Direct Numerical Simulation of Turbulent Condensation in Clouds

NASA Technical Reports Server (NTRS)

Shariff, K.; Paoli, R.

2004-01-01

In this brief, we investigate the turbulent condensation of a population of droplets by means of a direct numerical simulation. To that end, a coupled Navier-Stokes/Lagrangian solver is used where each particle is tracked and its growth by water vapor condensation is monitored exactly. The main goals of the study are to find out whether turbulence broadens the droplet size distribution, as observed in in situ measurements. The second issue is to understand if and for how long a correlation between the droplet radius and the local supersaturation exists for the purpose of modeling sub-grid scale microphysics in cloud-resolving codes. This brief is organized as follows. In Section 2 the governing equations are presented, including the droplet condensation model. The implementation of the forcing procedure is described in Section 3. The simulation results are presented in Section 4 together with a sketch of a simple stochastic model for turbulent condensation. Conclusions and the main outcomes of the study are given in Section 5.

Can Condensing Organic Aerosols Lead to Less Cloud Particles?

NASA Astrophysics Data System (ADS)

Gao, C. Y.; Tsigaridis, K.; Bauer, S.

2017-12-01

We examined the impact of condensing organic aerosols on activated cloud number concentration in a new aerosol microphysics box model, MATRIX-VBS. The model includes the volatility-basis set (VBS) framework in an aerosol microphysical scheme MATRIX (Multiconfiguration Aerosol TRacker of mIXing state) that resolves aerosol mass and number concentrations and aerosol mixing state. Preliminary results show that by including the condensation of organic aerosols, the new model (MATRIX-VBS) has less activated particles compared to the original model (MATRIX), which treats organic aerosols as non-volatile. Parameters such as aerosol chemical composition, mass and number concentrations, and particle sizes which affect activated cloud number concentration are thoroughly evaluated via a suite of Monte-Carlo simulations. The Monte-Carlo simulations also provide information on which climate-relevant parameters play a critical role in the aerosol evolution in the atmosphere. This study also helps simplifying the newly developed box model which will soon be implemented in the global model GISS ModelE as a module.

Organic Aerosols as Cloud Condensation Nuclei

NASA Astrophysics Data System (ADS)

Hudson, J. G.

2002-05-01

The large organic component of the atmospheric aerosol contributes to both natural and anthropogenic cloud condensation nuclei (CCN). Moreover, some organic substances may reduce droplet surface tension (Facchini et al. 1999), while others may be partially soluble (Laaksonen et al. 1998), and others may inhibit water condensation. The interaction of organics with water need to be understood in order to better understand the indirect aerosol effect. Therefore, laboratory CCN spectral measurements of organic aerosols are presented. These are measurements of the critical supersaturation (Sc), the supersaturation needed to produce an activated cloud droplet, as a function of the size of the organic particles. Substances include sodium lauryl (dodecyl) sulfate, oxalic, adipic, pinonic, hexadecanedioic, glutaric, stearic, succinic, phthalic, and benzoic acids. These size-Sc relationships are compared with theoretical and measured size-Sc relationships of common inorganic compounds (e.g., NaCl, KI, ammonium and calcium sulfate). Unlike most inorganics some organics display variations in solubility per unit mass as a function of particle size. Those showing relatively greater solubility at smaller sizes may be attributable to surface tension reduction, which is greater for less water dilution, as is the case for smaller particles, which are less diluted at the critical sizes. This was the case for sodium dodecyl sulfate, which does reduce surface tension. Relatively greater solubility for larger particles may be caused by greater dissolution at the higher dilutions that occur with larger particles; this is partial solubility. Measurements are also presented of internal mixtures of various organic and inorganic substances. These measurements were done with two CCN spectrometers (Hudson 1989) operating simultaneously. These two instruments usually displayed similar results in spite of the fact that they have different flow rates and supersaturation profiles. The degree of

Influence of Microphysical Variability on Stochastic Condensation in Turbulent Clouds

NASA Astrophysics Data System (ADS)

Desai, N.; Chandrakar, K. K.; Chang, K.; Glienke, S.; Cantrell, W. H.; Fugal, J. P.; Shaw, R. A.

2017-12-01

We investigate the influence of variability in droplet number concentration and radius on the evolution of cloud droplet size distributions. Measurements are made on the centimeter scale using digitial inline holography, both in a controlled laboratory setting and in the field using HOLODEC measurements from CSET. We created steady state cloud conditions in the laboratory Pi Chamber, in which a turbulent cloud can be sustained for long periods of time. Using holographic imaging, we directly observe the variations in local number concentration and droplet size distribution and, thereby, the integral radius. We interpret the measurements in the context of stochastic condensation theory to determine how fluctuations in integral radius contribute to droplet growth. We find that the variability in integral radius is primarily driven by variations in the droplet number concentration and not the droplet radius. This variability does not contribute significantly to the mean droplet growth rate, but contributes significantly to the rate of increase of the size distribution width. We compare these results with in-situ measurements and find evidence for microphysical signatures of stochastic condensation. The results suggest that supersaturation fluctuations lead to broader size distributions and allow droplets to reach the collision-coalescence stage.

Femtosecond laser filament induced condensation and precipitation in a cloud chamber

PubMed Central

Ju, Jingjing; Liu, Jiansheng; Liang, Hong; Chen, Yu; Sun, Haiyi; Liu, Yonghong; Wang, Jingwei; Wang, Cheng; Wang, Tiejun; Li, Ruxin; Xu, Zhizhan; Chin, See Leang

2016-01-01

A unified picture of femtosecond laser induced precipitation in a cloud chamber is proposed. Among the three principal consequences of filamentation from the point of view of thermodynamics, namely, generation of chemicals, shock waves and thermal air flow motion (due to convection), the last one turns out to be the principal cause. Much of the filament induced chemicals would stick onto the existing background CCN’s (Cloud Condensation Nuclei) through collision making the latter more active. Strong mixing of air having a large temperature gradient would result in supersaturation in which the background CCN’s would grow efficiently into water/ice/snow. This conclusion was supported by two independent experiments using pure heating or a fan to imitate the laser-induced thermal effect or the strong air flow motion, respectively. Without the assistance of any shock wave and chemical CCN’s arising from laser filament, condensation and precipitation occurred. Meanwhile we believe that latent heat release during condensation /precipitation would enhance the air flow for mixing. PMID:27143227

Titan's Aerosol and Condensation Cloud Properties in the Far-IR Between 2005 and 2010

NASA Technical Reports Server (NTRS)

Anderson, Carrie; Samuelson, Robert

2011-01-01

Analyses of far-IR spectra between 20 and 560 cm(exp -1) (500 to 18 micron) recorded by the Cassini Composite Infrared Spectrometer (CIRS) yield the spectral dependence and the vertical distribution of Titan's photochemical aerosol and ice clouds. Titan's aerosol appears to be well mixed between the surface and an altitude of 300 km, with a spectral shape that does not change with latitude or time. The aerosol exhibits an extremely broad emission feature with a spectral peak at 140 cm(exp -1) (71 micron), which is not evident in laboratory simulated Titan aerosols (tholin). This low- energy aerosol emission feature may arise from low-energy molecules such as polycyclic aromatic hydrocarbons and/or nitrogenated aromatics. Unlike the vertically well-mixed aerosol, Titan's condensate clouds are located in highly restricted altitudes in the lower stratosphere, ranging between 60 and 100 km at low and moderate latitudes, to between 150 and 165 km at high northern latitudes during northern winter. Such clouds are located at altitudes where nitrile vapors are expected to condense and appear to be dominated by HCN and HC3N, which are the two most abundant nitriles in Titan's atmosphere. Associated with this ice cloud is a broad emission feature that spectrally peaks near 160 cm(exp -1) (62.5 micron). This ice composite appears to chemically change with altitude and latitude, probably as a result of differences in vapor abundance and condensation temperature, and the ice cloud appears to be global in extent. Both CIRS and the Huygens Descent Imager and Spectral Radiometer (DISR) show evidence of cloud layering in Titan's lower stratosphere. The 15 km difference in cloud altitude indicated by the two instruments suggests a difference in ice composition. CIRS also indicates a second ice cloud that exists at isolated latitudes and is consistent with hydrocarbon condensation above the tropopause. This cloud exhibits an emission feature that spectrally peaks near 80 cm(exp -1

Organic condensation: a vital link connecting aerosol formation to cloud condensation nuclei (CCN) concentrations

NASA Astrophysics Data System (ADS)

Riipinen, I.; Pierce, J. R.; Yli-Juuti, T.; Nieminen, T.; Häkkinen, S.; Ehn, M.; Junninen, H.; Lehtipalo, K.; Petäjä, T.; Slowik, J.; Chang, R.; Shantz, N. C.; Abbatt, J.; Leaitch, W. R.; Kerminen, V.-M.; Worsnop, D. R.; Pandis, S. N.; Donahue, N. M.; Kulmala, M.

2011-04-01

Atmospheric aerosol particles influence global climate as well as impair air quality through their effects on atmospheric visibility and human health. Ultrafine (<100 nm) particles often dominate aerosol numbers, and nucleation of atmospheric vapors is an important source of these particles. To have climatic relevance, however, the freshly nucleated particles need to grow in size. We combine observations from two continental sites (Egbert, Canada and Hyytiälä, Finland) to show that condensation of organic vapors is a crucial factor governing the lifetimes and climatic importance of the smallest atmospheric particles. We model the observed ultrafine aerosol growth with a simplified scheme approximating the condensing species as a mixture of effectively non-volatile and semi-volatile species, demonstrate that state-of-the-art organic gas-particle partitioning models fail to reproduce the observations, and propose a modeling approach that is consistent with the measurements. We find that roughly half of the mass of the condensing mass needs to be distributed proportional to the aerosol surface area (thus implying that the condensation is governed by gas-phase concentration rather than the equilibrium vapour pressure) to explain the observed aerosol growth. We demonstrate the large sensitivity of predicted number concentrations of cloud condensation nuclei (CCN) to these interactions between organic vapors and the smallest atmospheric nanoparticles - highlighting the need for representing this process in global climate models.

Sensitivities of simulated satellite views of clouds to subgrid-scale overlap and condensate heterogeneity

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hillman, Benjamin R.; Marchand, Roger T.; Ackerman, Thomas P.

Satellite simulators are often used to account for limitations in satellite retrievals of cloud properties in comparisons between models and satellite observations. The purpose of the simulator framework is to enable more robust evaluation of model cloud properties, so that di erences between models and observations can more con dently be attributed to model errors. However, these simulators are subject to uncertainties themselves. A fundamental uncertainty exists in connecting the spatial scales at which cloud properties are retrieved with those at which clouds are simulated in global models. In this study, we create a series of sensitivity tests using 4more » km global model output from the Multiscale Modeling Framework to evaluate the sensitivity of simulated satellite retrievals when applied to climate models whose grid spacing is many tens to hundreds of kilometers. In particular, we examine the impact of cloud and precipitation overlap and of condensate spatial variability. We find the simulated retrievals are sensitive to these assumptions. Specifically, using maximum-random overlap with homogeneous cloud and precipitation condensate, which is often used in global climate models, leads to large errors in MISR and ISCCP-simulated cloud cover and in CloudSat-simulated radar reflectivity. To correct for these errors, an improved treatment of unresolved clouds and precipitation is implemented for use with the simulator framework and is shown to substantially reduce the identified errors.« less

Cloud Condensation Nuclei Activity of Aerosols during GoAmazon 2014/15 Field Campaign Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, J.; Martin, S. T.; Kleinman, L.

2016-03-01

Aerosol indirect effects, which represent the impact of aerosols on climate through influencing the properties of clouds, remain one of the main uncertainties in climate predictions (Stocker et al. 2013). Reducing this large uncertainty requires both improved understanding and representation of aerosol properties and processes in climate models, including the cloud activation properties of aerosols. The Atmospheric System Research (ASR) science program plan of January 2010 states that: “A key requirement for simulating aerosol-cloud interactions is the ability to calculate cloud condensation nuclei and ice nuclei (CCN and IN, respectively) concentrations as a function of supersaturation from the chemical andmore » microphysical properties of the aerosol.” The Observations and Modeling of the Green Ocean Amazon (GoAmazon 2014/15) study seeks to understand how aerosol and cloud life cycles are influenced by pollutant outflow from a tropical megacity (Manaus)—in particular, the differences in cloud-aerosol-precipitation interactions between polluted and pristine conditions. One key question of GoAmazon2014/5 is: “What is the influence of the Manaus pollution plume on the cloud condensation nuclei (CCN) activities of the aerosol particles and the secondary organic material in the particles?” To address this question, we measured size-resolved CCN spectra, a critical measurement for GoAmazon2014/5.« less

A Review of Spatial and Seasonal Changes in Condensation Clouds Observed During Aerobraking by MGS TES

NASA Technical Reports Server (NTRS)

Pearl, J. C.; Smith, M. D.; Conrath, B. J.; Bandfield, J. L.; Christensen, P. R.

1999-01-01

Successful operation of the Mars Global Surveyor spacecraft beginning in September 1997, has permitted extensive infrared observations of condensation clouds during the martian southern summer and fall seasons (184 degclouds and hazes were widespread, showing a latitudinal gradient. With the onset of a regional dust storm at L(sub s) = 224 deg, ice clouds essentially vanished in the southern hemisphere, to reappear gradually after the decay of the storm. The thickest clouds (optical depth approximately 0.6) were associated with major volcanic features. At L(sub s) =318 deg, the cloud at Ascraeus Mons was observed to disappear between 21:30 and 09:30, consistent with historically recorded diurnal behavior for clouds of this type. Limb observations showed extended optically thin (depth<0.04) stratiform clouds at altitudes up to 55 km. A water ice haze was present in the north polar night at altitudes up to 40 km; this probably provided heterogeneous nucleation sites for the formation of CO2 clouds at altitudes below the 1 mbar pressure level, where atmospheric temperatures dropped to the condensation point Of CO2.

Measurements of cloud condensation nuclei spectra within maritime cumulus cloud droplets: Implications for mixing processes

NASA Technical Reports Server (NTRS)

Twohy, Cynthia H.; Hudson, James G.

1995-01-01

In a cloud formed during adiabatic expansion, the droplet size distribution will be systematically related to the critical supersaturation of the cloud condensation nuclei (CNN), but this relationship can be complicated in entraining clouds. Useful information about cloud processes, such as mixing, can be obtained from direct measurements of the CNN involved in droplet nucleation. This was accomplished by interfacing two instruments for a series of flights in maritime cumulus clouds. One instrument, the counterflow virtual impactor, collected cloud droplets, and the nonvolatile residual nuclei of the droplets was then passed to a CCN spectrometer, which measured the critical supersaturation (S(sub c)) spectrum of the droplet nuclei. The measured S(sub c) spectra of the droplet nuclei were compared with the S(sub c) spectra of ambient aerosol particles in order to identify which CCN were actually incorporated into droplets and to determine when mixing processes were active at different cloud levels. The droplet nuclei nearly always exhibited lower median S(sub c)'s than the ambient aerosol, as expected since droplets nucleate perferentially on particles with lower critical supersaturations. Critical supersaturation spectra from nuclei of droplets near cloud base were similar to those predicted for cloud regions formed adiabatically, but spectra of droplet nuclei from middle cloud levels showed some evidence that mixing had occurred. Near cloud top, the greatest variation in the spectra of the droplet nuclei was observed, and nuclei with high S(sub c)'s were sometimes present even within relatively large droplets. This suggests that the extent of mixing increases with height in cumulus clouds and that inhomogeneous mixing may be important near cloud top. These promising initial results suggest improvements to the experimental technique that will permit more quantitative results in future experiments.

Effects of cloud condensate vertical alignment on radiative transfer calculations in deep convective regions

NASA Astrophysics Data System (ADS)

Wang, Xiaocong

2017-04-01

Effects of cloud condensate vertical alignment on radiative transfer process were investigated using cloud resolving model explicit simulations, which provide a surrogate for subgrid cloud geometry. Diagnostic results showed that the decorrelation length Lcw varies in the vertical dimension, with larger Lcw occurring in convective clouds and smaller Lcw in cirrus clouds. A new parameterization of Lcw is proposed that takes into account such varying features and gives rise to improvements in simulations of cloud radiative forcing (CRF) and radiative heating, i.e., the peak of bias is respectively reduced by 8 W m- 2 for SWCF and 2 W m- 2 for LWCF in comparison with Lcw = 1 km. The role of Lcw in modulating CRFs is twofold. On the one hand, larger Lcw tends to increase the standard deviation of optical depth στ, as dense and tenuous parts of the clouds would be increasingly aligned in the vertical dimension, thereby broadening the probability distribution. On the other hand, larger στ causes a decrease in the solar albedo and thermal emissivity, as implied in their convex functions on τ. As a result, increasing (decreasing) Lcwleads to decreased (increased) CRFs, as revealed by comparisons among Lcw = 0, Lcw = 1 km andLcw = ∞. It also affects the vertical structure of radiative flux and thus influences the radiative heating. A better representation of στ in the vertical dimension yields an improved simulation of radiative heating. Although the importance of vertical alignment of cloud condensate is found to be less than that of cloud cover in regards to their impacts on CRFs, it still has enough of an effect on modulating the cloud radiative transfer process.

Cloud Condensation Nuclei in Cumulus Humilis - Selected Case Study During the CHAPS Campaign

NASA Astrophysics Data System (ADS)

Yu, X.; Berg, L. K.; Berkowitz, C. M.; Alexander, M. L.; Lee, Y.; Laskin, A.; Ogren, J. A.; Andrews, B.

2009-12-01

The Cumulus Humilis Aerosol Processing Study (CHAPS) provided a unique opportunity to study aerosol and cloud processing. Clouds play an active role in the processing and cycling of atmospheric constituents. Gases and particles can partition to cloud droplets by absorption and condensation as well as activation and pact scavenging. The Department of Energy (DOE) G-1 aircraft was used as one of the main platforms in CHAPS. Flight tracks were designed and implemented to characterize freshly emitted aerosols on cloud top and cloud base as well as with cloud, i.e., cumulus humilis (or fair-weather cumulus), in the vicinity of Oklahoma City. Measurements of interstitial aerosols and residuals of activated condensation cloud nuclei were conducted simultaneously. The interstitial aerosols were determined downstream of an isokinetic inlet; and the activated particles downstream of a counter-flow virtual impactor (CVI). The sampling line to the Aerodyne Aerosol Mass Spectrometer was switched between the isokinetic inlet and the CVI to allow characterization of interstitial particles out of clouds in contrast to particles activated in clouds. Trace gases including ozone, carbon monoxide, sulfur dioxide, and a series of volatile organic compounds (VOCs) were also measured as were key meteorological state parameters including liquid water content, cloud drop size, and dew point temperature were measured. This work will focus on studying CCN properties in cumulus humilis. Several approaches will be taken. The first is single particle analysis of particles collected by the Time-Resolved Aerosol Sampler (TRAC) by SEM/TEM coupled with EDX. We will specifically look into differences in particle properties such as chemical composition and morphology between activated and interstitial ones. The second analysis will link in situ measurements with the snap shots observations by TRAC. For instance, by looking into the characteristic m/z obtained by AMS vs. CO or isoprene, one can gain

A Review of Spatial and Seasonal Changes in Condensation Clouds Observed During Aerobraking by MGS TES

NASA Technical Reports Server (NTRS)

Pearl, J. C.; Smith, M. D.; Conrath, B. J.; Bandfield, J. L.; Christensen, P. R.

1999-01-01

Successful operation of the Mars Global Surveyor spacecraft, beginning in September 1997, has permitted extensive infrared observations of condensation clouds during the martian southern summer and fall seasons (184 deg less than L(sub s) less than 28 deg). Initially, thin (normal optical depth less than 0.06 at 825/ cm) ice clouds and hazes were widespread, showing a latitudinal gradient. With the onset of a regional dust storm at L(sub s) = 224 deg, ice clouds essentially vanished in the southern hemisphere, to reappear gradually after the decay of the storm. The thickest clouds (optical depth approx. 0.6) were associated with major volcanic features. At L(exp s) = 318 deg, the cloud at Ascraeus Mons was observed to disappear between 21:30 and 09:30, consistent with historically recorded diurnal behavior for clouds of this type. Limb observations showed extended optically thin (depth less than 0.04) stratiform clouds at altitudes up to 55 km. A water ice haze was present in the north polar night at altitudes up to 40 km; this probably provided heterogeneous nucleation sites for the formation of CO2 clouds at altitudes below the 1 mbar pressure level, where atmospheric temperatures dropped to the condensation point of CO2.

On the Effect of Dust Particles on Global Cloud Condensation Nuclei and Cloud Droplet Number

NASA Technical Reports Server (NTRS)

Karydis, V. A.; Kumar, P.; Barahona, D.; Sokolik, I. N.; Nenes, A.

2011-01-01

Aerosol-cloud interaction studies to date consider aerosol with a substantial fraction of soluble material as the sole source of cloud condensation nuclei (CCN). Emerging evidence suggests that mineral dust can act as good CCN through water adsorption onto the surface of particles. This study provides a first assessment of the contribution of insoluble dust to global CCN and cloud droplet number concentration (CDNC). Simulations are carried out with the NASA Global Modeling Initiative chemical transport model with an online aerosol simulation, considering emissions from fossil fuel, biomass burning, marine, and dust sources. CDNC is calculated online and explicitly considers the competition of soluble and insoluble CCN for water vapor. The predicted annual average contribution of insoluble mineral dust to CCN and CDNC in cloud-forming areas is up to 40 and 23.8%, respectively. Sensitivity tests suggest that uncertainties in dust size distribution and water adsorption parameters modulate the contribution of mineral dust to CDNC by 23 and 56%, respectively. Coating of dust by hygroscopic salts during the atmospheric aging causes a twofold enhancement of the dust contribution to CCN; the aged dust, however, can substantially deplete in-cloud supersaturation during the initial stages of cloud formation and can eventually reduce CDNC. Considering the hydrophilicity from adsorption and hygroscopicity from solute is required to comprehensively capture the dust-warm cloud interactions. The framework presented here addresses this need and can be easily integrated in atmospheric models.

STORMVEX. Ice Nuclei and Cloud Condensation Nuclei Characterization Field Campaign Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cziczo, D.

2016-03-01

The relationship between aerosol particles and the formation of clouds is among the most uncertain aspects in our current understanding of climate change. Warm clouds have been the most extensively studied, in large part because they are normally close to the Earth’s surface and only contain large concentrations of liquid droplets. Ice and mixed-phase clouds have been less studied even though they have extensive global coverage and dominate precipitation formation. Because they require low temperatures to form, both cloud types are infrequently found at ground level, resulting in more difficult field studies. Complex mixtures of liquid and ice elements, normallymore » at much lower concentrations than found in warm clouds, require precise separation techniques and accurate identification of phase. Because they have proved so difficult to study, the climatic impact of ice-containing clouds remains unresolved. In this study, cloud condensation nuclei (CCN) concentrations and associated single particles’ composition and size were measured at a high-elevation research site—Storm Peak Lab, east of Steamboat Springs, Colorado, operated by the Desert Research Institute. Detailed composition analyses were presented to compare CCN activation with single-particle composition. In collaboration with the scientists of the Storm Peak Lab Cloud Property Validation Experiment (STORMVEX), our goal was to relate these findings to the cloud characteristics and the effect of anthropogenic activities.« less

Aircraft profile measurements of 18O/16O and D/H isotope ratios of cloud condensate and water vapor constrain precipitation efficiency and entrainment rates in tropical clouds

NASA Astrophysics Data System (ADS)

Noone, D. C.; Raudzens Bailey, A.; Toohey, D. W.; Twohy, C. H.; Heymsfield, A.; Rella, C.; Van Pelt, A. D.

2011-12-01

Convective clouds play a significant role in the moisture and heat balance of the tropics. The dynamics of organized and isolated convection are a function of the background thermodynamic profile and wind shear, buoyancy sources near the surface and the latent heating inside convective updrafts. The stable oxygen and hydrogen isotope ratios in water vapor and condensate can be used to identify dominant moisture exchanges and aspects of the cloud microphysics that are otherwise difficult to observe. Both the precipitation efficiency and the dilution of cloud updrafts by entrainment can be estimated since the isotopic composition outside the plume is distinct from inside. Measurements of the 18O/16O and D/H isotope ratios were made in July 2011 on 13 research flights of the NCAR C130 aircraft during the ICE-T (Ice in Clouds Experiment - Tropical) field campaign near St Croix. Measurements were made using an instrument based on the Picarro Wave-Length Scanning Cavity Ring Down platform that includes a number of optical, hardware and software modifications to allow measurements to be made at 5 Hz for deployment on aircraft. The measurement system was optimized to make precise measurements of the isotope ratio of liquid and ice cloud condensate by coupling the gas analyzer to the NCAR Counter flow Virtual Impactor inlet. The inlet system provides a particle enhancement while rejecting vapor. Sample air is vigorously heated before flowing into the gas phase analyzer. We present statistics that demonstrate the performance and calibration of the instrument. Measured profiles show that environmental air exhibits significant layering showing controls from boundary layer processes, large scale horizontal advection and regional subsidence. Condensate in clouds is consistent with generally low precipitation efficiency, although there is significant variability in the isotope ratios suggesting heterogeneity within plumes and the stochastic nature of detrainment processes

Cloud Condensation Nuclei Measurements in Tropical Cyclones

NASA Technical Reports Server (NTRS)

Hudson, J. G.; Simpson, J.

2002-01-01

The first measurements of cloud condensation nuclei (CCN) within and around tropical cyclones were made with the Desert Research Institute (DRI) CCN spectrometer (Hudson 1909) from a NOAA P-3 Hurricane Hunter aircraft throughout the 2001 season. Two penetrations of the closed eye of Hurricane Erin off the northeast US coast on Sept. 10 showed concentrations consistently well in excess of 1000 per cubic cm at approximately 1.4% supersaturation. Simultaneous condensation nuclei (CN--total particle) concentrations were consistently well in excess of 2000 per cubic cm throughout these closed eye penetrations. These within eye measurements at 4 km altitude for exceeded CCN and CN measurements just outside of the storm at similar altitudes--300 and 600 per cubic cm respectively. These CCN and CN concentrations within this closed eye were far above concentrations in maritime air masses; they are characteristic of continental or polluted air masses. Although there was a possibility that Saharan duct may have gotten into this storm these sub tenth micrometer particles are much too small and much too numerous to be dust. Such high concentrations may have originated from European air pollution, which may have been transported by similar airflow patterns to those that carry Saharan dust across the Atlantic. These high concentrations may be a manifestation of descending air that brings higher concentrations that are often characteristic of the upper troposphere (Clarke and Kapustin 2002). Later in the month measurements in Humberto showed highly variable CCN and CN concentrations that ranged from lots than 5 per cubic cm to more than 1000 per Cubic cm over km scale distances within and around the open eye of this tropical storm/hurricane. These very low concentrations suggest strong cloud scavenging.

