characterization as a function of time. Transmission electron microscopy (TEM) was used to visualize the evolution of phases at identical locations on TEM grids. The collective results show that the rates of Fh loss and emergence of product lepidocrocite (Lp) and goethite (Gt) as well as their phase proportions, nucleation mode and morphological properties depend directly on the rate of accumulation of the labile Fe(III) precursor to its critical concentration, which in our experiments was controlled simply by varying the available volume of solution into which it enters. Statistical analyses of TEM image data suggest that while both heterogeneous and homogeneous nucleation occurred in all experiments, the former was increasingly favored at lower Fh/solution ratio due to its lower nucleation barrier being more favorable at attendant lower supersaturations of Fe(III).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Growth of deuterium supersaturated surface layer with increasing ion flux and fluence in plasma-exposed tungsten

Deuterium supersaturated surface layer (DSSL) in tungsten, a few nm thick layer exhibiting extremely high deuterium content (> 5%), has been studied as a function of deuterium plasma ion flux and fluence. Tungsten samples were exposed at 400 K and deuterium ion energy of ∼ 60 eV. The deuterium ion flux spanned over an order of magnitude, being 7.3 × 10 20 , 4.2 × 10 21 , and 3.8 × 10 22 D/m 2 . The fluence ranged from 3.4 × 1024 to 3.4 × 1025 D/m2. The samples and their deuterium content were analyzed by nuclear reaction analysis (NRA), scanning transmission electron microscopy (STEM), and thermal desorption spectroscopy (TDS). The largest thickness of DSSL was found to be around 10.5 nm and was observed in the case of the highest exposure flux and fluence, whereas the layer was only about 3.8 nm thick in the case of the lowest value of the two parameters. The thickness of the DSSL was found to monotonically increase with both deuterium flux and fluence. Finally, similar to the thickness, the estimated D concentration seems to follow the same trend, increasing from the lowest value of around 3 at.% to the highest value of around 5 at.%.

Deuterium↗
DOE OSTI2023

Maximum Supersaturation in the Marine Boundary Layer Clouds Over the North Atlantic

Abstract The maximum supersaturation ( S x ) in clouds is a key parameter affecting the cloud's microphysical and radiative properties. We investigate the S x of the marine boundary layer clouds by combining airborne and surface observations in the Eastern North Atlantic. The cloud droplet number concentration ( N c ) in the least diluted cloud cores agrees well with the number concentration of particles larger than the Hoppel Minimum (HM) ( N >HM ) below clouds, indicating that the HM represents the average size threshold above which particles are activated to form cloud droplets. The S x values derived from surface observations vary from 0.10% to 0.50% from June 2017 to June 2018, with a clear seasonal variation exhibiting higher values during winter. Most of the S x variance (∼60%) can be explained by the cloud condensation nuclei (CCN) concentration and updraft velocity ( w ), with the CCN concentration playing a more important role than w in explaining the variation of S x . The influence of CCN concentration on S x leads to a buffered response of N c to aerosol perturbations. The response of N c to low aerosol concentration during winter is further buffered by the high w . The global Community Earth System Model (CESM) simulated S x values in the Azores have a positive bias compared to measured S x , likely due to overestimated w and underestimated CCN concentration. The CESM simulated S x exhibits higher values further north over the North Atlantic Ocean, which is attributed to stronger w . The suppression of S x by aerosol is also evident in regions with high CCN concentrations.

54 ENVIRONMENTAL SCIENCES↗