Bridging the condensation-collision size gap: a direct numerical simulation of continuous droplet growth in turbulent clouds

NASA Astrophysics Data System (ADS)

Chen, Sisi; Yau, Man-Kong; Bartello, Peter; Xue, Lulin

2018-05-01

In most previous direct numerical simulation (DNS) studies on droplet growth in turbulence, condensational growth and collisional growth were treated separately. Studies in recent decades have postulated that small-scale turbulence may accelerate droplet collisions when droplets are still small when condensational growth is effective. This implies that both processes should be considered simultaneously to unveil the full history of droplet growth and rain formation. This paper introduces the first direct numerical simulation approach to explicitly study the continuous droplet growth by condensation and collisions inside an adiabatic ascending cloud parcel. Results from the condensation-only, collision-only, and condensation-collision experiments are compared to examine the contribution to the broadening of droplet size distribution (DSD) by the individual process and by the combined processes. Simulations of different turbulent intensities are conducted to investigate the impact of turbulence on each process and on the condensation-induced collisions. The results show that the condensational process promotes the collisions in a turbulent environment and reduces the collisions when in still air, indicating a positive impact of condensation on turbulent collisions. This work suggests the necessity of including both processes simultaneously when studying droplet-turbulence interaction to quantify the turbulence effect on the evolution of cloud droplet spectrum and rain formation.

A Balloon-Borne Cloud Condensation Nuclei Counter

NASA Technical Reports Server (NTRS)

Delene, David J.; Deshler, Terry; Wechsler, Perry; Vali, Gabor A.

1997-01-01

A balloon-borne instrument was constructed for observations of vertical profiles of cloud condensation nucleus (CCN) concentrations, active at 1% supersaturation. Droplet concentration in the static thermal-gradient diffusion chamber is deduced from the amount of scattered laser light detected by a photodetector. The photodetector is calibrated using a video camera and computer system to count the number of droplets produced from NaCl aerosol. Preliminary data are available from nine early morning profiles obtained at Laramie, Wyoming, between June 1995 and January 1997. To complement the CCN measurements, instruments that measure condensation nuclei (CN) and aerosols with diameter greater than 0.30 micrometers (D(sub 0.3) were also included on the balloon package. CCN concentrations exhibited a general decrease from the surface to the top of the boundary layers, were generally uniform through well-mixed layers, and show variability above well-mixed layers. In general, the structure of the CCN profile appears to be closely related to the structure in the CN and D(sub 0.3) profiles. Summer profiles generally have CCN concentration greater than 200/cu cm up to 500 mbar, whereas winter profiles are less than 200/cu cm at all levels.

Planetary atmospheres program

NASA Technical Reports Server (NTRS)

1982-01-01

Non-solar compositional models of the troposphere of Jupiter, halide cloud condensation and volatile element inventories on Venus, and shock-wave processing of interstellar cloud materials are discussed.

Chinese SO2 pollution over Europe - Part 2: Simulation of aerosol and cloud condensation nuclei formation

NASA Astrophysics Data System (ADS)

Fiedler, V.; Arnold, F.; Schlager, H.; Pirjola, L.

2009-01-01

We report on sulfur dioxide (SO2) induced formation of aerosols and cloud condensation nuclei in an SO2 rich aged (9 days) pollution plume of Chinese origin, which we have detected at 5-7 km altitude during a research aircraft mission over the East Atlantic off the West coast of Ireland. Building on our measurements of SO2 and other trace gases along with plume trajectory simulations, we have performed model simulations of SO2 induced formation of gaseous sulfuric acid (GSA, H2SO4) followed by GSA induced formation and growth of aerosol particles. We find that efficient photochemical SO2 conversion to GSA took place in the plume followed by efficient formation and growth of H2SO4-H2O aerosol particles. Most particles reached sufficiently large sizes to act as cloud condensation nuclei whenever water vapor supersaturation exceeded 0.1-0.2%. As a consequence, smaller but more numerous cloud droplets are formed, which tend to increase the cloud albedo and to decrease the rainout efficiency. The detected plume represents an interesting example of the environmental impact of long range transport of fossil fuel combustion generated SO2.

Planetary atmospheres program

NASA Technical Reports Server (NTRS)

1982-01-01

Chemical and physical models of the Jovian subnebula are addressed. Halide cloud condensation and volatile element inventories on Venus and considered. Computation methods for isolated grain condensation behavior are examined.

The Impacts of an Observationally-Based Cloud Fraction and Condensate Overlap Parameterization on a GCM's Cloud Radiative Effect

NASA Technical Reports Server (NTRS)

Oreopoulos, Lazaros; Lee, Dongmin; Norris, Peter; Yuan, Tianle

2011-01-01

It has been shown that the details of how cloud fraction overlap is treated in GCMs has substantial impact on shortwave and longwave fluxes. Because cloud condensate is also horizontally heterogeneous at GCM grid scales, another aspect of cloud overlap should in principle also be assessed, namely the vertical overlap of hydrometeor distributions. This type of overlap is usually examined in terms of rank correlations, i.e., linear correlations between hydrometeor amount ranks of the overlapping parts of cloud layers at specific separation distances. The cloud fraction overlap parameter and the rank correlation of hydrometeor amounts can be both expressed as inverse exponential functions of separation distance characterized by their respective decorrelation lengths (e-folding distances). Larger decorrelation lengths mean that hydrometeor fractions and probability distribution functions have high levels of vertical alignment. An analysis of CloudSat and CALIPSO data reveals that the two aspects of cloud overlap are related and their respective decorrelation lengths have a distinct dependence on latitude that can be parameterized and included in a GCM. In our presentation we will contrast the Cloud Radiative Effect (CRE) of the GEOS-5 atmospheric GCM (AGCM) when the observationally-based parameterization of decorrelation lengths is used to represent overlap versus the simpler cases of maximum-random overlap and globally constant decorrelation lengths. The effects of specific overlap representations will be examined for both diagnostic and interactive radiation runs in GEOS-5 and comparisons will be made with observed CREs from CERES and CloudSat (2B-FLXHR product). Since the radiative effects of overlap depend on the cloud property distributions of the AGCM, the availability of two different cloud schemes in GEOS-5 will give us the opportunity to assess a wide range of potential cloud overlap consequences on the model's climate.

Cloud condensation nuclei droplet growth kinetics of ultrafine particles during anthropogenic nucleation events

NASA Astrophysics Data System (ADS)

Shantz, N. C.; Pierce, J. R.; Chang, R. Y.-W.; Vlasenko, A.; Riipinen, I.; Sjostedt, S.; Slowik, J. G.; Wiebe, A.; Liggio, J.; Abbatt, J. P. D.; Leaitch, W. R.

2012-02-01

Evolution of the cloud condensation nucleus (CCN) activity of 36 ± 4 nm diameter anthropogenic aerosol particles at a water supersaturation of 1.0 ± 0.1% is examined for particle nucleation and growth. During the early stages of one event, relatively few of the anthropogenic particles at 36 nm were CCN active and their growth rates by water condensation were delayed relative to ammonium sulphate particles. As the event progressed, the particle size distribution evolved to larger sizes and the relative numbers of particles at 36 nm that were CCN active increased until all the 36 nm particles were activating at the end of the event. Based on the chemistry of larger particles and the results from an aerosol chemical microphysics box model, the increase in CCN activity of the particles was most likely the result of the condensation of sulphate in this case. Despite the increased CCN activity, a delay was observed in the initial growth of these particles into cloud droplets, which persisted even when the aerosol was most CCN active later in the afternoon. Simulations show that the delay in water uptake is explained by a reduction of the mass accommodation coefficient assuming that the composition of the 36 nm particles is the same as the measured composition of the 60-100 nm particles.

Effect of the secondary organic aerosol coatings on black carbon water uptake, cloud condensation nuclei activity, and particle collapse

EPA Science Inventory

The ability of black carbon aerosols to absorb water and act as a cloud condensation nuclei (CCN) directly controls their lifetime in the atmosphere as well as their impact on cloud formation, thus impacting the earth’s climate. Black carbon emitted from most combustion pro...

The Exoplanet Cloud Atlas

NASA Astrophysics Data System (ADS)

Gao, Peter; Marley, Mark S.; Morley, Caroline; Fortney, Jonathan J.

2017-10-01

Clouds have been readily inferred from observations of exoplanet atmospheres, and there exists great variability in cloudiness between planets, such that no clear trend in exoplanet cloudiness has so far been discerned. Equilibrium condensation calculations suggest a myriad of species - salts, sulfides, silicates, and metals - could condense in exoplanet atmospheres, but how they behave as clouds is uncertain. The behavior of clouds - their formation, evolution, and equilibrium size distribution - is controlled by cloud microphysics, which includes processes such as nucleation, condensation, and evaporation. In this work, we explore the cloudy exoplanet phase space by using a cloud microphysics model to simulate a suite of cloud species ranging from cooler condensates such as KCl/ZnS, to hotter condensates like perovskite and corundum. We investigate how the cloudiness and cloud particle sizes of exoplanets change due to variations in temperature, metallicity, gravity, and cloud formation mechanisms, and how these changes may be reflected in current and future observations. In particular, we will evaluate where in phase space could cloud spectral features be observable using JWST MIRI at long wavelengths, which will be dependent on the cloud particle size distribution and cloud species.

Laser-filamentation-induced water condensation and snow formation in a cloud chamber filled with different ambient gases.

PubMed

Liu, Yonghong; Sun, Haiyi; Liu, Jiansheng; Liang, Hong; Ju, Jingjing; Wang, Tiejun; Tian, Ye; Wang, Cheng; Liu, Yi; Chin, See Leang; Li, Ruxin

2016-04-04

We investigated femtosecond laser-filamentation-induced airflow, water condensation and snow formation in a cloud chamber filled respectively with air, argon and helium. The mass of snow induced by laser filaments was found being the maximum when the chamber was filled with argon, followed by air and being the minimum with helium. We also discussed the mechanisms of water condensation in different gases. The results show that filaments with higher laser absorption efficiency, which result in higher plasma density, are beneficial for triggering intense airflow and thus more water condensation and precipitation.

Collocated observations of cloud condensation nuclei, particle size distributions, and chemical composition

NASA Astrophysics Data System (ADS)

Schmale, Julia; Henning, Silvia; Henzing, Bas; Keskinen, Helmi; Sellegri, Karine; Ovadnevaite, Jurgita; Bougiatioti, Aikaterini; Kalivitis, Nikos; Stavroulas, Iasonas; Jefferson, Anne; Park, Minsu; Schlag, Patrick; Kristensson, Adam; Iwamoto, Yoko; Pringle, Kirsty; Reddington, Carly; Aalto, Pasi; Äijälä, Mikko; Baltensperger, Urs; Bialek, Jakub; Birmili, Wolfram; Bukowiecki, Nicolas; Ehn, Mikael; Fjæraa, Ann Mari; Fiebig, Markus; Frank, Göran; Fröhlich, Roman; Frumau, Arnoud; Furuya, Masaki; Hammer, Emanuel; Heikkinen, Liine; Herrmann, Erik; Holzinger, Rupert; Hyono, Hiroyuki; Kanakidou, Maria; Kiendler-Scharr, Astrid; Kinouchi, Kento; Kos, Gerard; Kulmala, Markku; Mihalopoulos, Nikolaos; Motos, Ghislain; Nenes, Athanasios; O'Dowd, Colin; Paramonov, Mikhail; Petäjä, Tuukka; Picard, David; Poulain, Laurent; Prévôt, André Stephan Henry; Slowik, Jay; Sonntag, Andre; Swietlicki, Erik; Svenningsson, Birgitta; Tsurumaru, Hiroshi; Wiedensohler, Alfred; Wittbom, Cerina; Ogren, John A.; Matsuki, Atsushi; Yum, Seong Soo; Myhre, Cathrine Lund; Carslaw, Ken; Stratmann, Frank; Gysel, Martin

2017-03-01

Cloud condensation nuclei (CCN) number concentrations alongside with submicrometer particle number size distributions and particle chemical composition have been measured at atmospheric observatories of the Aerosols, Clouds, and Trace gases Research InfraStructure (ACTRIS) as well as other international sites over multiple years. Here, harmonized data records from 11 observatories are summarized, spanning 98,677 instrument hours for CCN data, 157,880 for particle number size distributions, and 70,817 for chemical composition data. The observatories represent nine different environments, e.g., Arctic, Atlantic, Pacific and Mediterranean maritime, boreal forest, or high alpine atmospheric conditions. This is a unique collection of aerosol particle properties most relevant for studying aerosol-cloud interactions which constitute the largest uncertainty in anthropogenic radiative forcing of the climate. The dataset is appropriate for comprehensive aerosol characterization (e.g., closure studies of CCN), model-measurement intercomparison and satellite retrieval method evaluation, among others. Data have been acquired and processed following international recommendations for quality assurance and have undergone multiple stages of quality assessment.

Aerosol partitioning between the interstitial and the condensed phase in mixed-phase clouds

NASA Astrophysics Data System (ADS)

Verheggen, Bart; Cozic, Julie; Weingartner, Ernest; Bower, Keith; Mertes, Stephan; Connolly, Paul; Gallagher, Martin; Flynn, Michael; Choularton, Tom; Baltensperger, Urs

2007-12-01

The partitioning of aerosol particles between the cloud and the interstitial phase (i.e., unactivated aerosol) has been investigated during several Cloud and Aerosol Characterization Experiments (CLACE-3, CLACE-3? and CLACE-4) conducted in winter and summer 2004 and winter 2005 at the high alpine research station Jungfraujoch (3580 m altitude, Switzerland). Ambient air was sampled using different inlets in order to determine the activated fraction of aerosol particles, FN, defined as the fraction of the total aerosol number concentration (with particle diameter dp > 100 nm) that has been incorporated into cloud particles. The liquid and ice water content of mixed-phase clouds were characterized by analyzing multiple cloud probes. The dependence of the activated fraction on several environmental factors is discussed on the basis of more than 900 h of in-cloud observations and parameterizations for key variables are given. FN is found to increase with increasing liquid water content and to decrease with increasing particle number concentration in liquid clouds. FN also decreases with increasing cloud ice mass fraction and with decreasing temperature from 0 to -25°C. The Wegener-Bergeron-Findeisen process probably contributed to this trend, since the presence of ice crystals causes liquid droplets to evaporate, thus releasing the formerly activated particles back into the interstitial phase. Ice nucleation could also have prevented additional cloud condensation nuclei from activating. The observed activation behavior has significant implications for our understanding of the indirect effect of aerosols on climate.

Clouds in GEOS-5

NASA Technical Reports Server (NTRS)

Bacmeister, Julio; Rienecker, Michele; Suarez, Max; Norris, Peter

2007-01-01

The GEOS-5 atmospheric model is being developed as a weather-and-climate capable model. It must perform well in assimilation mode as well as in weather and climate simulations and forecasts and in coupled chemistry-climate simulations. In developing GEOS-5, attention has focused on the representation of moist processes. The moist physics package uses a single phase prognostic condensate and a prognostic cloud fraction. Two separate cloud types are distinguished by their source: "anvil" cloud originates in detraining convection, and large-scale cloud originates in a PDF-based condensation calculation. Ice and liquid phases for each cloud type are considered. Once created, condensate and fraction from the anvil and statistical cloud types experience the same loss processes: evaporation of condensate and fraction, auto-conversion of liquid or mixed phase condensate, sedimentation of frozen condensate, and accretion of condensate by falling precipitation. The convective parameterization scheme is the Relaxed Arakawa-Schubert, or RAS, scheme. Satellite data are used to evaluate the performance of the moist physics packages and help in their tuning. In addition, analysis of and comparisons to cloud-resolving models such as the Goddard Cumulus Ensemble model are used to help improve the PDFs used in the moist physics. The presentation will show some of our evaluations including precipitation diagnostics.

Cloud Condensation Nuclei Measurements During the First Year of the ORACLES Study

NASA Astrophysics Data System (ADS)

Kacarab, M.; Howell, S. G.; Wood, R.; Redemann, J.; Nenes, A.

2016-12-01

Aerosols have significant impacts on air quality and climate. Their ability to scatter and absorb radiation and to act as cloud condensation nuclei (CCN) plays a very important role in the global climate. Biomass burning organic aerosol (BBOA) can drastically elevate the concentration of CCN in clouds, but the response in droplet number may be strongly suppressed (or even reversed) owing to low supersaturations that may develop from the strong competition of water vapor (Bougiatioti et al. 2016). Understanding and constraining the magnitude of droplet response to biomass burning plumes is an important component of the aerosol-cloud interaction problem. The southeastern Atlantic (SEA) cloud deck provides a unique opportunity to study these cloud-BBOA interactions for marine stratocumulus, as it is overlain by a large, optically thick biomass burning aerosol plume from Southern Africa during the burning season. The interaction between these biomass burning aerosols and the SEA cloud deck is being investigated in the NASA ObseRvations of Aerosols above Clouds and their intEractionS (ORACLES) study. The CCN activity of aerosol around the SEA cloud deck and associated biomass burning plume was evaluated during the first year of the ORACLES study with direct measurements of CCN concentration, aerosol size distribution and composition onboard the NASA P-3 aircraft during August and September of 2016. Here we present analysis of the observed CCN activity of the BBOA aerosol in and around the SEA cloud deck and its relationship to aerosol size, chemical composition, and plume mixing and aging. We also evaluate the predicted and observed droplet number sensitivity to the aerosol fluctuations and quantify, using the data, the drivers of droplet number variability (vertical velocity or aerosol properties) as a function of biomass burning plume characteristics.

Prebiotic chemistry in clouds

NASA Technical Reports Server (NTRS)

Oberbeck, Verne R.; Marshall, John; Shen, Thomas

1991-01-01

The chemical evolution hypothesis of Woese (1979), according to which prebiotic reactions occurred rapidly in droplets in giant atmospheric reflux columns was criticized by Scherer (1985). This paper proposes a mechanism for prebiotic chemistry in clouds that answers Scherer's concerns and supports Woese's hypothesis. According to this mechanism, rapid prebiotic chemical evolution was facilitated on the primordial earth by cycles of condensation and evaporation of cloud drops containing clay condensation nuclei and nonvolatile monomers. For example, amino acids supplied by, or synthesized during entry of meteorites, comets, and interplanetary dust, would have been scavenged by cloud drops containing clay condensation nuclei and would be polymerized within cloud systems during cycles of condensation, freezing, melting, and evaporation of cloud drops.

Response of Cloud Condensation Nuclei (> 50 nm) to changes in ion-nucleation

NASA Astrophysics Data System (ADS)

Pedersen, J. O.; Enghoff, M. B.; Svensmark, H.

2012-12-01

The role of ionization in the formation of clouds and aerosols has been debated for many years. A body of evidence exists that correlates cloud properties to galactic cosmic ray ionization; however these results are still contested. In recent years experimental evidence has also been produced showing that ionization can promote the nucleation of small aerosols at atmospheric conditions. The experiments showed that an increase in ionization leads to an increase in the formation of ultrafine aerosols (~3 nm), but in the real atmosphere such small particles have to grow by coagulation and condensation to become cloud condensation nuclei (CCN) in order to have an effect on clouds. However, numerical studies predict that variations in the count of ultra-fine aerosols will lead only to an insignificant change in the count of CCN. This is due to 1) the competition between the additional ultra-fine aerosols for the limited supply of condensable gases leading to a slower growth and 2) the increased loss rates of the additional particles during the longer growth-time. We investigated the growth of aerosols to CCN sizes using an 8 m3 reaction chamber made from electro-polished stainless steel. One side was fitted with a Teflon foil to allow ultraviolet light to illuminate the chamber, which was continuously flushed with dry purified air. Variable concentrations of water vapor, ozone, and sulfur dioxide could be added to the chamber. UV-lamps initiated photochemistry producing sulfuric acid. Ionization could be enhanced with two Cs-137 gamma sources (30 MBq), mounted on each side of the chamber. Figure 1 shows the evolution of the aerosols, following a nucleation event induced by the gamma sources. Previous to the event the aerosols were in steady state. Each curve represents a size bin: 3-10 nm (dark purple), 10-20 nm (purple), 20-30 nm (blue), 30-40 nm (light blue), 40-50 nm (green), 50-60 nm (yellow), and 60-68 nm (red). Black curves show a ~1 hour smoothing. The initial

Airborne observations of cloud condensation nuclei spectra and aerosols over East Inner Mongolia

NASA Astrophysics Data System (ADS)

Yang, Jiefan; Lei, Hengchi; Lü, Yuhuan

2017-08-01

A set of vertical profiles of aerosol number concentrations, size distributions and cloud condensation nuclei (CCN) spectra was observed using a passive cloud and aerosol spectrometer (PCASP) and cloud condensation nuclei counter, over the Tongliao area, East Inner Mongolia, China. The results showed that the average aerosol number concentration in this region was much lower than that in heavily polluted areas. Monthly average aerosol number concentrations within the boundary layer reached a maximum in May and a minimum in September, and the variations in CCN number concentrations at different supersaturations showed the same trend. The parameters c and k of the empirical function N = cS k were 539 and 1.477 under clean conditions, and their counterparts under polluted conditions were 1615 and 1.42. Measurements from the airborne probe mounted on a Yun-12 (Y12) aircraft, together with Hybrid Single-Particle Lagrangian Integrated Trajectory model backward trajectories indicated that the air mass from the south of Tongliao contained a high concentration of aerosol particles (1000-2500 cm-3) in the middle and lower parts of the troposphere. Moreover, detailed intercomparison of data obtained on two days in 2010 indicated that the activation efficiency in terms of the ratio of N CCN to N a (aerosols measured from PCASP) was 0.74 (0.4 supersaturations) when the air mass mainly came from south of Tongliao, and this value increased to 0.83 on the relatively cleaner day. Thus, long-range transport of anthropogenic pollutants from heavily polluted mega cities, such as Beijing and Tianjin, may result in slightly decreasing activation efficiencies.

Collocated observations of cloud condensation nuclei, particle size distributions, and chemical composition

PubMed Central

Schmale, Julia; Henning, Silvia; Henzing, Bas; Keskinen, Helmi; Sellegri, Karine; Ovadnevaite, Jurgita; Bougiatioti, Aikaterini; Kalivitis, Nikos; Stavroulas, Iasonas; Jefferson, Anne; Park, Minsu; Schlag, Patrick; Kristensson, Adam; Iwamoto, Yoko; Pringle, Kirsty; Reddington, Carly; Aalto, Pasi; Äijälä, Mikko; Baltensperger, Urs; Bialek, Jakub; Birmili, Wolfram; Bukowiecki, Nicolas; Ehn, Mikael; Fjæraa, Ann Mari; Fiebig, Markus; Frank, Göran; Fröhlich, Roman; Frumau, Arnoud; Furuya, Masaki; Hammer, Emanuel; Heikkinen, Liine; Herrmann, Erik; Holzinger, Rupert; Hyono, Hiroyuki; Kanakidou, Maria; Kiendler-Scharr, Astrid; Kinouchi, Kento; Kos, Gerard; Kulmala, Markku; Mihalopoulos, Nikolaos; Motos, Ghislain; Nenes, Athanasios; O’Dowd, Colin; Paramonov, Mikhail; Petäjä, Tuukka; Picard, David; Poulain, Laurent; Prévôt, André Stephan Henry; Slowik, Jay; Sonntag, Andre; Swietlicki, Erik; Svenningsson, Birgitta; Tsurumaru, Hiroshi; Wiedensohler, Alfred; Wittbom, Cerina; Ogren, John A.; Matsuki, Atsushi; Yum, Seong Soo; Myhre, Cathrine Lund; Carslaw, Ken; Stratmann, Frank; Gysel, Martin

2017-01-01

Cloud condensation nuclei (CCN) number concentrations alongside with submicrometer particle number size distributions and particle chemical composition have been measured at atmospheric observatories of the Aerosols, Clouds, and Trace gases Research InfraStructure (ACTRIS) as well as other international sites over multiple years. Here, harmonized data records from 11 observatories are summarized, spanning 98,677 instrument hours for CCN data, 157,880 for particle number size distributions, and 70,817 for chemical composition data. The observatories represent nine different environments, e.g., Arctic, Atlantic, Pacific and Mediterranean maritime, boreal forest, or high alpine atmospheric conditions. This is a unique collection of aerosol particle properties most relevant for studying aerosol-cloud interactions which constitute the largest uncertainty in anthropogenic radiative forcing of the climate. The dataset is appropriate for comprehensive aerosol characterization (e.g., closure studies of CCN), model-measurement intercomparison and satellite retrieval method evaluation, among others. Data have been acquired and processed following international recommendations for quality assurance and have undergone multiple stages of quality assessment. PMID:28291234

Use of In Situ Cloud Condensation Nuclei, Extinction, and Aerosol Size Distribution Measurements to Test a Method for Retrieving Cloud Condensation Nuclei Profiles From Surface Measurements

NASA Technical Reports Server (NTRS)

Ghan, Stephen J.; Rissman, Tracey A.; Ellman, Robert; Ferrare, Richard A.; Turner, David; Flynn, Connor; Wang, Jian; Ogren, John; Hudson, James; Jonsson, Haflidi H.;

Gravitationally Unstable Condensations Revealed by ALMA in the TUKH122 Prestellar Core in the Orion A Cloud

NASA Astrophysics Data System (ADS)

Ohashi, Satoshi; Sanhueza, Patricio; Sakai, Nami; Kandori, Ryo; Choi, Minho; Hirota, Tomoya; Nguyễn-Lu’o’ng, Quang; Tatematsu, Ken’ichi

2018-04-01

We have investigated the TUKH122 prestellar core in the Orion A cloud using ALMA 3 mm dust continuum, N2H+ (J = 1‑0), and CH3OH ({J}K={2}K-{1}K) molecular-line observations. Previous studies showed that TUKH122 is likely on the verge of star formation because the turbulence is almost dissipated and chemically evolved among other starless cores in the Orion A cloud. By combining ALMA 12 m and ACA data, we recover extended emission with a resolution of ∼5″ corresponding to 0.01 pc and identify six condensations with a mass range of 0.1–0.4 M ⊙ and a radius of ≲0.01 pc. These condensations are gravitationally bound following a virial analysis and are embedded in the filament, including the elongated core with a mass of ∼29 M ⊙ and a radial density profile of r ‑1.6 derived by Herschel. The separation of these condensations is ∼0.035 pc, consistent with the thermal Jeans length at a density of 4.4 × 105 cm‑3. This density is similar to the central part of the core. We also find a tendency for the N2H+ molecule to deplete at the dust peak condensation. This condensation may be beginning to collapse because the line width becomes broader. Therefore, the fragmentation still occurs in the prestellar core by thermal Jeans instability, and multiple stars are formed within the TUKH122 prestellar core. The CH3OH emission shows a large shell-like distribution and surrounds these condensations, suggesting that the CH3OH molecule formed on dust grains is released into the gas phase by nonthermal desorption such as photoevaporation caused by cosmic-ray-induced UV radiation.

Recent Findings Related to Giant Cloud Condensation Nuclei in the Marine Boundary Layer and Impacts on Clouds and Precipitation

NASA Astrophysics Data System (ADS)

Sorooshian, Armin; Dadashazar, Hossein; Wang, Zhen; Crosbie, Ewan; Brunke, Michael; Zeng, Xubin; Jonsson, Haflidi; Woods, Roy; Flagan, Richard; Seinfeld, John

2017-04-01

This presentation reports on findings from multiple airborne field campaigns off the California coast to understand the sources, nature, and impacts of giant cloud condensation nuclei (GCCN). Aside from sea spray emissions, measurements have revealed that ocean-going ships can be a source of GCCN due to wake and stack emissions off the California coast. Observed particle number concentrations behind 10 ships exceeded those in "control" areas, exhibiting number concentration enhancement ratios (ERs) for minimum threshold diameters of 2, 10, and 20 μm as high as 2.7, 5.5, and 7.5, respectively. The data provide insights into how ER is related to a variety of factors (downwind distance, altitude, ship characteristics such as gross tonnage, length, and beam). The data also provide insight into the extent to which a size distribution parameter and a cloud water chemical measurement can capture the effect of sea salt on marine stratocumulus cloud properties. The two GCCN proxy variables, near-surface particle number concentration for diameter > 5 µm and cloud water chloride concentration, are significantly correlated with each other, and both exhibit expected relationships with other parameters that typically coincide with sea salt emissions. Factors influencing the relationship between these two GCCN proxy measurements will be discussed. When comparing twelve pairs of high and low chloride cloud cases (at fixed liquid water path and cloud drop number concentration), the average drop spectra for high chloride cases exhibit enhanced drop number at diameters exceeding 20 µm, especially above 30 µm. In addition, high chloride cases coincide with enhanced mean columnar R and negative values of precipitation susceptibility. The difference in drop effective radius (re) between high and low chloride conditions decreases with height in cloud, suggesting that some GCCN-produced rain drops precipitate before reaching cloud tops. The sign of cloud responses (i.e., re, R) to

Fresh clouds: A parameterized updraft method for calculating cloud densities in one-dimensional models

NASA Astrophysics Data System (ADS)

Wong, Michael H.; Atreya, Sushil K.; Kuhn, William R.; Romani, Paul N.; Mihalka, Kristen M.

2015-01-01

Models of cloud condensation under thermodynamic equilibrium in planetary atmospheres are useful for several reasons. These equilibrium cloud condensation models (ECCMs) calculate the wet adiabatic lapse rate, determine saturation-limited mixing ratios of condensing species, calculate the stabilizing effect of latent heat release and molecular weight stratification, and locate cloud base levels. Many ECCMs trace their heritage to Lewis (Lewis, J.S. [1969]. Icarus 10, 365-378) and Weidenschilling and Lewis (Weidenschilling, S.J., Lewis, J.S. [1973]. Icarus 20, 465-476). Calculation of atmospheric structure and gas mixing ratios are correct in these models. We resolve errors affecting the cloud density calculation in these models by first calculating a cloud density rate: the change in cloud density with updraft length scale. The updraft length scale parameterizes the strength of the cloud-forming updraft, and converts the cloud density rate from the ECCM into cloud density. The method is validated by comparison with terrestrial cloud data. Our parameterized updraft method gives a first-order prediction of cloud densities in a “fresh” cloud, where condensation is the dominant microphysical process. Older evolved clouds may be better approximated by another 1-D method, the diffusive-precipitative Ackerman and Marley (Ackerman, A.S., Marley, M.S. [2001]. Astrophys. J. 556, 872-884) model, which represents a steady-state equilibrium between precipitation and condensation of vapor delivered by turbulent diffusion. We re-evaluate observed cloud densities in the Galileo Probe entry site (Ragent, B. et al. [1998]. J. Geophys. Res. 103, 22891-22910), and show that the upper and lower observed clouds at ∼0.5 and ∼3 bars are consistent with weak (cirrus-like) updrafts under conditions of saturated ammonia and water vapor, respectively. The densest observed cloud, near 1.3 bar, requires unexpectedly strong updraft conditions, or higher cloud density rates. The cloud

A Condensation–coalescence Cloud Model for Exoplanetary Atmospheres: Formulation and Test Applications to Terrestrial and Jovian Clouds

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ohno, Kazumasa; Okuzumi, Satoshi

A number of transiting exoplanets have featureless transmission spectra that might suggest the presence of clouds at high altitudes. A realistic cloud model is necessary to understand the atmospheric conditions under which such high-altitude clouds can form. In this study, we present a new cloud model that takes into account the microphysics of both condensation and coalescence. Our model provides the vertical profiles of the size and density of cloud and rain particles in an updraft for a given set of physical parameters, including the updraft velocity and the number density of cloud condensation nuclei (CCNs). We test our modelmore » by comparing with observations of trade-wind cumuli on Earth and ammonia ice clouds in Jupiter. For trade-wind cumuli, the model including both condensation and coalescence gives predictions that are consistent with observations, while the model including only condensation overestimates the mass density of cloud droplets by up to an order of magnitude. For Jovian ammonia clouds, the condensation–coalescence model simultaneously reproduces the effective particle radius, cloud optical thickness, and cloud geometric thickness inferred from Voyager observations if the updraft velocity and CCN number density are taken to be consistent with the results of moist convection simulations and Galileo probe measurements, respectively. These results suggest that the coalescence of condensate particles is important not only in terrestrial water clouds but also in Jovian ice clouds. Our model will be useful to understand how the dynamics, compositions, and nucleation processes in exoplanetary atmospheres affect the vertical extent and optical thickness of exoplanetary clouds via cloud microphysics.« less

Effects of cloud condensation nuclei and ice nucleating particles on precipitation processes and supercooled liquid in mixed-phase orographic clouds

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fan, Jiwen; Leung, L. Ruby; Rosenfeld, Daniel

How orographic mixed-phase clouds respond to the change in cloud condensation nuclei (CCN) and ice nucleating particles (INPs) are highly uncertain. The main snow production mechanism in warm and cold mixed-phase orographic clouds (referred to as WMOCs and CMOCs, respectively, distinguished here as those having cloud tops warmer and colder than -20°C) could be very different. We quantify the CCN and INP impacts on supercooled water content, cloud phases, and precipitation for a WMOC case and a CMOC case, with sensitivity tests using the same CCN and INP concentrations between the WMOC and CMOC cases. It was found that depositionmore » plays a more important role than riming for forming snow in the CMOC case, while the role of riming is dominant in the WMOC case. As expected, adding CCN suppresses precipitation, especially in WMOCs and low INPs. However, this reverses strongly for CCN of 1000 cm -3 and larger. We found a new mechanism through which CCN can invigorate mixed-phase clouds over the Sierra Nevada and drastically intensify snow precipitation when CCN concentrations are high (1000 cm -3 or higher). In this situation, more widespread shallow clouds with a greater amount of cloud water form in the Central Valley and foothills west of the mountain range. The increased latent heat release associated with the formation of these clouds strengthens the local transport of moisture to the windward slope, invigorating mixed-phase clouds over the mountains, and thereby producing higher amounts of snow precipitation. Under all CCN conditions, increasing the INPs leads to decreased riming and mixed-phase fraction in the CMOC as a result of liquid-limited conditions, but has the opposite effects in the WMOC as a result of ice-limited conditions. However, precipitation in both cases is increased by increasing INPs due to an increase in deposition for the CMOC but enhanced riming and deposition in the WMOC. Increasing the INPs dramatically reduces supercooled water

Effects of cloud condensation nuclei and ice nucleating particles on precipitation processes and supercooled liquid in mixed-phase orographic clouds

DOE PAGES

Fan, Jiwen; Leung, L. Ruby; Rosenfeld, Daniel; ...

2017-01-23

How orographic mixed-phase clouds respond to the change in cloud condensation nuclei (CCN) and ice nucleating particles (INPs) are highly uncertain. The main snow production mechanism in warm and cold mixed-phase orographic clouds (referred to as WMOCs and CMOCs, respectively, distinguished here as those having cloud tops warmer and colder than -20°C) could be very different. We quantify the CCN and INP impacts on supercooled water content, cloud phases, and precipitation for a WMOC case and a CMOC case, with sensitivity tests using the same CCN and INP concentrations between the WMOC and CMOC cases. It was found that depositionmore » plays a more important role than riming for forming snow in the CMOC case, while the role of riming is dominant in the WMOC case. As expected, adding CCN suppresses precipitation, especially in WMOCs and low INPs. However, this reverses strongly for CCN of 1000 cm -3 and larger. We found a new mechanism through which CCN can invigorate mixed-phase clouds over the Sierra Nevada and drastically intensify snow precipitation when CCN concentrations are high (1000 cm -3 or higher). In this situation, more widespread shallow clouds with a greater amount of cloud water form in the Central Valley and foothills west of the mountain range. The increased latent heat release associated with the formation of these clouds strengthens the local transport of moisture to the windward slope, invigorating mixed-phase clouds over the mountains, and thereby producing higher amounts of snow precipitation. Under all CCN conditions, increasing the INPs leads to decreased riming and mixed-phase fraction in the CMOC as a result of liquid-limited conditions, but has the opposite effects in the WMOC as a result of ice-limited conditions. However, precipitation in both cases is increased by increasing INPs due to an increase in deposition for the CMOC but enhanced riming and deposition in the WMOC. Increasing the INPs dramatically reduces supercooled water

Cloud condensation nuclei in Western Colorado: Observations and model predictions

NASA Astrophysics Data System (ADS)

Ward, Daniel Stewart

Variations in the warm cloud-active portion of atmospheric aerosols, or cloud condensation nuclei (CCN), have been shown to impact cloud droplet number concentration and subsequently cloud and precipitation processes. This issue carries special significance in western Colorado where a significant portion of the region's water resources is supplied by precipitation from winter season, orographic clouds, which are particularly sensitive to variations in CCN. Temporal and spatial variations in CCN in western Colorado were investigated using a combination of observations and a new method for modeling CCN. As part of the Inhibition of Snowfall by Pollution Aerosols (ISPA-III) field campaign, total particle and CCN number concentration were measured for a 24-day period in Mesa Verde National Park, climatologically upwind of the San Juan Mountains. These data were combined with CCN observations from Storm Peak Lab (SPL) in northwestern Colorado and from the King Air platform, flying north to south along the Western Slope. Altogether, the sampled aerosols were characteristic of a rural continental environment and the cloud-active portion varied slowly in time, and little in space. Estimates of the is hygroscopicity parameter indicated consistently low aerosol hygroscopicity typical of organic aerosol species. The modeling approach included the addition of prognostic CCN to the Regional Atmospheric Modeling System (RAMS). The RAMS droplet activation scheme was altered using parcel model simulations to include variations in aerosol hygroscopicity, represented by K. Analysis of the parcel model output and a supplemental sensitivity study showed that model CCN will be sensitive to changes in aerosol hygroscopicity, but only for conditions of low supersaturation or small particle sizes. Aerosol number, size distribution median radius, and hygroscopicity (represented by the K parameter) in RAMS were constrained by nudging to forecasts of these quantities from the Weather

A Numerical Study of Convection in a Condensing CO2 Atmosphere under Early Mars-Like Conditions

NASA Astrophysics Data System (ADS)

Nakajima, Kensuke; Yamashita, Tatsuya; Odaka, Masatsugu; Sugiyama, Ko-ichiro; Ishiwatari, Masaki; Nishizawa, Seiya; Takahashi, Yoshiyuki O.; Hayashi, Yoshi-Yuki

2017-10-01

Cloud convection of a CO2 atmosphere where the major constituent condenses is numerically investigated under a setup idealizing a possible warm atmosphere of early Mars, utilizing a two-dimensional cloud-resolving model forced by a fixed cooling profile as a substitute for a radiative process. The authors compare two cases with different critical saturation ratios as condensation criteria and also examine sensitivity to number mixing ratio of condensed particles given externally.When supersaturation is not necessary for condensation, the entire horizontal domain above the condensation level is continuously covered by clouds irrespective of number mixing ratio of condensed particles. Horizontal-mean cloud mass density decreases exponentially with height. The circulations below and above the condensation level are dominated by dry cellular convection and buoyancy waves, respectively.When 1.35 is adopted as the critical saturation ratio, clouds appear exclusively as intense, short-lived, quasi-periodic events. Clouds start just above the condensation level and develop upward, but intense updrafts exist only around the cloud top; they do not extend to the bottom of the condensation layer. The cloud layer is rapidly warmed by latent heat during the cloud events, and then the layer is slowly cooled by the specified thermal forcing, and supersaturation gradually develops leading to the next cloud event. The periodic appearance of cloud events does not occur when number mixing ratio of condensed particles is large.

Cohesive Energy-Lattice Constant and Bulk Modulus-Lattice Constant Relationships: Alkali Halides, Ag Halides, Tl Halides

NASA Technical Reports Server (NTRS)

Schlosser, Herbert

1992-01-01

In this note we present two expressions relating the cohesive energy, E(sub coh), and the zero pressure isothermal bulk modulus, B(sub 0), of the alkali halides. Ag halides and TI halides, with the nearest neighbor distances, d(sub nn). First, we show that the product E(sub coh)d(sub 0) within families of halide crystals with common crystal structure is to a good approximation constant, with maximum rms deviation of plus or minus 2%. Secondly, we demonstrate that within families of halide crystals with a common cation and common crystal structure the product B(sub 0)d(sup 3.5)(sub nn) is a good approximation constant, with maximum rms deviation of plus or minus 1.36%.

New particle formation events as a source for cloud condensation nuclei in an urban environment

NASA Astrophysics Data System (ADS)

Wonaschütz, Anna; Burkart, Julia; Wagner, Robert; Reischl, Georg; Steiner, Gerhard; Hitzenberger, Regina

2014-05-01

Nucleation and growth events have been observed in many remote, urban and rural environments. The new particles can contribute significantly to cloud condensation nuclei concentrations, after growing into the appropriate size range (Kerminen et al., 2012). Several studies have attempted to quantify this contribution (e.g. Asmi et al., 2011, Matsui et al., 2013), but only a limited number of them to date have used simultaneous measurements of CCN concentrations and particle size distributions for this purpose (e.g. Levin et al., 2012). In this study, a data set from an urban background station, consisting of 22 months of size distribution and 12 months of CCN concentration measurements (Burkart et al., 2011, Burkart et al., 2012) with 10 months of overlapping measurements is combined to explore the variability of CCN concentrations, their possible causes, and the contribution of nucleation and growth events to CCN concentrations. Consistent with observations in many other locations, nucleation and growth events occur on 30% of all days in spring and summer, on 11% of days in fall and on 4% of days in winter. This suggests a potentially large source of CCN from nucleation and growth events, particularly in the warm season. We acknowledge funding from FWF (Austrian Science Fund) P19515-N20 References: Asmi E., Kivekas, N., Kerminen, V. M., Komppula, M., Hyvarinen, A. P., Hatakka, J., Viisanen, Y., and Lihavainen, H.: Secondary new particle formation in Northern Finland Pallas site between the years 2000 and 2010, Atmos. Chem. Phys., 11, 12959-12972, doi: 10.5194/acp-11-12959-2011, 2011 Burkart J., Steiner, G., Reischl, G., and Hitzenberger, R.: Long-term study of cloud condensation nuclei (CCN) acticvation of the atmospheric aerosol in Vienna, Atmos. Environ., 45, 5751-5759, doi: 10.1016/j.atmosenv.2011.07.022, 2011. Burkart J., Hitzenberger, R., Reischl, G., Bauer, H., Leder, K., and Puxbaum, H.: Activation of "synthetic ambient" aerosols - relation to chemical

Shift Happens. How Halide Ion Defects Influence Photoinduced Segregation in Mixed Halide Perovskites

DOE PAGES

Yoon, Seog Joon; Kuno, Masaru; Kamat, Prashant V.

2017-06-01

Minimizing photoinduced segregation in mixed halide lead perovskites is important for achieving stable photovoltaic performance. The shift in the absorption and the rate of formation of iodide- and bromide-rich regions following visible excitation of mixed halide lead perovskites is found to strongly depend on the halide ion concentration. Slower formation and recovery rates observed in halide-deficient films indicate the involvement of defect sites in influencing halide phase segregation. At higher halide concentrations (in stoichiometric excess), segregation effects become less prominent, as evidenced by faster recovery kinetics. These results suggest that light-induced compositional segregation can be minimized in mixed halide perovskitemore » films by using excess halide ions. In conclusion, the findings from this study further reflect the importance of halide ion post-treatment of perovskite films to improve their solar cell performance.« less

Droplet Size Distributions as a function of rainy system type and Cloud Condensation Nuclei concentrations

NASA Astrophysics Data System (ADS)

Cecchini, Micael A.; Machado, Luiz A. T.; Artaxo, Paulo

2014-06-01

This work aims to study typical Droplet Size Distributions (DSDs) for different types of precipitation systems and Cloud Condensation Nuclei concentrations over the Vale do Paraíba region in southeastern Brazil. Numerous instruments were deployed during the CHUVA (Cloud processes of tHe main precipitation systems in Brazil: a contribUtion to cloud resolVing modeling and to the GPM) Project in Vale do Paraíba campaign, from November 22, 2011 through January 10, 2012. Measurements of CCN (Cloud Condensation Nuclei) and total particle concentrations, along with measurements of rain DSDs and standard atmospheric properties, including temperature, pressure and wind intensity and direction, were specifically made in this study. The measured DSDs were parameterized with a gamma function using the moment method. The three gamma parameters were disposed in a 3-dimensional space, and subclasses were classified using cluster analysis. Seven DSD categories were chosen to represent the different types of DSDs. The DSD classes were useful in characterizing precipitation events both individually and as a group of systems with similar properties. The rainfall regime classification system was employed to categorize rainy events as local convective rainfall, organized convection rainfall and stratiform rainfall. Furthermore, the frequencies of the seven DSD classes were associated to each type of rainy event. The rainfall categories were also employed to evaluate the impact of the CCN concentration on the DSDs. In the stratiform rain events, the polluted cases had a statistically significant increase in the total rain droplet concentrations (TDCs) compared to cleaner events. An average concentration increase from 668 cm- 3 to 2012 cm- 3 for CCN at 1% supersaturation was found to be associated with an increase of approximately 87 m- 3 in TDC for those events. For the local convection cases, polluted events presented a 10% higher mass weighted mean diameter (Dm) on average. For the

An uncertainty analysis for satellite-based estimates of cloud condensation nuclei number concentrations

NASA Astrophysics Data System (ADS)

Shinozuka, Y.; Clarke, A. D.; Nenes, A.; Jefferson, A.; Wood, R.; McNaughton, C. S.; Ström, J.; Tunved, P.; Redemann, J.; Thornhill, K. L., II; Moore, R.; Lathem, T. L.; Lin, J.; Yoon, Y. J.

2017-12-01

Aerosol-cloud interactions (ACI) are the largest source of uncertainty in estimates of anthropogenic radiative forcing responsible for the on-going climate change. ACI for warm clouds depend on the number concentration of cloud condensation nuclei (CCN), not on aerosol optical properties. Yet, aerosol optical depth (AOD) and its variants weighted by the spectral dependence over visible and near infrared wavelengths are commonly substituted for CCN in ACI studies. The substitution is motivated by the wide availability in space and time of satellite retrievals, an advantage over the sparse CCN measurements. If satellite-based CCN estimates are to continue to complement purely model-based ones, what CCN-AOD relationship should we assume and how large is the associated uncertainty? Our 2015 paper examines airborne and ground-based observations of aerosols to address these questions, focusing on the relationship between CCN and light extinction, σ, of dried particles averaged over one-kilometer horizontal distance. That paper discusses the way the CCN-AOD relationship is influenced not only by the CCN-σ relationship but also by the humidity response of light extinction, the vertical profile, the horizontal-temporal variability and the AOD measurement error. In this presentation, we apply these findings to passive satellite data to analyze the uncertainty in satellite-based CCN estimates.

Particles from a Diesel ship engine: Mixing state on the nano scale and cloud condensation abilities

NASA Astrophysics Data System (ADS)

Lieke, K. I.; Rosenørn, T.; Fuglsang, K.; Frederiksen, T.; Butcher, A. C.; King, S. M.; Bilde, M.

2012-04-01

Transport by ship plays an important role in global logistics. Current international policy initiatives by the International Maritime Organization (IMO) are taken to reduce emissions from ship propulsion systems (NO and SO, primarily). However, particulate emissions (e.g. soot) from ships are yet not regulated by legislations. To date, there is still a lack of knowledge regarding the global and local effects of the particulate matter emitted from ships at sea. Particles may influence the climate through their direct effects (scattering and absorption of long and shortwave radiation) and indirectly through formation of clouds. Many studies have been carried out estimating the mass and particle number from ship emissions (e.g. Petzold et al. 2008), many of them in test rig studies (e.g. Kasper et al. 2007). It is shown that particulate emissions vary with engine load and chemical composition of fuels. Only a few studies have been carried out to characterize the chemical composition and cloud-nucleating ability of the particulate matter (e.g. Corbett et al. 1997). In most cases, the cloud-nucleating ability of emission particles is estimated from number size distribution. We applied measurements to characterize particulate emissions from a MAN B&W Low Speed engine on test bed. A unique data set was obtained through the use of a scanning mobility particle sizing system (SMPS), combined with a cloud condensation nucleus (CCN) counter and a thermodenuder - all behind a dilution system. In addition, impactor samples were taken on nickel grids with carbon foil for use in an electron microscope (EM) to characterize the mineral phase and mixing state of the particles. The engine was operated at a series of different load conditions and an exhaust gas recirculation (EGR) system was applied. Measurements were carried out before and after the EGR system respectively. Our observations show significant changes in number size distribution and CCN activity with varying conditions

Global variability of cloud condensation nuclei concentrations

NASA Astrophysics Data System (ADS)

Makkonen, Risto; Krüger, Olaf

2017-04-01

Atmospheric aerosols can influence cloud optical and dynamical processes by acting as cloud condensation nuclei (CCN). Globally, these indirect aerosol effects are significant to the radiative budget as well as a source of high uncertainty in anthropogenic radiative forcing. While historically many global climate models have fixed CCN concentrations to a certain level, most state-of-the-art models calculate aerosol-cloud interactions with sophisticated methodologies based on interactively simulated aerosol size distributions. However, due to scarcity of atmospheric observations simulated global CCN concentrations remain poorly constrained. Here we assess global CCN variability with a climate model, and attribute potential trends during 2000-2010 to changes in emissions and meteorological fields. Here we have used ECHAM5.5-HAM2 with model M7 microphysical aerosol model. The model has been upgraded with a secondary organic aerosol (SOA) scheme including ELVOCs. Dust and sea salt emissions are calculated online, based on wind speed and hydrology. Each experiment is 11 years, analysed after a 6-month spin-up period. The MODIS CCN product (Terra platform) is used to evaluate model performance throughout 2000-2010. While optical remote observation of CCN column includes several deficiencies, the products serves as a proxy for changes during the simulation period. In our analysis we utilize the observed and simulated vertical column integrated CCN concentration, and limit our analysis only over marine regions. Simulated annual CCN column densities reach 2ṡ108 cm-2 near strong source regions in central Africa, Arabian Sea, Bay of Bengal and China sea. The spatial concentration gradient in CCN(0.2%) is steep, and column densities drop to <50% a few hundred kilometers away from the coasts. While the spatial distribution of CCN at 0.2% supersaturation is closer to that of MODIS proxy, as opposed to 1.0% supersaturation, the overall column integrated CCN are too low. Still

Two-stream Maxwellian kinetic theory of cloud droplet growth by condensation

NASA Technical Reports Server (NTRS)

Robinson, N. F.; Scott, W. T.

1981-01-01

A new growth rate formula (NGRF) is developed for the rate of growth of cloud droplets by condensation. The theory used is a modification of the Lees-Shankar theory in which the two-stream Maxwellian distribution function of Lees is used in Maxwell's method of moments to determine the transport of water vapor to and heat away from the droplet. Boundary conditions at the droplet are the usual conditions set in terms of accommodation coefficients, and the solution passes smoothly into diffusion flow in the far region. Comparisons are given between NGRF and the conventional formula showing close agreement (approximately 0.1%) for large radii with significant difference (approximately 5%) for small radii (not greater than 1 micron). Growth times for haze droplets in a Laktionov chamber are computed.

Improved Cloud Condensation Nucleus Spectrometer

NASA Technical Reports Server (NTRS)

Leu, Ming-Taun

2010-01-01

An improved thermal-gradient cloud condensation nucleus spectrometer (CCNS) has been designed to provide several enhancements over prior thermal- gradient counters, including fast response and high-sensitivity detection covering a wide range of supersaturations. CCNSs are used in laboratory research on the relationships among aerosols, supersaturation of air, and the formation of clouds. The operational characteristics of prior counters are such that it takes long times to determine aerosol critical supersaturations. Hence, there is a need for a CCNS capable of rapid scanning through a wide range of supersaturations. The present improved CCNS satisfies this need. The improved thermal-gradient CCNS (see Figure 1) incorporates the following notable features: a) The main chamber is bounded on the top and bottom by parallel thick copper plates, which are joined by a thermally conductive vertical wall on one side and a thermally nonconductive wall on the opposite side. b) To establish a temperature gradient needed to establish a supersaturation gradient, water at two different regulated temperatures is pumped through tubes along the edges of the copper plates at the thermally-nonconductive-wall side. Figure 2 presents an example of temperature and supersaturation gradients for one combination of regulated temperatures at the thermally-nonconductive-wall edges of the copper plates. c) To enable measurement of the temperature gradient, ten thermocouples are cemented to the external surfaces of the copper plates (five on the top plate and five on the bottom plate), spaced at equal intervals along the width axis of the main chamber near the outlet end. d) Pieces of filter paper or cotton felt are cemented onto the interior surfaces of the copper plates and, prior to each experimental run, are saturated with water to establish a supersaturation field inside the main chamber. e) A flow of monodisperse aerosol and a dilution flow of humid air are introduced into the main

Cold and transition season cloud condensation nuclei measurements in western Colorado

NASA Astrophysics Data System (ADS)

Ward, D. S.; Cotton, W. R.

2010-11-01

Recent research has shown that orographic precipitation and the water resources that depend on it in the Colorado Rocky Mountains are sensitive to the variability of the region's aerosols, whether emitted locally or from distant sources. However, observations of cloud-active aerosols in western Colorado, climatologically upwind of the Colorado Rocky Mountains, have been limited to a few studies at a single, northern site. To address this knowledge gap, atmospheric aerosols were sampled at a ground site in southwestern Colorado and in low-level north to south transects of the Colorado Western Slope as part of the Inhibition of Snowfall by Pollution Aerosols (ISPA-III) field campaign. Total particle and cloud condensation nuclei (CCN) number concentration were measured for a 24-day period in Mesa Verde National Park, climatologically upwind of the San Juan Mountains, in Sept. and Oct. 2009. Regression analysis showed a positive relationship between mid-troposphere atmospheric pressure to the west of the site and the total particle count at the ground site, but no similar statistically significant relationship for the observed CCN. These data were supplemented with particle and CCN number concentration, as well as particle size distribution measurements aboard the KingAir platform during December 2009. A CCN closure attempt was performed using the size distribution information and suggested that the sampled aerosol in general had low hygroscopicity that changed slightly with the large-scale wind direction. Together, the sampled aerosols from these field programs were characteristic of a rural continental environment with a cloud active portion that varied slowly in time, and little in space along the Western Slope.

The Effect of Carbon Dioxide (CO 2) Ice Cloud Condensation on the Habitable Zone

NASA Astrophysics Data System (ADS)

Lincowski, Andrew; Meadows, Victoria; Robinson, Tyler D.; Crisp, David

2016-10-01

The currently accepted outer limit of the habitable zone (OHZ) is defined by the "maximum greenhouse" limit, where Rayleigh scattering from additional CO2 gas overwhelms greenhouse warming. However, this long-standing definition neglects the radiative effects of CO2 clouds (Kopparapu, 2013); this omission was justified based on studies using the two-stream approximation, which found CO2 clouds to be highly likely to produce a net warming. However, recent comparisons of the radiative effect of CO2 clouds using both a two-stream and multi-stream radiative transfer model (Kitzmann et al, 2013; Kitzmann, 2016) found that the warming effect was reduced when the more sophisticated multi-stream models were used. In many cases CO2 clouds caused a cooling effect, meaning that their impact on climate could not be neglected when calculating the outer edge of the habitable zone. To better understand the impact of CO2 ice clouds on the OHZ, we have integrated CO2 cloud condensation into a versatile 1-D climate model for terrestrial planets (Robinson et al, 2012) that uses the validated multi-stream SMART radiative transfer code (Meadows & Crisp, 1996; Crisp, 1997) with a simple microphysical model. We present preliminary results on the habitable zone with self-consistent CO2 clouds for a range of atmospheric masses, compositions and host star spectra, and the subsequent effect on surface temperature. In particular, we evaluate the habitable zone for TRAPPIST-1d (Gillon et al, 2016) with a variety of atmospheric compositions and masses. We present reflectance and transit spectra of these cold terrestrial planets. We identify any consequences for the OHZ in general and TRAPPIST-1d in particular. This more comprehensive treatment of the OHZ could impact our understanding of the distribution of habitable planets in the universe, and provide better constraints for statistical target selection techniques, such as the habitability index (Barnes et al, 2015), for missions like JWST

Aerosol properties and their influences on surface cloud condensation nuclei during CAP-MBL and MC3E

NASA Astrophysics Data System (ADS)

Logan, T.; Dong, X.; Xi, B.

2016-12-01

Aerosol particles are of particular importance because of their influences on cloud development and precipitation processes over land and ocean. Aerosol physical and chemical properties and their ability to activate as cloud condensation nuclei (CCN) as well as influence CCN number concentration (NCCN) during the 2011 Midlatitude Continental Convective Clouds Experiment (MC3E) over the Southern Great Plains (SGP) region and the 2009-2010 Clouds, Aerosol, and Precipitation in the Marine Boundary Layer (CAP-MBL) over the Azores are presented in this study. Both regions periodically observe increases in NCCN when sulfate pollution and biomass burning smoke are present but over ocean, mineral dust diminishes NCCN. During clean conditions over the ocean, sea salt is the main contributor to CCN production, and strong (weak) surface winds and turbulent conditions can enhance (diminish) NCCN. Over the SGP, there were moderate to high correlations (R > 0.5) between increased magnitudes of aerosol loading (ssp), NCCN, chemical species, and PWV suggesting a shared common transport mechanism via the Gulf of Mexico further indicating the strong dependence on air mass type (e.g., marine vs. continental). Further investigations will greatly help to understand the seasonal influences of air masses on aerosol, NCCN, and cloud properties.

Substantial Seasonal Contribution of Observed Biogenic Sulfate Particles to Cloud Condensation Nuclei.

PubMed

Sanchez, Kevin J; Chen, Chia-Li; Russell, Lynn M; Betha, Raghu; Liu, Jun; Price, Derek J; Massoli, Paola; Ziemba, Luke D; Crosbie, Ewan C; Moore, Richard H; Müller, Markus; Schiller, Sven A; Wisthaler, Armin; Lee, Alex K Y; Quinn, Patricia K; Bates, Timothy S; Porter, Jack; Bell, Thomas G; Saltzman, Eric S; Vaillancourt, Robert D; Behrenfeld, Mike J

2018-02-19

Biogenic sources contribute to cloud condensation nuclei (CCN) in the clean marine atmosphere, but few measurements exist to constrain climate model simulations of their importance. The chemical composition of individual atmospheric aerosol particles showed two types of sulfate-containing particles in clean marine air masses in addition to mass-based Estimated Salt particles. Both types of sulfate particles lack combustion tracers and correlate, for some conditions, to atmospheric or seawater dimethyl sulfide (DMS) concentrations, which means their source was largely biogenic. The first type is identified as New Sulfate because their large sulfate mass fraction (63% sulfate) and association with entrainment conditions means they could have formed by nucleation in the free troposphere. The second type is Added Sulfate particles (38% sulfate), because they are preexisting particles onto which additional sulfate condensed. New Sulfate particles accounted for 31% (7 cm -3 ) and 33% (36 cm -3 ) CCN at 0.1% supersaturation in late-autumn and late-spring, respectively, whereas sea spray provided 55% (13 cm -3 ) in late-autumn but only 4% (4 cm -3 ) in late-spring. Our results show a clear seasonal difference in the marine CCN budget, which illustrates how important phytoplankton-produced DMS emissions are for CCN in the North Atlantic.

Are Organic Aerosols Good Cloud Condensation Nuclei?

NASA Astrophysics Data System (ADS)

Abbatt, J. P.; Broekhuizen, K.; Kumar, P. P.

2002-12-01

The ability of a set of organic-containing aerosols to act as cloud condensation nuclei has been measured in the laboratory using a thermal-gradient diffusion chamber operated at a fixed supersaturation. We observe that particles composed of soluble organics, such as malonic acid and adipic acid, activate at dry particle diameters in agreement with Kohler theory predications assuming the solutes are fully soluble and the droplet has the surface tension of water. Surprisingly, we also observe that sparingly soluble azelaic acid and cis-pinonic acid particles also activate, perhaps because they are being formed in a supersaturated, amorphous state or that their activation is aided by surface uptake of water. Mixed organic/ammonium sulfate particles have also been studied, and a range of behavior is observed. Soluble species such as malonic acid enhance activation through the vapour-pressure lowering effect whereas a thick coating of stearic acid on ammonium sulfate makes the particles totally inactive. Lastly, we have observed that pure oleic acid particles, which show no indication of activation when pure, can be activated after exposure to gas-phase ozone. The atmospheric implications of our results will be discussed. An interesting issue is the degree to which we can quantitatively model our results by assuming the surface tension of the growing droplet is that of water, i.e. without the need to invoke the surface-tension-lowering effect due to surface-active organics.

Estimation of the Cloud condensation nuclei concentration(CCN) and aerosol optical depth(AOD) relation in the Arctic region

NASA Astrophysics Data System (ADS)

Jung, C. H.; Yoon, Y. J.; Ahn, S. H.; Kang, H. J.; Gim, Y. T.; Lee, B. Y.

2017-12-01

Information of the spatial and temporal variations of cloud condensation nuclei (CCN) concentrations is important in estimating aerosol indirect effects. Generally, CCN aerosol is difficult to estimate using remote sensing methods. Although there are many CCN measurements data, extensive measurements of CCN are not feasible because of the complex nature of the operation and high cost, especially in the Arctic region. Thus, there have been many attempts to estimate CCN concentrations from more easily obtainable parameters such as aerosol optical depth (AOD) because AOD has the advantage of being readily observed by remote sensing from space by several sensors. For example, some form of correlation was derived between AOD and the number concentration of cloud condensation nuclei (CCN) through the comparison results from AERONET network and CCN measurements (Andreae 2009). In this study, a parameterization of CCN concentration as a function of AOD at 500 nm is given in the Arctic region. CCN data was collected during the period 2007-2013 at the Zeppelin observatory (78.91° N, 11.89° E, 474 masl). The AERONET network and MODIS AOD data are compared with ground measured CCN measurement and the relations between AOD and CCN are parameterized. The seasonal characteristics as well as long term trends are also considered. Through the measurement, CCN concentration remains high during spring because of aerosol transportation from the mid-latitudes, known as Arctic Haze. Lowest CCN number densities were observed during Arctic autumn and early winter when aerosol long-range transport into the Arctic is not effective and new particle formation ceases. The results show that the relation between AOD and CCN shows a different parameter depending on the seasonal aerosol and CCN characteristics. This seasonal different CCN-AOD relation can be interpreted as many physico-chemical aerosol properties including aerosol size distribution, composition. ReferenceAndreae, M. O. (2009

Cloud condensation nuclei closure study on summer arctic aerosol

NASA Astrophysics Data System (ADS)

Martin, M.; Chang, R. Y.-W.; Sierau, B.; Sjogren, S.; Swietlicki, E.; Abbatt, J. P. D.; Leck, C.; Lohmann, U.

2011-03-01

We present an aerosol - cloud condensation nuclei CCN) closure study on summer high Arctic aerosol based on measurements that were carried out in summer 2008 during the Arctic Summer Cloud Ocean Study (ASCOS) on board the Swedish ice breaker Oden. The data presented here were collected during a three-week time period in the pack ice (>85° N) when the icebreaker Oden was moored to an ice floe and drifted passively during the most biological active period into autumn freeze up conditions. CCN number concentrations were obtained using two CCN counters measuring at different supersaturations. The directly measured CCN number concentration is then compared with a CCN number concentration calculated using both bulk aerosol mass composition data from an aerosol mass spectrometer and aerosol number size distributions obtained from a differential mobility particle sizer, assuming κ-Köhler theory and an internally mixed aerosol. For the two highest measured supersaturations, 0.73 and 0.41%, closure could not be achieved with the investigated settings concerning hygroscopicity and density. The calculated CCN number concentration was always higher than the measured one. One possible explanation is that the smaller particles that activate at these supersaturations have a relative larger insoluble organic mass fraction and thus are less good CCN than the larger particles. At 0.20, 0.15 and 0.10% supersaturation, the measured CCN number can be represented with different parameters for the hygroscopicity and density of the particles. For the best agreement of the calculated CCNnumber concentration with the measured one the organic fraction of the aerosol needs to be nearly insoluble (қorg=0.02). However, this is not unambigious and қorg=0.2 is found as an upper limit at 0.1% supersaturation.

Peroxidative oxidation of halides catalysed by myeloperoxidase. Effect of fluoride on halide oxidation.

PubMed

Zgliczyński, J M; Stelmaszyńska, T; Olszowska, E; Krawczyk, A; Kwasnowska, E; Wróbel, J T

1983-01-01

It was found that all halides can compete with cyanide for binding with myeloperoxidase. The lower is the pH, the higher is the affinity of halides. The apparent dissociation constants (Kd) of myeloperoxidase-cyanide complex were determined in the presence of F-, Cl-, Br- and I- in the pH range of 4 to 7. In slightly acidic pH (4 - 6) fluoride and chloride exhibit a higher affinity towards the enzyme than bromide and iodide. Taking into account competition between cyanide and halides for binding with myeloperoxidase the dissociation constants of halide-myeloperoxidase complexes were calculated. All halides except fluoride can be oxidized by H2O2 in the presence of myeloperoxidase. However, since fluoride can bind with myeloperoxidase, it can competitively inhibit the oxidation of other halides. Fluoride was a competitive inhibitor with respect to other halides as well as to H2O2. Inhibition constants (Ki) for fluoride as a competitive inhibitor with respect to H2O2 increased from iodide oxidation through bromide to chloride oxidation.

Long-term observations of aerosol and cloud condensation nuclei concentrations in Barbados

NASA Astrophysics Data System (ADS)

Pöhlker, Mira L.; Klimach, Thomas; Krüger, Ovid O.; Hrabe de Angelis, Isabella; Ditas, Florian; Praß, Maria; Holanda, Bruna; Su, Hang; Weber, Bettina; Pöhlker, Christopher; Farrell, David A.; Stevens, Bjorn; Prospero, Joseph M.; Andreae, Meinrat O.; Pöschl, Ulrich

2017-04-01

Long-term observation of atmospheric aerosol and cloud condensation nuclei (CCN) concentrations has been conducted at the Ragged Point site in Barbados since August 2016. Ragged Point is a well-established station to monitor the transatlantic transport of Saharan dust outbreaks [1]. In the absence of dust plumes, it represents an ideal site to analyze the maritime boundary layer aerosol that is transported with the trade winds over the Atlantic towards Barbados [2,3]. Broad aerosol size distribution (10 nm to 10 µm) as well as size-resolved CCN measurements at 10 different supersaturations from 0.05 % to 0.84 % have been conducted. The continuous online analyses are supplemented by intensive sampling periods to probe specific aerosol properties with various offline techniques (i.e., microscopy and spectroscopy). Aerosol key properties from our measurements are compared with the continuous and in depth observation of cloud properties at Deebles Point, which is in close neighborhood to the Ragged Point site [2]. Moreover, our activities have been synchronized with the HALO-NARVAL-2 aircraft campaign in August 2016 that added further detailed information on shallow cumulus clouds, which are characteristic for the Atlantic trade winds and represent a crucial factor in the Earth climate system. Our measurements have the following two focal points: (i) We aim to obtain a detailed CCN climatology for the alternation of maritime and dust-impacted episodes at this unique coastal location. This study will complement our recent in-depth analysis for the long-term CCN variability at a remote rain forest location [4]. (ii) Furthermore, we aim to collect detailed information on the role of different aerosol populations on the properties of the climatically important shallow cumulus clouds. References: [1] Prospero, J. M., Collard, F. X., Molinie, J., Jeannot, A. (2014), Global Biogeochemical Cycles, 28, 757-773. [2] Stevens, B., et al. (2016), Bulletin of the American

Global synthesis of long-term cloud condensation nuclei observations

NASA Astrophysics Data System (ADS)

Schmale, Julia; Henning, Silvia; Stratmann, Frank; Henzing, Bas; Schlag, Patrick; Aalto, Pasi; Keskinen, Helmi; Sellegri, Karine; Ovadnevaite, Jurgita; Krüger, Mira; Jefferson, Anne; Whitehead, James; Carslaw, Ken; Yum, Seong Soo; Kristensson, Adam; Baltensperger, Urs; Gysel, Martin

2016-04-01

Cloud condensation nuclei (CCN) are aerosol particles with the ability to activate into droplets at a given super saturation and therefore influence the microphysical and optical properties of clouds. To predict cloud radiative properties understanding the spatial and temporal variability of CCN concentrations in different environments is important. However, currently, the effects of atmospheric particles on changes in cloud radiative forcing are still the largest contribution of uncertainty in climate forcing prediction (IPCC, 2013). Numerous intensive field campaigns have already explored detailed characteristics of CCN in many locations around the world. However, these rather short-term observations can generally not address seasonal or inter-annual variations and a comparison between campaign sites is difficult due to the higher influence of specific environmental circumstances on short-term measurements results. Here, we present results of more long-term CCN and aerosol number concentrations as well as size distribution data covering at least one full year between 2006 and 2014. The 12 locations include ACTRIS stations (http://www.actris.net/) in Europe, and further sites in North America, Brazil and Korea. The sites are located in different environments allowing for temporal and spatial characterization of CCN variability in different atmospheric regimes. Those include marine, remote-continental, boreal forest, rain forest, Arctic and monsoon-influenced environments, as well as boundary layer and free tropospheric conditions. The aerosol populations and their activation behavior show significant differences across the stations. While peak concentrations of CCN are observed in summer at the high altitude sites, in the Arctic the highest concentrations occur during the Haze period in spring. The rural-marine and rural-continental sites exhibit similar CCN concentration characteristics with a relatively flat annual cycle. At some stations, e.g. in the boreal

Cloud Microphysics Budget in the Tropical Deep Convective Regime

NASA Technical Reports Server (NTRS)

Li, Xiao-Fan; Sui, C.-H.; Lau, K.-M.; Einaudi, Franco (Technical Monitor)

2001-01-01

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.

Clouds Composition in Super-Earth Atmospheres: Chemical Equilibrium Calculations

NASA Astrophysics Data System (ADS)

Kempton, Eliza M.-R.; Mbarek, Rostom

2015-12-01

Attempts to determine the composition of super-Earth atmospheres have so far been plagued by the presence of clouds. Yet the theoretical framework to understand these clouds is still in its infancy. For the super-Earth archetype GJ 1214b, KCl, Na2S, and ZnS have been proposed as condensates that would form under the condition of chemical equilibrium, if the planet’s atmosphere has a bulk composition near solar. Condensation chemistry calculations have not been presented for a wider range of atmospheric bulk composition that is to be expected for super-Earth exoplanets. Here we provide a theoretical context for the formation of super-Earth clouds in atmospheres of varied composition by determining which condensates are likely to form, under the assumption of chemical equilibrium. We model super-Earth atmospheres assuming they are formed by degassing of volatiles from a solid planetary core of chondritic material. Given the atomic makeup of these atmospheres, we minimize the global Gibbs free energy of over 550 gases and condensates to obtain the molecular composition of the atmospheres over a temperature range of 350-3,000 K. Clouds should form along the temperature-pressure boundaries where the condensed species appear in our calculations. The super-Earth atmospheres that we study range from highly reducing to oxidizing and have carbon to oxygen (C:O) ratios that are both sub-solar and super-solar, thereby spanning a diverse range of atmospheric composition that is appropriate for low-mass exoplanets. Some condensates appear across all of our models. However, the majority of condensed species appear only over specific ranges of H:O and C:O ratios. We find that for GJ 1214b, KCl is the primary cloud-forming condensate at solar composition, in agreement with previous work. However, for oxidizing atmospheres, where H:O is less than unity, K2SO4 clouds form instead. For carbon-rich atmospheres with super-solar C:O ratios, graphite clouds additionally appear. At

CLOUDS IN SUPER-EARTH ATMOSPHERES: CHEMICAL EQUILIBRIUM CALCULATIONS

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mbarek, Rostom; Kempton, Eliza M.-R., E-mail: mbarekro@grinnell.edu, E-mail: kemptone@grinnell.edu

Recent studies have unequivocally proven the existence of clouds in super-Earth atmospheres. Here we provide a theoretical context for the formation of super-Earth clouds by determining which condensates are likely to form under the assumption of chemical equilibrium. We study super-Earth atmospheres of diverse bulk composition, which are assumed to form by outgassing from a solid core of chondritic material, following Schaefer and Fegley. The super-Earth atmospheres that we study arise from planetary cores made up of individual types of chondritic meteorites. They range from highly reducing to oxidizing and have carbon to oxygen (C:O) ratios that are both sub-solarmore » and super-solar, thereby spanning a range of atmospheric composition that is appropriate for low-mass exoplanets. Given the atomic makeup of these atmospheres, we minimize the global Gibbs free energy of formation for over 550 gases and condensates to obtain the molecular composition of the atmospheres over a temperature range of 350–3000 K. Clouds should form along the temperature–pressure boundaries where the condensed species appear in our calculation. We find that the composition of condensate clouds depends strongly on both the H:O and C:O ratios. For the super-Earth archetype GJ 1214b, KCl and ZnS are the primary cloud-forming condensates at solar composition, in agreement with previous work. However, for oxidizing atmospheres, K{sub 2}SO{sub 4} and ZnO condensates are favored instead, and for carbon-rich atmospheres with super-solar C:O ratios, graphite clouds appear. For even hotter planets, clouds form from a wide variety of rock-forming and metallic species.« less

Clouds in Super-Earth Atmospheres: Chemical Equilibrium Calculations

NASA Astrophysics Data System (ADS)

Mbarek, Rostom; Kempton, Eliza M.-R.

2016-08-01

Recent studies have unequivocally proven the existence of clouds in super-Earth atmospheres. Here we provide a theoretical context for the formation of super-Earth clouds by determining which condensates are likely to form under the assumption of chemical equilibrium. We study super-Earth atmospheres of diverse bulk composition, which are assumed to form by outgassing from a solid core of chondritic material, following Schaefer & Fegley. The super-Earth atmospheres that we study arise from planetary cores made up of individual types of chondritic meteorites. They range from highly reducing to oxidizing and have carbon to oxygen (C:O) ratios that are both sub-solar and super-solar, thereby spanning a range of atmospheric composition that is appropriate for low-mass exoplanets. Given the atomic makeup of these atmospheres, we minimize the global Gibbs free energy of formation for over 550 gases and condensates to obtain the molecular composition of the atmospheres over a temperature range of 350-3000 K. Clouds should form along the temperature-pressure boundaries where the condensed species appear in our calculation. We find that the composition of condensate clouds depends strongly on both the H:O and C:O ratios. For the super-Earth archetype GJ 1214b, KCl and ZnS are the primary cloud-forming condensates at solar composition, in agreement with previous work. However, for oxidizing atmospheres, K2SO4 and ZnO condensates are favored instead, and for carbon-rich atmospheres with super-solar C:O ratios, graphite clouds appear. For even hotter planets, clouds form from a wide variety of rock-forming and metallic species.

Aerosol effects on cloud water amounts were successfully simulated by a global cloud-system resolving model.

PubMed

Sato, Yousuke; Goto, Daisuke; Michibata, Takuro; Suzuki, Kentaroh; Takemura, Toshihiko; Tomita, Hirofumi; Nakajima, Teruyuki

2018-03-07

Aerosols affect climate by modifying cloud properties through their role as cloud condensation nuclei or ice nuclei, called aerosol-cloud interactions. In most global climate models (GCMs), the aerosol-cloud interactions are represented by empirical parameterisations, in which the mass of cloud liquid water (LWP) is assumed to increase monotonically with increasing aerosol loading. Recent satellite observations, however, have yielded contradictory results: LWP can decrease with increasing aerosol loading. This difference implies that GCMs overestimate the aerosol effect, but the reasons for the difference are not obvious. Here, we reproduce satellite-observed LWP responses using a global simulation with explicit representations of cloud microphysics, instead of the parameterisations. Our analyses reveal that the decrease in LWP originates from the response of evaporation and condensation processes to aerosol perturbations, which are not represented in GCMs. The explicit representation of cloud microphysics in global scale modelling reduces the uncertainty of climate prediction.

Cloud condensation nuclei activation of limited solubility organic aerosol

NASA Astrophysics Data System (ADS)

Huff Hartz, Kara E.; Tischuk, Joshua E.; Chan, Man Nin; Chan, Chak K.; Donahue, Neil M.; Pandis, Spyros N.

The cloud condensation nuclei (CCN) activation of 19 organic species with water solubilities ( Csat) ranging from 10 -4 to 10 2 g solute 100 g -1 H 2O was measured. The organic particles were generated by nebulization of an aqueous or an alcohol solution. Use of alcohols as solvents enables the measurement of low solubility, non-volatile organic CCN activity and reduces the likelihood of residual water in the aerosol. The activation diameter of organic species with very low solubility in water ( Csat<0.3 g 100 g -1 H 2O) is in agreement with Köhler theory using the bulk solubility (limited solubility case) of the organic in water. Many species, including 2-acetylbenzoic acid, aspartic acid, azelaic acid, glutamic acid, homophthalic acid, phthalic acid, cis-pinonic acid, and salicylic acid are highly CCN active in spite of their low solubility (0.3 g 100 g -1 H 2O< Csat<1 g 100 g -1 H 2O), and activate almost as if completely water soluble. The CCN activity of most species is reduced, if the particles are produced using non-aqueous solvents. The existence of the particles in a metastable state at low RH can explain the observed enhancement in CCN activity beyond the levels suggested by their solubility.

Calibration Uncertainties in the Droplet Measurement Technologies Cloud Condensation Nuclei Counter

NASA Astrophysics Data System (ADS)

Hibert, Kurt James

Cloud condensation nuclei (CCN) serve as the nucleation sites for the condensation of water vapor in Earth's atmosphere and are important for their effect on climate and weather. The influence of CCN on cloud radiative properties (aerosol indirect effect) is the most uncertain of quantified radiative forcing changes that have occurred since pre-industrial times. CCN influence the weather because intrinsic and extrinsic aerosol properties affect cloud formation and precipitation development. To quantify these effects, it is necessary to accurately measure CCN, which requires accurate calibrations using a consistent methodology. Furthermore, the calibration uncertainties are required to compare measurements from different field projects. CCN uncertainties also aid the integration of CCN measurements with atmospheric models. The commercially available Droplet Measurement Technologies (DMT) CCN Counter is used by many research groups, so it is important to quantify its calibration uncertainty. Uncertainties in the calibration of the DMT CCN counter exist in the flow rate and supersaturation values. The concentration depends on the accuracy of the flow rate calibration, which does not have a large (4.3 %) uncertainty. The supersaturation depends on chamber pressure, temperature, and flow rate. The supersaturation calibration is a complex process since the chamber's supersaturation must be inferred from a temperature difference measurement. Additionally, calibration errors can result from the Kohler theory assumptions, fitting methods utilized, the influence of multiply-charged particles, and calibration points used. In order to determine the calibration uncertainties and the pressure dependence of the supersaturation calibration, three calibrations are done at each pressure level: 700, 840, and 980 hPa. Typically 700 hPa is the pressure used for aircraft measurements in the boundary layer, 840 hPa is the calibration pressure at DMT in Boulder, CO, and 980 hPa is the

Partially soluble organics as cloud condensation nuclei: Role of trace soluble and surface active species

NASA Astrophysics Data System (ADS)

Broekhuizen, K.; Kumar, P. Pradeep; Abbatt, J. P. D.

2004-01-01

The ability of partially soluble organic species to act as cloud condensation nuclei (CCN) has been studied. A Köhler model incorporating solute solubility and droplet surface tension describes the behavior of solid adipic and succinic acid particles, whereas solid azelaic acid activates much more efficiently that predicted. In addition, it was shown that trace levels of either sulfate or surface active species have a dramatic effect on the activation of adipic acid, a moderately soluble organic, as predicted by the full Köhler model. For internally mixed particles in the atmosphere, these effects will greatly enhance the role of organic aerosols as CCN.

Cold and transition season cloud condensation nuclei measurements in western Colorado

NASA Astrophysics Data System (ADS)

Ward, D. S.; Cotton, W. R.

2011-05-01

Recent studies have shown that orographic precipitation and the water resources that depend on it in the Colorado Rocky Mountains are sensitive to the variability of the region's aerosols, whether emitted locally or from distant sources. However, observations of cloud droplet nucleating aerosols in western Colorado, climatologically upwind of the Colorado Rocky Mountains, have been limited to a few studies at a single, northern site. To address this knowledge gap, atmospheric aerosols were sampled at a ground site in southwestern Colorado and in low-level north to south transects of the Colorado Western Slope as part of the Inhibition of Snowfall by Pollution Aerosols (ISPA-III) field campaign. Total particle and cloud condensation nuclei (CCN) number concentrations were measured for a 24-day period in Mesa Verde National Park, in September and October 2009. Regression analysis showed a positive relationship between mid-troposphere atmospheric pressure to the west of the site and the total particle count at the ground site, but no similar statistically significant relationship was found for the observed CCN. These data were supplemented with particle and CCN number concentration, as well as particle size distribution measurements collected aboard the King Air platform during December 2009. A CCN closure attempt was performed and suggested that the sampled aerosol may have had a low hygroscopicity that changed little with the large-scale wind direction. Together, the sampled aerosols from these field programs were characteristic of a rural continental environment with CCN number concentrations that varied slowly in time, and little in space along the Western Slope.

Aerosol-cloud interactions in mixed-phase convective clouds - Part 1: Aerosol perturbations

NASA Astrophysics Data System (ADS)

Miltenberger, Annette K.; Field, Paul R.; Hill, Adrian A.; Rosenberg, Phil; Shipway, Ben J.; Wilkinson, Jonathan M.; Scovell, Robert; Blyth, Alan M.

2018-03-01

Changes induced by perturbed aerosol conditions in moderately deep mixed-phase convective clouds (cloud top height ˜ 5 km) developing along sea-breeze convergence lines are investigated with high-resolution numerical model simulations. The simulations utilise the newly developed Cloud-AeroSol Interacting Microphysics (CASIM) module for the Unified Model (UM), which allows for the representation of the two-way interaction between cloud and aerosol fields. Simulations are evaluated against observations collected during the COnvective Precipitation Experiment (COPE) field campaign over the southwestern peninsula of the UK in 2013. The simulations compare favourably with observed thermodynamic profiles, cloud base cloud droplet number concentrations (CDNC), cloud depth, and radar reflectivity statistics. Including the modification of aerosol fields by cloud microphysical processes improves the correspondence with observed CDNC values and spatial variability, but reduces the agreement with observations for average cloud size and cloud top height. Accumulated precipitation is suppressed for higher-aerosol conditions before clouds become organised along the sea-breeze convergence lines. Changes in precipitation are smaller in simulations with aerosol processing. The precipitation suppression is due to less efficient precipitation production by warm-phase microphysics, consistent with parcel model predictions. In contrast, after convective cells organise along the sea-breeze convergence zone, accumulated precipitation increases with aerosol concentrations. Condensate production increases with the aerosol concentrations due to higher vertical velocities in the convective cores and higher cloud top heights. However, for the highest-aerosol scenarios, no further increase in the condensate production occurs, as clouds grow into an upper-level stable layer. In these cases, the reduced precipitation efficiency (PE) dominates the precipitation response and no further

Structure and chemistry in the northwestern condensation of the Serpens molecular cloud core

NASA Technical Reports Server (NTRS)

Mcmullin, Joseph P.; Mundy, Lee G.; Wilking, Bruce A.; Hezel, T.; Blake, Geoff A.

1994-01-01

We present single-dish and interferometric observations of gas and dust in the core of the Serpens molecular cloud, focusing on the northwestern condensation. Single-dish molecular line observations are used to probe the structure and chemistry of the condensation while high-resolution images of CS and CH30H are combined with continuum observations from lambda = 1.3 mm to lambda = 3.5 cm to study the subcondensations and overall distribution of dust. For the northwestern condensation, we derive a characteristic density of 3 x 10(exp 5)/ cu cm and an estimated total mass of approximately 70 solar mass. We find compact molecular emission associated with the far-infrared source S68 FIRS 1, and with a newly detected subcondensation named S68 N. Comparison of the large-and small-scale emission reveals that most of the material in the northwest condensation is not directly associated with these compact sources, suggesting a youthful age for this region. CO J = 1 approaches 0 observations indicate widespread outflow activity. However, no unique association of embedded objects with outflows is possible with our observations. The SiO emission is found to be extended with the overall emission centered about S68 FIRS 1; the offset of the peak emission from all of the known continuum sources and the coincidence between the blueshifted SiO emission and blueshifted high-velocity gas traced by CO and CS is consistent with formation of SiO in shocks. Derived abundances of CO and HCO(+) are consistent with quiescent and other star-forming regions while CS, HCN, and H2CO abundances indicate mild depletions within the condensation. Spectral energy distribution fits to S68 FIRS 1 indicate a modest luminosity (50-60 solar luminosity), implying that it is a low-mass (0.5-3 solar mass) young stellar object. Radio continuum observations of the triple source toward S68 FIRS 1 indicate that the lobe emission is varying on timescales less than or equal to 1 yr while the central component is

Stratus Cloud Radiative Effects from Cloud Processed Bimodal CCN Distributions

NASA Astrophysics Data System (ADS)

Noble, S. R., Jr.; Hudson, J. G.

2016-12-01

Inability to understand cloud processes is a large component of climate uncertainty. Increases in cloud condensation nuclei (CCN) concentrations are known to increase cloud droplet number concentrations (Nc). This aerosol-cloud interaction (ACI) produces greater Nc at smaller sizes, which brightens clouds. A lesser understood ACI is cloud processing of CCN. This improves CCN that then more easily activate at lower cloud supersaturations (S). Bimodal CCN distributions thus ensue from these evaporated cloud droplets. Hudson et al. (2015) related CCN bimodality to Nc. In stratus clouds, bimodal CCN created greater Nc whereas in cumulus less Nc. Thus, CCN distribution shape influences cloud properties; microphysics and radiative properties. Measured uni- and bimodal CCN distributions were input into an adiabatic droplet growth model using various specified vertical wind speeds (W). Bimodal CCN produced greater Nc (Fig. 1a) and smaller mean diameters (MD; Fig. 1b) at lower W typical of stratus clouds (<70 cm/s). Improved CCN (low critical S) were more easily activated at the lower S of stratus from low W, thus, creating greater Nc. Competition for condensate thus reduced MD and drizzle. At greater W, typical of cumulus clouds (>70 cm/s), bimodal CCN made lower Nc with larger MD thus enhancing drizzle whereas unimodal CCN made greater Nc with smaller MD, thus reducing drizzle. Thus, theoretical predictions of Nc and MD for uni- and bimodal CCN agree with the sense of the observations. Radiative effects were determined using a cloud grown to a 250-meter thickness. Bimodal CCN at low W reduced cloud effective radius (re), made greater cloud optical thickness (COT), and made greater cloud albedo (Fig. 1c). At very low W changes were as much as +9% for albedo, +17% for COT, and -12% for re. Stratus clouds typically have low W and cover large areas. Thus, these changes in cloud radiative properties at low W impact climate. Stratus cloud susceptibility to CCN distribution thus

Cloud condensation nucleus activity of internally mixed ammonium sulfate/organic acid aerosol particles

NASA Astrophysics Data System (ADS)

Abbatt, J. P. D.; Broekhuizen, K.; Pradeep Kumar, P.

The ability of mixed ammonium sulfate/organic acid particles to act as cloud condensation nuclei (CCN) has been studied in the laboratory using a continuous flow, thermal-gradient diffusion chamber operated at supersaturations between 0.3% and 0.6%. The organic acids studied were malonic acid, azelaic acid, hexanoic acid, cis-pinonic acid, oleic acid and stearic acid, and the particles were largely prepared by condensation of the organic vapor onto a dry ammonium sulfate core. For malonic acid and hexanoic acid, the mixed particles activated as predicted by a simple Köhler theory model where both species are assumed to be fully soluble and the droplet has the surface tension of water. Three low-solubility species, cis-pinonic acid, azelaic acid and oleic acid, are well modeled where the acid was assumed to be either partially or fully insoluble. Interestingly, although thin coats of stearic acid behaved in a manner similar to that displayed by oleic and cis-pinonic acid, we observed that thick coats led to a complete deactivation of the ammonium sulfate, presumably because the water vapor could not diffuse through the solid stearic acid. We observed no CCN behavior that could be clearly attributed to a lowering of the surface tension of the growing droplet by the presence of the organic constituents, some of which are highly surface active.

Microphysical Model Studies of Venus Clouds

NASA Astrophysics Data System (ADS)

Meade, P. E.; Bullock, M. A.; Grinspoon, D. H.

2004-11-01

We have adapted a standard cloud microphysics model to construct a self-consistent microphysical model of Venus' cloud layer which reproduces and extends previous studies (e.g. James et al. 1997). Our model is based on the Community Aerosol and Radiation Model Atmosphere (CARMA), which is a widely used computer code for terrestrial cloud microphysics, derived from the work of Toon et al. (1988). The standard code has been adapted to treat H2O and H2SO4 as co-condensing vapor species onto aqueous H2SO4 cloud droplets, as well as the nucleation of condensation nuclei to droplets. Vapor condensation and evaporation follows the method of James et al. (1997). Microphysical processes included in this model include nucleation of condensation nuclei, condensation and evaporation of H2O and H2SO4 vapor, and droplet coagulation. Vertical transport occurs though advection, eddy diffusion, sedimentation for both droplets and condensation nuclei. The cloud model is used to explore the sensitivity of Venus' cloud layer to environmental changes. Observations of the Venus' lower cloud from the Pioneer Venus, Venera, and Galileo spacecraft have suggested that the properties of the lower cloud may be time-variable, and at times may be entirely absent (Carlson et al. 1993, Grinspoon et al. 1993, Esposito et al. 1997). Our model explores the dependence of such behavior on environment factors such as variations in water or SO2 abundance. We have also calculated the optical properties of the model atmosphere using both the conventional optical constants for H2SO4 (Palmer and Williams, 1975), and the new data of Tisdale et al. (1998). This work has been supported by NASA's Exobiology Program. References Carlson, R.W., et al., 1993. Planetary and Space Science, 41, 477-486. Esposito, L.W., et al., 1997. In Venus II, eds. S.W. Bougher et al., pp. 415-458, University of Arizona Press, Tucson. Grinspoon, D.H., et al., 1993. Planetary and Space Science, 41 (July 1993), 515-542. James, E. P

Multivariate quadrature for representing cloud condensation nuclei activity of aerosol populations

DOE PAGES

Fierce, Laura; McGraw, Robert L.

2017-07-26

Here, sparse representations of atmospheric aerosols are needed for efficient regional- and global-scale chemical transport models. Here we introduce a new framework for representing aerosol distributions, based on the quadrature method of moments. Given a set of moment constraints, we show how linear programming, combined with an entropy-inspired cost function, can be used to construct optimized quadrature representations of aerosol distributions. The sparse representations derived from this approach accurately reproduce cloud condensation nuclei (CCN) activity for realistically complex distributions simulated by a particleresolved model. Additionally, the linear programming techniques described in this study can be used to bound key aerosolmore » properties, such as the number concentration of CCN. Unlike the commonly used sparse representations, such as modal and sectional schemes, the maximum-entropy approach described here is not constrained to pre-determined size bins or assumed distribution shapes. This study is a first step toward a particle-based aerosol scheme that will track multivariate aerosol distributions with sufficient computational efficiency for large-scale simulations.« less

Multivariate quadrature for representing cloud condensation nuclei activity of aerosol populations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fierce, Laura; McGraw, Robert L.

Here, sparse representations of atmospheric aerosols are needed for efficient regional- and global-scale chemical transport models. Here we introduce a new framework for representing aerosol distributions, based on the quadrature method of moments. Given a set of moment constraints, we show how linear programming, combined with an entropy-inspired cost function, can be used to construct optimized quadrature representations of aerosol distributions. The sparse representations derived from this approach accurately reproduce cloud condensation nuclei (CCN) activity for realistically complex distributions simulated by a particleresolved model. Additionally, the linear programming techniques described in this study can be used to bound key aerosolmore » properties, such as the number concentration of CCN. Unlike the commonly used sparse representations, such as modal and sectional schemes, the maximum-entropy approach described here is not constrained to pre-determined size bins or assumed distribution shapes. This study is a first step toward a particle-based aerosol scheme that will track multivariate aerosol distributions with sufficient computational efficiency for large-scale simulations.« less

CO2 Condensation Models for Mars

NASA Technical Reports Server (NTRS)

Colaprete, A.; Haberle, R.

2004-01-01

During the polar night in both hemispheres of Mars, regions of low thermal emission, frequently referred to as "cold spots", have been observed by Mariner 9, Viking and Mars Global Surveyor (MGS) spacecraft. These cold spots vary in time and appear to be associated with topographic features suggesting that they are the result of a spectral-emission effect due to surface accumulation of fine-grained frost or snow. Presented here are simulations of the Martian polar night using the NASA Ames General Circulation Cloud Model. This cloud model incorporates all the microphysical processes of carbon dioxide cloud formation, including nucleation, condensation and sedimentation and is coupled to a surface frost scheme that includes both direct surface condensation and precipitation. Using this cloud model we simulate the Mars polar nights and compare model results to observations from the Thermal Emission Spectrometer (TES) and the Mars Orbiter Laser Altimeter (MOLA). Model predictions of "cold spots" compare well with TES observations of low emissivity regions, both spatially and as a function of season. The model predicted frequency of CO2 cloud formation also agrees well with MOLA observations of polar night cloud echoes. Together the simulations and observations in the North indicate a distinct shift in atmospheric state centered about Ls 270 which we believe may be associated with the strength of the polar vortex.

Jets and Water Clouds on Jupiter

NASA Astrophysics Data System (ADS)

Lian, Yuan; Showman, A. P.

2012-10-01

Ground-based and spacecraft observations show that Jupiter exhibits multiple banded zonal jet structures. These banded jets correlate with dark and bright clouds, often called "belts" and "zones". The mechanisms that produce these banded zonal jets and clouds are poorly understood. Our previous studies showed that the latent heat released by condensation of water vapor could produce equatorial superrotation along with multiple zonal jets in the mid-to-high latitudes. However, that previous work assumed complete and instant removal of condensate and therefore could not predict the cloud formation. Here we present an improved 3D Jupiter model to investigate some effects of cloud microphysics on large-scale dynamics using a closed water cycle that includes condensation, three-dimensional advection of cloud material by the large-scale circulation, evaporation and sedimentation. We use a dry convective adjustment scheme to adjust the temperature towards a dry adiabat when atmospheric columns become convectively unstable, and the tracers are mixed within the unstable layers accordingly. Other physics parameterizations included in our model are the bottom drag and internal heat flux as well as the choices of either Newtonian heating scheme or gray radiative transfer. Given the poorly understood cloud microphysics, we perform case studies by treating the particle size and condensation/evaporation time scale as free parameters. We find that, in some cases, the active water cycle can produce multiple banded jets and clouds. However, the equatorial jet is generally very weak in all the cases because of insufficient supply of eastward eddy momentum fluxes. These differences may result from differences in the overall vertical stratification, baroclinicity, and moisture distribution in our new models relative to the older ones; we expect to elucidate the dynamical mechanisms in continuing work.

Cloud condensation nucleation activities of calcium carbonate and its atmospheric ageing products.

PubMed

Tang, M J; Whitehead, J; Davidson, N M; Pope, F D; Alfarra, M R; McFiggans, G; Kalberer, M

2015-12-28

Aerosol particles can serve as cloud condensation nuclei (CCN) to form cloud droplets, and its composition is a main factor governing whether an aerosol particle is an effective CCN. Pure mineral dust particles are poor CCN; however, changes in chemical composition of mineral dust aerosol particles, due to heterogeneous reactions with reactive trace gases in the troposphere, can modify their CCN properties. In this study we investigated the CCN activities of CaCO3 (as a surrogate for mineral dust) and its six atmospheric ageing products: Ca(NO3)2, CaCl2, CaSO4, Ca(CH3SO3)2, Ca(HCOO)2, and Ca(CH3COO)2. CaCO3 has a very low CCN activity with a hygroscopicity parameter (κ) of 0.001-0.003. The CCN activities of its potential atmospheric ageing products are significantly higher. For example, we determined that Ca(NO3)2, CaCl2 and Ca(HCOO)2 have κ values of ∼0.50, similar to that of (NH4)2SO4. Ca(CH3COO)2 has slightly lower CCN activity with a κ value of ∼0.40, and the κ value of CaSO4 is around 0.02. We further show that exposure of CaCO3 particles to N2O5 at 0% relative humidity (RH) significantly enhances their CCN activity, with κ values increasing to around 0.02-0.04. Within the experimental uncertainties, it appears that the variation in exposure to N2O5 from ∼550 to 15,000 ppbv s does not change the CCN activities of aged CaCO3 particles. This observation indicates that the CaCO3 surface may be already saturated at the shortest exposure. We also discussed the atmospheric implications of our study, and suggested that the rate of change in CCN activities of mineral dust particles in the troposphere is important to determine their roles in cloud formation.

Nitric Acid Uptake on Subtropical Cirrus Cloud Particles

NASA Technical Reports Server (NTRS)

2004-01-01

The redistribution of HNO3 via uptake and sedimentation by cirrus cloud particles is considered an important term in the upper tropospheric budget of reactive nitrogen. Numerous cirrus cloud encounters by the NASA WB-57F high-altitude research aircraft during CRYSTAL-FACE were accompanied by the observation of condensed-phase HNO3 with the NOAA chemical ionization mass spectrometer. The instrument measures HNO3 with two independent channels of detection connected to separate forward- and downward-facing inlets that allow a determination of the amount of HNO3 condensed on ice particles. Subtropical cirrus clouds, as indicated by the presence of ice particles, were observed coincident with condensed-phase HNO3 at temperatures of 197 K - 224 K and pressures of 122 hPa - 224 hPa. Maximum levels of condensed-phase HNO3 approached the gas-phase equivalent of 0.8 ppbv. Ice particle surface coverages as high as 1.4- 10(exp 14) molecules/sq cm were observed. A dissociative Langmuir adsorption model, when using an empirically derived HNO3 adsorption enthalpy of -11.0 kcal/mol, effectively describes the observed molecular coverages to within a factor of 5. The percentage of total HNO3 in the condensed phase ranged from near zero to 100% in the observed cirrus clouds. With volume-weighted mean particle diameters up to 700 pm and particle fall velocities up to 10 m/s, some observed clouds have significant potential to redistribute HNO3 in the upper troposphere.

Silver-halide gelatin holograms

NASA Astrophysics Data System (ADS)

Chang, B. J.; Winick, K.

1980-05-01

The use of a silver-halide gelatin for volume phase holograms having a wide spectral response and lower exposure requirements than alternatives and using commercially available silver salts, is proposed. The main difference between the dichromated gelatin and silver-halide processes is the creation of a hologram latent image, which is given in the form of a hardness differential between exposed and unexposed regions in the silver halide hologram; the differential is in turn created by the reaction products of either tanning development or tanning bleach, which harden the gelatin with link-bonds between molecules.

On signatures of clouds in exoplanetary transit spectra

NASA Astrophysics Data System (ADS)

Pinhas, Arazi; Madhusudhan, Nikku

2017-11-01

Transmission spectra of exoplanetary atmospheres have been used to infer the presence of clouds/hazes. Such inferences are typically based on spectral slopes in the optical deviant from gaseous Rayleigh scattering or low-amplitude spectral features in the infrared. We investigate three observable metrics that could allow constraints on cloud properties from transmission spectra, namely the optical slope, the uniformity of this slope and condensate features in the infrared. We derive these metrics using model transmission spectra considering Mie extinction from a wide range of condensate species, particle sizes and scaleheights. First, we investigate possible degeneracies among the cloud properties for an observed slope. We find, for example, that spectra with very steep optical slopes suggest sulphide clouds (e.g. MnS, ZnS, Na2S) in the atmospheres. Secondly, (non)uniformities in optical slopes provide additional constraints on cloud properties, e.g. MnS, ZnS, TiO2 and Fe2O3 have significantly non-uniform slopes. Thirdly, infrared spectra provide an additional powerful probe into cloud properties, with SiO2, Fe2O3, Mg2SiO4 and MgSiO3 bearing strong infrared features observable with James Webb Space Telescope. We investigate observed spectra of eight hot Jupiters and discuss their implications. In particular, no single or composite condensate species considered here conforms to the steep and non-uniform optical slope observed for HD 189733b. Our work highlights the importance of the three above metrics to investigate cloud properties in exoplanetary atmospheres using high-precision transmission spectra and detailed cloud models. We make our Mie scattering data for condensates publicly available to the community.

Toward Aerosol/Cloud Condensation Nuclei (CCN) Closure during CRYSTAL-FACE

NASA Technical Reports Server (NTRS)

VanReken, Timothy M.; Rissman, Tracey, A.; Roberts, Gregory C.; Varutbangkul, Varuntida; Jonsson, Haflidi H.; Flagan, Richard C.; Seinfeld, John H.

2003-01-01

During July 2002, measurements of cloud condensation nuclei were made in the vicinity of southwest Florida as part of the Cirrus Regional Study of Tropical Anvils and Cirrus Layers-Florida Area Cirrus Experiment (CRYSTAL-FACE) field campaign. These observations, at supersaturations of 0.2 and 0.85%, are presented here. The performance of each of the two CCN counters was validated through laboratory calibration and an in situ intercomparison. The measurements indicate that the aerosol sampled during the campaign was predominantly marine in character: the median concentrations were 233 cm-3 (at S = 0.2%) and 371 cm(sup -3) (at S = 0.85%). Three flights during the experiment differed from this general trend; the aerosol sampled during the two flights on 18 July was more continental in character, and the observations on 28 July indicate high spatial variability and periods of very high aerosol concentrations. This study also includes a simplified aerosol/CCN closure analysis. Aerosol size distributions were measured simultaneously with the CCN observations, and these data are used to predict a CCN concentration using Kohler theory. For the purpose of this analysis, an idealized composition of pure ammonium sulfate was assumed. The analysis indicates that in this case, there was good general agreement between the predicted and observed CCN concentrations: at S = 0.2%, N(sub predicted)/N(sub observed)= 1.047 (R(sup 2)= 0.911)); at S = 0.85%, N(sub predicted)/N(sub observed)=1.201 (R(sup 2)= 0.835)). The impacts of the compositional assumption and of including in-cloud data in the analysis are addressed. The effect of removing the data from the 28 July flight is also examined; doing so improves the result of the closure analysis at S = 0.85%. When omitting that atypical flight, N(sub predicted)/N(sub observed) = 1.085 (R(sup 2) = 0.770) at S = 0.85%.

Nitric Acid Uptake on Subtropical Cirrus Cloud Particles

NASA Technical Reports Server (NTRS)

Popp, P. J.; Gao, R. S.; Marcy, T. P.; Fahey, D. W.; Hudson, P. K.; Thompson, T. L.; Kaercher, B.; Ridley, B. A.; Weinheimer, A. J.; Knapp, D. J.;

Condensed Acids In Antartic Stratospheric Clouds

NASA Technical Reports Server (NTRS)

Pueschel, R. F.; Snetsinger, K. G.; Toon, O. B.; Ferry, G. V.; Starr, W. L.; Oberbeck, V. R.; Chan, K. R.; Goodman, J. K.; Livingston, J. M.; Verma, S.;

Hybrid Lead Halide Layered Perovskites with Silsesquioxane Interlayers.

PubMed

Kataoka, Sho; Kaburagi, Wako; Mochizuki, Hiroyuki; Kamimura, Yoshihiro; Sato, Kazuhiko; Endo, Akira

2018-01-01

Hybrid organic-lead halide perovskites exhibit remarkable properties as semiconductors and light absorbers. Here, we report the formation of silsesquioxane-lead halide hybrid layered perovskites. We prepared silsesquioxane with a cubic cage-like structure and fabricated hybrid silsesquioxane-lead halide layered perovskites in a self-assembled manner. It is demonstrated that the silsesquioxane maintain their cage-like structure between lead halide perovskite layers. The silsesquioxane-lead halide perovskites also show excitonic absorption and emission in the visible light region similar to typical lead halide layered perovskites.

Heat capacity of molten halides.

PubMed

Redkin, Alexander A; Zaikov, Yurii P; Korzun, Iraida V; Reznitskikh, Olga G; Yaroslavtseva, Tatiana V; Kumkov, Sergey I

2015-01-15

The heat capacities of molten salts are very important for their practical use. Experimental investigation of this property is challenging because of the high temperatures involved and the corrosive nature of these materials. It is preferable to combine experimental investigations with empirical relationships, which allows for the evaluation of the heat capacity of molten salt mixtures. The isobaric molar heat capacities of all molten alkali and alkaline-earth halides were found to be constant for each group of salts. The value depends on the number of atoms in the salt, and the molar heat capacity per atom is constant for all molten halide salts with the exception of the lithium halides. The molar heat capacities of molten halides do not change when the anions are changed.

Methods for producing single crystal mixed halide perovskites

DOEpatents

Zhu, Kai; Zhao, Yixin

2017-07-11

An aspect of the present invention is a method that includes contacting a metal halide and a first alkylammonium halide in a solvent to form a solution and maintaining the solution at a first temperature, resulting in the formation of at least one alkylammonium halide perovskite crystal, where the metal halide includes a first halogen and a metal, the first alkylammonium halide includes the first halogen, the at least one alkylammonium halide perovskite crystal includes the metal and the first halogen, and the first temperature is above about 21.degree. C.

Vertical Profiles of Cloud Condensation Nuclei, Condensation Nuclei, Optical Aerosol, Aerosol Optical Properties, and Aerosol Volatility Measured from Balloons

NASA Technical Reports Server (NTRS)

Deshler, T.; Snider, J. R.; Vali, G.

1998-01-01

Under the support of this grant a balloon-borne gondola containing a variety of aerosol instruments was developed and flown from Laramie, Wyoming, (41 deg N, 105 deg W) and from Lauder, New Zealand (45 deg S, 170 deg E). The gondola includes instruments to measure the concentrations of condensation nuclei (CN), cloud condensation nuclei (CCN), optically detectable aerosol (OA.) (r greater than or equal to 0.15 - 2.0 microns), and optical scattering properties using a nephelometer (lambda = 530 microns). All instruments sampled from a common inlet which was heated to 40 C on ascent and to 160 C on descent. Flights with the CN counter, OA counter, and nephelometer began in July 1994. The CCN counter was added in November 1994, and the engineering problems were solved by June 1995. Since then the flights have included all four instruments, and were completed in January 1998. Altogether there were 20 flights from Laramie, approximately 5 per year, and 2 from Lauder. Of these there were one or more engineering problems on 6 of the flights from Laramie, hence the data are somewhat limited on those 6 flights, while a complete data set was obtained from the other 14 flights. Good CCN data are available from 12 of the Laramie flights. The two flights from Lauder in January 1998 were successful for all measurements. The results from these flights, and the development of the balloon-bome CCN counter have formed the basis for five conference presentations. The heated and unheated CN and OA measurements have been used to estimate the mass fraction of the aerosol volatile, while comparisons of the nephelometer measurements were used to estimate the light scattering, associated with the volatile aerosol. These estimates were calculated for 0.5 km averages of the ascent and descent data between 2.5 km and the tropopause, near 11.5 km.

Plume-exit modeling to determine cloud condensation nuclei activity of aerosols from residential biofuel combustion

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mena, Francisco; Bond, Tami C.; Riemer, Nicole

Residential biofuel combustion is an important source of aerosols and gases in the atmosphere. The change in cloud characteristics due to biofuel burning aerosols is uncertain, in part, due to the uncertainty in the added number of cloud condensation nuclei (CCN) from biofuel burning. We provide estimates of the CCN activity of biofuel burning aerosols by explicitly modeling plume dynamics (coagulation, condensation, chemical reactions, and dilution) in a young biofuel burning plume from emission until plume exit, defined here as the condition when the plume reaches ambient temperature and specific humidity through entrainment. We found that aerosol-scale dynamics affect CCNmore » activity only during the first few seconds of evolution, after which the CCN efficiency reaches a constant value. Homogenizing factors in a plume are co-emission of semi-volatile organic compounds (SVOCs) or emission at small particle sizes; SVOC co-emission can be the main factor determining plume-exit CCN for hydrophobic or small particles. Coagulation limits emission of CCN to about 10 16 per kilogram of fuel. Depending on emission factor, particle size, and composition, some of these particles may not activate at low supersaturation ( s sat). Hygroscopic Aitken-mode particles can contribute to CCN through self-coagulation but have a small effect on the CCN activity of accumulation-mode particles, regardless of composition differences. Simple models (monodisperse coagulation and average hygroscopicity) can be used to estimate plume-exit CCN within about 20 % if particles are unimodal and have homogeneous composition, or when particles are emitted in the Aitken mode even if they are not homogeneous. On the other hand, if externally mixed particles are emitted in the accumulation mode without SVOCs, an average hygroscopicity overestimates emitted CCN by up to a factor of 2. This work has identified conditions under which particle populations become more homogeneous during plume

Plume-exit modeling to determine cloud condensation nuclei activity of aerosols from residential biofuel combustion

NASA Astrophysics Data System (ADS)

Mena, Francisco; Bond, Tami C.; Riemer, Nicole

2017-08-01

Residential biofuel combustion is an important source of aerosols and gases in the atmosphere. The change in cloud characteristics due to biofuel burning aerosols is uncertain, in part, due to the uncertainty in the added number of cloud condensation nuclei (CCN) from biofuel burning. We provide estimates of the CCN activity of biofuel burning aerosols by explicitly modeling plume dynamics (coagulation, condensation, chemical reactions, and dilution) in a young biofuel burning plume from emission until plume exit, defined here as the condition when the plume reaches ambient temperature and specific humidity through entrainment. We found that aerosol-scale dynamics affect CCN activity only during the first few seconds of evolution, after which the CCN efficiency reaches a constant value. Homogenizing factors in a plume are co-emission of semi-volatile organic compounds (SVOCs) or emission at small particle sizes; SVOC co-emission can be the main factor determining plume-exit CCN for hydrophobic or small particles. Coagulation limits emission of CCN to about 1016 per kilogram of fuel. Depending on emission factor, particle size, and composition, some of these particles may not activate at low supersaturation (ssat). Hygroscopic Aitken-mode particles can contribute to CCN through self-coagulation but have a small effect on the CCN activity of accumulation-mode particles, regardless of composition differences. Simple models (monodisperse coagulation and average hygroscopicity) can be used to estimate plume-exit CCN within about 20 % if particles are unimodal and have homogeneous composition, or when particles are emitted in the Aitken mode even if they are not homogeneous. On the other hand, if externally mixed particles are emitted in the accumulation mode without SVOCs, an average hygroscopicity overestimates emitted CCN by up to a factor of 2. This work has identified conditions under which particle populations become more homogeneous during plume processes. This

Plume-exit modeling to determine cloud condensation nuclei activity of aerosols from residential biofuel combustion

DOE PAGES

Mena, Francisco; Bond, Tami C.; Riemer, Nicole

2017-08-07

Residential biofuel combustion is an important source of aerosols and gases in the atmosphere. The change in cloud characteristics due to biofuel burning aerosols is uncertain, in part, due to the uncertainty in the added number of cloud condensation nuclei (CCN) from biofuel burning. We provide estimates of the CCN activity of biofuel burning aerosols by explicitly modeling plume dynamics (coagulation, condensation, chemical reactions, and dilution) in a young biofuel burning plume from emission until plume exit, defined here as the condition when the plume reaches ambient temperature and specific humidity through entrainment. We found that aerosol-scale dynamics affect CCNmore » activity only during the first few seconds of evolution, after which the CCN efficiency reaches a constant value. Homogenizing factors in a plume are co-emission of semi-volatile organic compounds (SVOCs) or emission at small particle sizes; SVOC co-emission can be the main factor determining plume-exit CCN for hydrophobic or small particles. Coagulation limits emission of CCN to about 10 16 per kilogram of fuel. Depending on emission factor, particle size, and composition, some of these particles may not activate at low supersaturation ( s sat). Hygroscopic Aitken-mode particles can contribute to CCN through self-coagulation but have a small effect on the CCN activity of accumulation-mode particles, regardless of composition differences. Simple models (monodisperse coagulation and average hygroscopicity) can be used to estimate plume-exit CCN within about 20 % if particles are unimodal and have homogeneous composition, or when particles are emitted in the Aitken mode even if they are not homogeneous. On the other hand, if externally mixed particles are emitted in the accumulation mode without SVOCs, an average hygroscopicity overestimates emitted CCN by up to a factor of 2. This work has identified conditions under which particle populations become more homogeneous during plume

Cloud Condensation Nuclei Prediction Error from Application of Kohler Theory: Importance for the Aerosol Indirect Effect

NASA Technical Reports Server (NTRS)

Sotiropoulou, Rafaella-Eleni P.; Nenes, Athanasios; Adams, Peter J.; Seinfeld, John H.

2007-01-01

In situ observations of aerosol and cloud condensation nuclei (CCN) and the GISS GCM Model II' with an online aerosol simulation and explicit aerosol-cloud interactions are used to quantify the uncertainty in radiative forcing and autoconversion rate from application of Kohler theory. Simulations suggest that application of Koehler theory introduces a 10-20% uncertainty in global average indirect forcing and 2-11% uncertainty in autoconversion. Regionally, the uncertainty in indirect forcing ranges between 10-20%, and 5-50% for autoconversion. These results are insensitive to the range of updraft velocity and water vapor uptake coefficient considered. This study suggests that Koehler theory (as implemented in climate models) is not a significant source of uncertainty for aerosol indirect forcing but can be substantial for assessments of aerosol effects on the hydrological cycle in climatically sensitive regions of the globe. This implies that improvements in the representation of GCM subgrid processes and aerosol size distribution will mostly benefit indirect forcing assessments. Predictions of autoconversion, by nature, will be subject to considerable uncertainty; its reduction may require explicit representation of size-resolved aerosol composition and mixing state.

Airborne measurements of cloud-forming nuclei and aerosol particles in stabilized ground clouds produced by solid rocket booster firings

NASA Technical Reports Server (NTRS)

Hindman, E. E., II; Ala, G. G.; Parungo, F. P.; Willis, P. T.; Bendura, R. J.; Woods, D.

1978-01-01

Airborne measurements of cloud volumes, ice nuclei and cloud condensation nuclei, liquid particles, and aerosol particles were obtained from stabilized ground clouds (SGCs) produced by Titan 3 launches at Kennedy Space Center, 20 August and 5 September 1977. The SGCs were bright, white, cumulus clouds early in their life and contained up to 3.5 g/m3 of liquid in micron to millimeter size droplets. The measured cloud volumes were 40 to 60 cu km five hours after launch. The SGCs contained high concentrations of cloud condensation nuclei active at 0.2%, 0.5%, and 1.0% supersaturation for periods of three to five hours. The SGCs also contained high concentrations of submicron particles. Three modes existed in the particle population: a 0.05 to 0.1 micron mode composed of aluminum-containing particles, a 0.2 to 0.8 micron mode, and a 2.0 to 10 micron mode composed of particles that contained primarily aluminum.

Preparation of cerium halide solvate complexes

DOEpatents

Vasudevan, Kalyan V; Smith, Nickolaus A; Gordon, John C; McKigney, Edward A; Muenchaussen, Ross E

2013-08-06

Crystals of a solvated cerium(III) halide solvate complex resulted from a process of forming a paste of a cerium(III) halide in an ionic liquid, adding a solvent to the paste, removing any undissolved solid, and then cooling the liquid phase. Diffusing a solvent vapor into the liquid phase also resulted in crystals of a solvated cerium(III) halide complex.

Clouds over Tharsis

NASA Technical Reports Server (NTRS)

1998-01-01

Color composite of condensate clouds over Tharsis made from red and blue images with a synthesized green channel. Mars Orbiter Camera wide angle frames from Orbit 48.

Figure caption from Science Magazine

Clouds in the Martian Atmosphere

NASA Astrophysics Data System (ADS)

Määttänen, Anni; Montmessin, Franck

2018-01-01

Although resembling an extremely dry desert, planet Mars hosts clouds in its atmosphere. Every day somewhere on the planet a part of the tiny amount of water vapor held by the atmosphere can condense as ice crystals to form cirrus-type clouds. The existence of water ice clouds has been known for a long time, and they have been studied for decades, leading to the establishment of a well-known climatology and understanding of their formation and properties. Despite their thinness, they have a clear impact on the atmospheric temperatures, thus affecting the Martian climate. Another, more exotic type of clouds forms as well on Mars. The atmospheric temperatures can plunge to such frigid values that the major gaseous component of the atmosphere, CO2, condenses as ice crystals. These clouds form in the cold polar night where they also contribute to the formation of the CO2 ice polar cap, and also in the mesosphere at very high altitudes, near the edge of space, analogously to the noctilucent clouds on Earth. The mesospheric clouds are a fairly recent discovery and have put our understanding of the Martian atmosphere to a test. On Mars, cloud crystals form on ice nuclei, mostly provided by the omnipresent dust. Thus, the clouds link the three major climatic cycles: those of the two major volatiles, H2O and CO2; and that of dust, which is a major climatic agent itself.

Cloud condensation nuclei closure study on summer arctic aerosol

NASA Astrophysics Data System (ADS)

Martin, M.; Chang, R. Y.-W.; Sierau, B.; Sjogren, S.; Swietlicki, E.; Abbatt, J. P. D.; Leck, C.; Lohmann, U.

2011-11-01

We present an aerosol - cloud condensation nuclei (CCN) closure study on summer high Arctic aerosol based on measurements that were carried out in 2008 during the Arctic Summer Cloud Ocean Study (ASCOS) on board the Swedish ice breaker Oden. The data presented here were collected during a three-week time period in the pack ice (>85° N) when the icebreaker Oden was moored to an ice floe and drifted passively during the most biological active period into autumn freeze up conditions. CCN number concentrations were obtained using two CCN counters measuring at different supersaturations. The directly measured CCN number concentration was then compared with a CCN number concentration calculated using both bulk aerosol mass composition data from an aerosol mass spectrometer (AMS) and aerosol number size distributions obtained from a differential mobility particle sizer, assuming κ-Köhler theory, surface tension of water and an internally mixed aerosol. The last assumption was supported by measurements made with a hygroscopic tandem differential mobility analyzer (HTDMA) for particles >70 nm. For the two highest measured supersaturations, 0.73 and 0.41%, closure could not be achieved with the investigated settings concerning hygroscopicity and density. The calculated CCN number concentration was always higher than the measured one for those two supersaturations. This might be caused by a relative larger insoluble organic mass fraction of the smaller particles that activate at these supersaturations, which are thus less good CCN than the larger particles. On average, 36% of the mass measured with the AMS was organic mass. At 0.20, 0.15 and 0.10% supersaturation, closure could be achieved with different combinations of hygroscopic parameters and densities within the uncertainty range of the fit. The best agreement of the calculated CCN number concentration with the observed one was achieved when the organic fraction of the aerosol was treated as nearly water insoluble

In-Situ Characterization of Cloud Condensation Nuclei, Interstitial, and background Particles using Single Particle Mass Spectrometer, SPLAT II

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zelenyuk, Alla; Imre, D.; Earle, Michael

2010-10-01

Aerosol indirect effect remains the most uncertain aspect of climate change modeling because proper test requires knowledge of individual particles sizes and compositions with high spatial and temporal resolution. We present the first deployment of a single particle mass spectrometer (SPLAT II) that is operated in a dual data acquisition mode to measure all the required individual particle properties with sufficient temporal resolution to definitively resolve the aerosol-cloud interaction in this exemplary case. We measured particle number concentrations, asphericity, and individual particle size, composition, and density with better than 60 seconds resolution. SPLAT II measured particle number concentrations between 70more » particles cm-3and 300 particles cm-3, an average particle density of 1.4 g cm-3. Found that most particles are composed of oxygenated organics, many of which are mixed with sulfates. Biomass burn particles some with sulfates were prevalent, particularly at higher altitudes, and processed sea-salt was observed over the ocean. Analysis of cloud residuals shows that with time cloud droplets acquire sulfate by the reaction of peroxide with SO2. Based on the particle mass spectra and densities we find that the compositions of cloud condensation nuclei are similar to those of background aerosol but, contain on average ~7% more sulfate, and do not include dust and metallic particles. A comparison between the size distributions of background, activated, and interstitial particles shows that while nearly none of the activated particles is smaller than 115 nm, more than 80% of interstitial particles are smaller than 115 nm. We conclude that for this cloud the most important difference between CCN and background aerosol is particle size although having more sulfate also helps.« less

Clouds over Tharsis

NASA Image and Video Library

1998-03-13

Color composite of condensate clouds over Tharsis made from red and blue images with a synthesized green channel. Mars Orbiter Camera wide angle frames from Orbit 48. http://photojournal.jpl.nasa.gov/catalog/PIA00812

A numerical determination of the evolution of cloud drop spectra due to condensation on natural aerosol particles

NASA Technical Reports Server (NTRS)

Lee, I. Y.; Haenel, G.; Pruppacher, H. R.

1980-01-01

The time variation in size of aerosol particles growing by condensation is studied numerically by means of an air parcel model which allows entrainment of air and aerosol particles. Particles of four types of aerosols typically occurring in atmospheric air masses were considered. The present model circumvents any assumption about the size distribution and chemical composition of the aerosol particles by basing the aerosol particle growth on actually observed size distributions and on observed amounts of water taken up under equilibrium by a deposit of the aerosol particles. Characteristic differences in the drop size distribution, liquid water content and supersaturation were found for the clouds which evolved from the four aerosol types considered.

Prediction of cloud condensation nuclei activity for organic compounds using functional group contribution methods

DOE PAGES

Petters, M. D.; Kreidenweis, S. M.; Ziemann, P. J.

2016-01-19

A wealth of recent laboratory and field experiments demonstrate that organic aerosol composition evolves with time in the atmosphere, leading to changes in the influence of the organic fraction to cloud condensation nuclei (CCN) spectra. There is a need for tools that can realistically represent the evolution of CCN activity to better predict indirect effects of organic aerosol on clouds and climate. This work describes a model to predict the CCN activity of organic compounds from functional group composition. Following previous methods in the literature, we test the ability of semi-empirical group contribution methods in Kohler theory to predict themore » effective hygroscopicity parameter, kappa. However, in our approach we also account for liquid–liquid phase boundaries to simulate phase-limited activation behavior. Model evaluation against a selected database of published laboratory measurements demonstrates that kappa can be predicted within a factor of 2. Simulation of homologous series is used to identify the relative effectiveness of different functional groups in increasing the CCN activity of weakly functionalized organic compounds. Hydroxyl, carboxyl, aldehyde, hydroperoxide, carbonyl, and ether moieties promote CCN activity while methylene and nitrate moieties inhibit CCN activity. Furthermore, the model can be incorporated into scale-bridging test beds such as the Generator of Explicit Chemistry and Kinetics of Organics in the Atmosphere (GECKO-A) to evaluate the evolution of kappa for a complex mix of organic compounds and to develop suitable parameterizations of CCN evolution for larger-scale models.« less

Impact of new particle formation on the concentrations of aerosols and cloud condensation nuclei around Beijing

NASA Astrophysics Data System (ADS)

Matsui, H.; Koike, M.; Kondo, Y.; Takegawa, N.; Wiedensohler, A.; Fast, J. D.; Zaveri, R. A.

2011-10-01

New particle formation (NPF) is one of the most important processes in controlling the concentrations of aerosols (condensation nuclei, CN) and cloud condensation nuclei (CCN) in the atmosphere. In this study, we introduce a new aerosol model representation with 20 size bins between 1 nm and 10 μm and activation-type and kinetic nucleation parameterizations into the WRF-chem model (called NPF-explicit WRF-chem). Model calculations were conducted in the Beijing region in China for the periods during the Campaign of Air Quality Research in Beijing and Surrounding Region 2006 (CARE-Beijing 2006) campaign conducted in August and September 2006. Model calculations successfully reproduced the timing of NPF and no-NPF days in the measurements (21 of 26 days). Model calculations also reproduced the subsequent rapid growth of new particles with a time scale of half a day. These results suggest that once a reasonable nucleation rate at a diameter of 1 nm is given, explicit calculations of condensation and coagulation processes can reproduce the clear contrast between NPF and no-NPF days as well as further growth up to several tens of nanometers. With this reasonable representation of the NPF process, we show that NPF contributed 20%-30% of the CN concentrations (>10 nm in diameter) in and around Beijing on average. We also show that NPF increases CCN concentrations at higher supersaturations (S > 0.2%), while it decreases them at lower supersaturations (S < 0.1%). This is likely because NPF suppresses the increases in both the size and hygroscopicity of preexisting particles through the competition of condensable gases between new particles and preexisting particles. Sensitivity calculations show that a reduction of primary aerosol emissions, such as black carbon (BC), would not necessarily decrease CCN concentrations because of an increase in NPF. Sensitivity calculations also suggest that the reduction ratio of primary aerosol and SO2 emissions will be key in enhancing or

Shallow halogen vacancies in halide optoelectronic materials

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shi, Hongliang; Du, Mao -Hua

2014-11-05

Halogen vacancies (V H) are usually deep color centers (F centers) in halides and can act as major electron traps or recombination centers. The deep V H contributes to the typically poor carrier transport properties in halides. However, several halides have recently emerged as excellent optoelectronic materials, e.g., CH 3NH 3PbI 3 and TlBr. Both CH 3NH 3PbI 3 and TlBr have been found to have shallow V H, in contrast to commonly seen deep V H in halides. In this paper, several halide optoelectronic materials, i.e., CH 3NH 3PbI 3, CH 3NH 3SnI 3 (photovoltaic materials), TlBr, and CsPbBrmore » 3, (gamma-ray detection materials) are studied to understand the material chemistry and structure that determine whether V H is a shallow or deep defect in a halide material. It is found that crystal structure and chemistry of ns 2 ions both play important roles in creating shallow V H in halides such as CH 3NH 3PbI 3, CH 3NH 3SnI 3, and TlBr. The key to identifying halides with shallow V H is to find the right crystal structures and compounds that suppress cation orbital hybridization at V H, such as those with long cation-cation distances and low anion coordination numbers, and those with crystal symmetry that prevents strong hybridization of cation dangling bond orbitals at V H. Furthermore, the results of this paper provide insight and guidance to identifying halides with shallow V H as good electronic and optoelectronic materials.« less

Shallow halogen vacancies in halide optoelectronic materials

NASA Astrophysics Data System (ADS)

Shi, Hongliang; Du, Mao-Hua

2014-11-01

Halogen vacancies (VH ) are usually deep color centers (F centers) in halides and can act as major electron traps or recombination centers. The deep VH contributes to the typically poor carrier transport properties in halides. However, several halides have recently emerged as excellent optoelectronic materials, e.g., C H3N H3Pb I3 and TlBr. Both C H3N H3Pb I3 and TlBr have been found to have shallow VH , in contrast to commonly seen deep VH in halides. In this paper, several halide optoelectronic materials, i.e., C H3N H3Pb I3 , C H3N H3Sn I3 (photovoltaic materials), TlBr, and CsPbB r3 (gamma-ray detection materials) are studied to understand the material chemistry and structure that determine whether VH is a shallow or deep defect in a halide material. It is found that crystal structure and chemistry of n s2 ions both play important roles in creating shallow VH in halides such as C H3N H3Pb I3 , C H3N H3Sn I3 , and TlBr. The key to identifying halides with shallow VH is to find the right crystal structures and compounds that suppress cation orbital hybridization at VH , such as those with large cation-cation distances and low anion coordination numbers and those with crystal symmetry that prevents strong hybridization of cation dangling bond orbitals at VH . The results of this paper provide insight and guidance to identifying halides with shallow VH as good electronic and optoelectronic materials.

Benzoyl Halides as Alternative Precursors for the Colloidal Synthesis of Lead-Based Halide Perovskite Nanocrystals

PubMed Central

2018-01-01

We propose here a new colloidal approach for the synthesis of both all-inorganic and hybrid organic–inorganic lead halide perovskite nanocrystals (NCs). The main limitation of the protocols that are currently in use, such as the hot injection and the ligand-assisted reprecipitation routes, is that they employ PbX2 (X = Cl, Br, or I) salts as both lead and halide precursors. This imposes restrictions on being able to precisely tune the amount of reaction species and, consequently, on being able to regulate the composition of the final NCs. In order to overcome this issue, we show here that benzoyl halides can be efficiently used as halide sources to be injected in a solution of metal cations (mainly in the form of metal carboxylates) for the synthesis of APbX3 NCs (in which A = Cs+, CH3NH3+, or CH(NH2)2+). In this way, it is possible to independently tune the amount of both cations and halide precursors in the synthesis. The APbX3 NCs that were prepared with our protocol show excellent optical properties, such as high photoluminescence quantum yields, low amplified spontaneous emission thresholds, and enhanced stability in air. It is noteworthy that CsPbI3 NCs, which crystallize in the cubic α phase, are stable in air for weeks without any postsynthesis treatment. The improved properties of our CsPbX3 perovskite NCs can be ascribed to the formation of lead halide terminated surfaces, in which Cs cations are replaced by alkylammonium ions. PMID:29378131

Benzoyl Halides as Alternative Precursors for the Colloidal Synthesis of Lead-Based Halide Perovskite Nanocrystals.

PubMed

Imran, Muhammad; Caligiuri, Vincenzo; Wang, Mengjiao; Goldoni, Luca; Prato, Mirko; Krahne, Roman; De Trizio, Luca; Manna, Liberato

2018-02-21

We propose here a new colloidal approach for the synthesis of both all-inorganic and hybrid organic-inorganic lead halide perovskite nanocrystals (NCs). The main limitation of the protocols that are currently in use, such as the hot injection and the ligand-assisted reprecipitation routes, is that they employ PbX 2 (X = Cl, Br, or I) salts as both lead and halide precursors. This imposes restrictions on being able to precisely tune the amount of reaction species and, consequently, on being able to regulate the composition of the final NCs. In order to overcome this issue, we show here that benzoyl halides can be efficiently used as halide sources to be injected in a solution of metal cations (mainly in the form of metal carboxylates) for the synthesis of APbX 3 NCs (in which A = Cs + , CH 3 NH 3 + , or CH(NH 2 ) 2 + ). In this way, it is possible to independently tune the amount of both cations and halide precursors in the synthesis. The APbX 3 NCs that were prepared with our protocol show excellent optical properties, such as high photoluminescence quantum yields, low amplified spontaneous emission thresholds, and enhanced stability in air. It is noteworthy that CsPbI 3 NCs, which crystallize in the cubic α phase, are stable in air for weeks without any postsynthesis treatment. The improved properties of our CsPbX 3 perovskite NCs can be ascribed to the formation of lead halide terminated surfaces, in which Cs cations are replaced by alkylammonium ions.

Worldwide data sets constrain the water vapor uptake coefficient in cloud formation.

PubMed

Raatikainen, Tomi; Nenes, Athanasios; Seinfeld, John H; Morales, Ricardo; Moore, Richard H; Lathem, Terry L; Lance, Sara; Padró, Luz T; Lin, Jack J; Cerully, Kate M; Bougiatioti, Aikaterini; Cozic, Julie; Ruehl, Christopher R; Chuang, Patrick Y; Anderson, Bruce E; Flagan, Richard C; Jonsson, Haflidi; Mihalopoulos, Nikos; Smith, James N

2013-03-05

Cloud droplet formation depends on the condensation of water vapor on ambient aerosols, the rate of which is strongly affected by the kinetics of water uptake as expressed by the condensation (or mass accommodation) coefficient, αc. Estimates of αc for droplet growth from activation of ambient particles vary considerably and represent a critical source of uncertainty in estimates of global cloud droplet distributions and the aerosol indirect forcing of climate. We present an analysis of 10 globally relevant data sets of cloud condensation nuclei to constrain the value of αc for ambient aerosol. We find that rapid activation kinetics (αc > 0.1) is uniformly prevalent. This finding resolves a long-standing issue in cloud physics, as the uncertainty in water vapor accommodation on droplets is considerably less than previously thought.

Radiative Impacts of Cloud Heterogeneity and Overlap in an Atmospheric General Circulation Model

NASA Technical Reports Server (NTRS)

Oreopoulos, L.; Lee, D.; Sud, Y. C.; Suarez, M. J.

2012-01-01

The radiative impacts of introducing horizontal heterogeneity of layer cloud condensate, and vertical overlap of condensate and cloud fraction are examined with the aid of a new radiation package operating in the GEOS-5 Atmospheric General Circulation Model. The impacts are examined in terms of diagnostic top-of-the-atmosphere shortwave (SW) and longwave (LW) cloud radiative effect (CRE) calculations for a range of assumptions and parameter specifications about the overlap. The investigation is conducted for two distinct cloud schemes, the one that comes with the standard GEOS-5 distribution, and another which has been recently used experimentally for its enhanced GEOS-5 distribution, and another which has been recently used experimentally for its enhanced cloud microphysical capabilities; both are coupled to a cloud generator allowing arbitrary cloud overlap specification. We find that cloud overlap radiative impacts are significantly stronger for the operational cloud scheme for which a change of cloud fraction overlap from maximum-random to generalized results to global changes of SW and LW CRE of approximately 4 Watts per square meter, and zonal changes of up to approximately 10 Watts per square meter. This is because of fewer occurrences compared to the other scheme of large layer cloud fractions and of multi-layer situations with large numbers of atmospheric being simultaneously cloudy, conditions that make overlap details more important. The impact on CRE of the details of condensate distribution overlap is much weaker. Once generalized overlap is adopted, both cloud schemes are only modestly sensitive to the exact values of the overlap parameters. We also find that if one of the CRE components is overestimated and the other underestimated, both cannot be driven towards observed values by adjustments to cloud condensate heterogeneity and overlap alone.

Process and composition for drying of gaseous hydrogen halides

DOEpatents

Tom, Glenn M.; Brown, Duncan W.

1989-08-01

A process for drying a gaseous hydrogen halide of the formula HX, wherein X is selected from the group consisting of bromine, chlorine, fluorine, and iodine, to remove water impurity therefrom, comprising: contacting the water impurity-containing gaseous hydrogen halide with a scavenger including a support having associated therewith one or more members of the group consisting of: (a) an active scavenging moiety selected from one or more members of the group consisting of: (i) metal halide compounds dispersed in the support, of the formula MX.sub.y ; and (ii) metal halide pendant functional groups of the formula -MX.sub.y-1 covalently bonded to the support, wherein M is a y-valent metal, and y is an integer whose value is from 1 to 3; (b) corresponding partially or fully alkylated compounds and/or pendant functional groups, of the metal halide compounds and/or pendant functional groups of (a); wherein the alkylated compounds and/or pendant functional groups, when present, are reactive with the gaseous hydrogen halide to form the corresponding halide compounds and/or pendant functional groups of (a); and M being selected such that the heat of formation, .DELTA.H.sub.f of its hydrated halide, MX.sub.y.(H.sub.2 O).sub.n, is governed by the relationship: .DELTA.H.sub.f .gtoreq.n.times.10.1 kilocalories/mole of such hydrated halide compound wherein n is the number of water molecules bound to the metal halide in the metal halide hydrate. Also disclosed is an appertaining scavenger composition and a contacting apparatus wherein the scavenger is deployed in a bed for contacting with the water impurity-containing gaseous hydrogen halide.

An observational search for CO2 ice clouds on Mars

NASA Technical Reports Server (NTRS)

Bell, James F., III; Calvin, Wendy M.; Pollack, James B.; Crisp, David

1993-01-01

CO2 ice clouds were first directly identified on Mars by the Mariner 6 and 7 infrared spectrometer limb scans. These observations provided support for early theoretical modeling efforts of CO2 condensation. Mariner 9 IRIS temperature profiles of north polar hood clouds were interpreted as indicating that these clouds were composed of H2O ice at lower latitudes and CO2 ice at higher latitudes. The role of CO2 condensation on Mars has recently received increased attention because (1) Kasting's model results indicated that CO2 cloud condensation limits the magnitude of the proposed early Mars CO2/H2O greenhouse, and (2) Pollack el al.'s GCM results indicated that the formation of CO2 ice clouds is favorable at all polar latitudes during the fall and winter seasons. These latter authors have shown that CO2 clouds play an important role in the polar energy balance, as the amount of CO2 contained in the polar caps is constrained by a balance between latent heat release, heat advected from lower latitudes, and thermal emission to space. The polar hood clouds reduce the amount of CO2 condensation on the polar caps because they reduce the net emission to space. There have been many extensive laboratory spectroscopic studies of H2O and CO2 ices and frosts. In this study, we use results from these and other sources to search for the occurrence of diagnostic CO2 (and H2O) ice and/or frost absorption features in ground based near-infrared imaging spectroscopic data of Mars. Our primary goals are (1) to try to confirm the previous direct observations of CO2 clouds on Mars; (2) to determine the spatial extent, temporal variability, and composition (H2O/CO2 ratio) of any clouds detected; and (3) through radiative transfer modeling, to try to determine the mean particle size and optical depth of polar hood clouds, thus, assessing their role in the polar heat budget.

Worldwide data sets constrain the water vapor uptake coefficient in cloud formation

PubMed Central

Raatikainen, Tomi; Nenes, Athanasios; Seinfeld, John H.; Morales, Ricardo; Moore, Richard H.; Lathem, Terry L.; Lance, Sara; Padró, Luz T.; Lin, Jack J.; Cerully, Kate M.; Bougiatioti, Aikaterini; Cozic, Julie; Ruehl, Christopher R.; Chuang, Patrick Y.; Anderson, Bruce E.; Flagan, Richard C.; Jonsson, Haflidi; Mihalopoulos, Nikos; Smith, James N.

2013-01-01

Cloud droplet formation depends on the condensation of water vapor on ambient aerosols, the rate of which is strongly affected by the kinetics of water uptake as expressed by the condensation (or mass accommodation) coefficient, αc. Estimates of αc for droplet growth from activation of ambient particles vary considerably and represent a critical source of uncertainty in estimates of global cloud droplet distributions and the aerosol indirect forcing of climate. We present an analysis of 10 globally relevant data sets of cloud condensation nuclei to constrain the value of αc for ambient aerosol. We find that rapid activation kinetics (αc > 0.1) is uniformly prevalent. This finding resolves a long-standing issue in cloud physics, as the uncertainty in water vapor accommodation on droplets is considerably less than previously thought. PMID:23431189

Balloon-borne measurements of aerosol, condensation nuclei, and cloud particles in the stratosphere at McMurdo Station, Antarctica, during the spring of 1987

NASA Technical Reports Server (NTRS)

Hofmann, D. J.; Rosen, J. M.; Harder, J. W.; Hereford, J. V.

1989-01-01

Measurements of the vertical profile of particles with condensation nuclei counters and eight channel aerosol detectors at McMurdo Station, Antarctica, in 1987 verified observations made in 1986 concerning the absence of upwelling in the polar vortex and the presence of a condensation nuclei layer in conjunction with the ozone hole region. New observations of a bimodal aerosol size distribution, consisting of a large-particle mode mixed in with the small-particle sulfate mode, at temperatures below -79 C are consistent with the presence of nitric acid-water particles at low concentrations. Higher concentrations of large particles were observed in association with nacreous clouds. An unusual particle layer which contained enhanced concentrations of both the small-particle (sulfate) mode and the large-particle (nitric acid) mode was detected at temperatures below -85 C, suggesting simultaneous nucleation and growth phenomena. The vortex condensation nuclei layer was observed to form at the same time as the ozone hole, indicating that formation of the layer is triggered by photochemical processes and may be important in controlling ozone depletion above 22 km.

EDITORIAL: Focus on Cloud Physics FOCUS ON CLOUD PHYSICS

NASA Astrophysics Data System (ADS)

Falkovich, Gregory; Malinowski, Szymon P.

2008-07-01

Cloud physics has for a long time been an important segment of atmospheric science. It is common knowledge that clouds are crucial for our understanding of weather and climate. Clouds are also interesting by themselves (not to mention that they are beautiful). Complexity is hidden behind the common picture of these beautiful and interesting objects. The typical school textbook definition that a cloud is 'a set of droplets or particles suspended in the atmosphere' is not adequate. Clouds are complicated phenomena in which dynamics, turbulence, microphysics, thermodynamics and radiative transfer interact on a wide range of scales, from sub-micron to kilometres. Some of these interactions are subtle and others are more straightforward. Large and small-scale motions lead to activation of cloud condensation nuclei, condensational growth and collisions; small changes in composition and concentration of atmospheric aerosol lead to significant differences in radiative properties of the clouds and influence rainfall formation. It is justified to look at a cloud as a composite, nonlinear system which involves many interactions and feedback. This system is actively linked into a web of atmospheric, oceanic and even cosmic interactions. Due to the complexity of the cloud system, present-day descriptions of clouds suffer from simplifications, inadequate parameterizations, and omissions. Sometimes the most fundamental physics hidden behind these simplifications and parameterizations is not known, and a wide scope of view can sometimes prevent a 'microscopic', deep insight into the detail. Only the expertise offered by scientists focused on particular elementary processes involved in this complicated pattern of interactions allows us to shape elements of the puzzle from which a general picture of clouds can be created. To be useful, every element of the puzzle must be shaped precisely. This often creates problems in communication between the sciences responsible for shaping

Mixed-Halide Perovskites with Stabilized Bandgaps.

PubMed

Xiao, Zhengguo; Zhao, Lianfeng; Tran, Nhu L; Lin, Yunhui Lisa; Silver, Scott H; Kerner, Ross A; Yao, Nan; Kahn, Antoine; Scholes, Gregory D; Rand, Barry P

2017-11-08

One merit of organic-inorganic hybrid perovskites is their tunable bandgap by adjusting the halide stoichiometry, an aspect critical to their application in tandem solar cells, wavelength-tunable light emitting diodes (LEDs), and lasers. However, the phase separation of mixed-halide perovskites caused by light or applied bias results in undesirable recombination at iodide-rich domains, meaning open-circuit voltage (V OC ) pinning in solar cells and infrared emission in LEDs. Here, we report an approach to suppress halide redistribution by self-assembled long-chain organic ammonium capping layers at nanometer-sized grain surfaces. Using the stable mixed-halide perovskite films, we are able to fabricate efficient and wavelength-tunable perovskite LEDs from infrared to green with high external quantum efficiencies of up to 5%, as well as linearly tuned V OC from 1.05 to 1.45 V in solar cells.

New particle formation leads to cloud dimming

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sullivan, Ryan C.; Crippa, Paola; Matsui, Hitoshi

New particle formation (NPF), nucleation of condensable vapors to the solid or liquid phase, is a significant source of atmospheric aerosol particle number concentrations. With sufficient growth, these nucleated particles may be a significant source of cloud condensation nuclei (CCN), thus altering cloud albedo, structure, and lifetimes, and insolation reaching the Earth's surface. Herein we present one of the first numerical experiments to quantify the impact of NPF on cloud radiative properties that is conducted at a convection permitting resolution and that explicitly simulates cloud droplet number concentrations. Consistent with observations, these simulations suggest that in spring over the Midwesternmore » U.S.A., NPF occurs frequently and on regional scales. However, the simulations suggest that NPF is not associated with enhancement of regional cloud albedos as would be expected from an increase of CCN. These simulations indicate that NPF reduces ambient sulfuric acid concentrations sufficiently to inhibit growth of preexisting particles to CCN sizes. This reduction in CCN-sized particles reduces cloud albedo, resulting in a domain average positive top of atmosphere cloud radiative forcing of 10 W m-2 and up to ~ 50 W m-2 in individual grid cells relative to a simulation in which NPF is excluded.« less

PREPARATION OF HALIDES OF PLUTONIUM

DOEpatents

Garner, C.S.; Johns, I.B.

1958-09-01

A dry chemical method is described for preparing plutonium halides, which consists in contacting plutonyl nitrate with dry gaseous HCl or HF at an elevated temperature. The addition to the reaction gas of a small quantity of an oxidizing gas or a reducing gas will cause formation of the tetra- or tri-halide of plutonium as desired.

Impact of new particle formation on the concentrations of aerosol number and cloud condensation nuclei around Beijing

DOE Office of Scientific and Technical Information (OSTI.GOV)

Matsui, H.; Koike, Makoto; Kondo, Yutaka

New particle formation (NPF) is one of the most important processes in controlling the concentrations of aerosol number (condensation nuclei, CN) and cloud condensation nuclei (CCN) in the atmosphere. In this study, we introduced a new aerosol model representation with 20 size bins between 1 nm and 10 {mu}m and activation-type and kinetic nucleation parameterizations into the WRF-chem model (called NPF-explicit WRF-chem). Model calculations were conducted in the Beijing region in China for the periods during the CARE-Beijing 2006 campaign conducted in August and September 2006. Model calculations successfully reproduced the timing of NPF and no-NPF days in the measurementsmore » (21 of 26 days). Model calculations also reproduced the subsequent rapid growth of new particles with a time scale of half a day. These results suggest that once a reasonable nucleation rate at a diameter of 1 nm is given, explicit calculations of condensation and coagulation processes can reproduce the clear contrast between NPF and no-NPF days as well as further growth up to several tens nanometers. With this reasonable representation of the NPF process, we show that NPF contributed 20-30% of CN concentrations (> 10 nm in diameter) in and around Beijing on average. We also show that NPF increases CCN concentrations at higher supersaturations (S > 0.2%), while it decreases them at lower supersaturations (S < 0.1%). This is likely because NPF suppresses the increases in both the size and hygroscopicity of pre-existing particles through the competition of condensable gases between new particles and pre-existing particles. Sensitivity calculations show that a reduction of primary aerosol emissions, such as black carbon (BC), would not necessarily decrease CCN concentrations because of an increase in NPF. Sensitivity calculations also suggest that the reduction ratio of primary aerosol and SO2 emissions will be key in enhancing or damping the BC mitigation effect.« less

Tropical High Cloud Fraction Controlled by Cloud Lifetime Rather Than Clear-sky Convergence

NASA Astrophysics Data System (ADS)

Seeley, J.; Jeevanjee, N.; Romps, D. M.

2016-12-01

Observations and simulations show a peak in cloud fraction below the tropopause. This peak is usually attributed to a roughly co-located peak in radiatively-driven clear-sky convergence, which is presumed to force convective detrainment and thus promote large cloud fraction. Using simulations of radiative-convective equilibrium forced by various radiative cooling profiles, we refute this mechanism by showing that an upper-tropospheric peak in cloud fraction persists even in simulations with no peak in clear-sky convergence. Instead, cloud fraction profiles seem to be controlled by cloud lifetimes — i.e., how long it takes for clouds to dissipate after they have detrained. A simple model of cloud evaporation shows that the small saturation deficit in the upper troposphere greatly extends cloud lifetimes there, while the large saturation deficit in the lower troposphere causes condensate to evaporate quickly. Since cloud mass flux must go to zero at the tropopause, a peak in cloud fraction emerges at a "sweet spot" below the tropopause where cloud lifetimes are long and there is still sufficient mass flux to be detrained.

Evolution of the Far-Infrared Cloud at Titan's South Pole

NASA Technical Reports Server (NTRS)

Jennings, Donald E.; Achterberg, R. K.; Cottini, V.; Anderson, C. M.; Flasar, F. M.; Nixon, C. A.; Bjoraker, G. L.; Kunde, V. G.; Carlson, R. C.; Guandique, E.;

Wave-Modulated CO2 Condensation in Mars' Polar Atmosphere From MGS/TES & MOLA and MRO/MCS.

NASA Astrophysics Data System (ADS)

Banfield, D. J.

2016-12-01

In Mars' polar night, atmospheric temperatures fall low enough to cause CO2 condensation. This has been empirically demonstrated by Mars Global Surveyor's (MGS) Mars Orbiter Laser Altimeter (MOLA), which identified reflections from above the surface, and MGS Radio Science (RS) and Thermal Emission Spectrometer (TES) and Mars Reconnaissance Orbiter's (MRO) Mars Climate Sounder (MCS), all of which showed polar night temperature profiles that were super-saturated. Detailed analysis of TES temperature profiles as well as numerical modeling both suggest that the stationary and traveling waves on the polar vortices are strong enough to significantly modulate the CO2 cloud condensation. However the extent to which this is actually occurring has not been quantified. The polar night CO2 condensation represents a significant amount of energy deposition, even if it were uniformly distributed. If instead it is concentrated in the cold sectors of the various waves, this can be a tremendous perturbation not only to the wave amplitudes (clipping them from going much below the CO2 condensation temperature), but also impacting their ability to transport heat and momentum poleward and upward, and thus it may also impact the maintenance and shape of the polar vortex itself. Mars' polar vortices remain barotropically unstable throughout the winter in spite of large amplitude waves in their vicinity. We have identified when and where the various waves (with their specific amplitudes and phases) in the vicinity of the polar vortex should modulate the CO2 condensation (see Figure of a meridional cross-section showing where no clouds are expected (blue), clouds should be ubiquitous (green) and waves should be required to form clouds (red)). We have also correlated this with the distribution of the actual observed cloud identifications from MGS MOLA and MRO MCS. We find only poor correlations between the MGS/TES identified wave modulated condensation predictions and actual simultaneous

Turbulence and cloud droplets in cumulus clouds

NASA Astrophysics Data System (ADS)

Saito, Izumi; Gotoh, Toshiyuki

2018-02-01

In this paper, we report on the successful and seamless simulation of turbulence and the evolution of cloud droplets to raindrops over 10 minutes from microscopic viewpoints by using direct numerical simulation. Included processes are condensation-evaporation, collision-coalescence of droplets with hydrodynamic interaction, Reynolds number dependent drag, and turbulent flow within a parcel that is ascending within a self-consistently determined updraft inside a cumulus cloud. We found that the altitude and the updraft velocity of the parcel, the mean supersaturation, and the liquid water content are insensitive to the turbulence intensity, and that when the turbulence intensity increases, the droplet number density swiftly decreases while the spectral width of droplets rapidly increases. This study marks the first time the evolution of the mass density distribution function has been successfully calculated from microscopic computations. The turbulence accelerated to form a second peak in the mass density distribution function, leading to the raindrop formation, and the radius of the largest drop was over 300 μm at the end of the simulation. We also found that cloud droplets modify the turbulence in a way that is unlike the Kolmogorov-Obukhov-Corrsin theory. For example, the temperature and water vapor spectra at low wavenumbers become shallower than {k}-5/3 in the inertial-convective range, and decrease slower than exponentially in the diffusive range. This spectra modification is explained by nonlinear interactions between turbulent mixing and the evaporation-condensation process associated with large numbers of droplets.

Stratocumulus Cloud Top Radiative Cooling and Cloud Base Updraft Speeds

NASA Astrophysics Data System (ADS)

Kazil, J.; Feingold, G.; Balsells, J.; Klinger, C.

2017-12-01

Cloud top radiative cooling is a primary driver of turbulence in the stratocumulus-topped marine boundary. A functional relationship between cloud top cooling and cloud base updraft speeds may therefore exist. A correlation of cloud top radiative cooling and cloud base updraft speeds has been recently identified empirically, providing a basis for satellite retrieval of cloud base updraft speeds. Such retrievals may enable analysis of aerosol-cloud interactions using satellite observations: Updraft speeds at cloud base co-determine supersaturation and therefore the activation of cloud condensation nuclei, which in turn co-determine cloud properties and precipitation formation. We use large eddy simulation and an off-line radiative transfer model to explore the relationship between cloud-top radiative cooling and cloud base updraft speeds in a marine stratocumulus cloud over the course of the diurnal cycle. We find that during daytime, at low cloud water path (CWP < 50 g m-2), cloud base updraft speeds and cloud top cooling are well-correlated, in agreement with the reported empirical relationship. During the night, in the absence of short-wave heating, CWP builds up (CWP > 50 g m-2) and long-wave emissions from cloud top saturate, while cloud base heating increases. In combination, cloud top cooling and cloud base updrafts become weakly anti-correlated. A functional relationship between cloud top cooling and cloud base updraft speed can hence be expected for stratocumulus clouds with a sufficiently low CWP and sub-saturated long-wave emissions, in particular during daytime. At higher CWPs, in particular at night, the relationship breaks down due to saturation of long-wave emissions from cloud top.

Cloud condensation nuclei activity and hygroscopicity of fresh and aged cooking organic aerosol

NASA Astrophysics Data System (ADS)

Li, Yanwei; Tasoglou, Antonios; Liangou, Aikaterini; Cain, Kerrigan P.; Jahn, Leif; Gu, Peishi; Kostenidou, Evangelia; Pandis, Spyros N.

2018-03-01

Cooking organic aerosol (COA) is potentially a significant fraction of organic particulate matter in urban areas. COA chemical aging experiments, using aerosol produced by grilling hamburgers, took place in a smog chamber in the presence of UV light or excess ozone. The water solubility distributions, cloud condensation nuclei (CCN) activity, and corresponding hygroscopicity of fresh and aged COA were measured. The average mobility equivalent activation diameter of the fresh particles at 0.4% supersaturation ranged from 87 to 126 nm and decreased for aged particles, ranging from 65 to 88 nm. Most of the fresh COA had water solubility less than 0.1 g L-1, even though the corresponding particles were quite CCN active. After aging, the COA fraction with water solubility greater than 0.1 g L-1 increased more than 2 times. Using the extended Köhler theory for multiple partially soluble components in order to predict the measured activation diameters, the COA solubility distribution alone could not explain the CCN activity. Surface tensions less than 30 dyn cm-1 were required to explain the measured activation diameters. In addition, COA particles appear to not be spherical, which can introduce uncertainties into the corresponding calculations.

A study of cloud microphysics and precipitation over the Tibetan Plateau by radar observations and cloud-resolving model simulations: Cloud Microphysics over Tibetan Plateau

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gao, Wenhua; Sui, Chung-Hsiung; Fan, Jiwen

Cloud microphysical properties and precipitation over the Tibetan Plateau (TP) are unique because of the high terrains, clean atmosphere, and sufficient water vapor. With dual-polarization precipitation radar and cloud radar measurements during the Third Tibetan Plateau Atmospheric Scientific Experiment (TIPEX-III), the simulated microphysics and precipitation by the Weather Research and Forecasting model (WRF) with the Chinese Academy of Meteorological Sciences (CAMS) microphysics and other microphysical schemes are investigated through a typical plateau rainfall event on 22 July 2014. Results show that the WRF-CAMS simulation reasonably reproduces the spatial distribution of 24-h accumulated precipitation, but has limitations in simulating time evolutionmore » of precipitation rates. The model-calculated polarimetric radar variables have biases as well, suggesting bias in modeled hydrometeor types. The raindrop sizes in convective region are larger than those in stratiform region indicated by the small intercept of raindrop size distribution in the former. The sensitivity experiments show that precipitation processes are sensitive to the changes of warm rain processes in condensation and nucleated droplet size (but less sensitive to evaporation process). Increasing droplet condensation produces the best area-averaged rain rate during weak convection period compared with the observation, suggesting a considerable bias in thermodynamics in the baseline simulation. Increasing the initial cloud droplet size causes the rain rate reduced by half, an opposite effect to that of increasing droplet condensation.« less

Cloud/climate sensitivity experiments

NASA Technical Reports Server (NTRS)

Roads, J. O.; Vallis, G. K.; Remer, L.

1982-01-01

A study of the relationships between large-scale cloud fields and large scale circulation patterns is presented. The basic tool is a multi-level numerical model comprising conservation equations for temperature, water vapor and cloud water and appropriate parameterizations for evaporation, condensation, precipitation and radiative feedbacks. Incorporating an equation for cloud water in a large-scale model is somewhat novel and allows the formation and advection of clouds to be treated explicitly. The model is run on a two-dimensional, vertical-horizontal grid with constant winds. It is shown that cloud cover increases with decreased eddy vertical velocity, decreased horizontal advection, decreased atmospheric temperature, increased surface temperature, and decreased precipitation efficiency. The cloud field is found to be well correlated with the relative humidity field except at the highest levels. When radiative feedbacks are incorporated and the temperature increased by increasing CO2 content, cloud amounts decrease at upper-levels or equivalently cloud top height falls. This reduces the temperature response, especially at upper levels, compared with an experiment in which cloud cover is fixed.

Morphology-Controlled Synthesis of Organometal Halide Perovskite Inverse Opals.

PubMed

Chen, Kun; Tüysüz, Harun

2015-11-09

The booming development of organometal halide perovskites in recent years has prompted the exploration of morphology-control strategies to improve their performance in photovoltaic, photonic, and optoelectronic applications. However, the preparation of organometal halide perovskites with high hierarchical architecture is still highly challenging and a general morphology-control method for various organometal halide perovskites has not been achieved. A mild and scalable method to prepare organometal halide perovskites in inverse opal morphology is presented that uses a polystyrene-based artificial opal as hard template. Our method is flexible and compatible with different halides and organic ammonium compositions. Thus, the perovskite inverse opal maintains the advantage of straightforward structure and band gap engineering. Furthermore, optoelectronic investigations reveal that morphology exerted influence on the conducting nature of organometal halide perovskites. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Influence of organic films on the evaporation and condensation of water in aerosol

PubMed Central

Davies, James F.; Miles, Rachael E. H.; Haddrell, Allen E.; Reid, Jonathan P.

2013-01-01

Uncertainties in quantifying the kinetics of evaporation and condensation of water from atmospheric aerosol are a significant contributor to the uncertainty in predicting cloud droplet number and the indirect effect of aerosols on climate. The influence of aerosol particle surface composition, particularly the impact of surface active organic films, on the condensation and evaporation coefficients remains ambiguous. Here, we report measurements of the influence of organic films on the evaporation and condensation of water from aerosol particles. Significant reductions in the evaporation coefficient are shown to result when condensed films are formed by monolayers of long-chain alcohols [CnH(2n+1)OH], with the value decreasing from 2.4 × 10−3 to 1.7 × 10−5 as n increases from 12 to 17. Temperature-dependent measurements confirm that a condensed film of long-range order must be formed to suppress the evaporation coefficient below 0.05. The condensation of water on a droplet coated in a condensed film is shown to be fast, with strong coherence of the long-chain alcohol molecules leading to islanding as the water droplet grows, opening up broad areas of uncoated surface on which water can condense rapidly. We conclude that multicomponent composition of organic films on the surface of atmospheric aerosol particles is likely to preclude the formation of condensed films and that the kinetics of water condensation during the activation of aerosol to form cloud droplets is likely to remain rapid. PMID:23674675

Influence of organic films on the evaporation and condensation of water in aerosol.

PubMed

Davies, James F; Miles, Rachael E H; Haddrell, Allen E; Reid, Jonathan P

2013-05-28

Uncertainties in quantifying the kinetics of evaporation and condensation of water from atmospheric aerosol are a significant contributor to the uncertainty in predicting cloud droplet number and the indirect effect of aerosols on climate. The influence of aerosol particle surface composition, particularly the impact of surface active organic films, on the condensation and evaporation coefficients remains ambiguous. Here, we report measurements of the influence of organic films on the evaporation and condensation of water from aerosol particles. Significant reductions in the evaporation coefficient are shown to result when condensed films are formed by monolayers of long-chain alcohols [C(n)H(2n+1)OH], with the value decreasing from 2.4 × 10(-3) to 1.7 × 10(-5) as n increases from 12 to 17. Temperature-dependent measurements confirm that a condensed film of long-range order must be formed to suppress the evaporation coefficient below 0.05. The condensation of water on a droplet coated in a condensed film is shown to be fast, with strong coherence of the long-chain alcohol molecules leading to islanding as the water droplet grows, opening up broad areas of uncoated surface on which water can condense rapidly. We conclude that multicomponent composition of organic films on the surface of atmospheric aerosol particles is likely to preclude the formation of condensed films and that the kinetics of water condensation during the activation of aerosol to form cloud droplets is likely to remain rapid.

Bulk assembly of organic metal halide nanotubes

DOE PAGES

Lin, Haoran; Zhou, Chenkun; Tian, Yu; ...

2017-10-16

The organic metal halide hybrids welcome a new member with a one-dimensional (1D) tubular structure. Herein we report the synthesis and characterization of a single crystalline bulk assembly of organic metal halide nanotubes, (C 6H 13N 4) 3Pb 2Br 7. In a metal halide nanotube, six face-sharing metal halide dimers (Pb 2Br 9 5–) connect at the corners to form rings that extend in one dimension, of which the inside and outside surfaces are coated with protonated hexamethylenetetramine (HMTA) cations (C 6H 13N 4 +). This unique 1D tubular structure possesses highly localized electronic states with strong quantum confinement, resultingmore » in the formation of self-trapped excitons that give strongly Stokes shifted broadband yellowish-white emission with a photoluminescence quantum efficiency (PLQE) of ~7%. Finally, having realized single crystalline bulk assemblies of two-dimensional (2D) wells, 1D wires, and now 1D tubes using organic metal halide hybrids, our work significantly advances the research on bulk assemblies of quantum-confined materials.« less

HCl in rocket exhaust clouds - Atmospheric dispersion, acid aerosol characteristics, and acid rain deposition

NASA Technical Reports Server (NTRS)

Pellett, G. L.; Sebacher, D. I.; Bendura, R. J.; Wornom, D. E.

1983-01-01

Both measurements and model calculations of the temporal dispersion of peak HCl (g + aq) concentration in Titan III exhaust clouds are found to be well characterized by one-term power-law decay expressions. The respective coefficients and decay exponents, however, are found to vary widely with meteorology. The HCl (g), HCl (g + aq), dewpoint, and temperature-pressure-altitude data for Titan III exhaust clouds are consistent with accurately calculated HCl/H2O vapor-liquid compositions for a model quasi-equilibrated flat surface aqueous aerosol. Some cloud evolution characteristics are also defined. Rapid and extensive condensation of aqueous acid clearly occurs during the first three min of cloud rise. Condensation is found to be intensified by the initial entrainment of relatively moist ambient air from lower levels, that is, from levels below eventual cloud stabilization. It is pointed out that if subsequent dilution air at stabilization altitude is significantly drier, a state of maximum condensation soon occurs, followed by an aerosol evaporation phase.

Simulation of the Upper Clouds and Hazes of Venus Using a Microphysical Cloud Model

NASA Astrophysics Data System (ADS)

McGouldrick, K.

2012-12-01

Several different microphysical and chemical models of the clouds of Venus have been developed in attempts to reproduce the in situ observations of the Venus clouds made by Pioneer Venus, Venera, and Vega descent probes (Turco et al., 1983 (Icarus 53:18-25), James et al, 1997 (Icarus 129:147-171), Imamura and Hashimoto, 2001 (J. Atm. Sci. 58:3597-3612), and McGouldrick and Toon, 2007 (Icarus 191:1-24)). The model of McGouldrick and Toon has successfully reproduced observations within the condensational middle and lower cloud decks of Venus (between about 48 and 57 km altitude, experiencing conditions similar to Earth's troposphere) and it now being extended to also simulate the microphysics occurring in the upper cloud deck (between altitudes of about 57 km and 70 km, experiencing conditions similar to Earth's stratosphere). In the upper clouds, aerosols composed of a solution of sulfuric acid in water are generated from the reservoir of available water vapor and sulfuric acid vapor that is photochemically produced. The manner of particle creation (e.g., activation of cloud condensation nuclei, or homogeneous or heterogeneous nucleation) is still incompletely understood, and the atmospheric environment has been measured to be not inconsistent with frozen aerosol particles (either sulfuric acid monohydrate or water ice). The material phase, viscosity, and surface tension of the aerosols (which are strongly dependent up on the local temperature and water vapor concentration) can affect the coagulation efficiencies of the aerosol, leading to variations in the size distributions, and other microphysical and radiative properties. Here, I present recent work exploring the effects of nucleation rates and coalescence efficiencies on the simulated Venus upper clouds.

The chemical evolution of molecular clouds

NASA Technical Reports Server (NTRS)

Iglesias, E.

1977-01-01

The nonequilibrium chemistry of dense molecular clouds (10,000 to 1 million hydrogen molecules per cu cm) is studied in the framework of a model that includes the latest published chemical data and most of the recent theoretical advances. In this model the only important external source of ionization is assumed to be high-energy cosmic-ray bombardment; standard charge-transfer reactions are taken into account as well as reactions that transfer charge from molecular ions to trace-metal atoms. Schemes are proposed for the synthesis of such species as NCO, HNCO, and CN. The role played by adsorption and condensation of molecules on the surface of dust grains is investigated, and effects on the chemical evolution of a dense molecular cloud are considered which result from varying the total density or the elemental abundances and from assuming negligible or severe condensation of gaseous species on dust grains. It is shown that the chemical-equilibrium time scale is given approximately by the depletion times of oxygen and nitrogen when the condensation efficiency is negligible; that this time scale is probably in the range from 1 to 4 million years, depending on the elemental composition and initial conditions in the cloud; and that this time scale is insensitive to variations in the total density.

Bose-Einstein condensates in charged black-hole spacetimes

NASA Astrophysics Data System (ADS)

Castellanos, Elías; Degollado, Juan Carlos; Lämmerzahl, Claus; Macías, Alfredo; Perlick, Volker

2018-01-01

We analyze Bose-Einstein condensates on three types of spherically symmetric and static charged black-hole spacetimes: the Reissner-Nordström spacetime, Hoffmann's Born-Infeld black-hole spacetime, and the regular Ayón-Beato-García spacetime. The Bose-Einstein condensate is modeled in terms of a massive scalar field that satisfies a Klein-Gordon equation with a self-interaction term. The scalar field is assumed to be uncharged and not self-gravitating. If the mass parameter of the scalar field is chosen sufficiently small, there are quasi-bound states of the scalar field that may be interpreted as dark matter clouds. We estimate the size and the total energy of such clouds around charged supermassive black holes and we investigate if their observable features can be used for discriminating between the different types of charged black holes.

Turbulence and star formation in molecular clouds

NASA Astrophysics Data System (ADS)

Larson, R. B.

1981-03-01

Consideration is given to the turbulence properties of molecular clouds and their implications for star formation. Data for 54 molecular clouds and condensations is presented which reveals cloud velocity dispersion and region size to follow a power-law relation, similar to the Kolmogoroff law for subsonic turbulence. Examination of the dynamics of the molecular clouds for which mass determinations are available reveals essentially all of them to be gravitationally bound, and to approximately satisfy the virial theorem. The observation of moderate scatter in the dispersion-size relation is noted to imply that most regions have not collapsed much since formation, suggesting that processes of turbulent hydrodynamics have played an important role in producing the observed substructures. A lower limit to the size of subcondensations at which their internal motions are no longer supersonic is shown to predict a minimum protostellar mass on the order of a few tenths of a solar mass, while massive protostellar clumps are found to develop complex internal structures, probably leading to the formation of prestellar condensation nuclei. The observed turbulence of molecular clouds is noted to imply lifetimes of less than 10 million years.

The Impact of Aerosols on Cloud and Precipitation Processes: Cloud-Resolving Model Simulations

NASA Technical Reports Server (NTRS)

Tao, Wei-Kuo; Li, X.; Khain, A.; Simpson, S.

2005-01-01

Cloud microphysics are inevitable affected by the smoke particle (CCN, cloud condensation nuclei) size distributions below the clouds, Therefore, size distributions parameterized as spectral bin microphysics are needed to explicitly study the effect of atmospheric aerosol concentration on cloud development, rainfall production, and rainfall rates for convective clouds. Recently, a detailed spectral-bin microphysical scheme was implemented into the the Goddard Cumulus Ensemble (GCE) model. The formulation for the explicit spectral-bim microphysical processes is based on solving stochastic kinetic equations for the size distribution functions of water droplets (i.e., cloud droplets and raindrops), and several types of ice particles [i.e., pristine ice crystals (columnar and plate-like), snow (dendrites and aggregates), graupel and frozen drops/hail]. Each type is described by a special size distribution function containing many categories (i.e., 33 bins). Atmospheric aerosols are also described using number density size-distribution functions.

Lagrangian condensation microphysics with Twomey CCN activation

NASA Astrophysics Data System (ADS)

Grabowski, Wojciech W.; Dziekan, Piotr; Pawlowska, Hanna

2018-01-01

We report the development of a novel Lagrangian microphysics methodology for simulations of warm ice-free clouds. The approach applies the traditional Eulerian method for the momentum and continuous thermodynamic fields such as the temperature and water vapor mixing ratio, and uses Lagrangian super-droplets to represent condensed phase such as cloud droplets and drizzle or rain drops. In other applications of the Lagrangian warm-rain microphysics, the super-droplets outside clouds represent unactivated cloud condensation nuclei (CCN) that become activated upon entering a cloud and can further grow through diffusional and collisional processes. The original methodology allows for the detailed study of not only effects of CCN on cloud microphysics and dynamics, but also CCN processing by a cloud. However, when cloud processing is not of interest, a simpler and computationally more efficient approach can be used with super-droplets forming only when CCN is activated and no super-droplet existing outside a cloud. This is possible by applying the Twomey activation scheme where the local supersaturation dictates the concentration of cloud droplets that need to be present inside a cloudy volume, as typically used in Eulerian bin microphysics schemes. Since a cloud volume is a small fraction of the computational domain volume, the Twomey super-droplets provide significant computational advantage when compared to the original super-droplet methodology. Additional advantage comes from significantly longer time steps that can be used when modeling of CCN deliquescence is avoided. Moreover, other formulation of the droplet activation can be applied in case of low vertical resolution of the host model, for instance, linking the concentration of activated cloud droplets to the local updraft speed. This paper discusses the development and testing of the Twomey super-droplet methodology, focusing on the activation and diffusional growth. Details of the activation

Method for recovering hydrocarbons from molten metal halides

DOEpatents

Pell, Melvyn B.

1979-01-01

In a process for hydrocracking heavy carbonaceous materials by contacting such carbonaceous materials with hydrogen in the presence of a molten metal halide catalyst to produce hydrocarbons having lower molecular weights and thereafter recovering the hydrocarbons so produced from the molten metal halide, an improvement comprising injecting into the spent molten metal halide, a liquid low-boiling hydrocarbon stream is disclosed.

Evolution of the Far-Infrared Cloud at Titan's South Pole

NASA Technical Reports Server (NTRS)

Jennings, Donald E.; Achterberg, R. K.; Cottini, V.; Anderson, C. M.; Flasar, F. M.; Nixon, C. A.; Bjoraker, G. L.; Kunde, V. G.; Carlson, R. C.; Guandique, E.;

Divergent electronic structures of isoelectronic metalloclusters: tungsten(II) halides and rhenium(III) chalcogenide halides.

PubMed

Gray, Thomas G

2009-03-02

Same but different: DFT calculations on hexanuclear tungsten(II) halide clusters [W(6)X(8)X'(6)](2-) (X, X'=Cl, Br, I) indicate a breakdown in the isoelectronic analogy between themselves and the isostructural rhenium(III) chalcogenide clusters [Re(6)S(8)X(6)](4-) (see figure).The hexanuclear tungsten(II) halide clusters and the sulfido-halide clusters of rhenium(III) are subsets of a broad system of 24-electron metal-metal bonded assemblies that share a common structure. Tungsten(II) halide clusters and rhenium(III) sulfide clusters luminesce from triplet excited states upon ultraviolet or visible excitation; emission from both cluster series has been extensively characterized elsewhere. Reported here are density-functional theory studies of the nine permutations of [W(6)X(8)X'(6)](2-) (X, X'=Cl, Br, I). Ground-state properties including geometries, harmonic vibrational frequencies, and orbital energy-level diagrams, have been calculated. Comparison is made to the sulfide clusters of rhenium(III), of which [Re(6)S(8)Cl(6)](4-) is representative. [W(6)X(8)X'(6)](2-) and [Re(6)S(8)Cl(6)](4-) possess disparate electronic structures owing to the greater covalency of the metal-sulfur bond and hence of the [Re(6)S(8)](2+) core. Low-lying virtual orbitals are raised in energy in [Re(6)S(8)Cl(6)](4-) with the result that the LUMO+7 (or LUMO+8 in some cases) of tungsten(II) halide clusters is the LUMO of [Re(6)S(8)Cl(6)](4-) species. An inversion of the HOMO and HOMO-1 between the two cluster series also occurs. Time-dependent density-functional calculations using asymptotically correct functionals do not recapture the experimentally observed periodic trend in [W(6)X(14)](2-) luminescence (E(em) increasing in the order [W(6)Cl(14)](2-) < [W(6)Br(14)](2-) < [W(6)I(14)](2-)), predicting instead that emission energies decrease with incorporation of the heavier halides. This circumstance is either a gross failure of the time-dependent formalism of DFT or it indicates extensive

METHOD OF PREPARING METAL HALIDES

DOEpatents

Hendrickson, A.V.

1958-11-18

The conversion of plutonium halides from plutonium peroxide can be done by washing the peroxide with hydrogen peroxide, drying the peroxide, passing a dry gaseous hydrohalide over the surface of the peroxide at a temperature of about lOO icient laborato C until the reaction rate has stabillzed, and then ralsing the reaction temperature to between 400 and 600 icient laborato C until the conversion to plutonium halide is substantially complete.

Reducing Errors in Satellite Simulated Views of Clouds with an Improved Parameterization of Unresolved Scales

NASA Astrophysics Data System (ADS)

Hillman, B. R.; Marchand, R.; Ackerman, T. P.

2016-12-01

Satellite instrument simulators have emerged as a means to reduce errors in model evaluation by producing simulated or psuedo-retrievals from model fields, which account for limitations in the satellite retrieval process. Because of the mismatch in resolved scales between satellite retrievals and large-scale models, model cloud fields must first be downscaled to scales consistent with satellite retrievals. This downscaling is analogous to that required for model radiative transfer calculations. The assumption is often made in both model radiative transfer codes and satellite simulators that the unresolved clouds follow maximum-random overlap with horizontally homogeneous cloud condensate amounts. We examine errors in simulated MISR and CloudSat retrievals that arise due to these assumptions by applying the MISR and CloudSat simulators to cloud resolving model (CRM) output generated by the Super-parameterized Community Atmosphere Model (SP-CAM). Errors are quantified by comparing simulated retrievals performed directly on the CRM fields with those simulated by first averaging the CRM fields to approximately 2-degree resolution, applying a "subcolumn generator" to regenerate psuedo-resolved cloud and precipitation condensate fields, and then applying the MISR and CloudSat simulators on the regenerated condensate fields. We show that errors due to both assumptions of maximum-random overlap and homogeneous condensate are significant (relative to uncertainties in the observations and other simulator limitations). The treatment of precipitation is particularly problematic for CloudSat-simulated radar reflectivity. We introduce an improved subcolumn generator for use with the simulators, and show that these errors can be greatly reduced by replacing the maximum-random overlap assumption with the more realistic generalized overlap and incorporating a simple parameterization of subgrid-scale cloud and precipitation condensate heterogeneity. Sandia National Laboratories is a

Development of a thermal gradient cloud condensation nucleus spectrometer

NASA Technical Reports Server (NTRS)

Leu, Ming-Taun; Friedl, R.

2004-01-01

Droplet clouds are one of the most important factors controlling the albedo and hence the temperature of out planet. Anthropogenic aerosols, such as black carbon (BC) organic carbon (OC) and sulfate, have a strong influence on cloud albedo. IPCC (2001) has estimated the global mean forcing from aerosols to be potentially as large as that of green house gases but opposite in sign. However, the uncertainties associated with the indirect aerosol forcing preclude a quantitative estimate. An additional impact on the indirect aerosol forcing, not quantified by IPCC, arises from recently identified chemical factors, for examples, interactions of atmospheric soluble gases, slightly soluble solutes, and organic substance with aerosols, which may influence the formation of cloud droplets. Recent studies suggest that inclusion of chemical effects on aerosol droplets. We plan to conduct several critical laboratory experiments that will reduce the uncertainty associated with indirect radiative forcing due to chemical modification of sulfate and BC aerosols by ambient gases.

Corona discharge induced snow formation in a cloud chamber.

PubMed

Ju, Jingjing; Wang, Tie-Jun; Li, Ruxin; Du, Shengzhe; Sun, Haiyi; Liu, Yonghong; Tian, Ye; Bai, Yafeng; Liu, Yaoxiang; Chen, Na; Wang, Jingwei; Wang, Cheng; Liu, Jiansheng; Chin, S L; Xu, Zhizhan

2017-09-18

Artificial rainmaking is in strong demand especially in arid regions. Traditional methods of seeding various Cloud Condensation Nuclei (CCN) into the clouds are costly and not environment friendly. Possible solutions based on ionization were proposed more than 100 years ago but there is still a lack of convincing verification or evidence. In this report, we demonstrated for the first time the condensation and precipitation (or snowfall) induced by a corona discharge inside a cloud chamber. Ionic wind was found to have played a more significant role than ions as extra CCN. In comparison with another newly emerging femtosecond laser filamentation ionization method, the snow precipitation induced by the corona discharge has about 4 orders of magnitude higher wall-plug efficiency under similar conditions.

TRANSURANIC METAL HALIDES AND A PROCESS FOR THE PRODUCTION THEREOF

DOEpatents

Fried, S.

1951-03-20

Halides of transuranic elements are prepared by contacting with aluminum and a halogen, or with an aluminum halide, a transuranic metal oxide, oxyhalide, halide, or mixture thereof at an elevated temperature.

Broadening of cloud droplet spectra through turbulent entrainment and eddy hopping

NASA Astrophysics Data System (ADS)

Abade, Gustavo; Grabowski, Wojciech; Pawlowska, Hanna

2017-11-01

This work discusses the effect of cloud turbulence and turbulent entrainment on the evolution of the cloud droplet-size spectrum. We simulate an ensemble of idealized turbulent cloud parcels that are subject to entrainment events, modeled as a random Poisson process. Entrainment events, subsequent turbulent mixing inside the parcel, supersaturation fluctuations, and the resulting stochastic droplet growth by condensation are simulated using a Monte Carlo scheme. Quantities characterizing the turbulence intensity, entrainment rate and the mean fraction of environmental air entrained in an event are specified as external parameters. Cloud microphysics is described by applying Lagrangian particles, the so-called superdroplets. They are either unactivated cloud condensation nuclei (CCN) or cloud droplets that form from activated CCN. The model accounts for the transport of environmental CCN into the cloud by the entraining eddies at the cloud edge. Turbulent mixing of the entrained dry air with cloudy air is described using a linear model. We show that turbulence plays an important role in aiding entrained CCN to activate, providing a source of small cloud droplets and thus broadening the droplet size distribution. Further simulation results will be reported at the meeting.

Unraveling the Role of Monovalent Halides in Mixed-Halide Organic-Inorganic Perovskites.

PubMed

Deepa, Melepurath; Ramos, F Javier; Shivaprasad, S M; Ahmad, Shahzada

2016-03-16

The performance of perovskite solar cells is strongly influenced by the composition and microstructure of the perovskite. A recent approach to improve the power conversion efficiencies utilized mixed-halide perovskites, but the halide ions and their roles were not directly studied. Unraveling their precise location in the perovskite layer is of paramount importance. Here, we investigated four different perovskites by using X-ray photoelectron spectroscopy, and found that among the three studied mixed-halide perovskites, CH3 NH3 Pb(I0.74 Br0.26 )3 and CH3 NH3 PbBr3-x Clx show peaks that unambiguously demonstrate the presence of iodide and bromide in the former, and bromide and chloride in the latter. The CH3 NH3 PbI3-x Clx perovskite shows anomalous behavior, the iodide content far outweighs that of the chloride; a small proportion of chloride, in all likelihood, resides deep within the TiO2 /absorber layer. Our study reveals that there are many distinguishable structural differences between these perovskites, and that these directly impact the photovoltaic performances. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Compositional Grading in an Impact-produced Spherule Bed, Barberton Greenstone Belt, South Africa: A Key to Condensation History of Rock Vapor Clouds

NASA Technical Reports Server (NTRS)

Krull, A. E.; Lowe, D. R.; Byerly, G. R.

2003-01-01

The chemical and physical processes by which spherules form during the condensation of impact-produced rock vapor clouds are poorly understood. Although efforts have been made to model the processes of spherule formation, there is presently a paucity of field data to constrain the resulting theoretical models. The present study examines the vertical compositional variability in a single early Archean spherule bed in the Barberton Greenstone Belt (BGB), South Africa, in order to better identify the process by which impact vapor clouds condense and spherules form and accumulate. The BGB spherule beds are suitable for this type of study because of their great thickness, often exceeding 25cm of pure spherules, due to the massive sizes of the impactors. Two main problems complicate analysis of vertical compositional variability of graded spherule beds: (1) differential settling of particles in both the vapor and water column due to density and size differences and (2) turbulence within the vapor cloud. The present study compares sections of spherule bed S3 from four different depositional environments in the Barberton Greenstone Belt: (1) The Sheba Mine section (SAF-381) was deposited under fairly low energy conditions in deep water, providing a nice fallout sequence, and also has abundant Ni-rich spinels; (2) Jay's Chert section (SAF-380) was deposited in subaerial to shallow-water conditions with extensive post-depositional reworking by currents. The spherules also have preserved spinels; (3) the Loop Road section (loc. SAF-295; samp. KSA-7) was moderately reworked and has only rare preservation of spinels; and (4) the shallow-water Barite Syncline section (loc. SAF-206; samp KSA-1) has few to no spinels preserved and is not reworked. Although all of the spherule beds have been altered by silica diagenesis and K-metasomatism, most of the compositional differences between these sections appear to reflect their diagenetic histories, possibly related to their differing

The Impact of Aerosols on Cloud and Precipitation Processes: Cloud-Resolving Model Simulations

NASA Technical Reports Server (NTRS)

Tao, Wei-Kuo; Khain, A.; Simpson, S.; Johnson, D.; Li, X.; Remer, L.

2003-01-01

Cloud microphysics are inevitably affected by the smoke particle (CCN, cloud condensation nuclei) size distributions below the clouds. Therefore, size distributions parameterized as spectral bin microphysics are needed to explicitly study the effects of atmospheric aerosol concentration on cloud development, rainfall production, and rainfall rates for convective clouds. Recently, two detailed spectral-bin microphysical schemes were implemented into the Goddard Cumulus Ensemble (GCE) model. The formulation for the explicit spectral-bin microphysical processes is based on solving stochastic kinetic equations for the size distribution functions of water droplets (i.e., cloud droplets and raindrops), and several types of ice particles [i.e.,pristine ice crystals (columnar and plate-like), snow (dendrites and aggregates), graupel and frozen drops/hail]. Each type is described by a special size distribution function containing many categories (i.e. 33 bins). Atmospheric aerosols are also described using number density size-distribution functions.A spectral-bin microphysical model is very expensive from a from a computational point of view and has only been implemented into the 2D version of the GCE at the present time. The model is tested by studying the evolution of deep tropical clouds in the west Pacific warm pool region using identical thermodynamic conditions but with different concentrations of CCN: a low "clean" concentration and a high "dirty" concentration. Besides the initial differences in aerosol concentration, preliminary results indicate that the low CCN concentration case produces rainfall at the surface sooner than the high CCN case but has less cloud water mass aloft. Because the spectral-bin model explicitly calculates and allows for the examination of both the mass and number concentration of species in each size categor, a detailed analysis of the instantaneous size spectrum can be obtained for the two cases. It is shown that since the low CCN case

New particle formation and growth in biomass burning plumes: An important source of cloud condensation nuclei

NASA Astrophysics Data System (ADS)

Hennigan, Christopher J.; Westervelt, Daniel M.; Riipinen, Ilona; Engelhart, Gabriella J.; Lee, Taehyoung; Collett, Jeffrey L., Jr.; Pandis, Spyros N.; Adams, Peter J.; Robinson, Allen L.

2012-05-01

Experiments were performed in an environmental chamber to characterize the effects of photo-chemical aging on biomass burning emissions. Photo-oxidation of dilute exhaust from combustion of 12 different North American fuels induced significant new particle formation that increased the particle number concentration by a factor of four (median value). The production of secondary organic aerosol caused these new particles to grow rapidly, significantly enhancing cloud condensation nuclei (CCN) concentrations. Using inputs derived from these new data, global model simulations predict that nucleation in photo-chemically aging fire plumes produces dramatically higher CCN concentrations over widespread areas of the southern hemisphere during the dry, burning season (Sept.-Oct.), improving model predictions of surface CCN concentrations. The annual indirect forcing from CCN resulting from nucleation and growth in biomass burning plumes is predicted to be -0.2 W m-2, demonstrating that this effect has a significant impact on climate that has not been previously considered.

Characterization and parameterization of aerosol cloud condensation nuclei activation under different pollution conditions

PubMed Central

Che, H. C.; Zhang, X. Y.; Wang, Y. Q.; Zhang, L.; Shen, X. J.; Zhang, Y. M.; Ma, Q. L.; Sun, J. Y.; Zhang, Y. W.; Wang, T. T.

2016-01-01

To better understand the cloud condensation nuclei (CCN) activation capacity of aerosol particles in different pollution conditions, a long-term field experiment was carried out at a regional GAW (Global Atmosphere Watch) station in the Yangtze River Delta area of China. The homogeneity of aerosol particles was the highest in clean weather, with the highest active fraction of all the weather types. For pollution with the same visibility, the residual aerosol particles in higher relative humidity weather conditions were more externally mixed and heterogeneous, with a lower hygroscopic capacity. The hygroscopic capacity (κ) of organic aerosols can be classified into 0.1 and 0.2 in different weather types. The particles at ~150 nm were easily activated in haze weather conditions. For CCN predictions, the bulk chemical composition method was closer to observations at low supersaturations (≤0.1%), whereas when the supersaturation was ≥0.2%, the size-resolved chemical composition method was more accurate. As for the mixing state of the aerosol particles, in haze, heavy haze, and severe haze weather conditions CCN predictions based on the internal mixing assumption were robust, whereas for other weather conditions, predictions based on the external mixing assumption were more accurate. PMID:27075947

A cloud-resolving model study of aerosol-cloud correlation in a pristine maritime environment

NASA Astrophysics Data System (ADS)

Nishant, Nidhi; Sherwood, Steven C.

2017-06-01

In convective clouds, satellite-observed deepening or increased amount of clouds with increasing aerosol concentration has been reported and is sometimes interpreted as aerosol-induced invigoration of the clouds. However, such correlations can be affected by meteorological factors that affect both aerosol and clouds, as well as observational issues. In this study, we examine the behavior in a 660 × 660 km2 region of the South Pacific during June 2007, previously found by Koren et al. (2014) to show strong correlation between cloud fraction, cloud top pressure, and aerosols, using a cloud-resolving model with meteorological boundary conditions specified from a reanalysis. The model assumes constant aerosol loading, yet reproduces vigorous clouds at times of high real-world aerosol concentrations. Days with high- and low-aerosol loading exhibit deep-convective and shallow clouds, respectively, in both observations and the simulation. Synoptic analysis shows that vigorous clouds occur at times of strong surface troughs, which are associated with high winds and advection of boundary layer air from the Southern Ocean where sea-salt aerosol is abundant, thus accounting for the high correlation. Our model results show that aerosol-cloud relationships can be explained by coexisting but independent wind-aerosol and wind-cloud relationships and that no cloud condensation nuclei effect is required.

Aerosol-Cloud Interactions and Cloud Microphysical Properties in the Asir Region of Saudi Arabia

NASA Astrophysics Data System (ADS)

Kucera, P. A.; Axisa, D.; Burger, R. P.; Li, R.; Collins, D. R.; Freney, E. J.; Buseck, P. R.

2009-12-01

In recent advertent and inadvertent weather modification studies, a considerable effort has been made to understand the impact of varying aerosol properties and concentration on cloud properties. Significant uncertainties exist with aerosol-cloud interactions for which complex microphysical processes link the aerosol and cloud properties. Under almost all environmental conditions, increased aerosol concentrations within polluted air masses will enhance cloud droplet concentration relative to that in unperturbed regions. The interaction between dust particles and clouds are significant, yet the conditions in which dust particles become cloud condensation nuclei (CCN) are uncertain. In order to quantify this aerosol effect on clouds and precipitation, a field campaign was launched in the Asir region, located adjacent to the Red Sea in the southwest region of Saudi Arabia. Ground measurements of aerosol size distributions, hygroscopic growth factors, CCN concentrations as well as aircraft measurements of cloud hydrometeor size distributions were observed in the Asir region in August 2009. The presentation will include a summary of the analysis and results with a focus on aerosol-cloud interactions and cloud microphysical properties observed during the convective season in the Asir region.

Investigation of surface halide modification of nitrile butadiene rubber

NASA Astrophysics Data System (ADS)

Sukhareva, K. V.; Mikhailov, I. A.; Andriasyan, Yu O.; Mastalygina, E. E.; Popov, A. A.

2017-12-01

The investigation is devoted to the novel technology of surface halide modification of rubber samples based on nitrile butadiene rubber (NBR). 1,1,2-trifluoro-1,2,2-trichlorethane was used as halide modifier. The developed technology is characterized by production stages reduction to one by means of treating the rubber compound with a halide modifier. The surface halide modification of compounds based on nitrile butadiene rubber (NBR) was determined to result in increase of resistance to thermal oxidation and aggressive media. The conducted research revealed the influence of modification time on chemical resistance and physical-mechanical properties of rubbers under investigation.

Unraveling luminescence mechanisms in zero-dimensional halide perovskites

DOE PAGES

Han, Dan; Shi, Hongliang; Ming, Wenmei; ...

2018-01-01

Zero-dimensional (0D) halides perovskites, in which anionic metal-halide octahedra (MX 6 ) 4− are separated by organic or inorganic countercations, have recently shown promise as excellent luminescent materials.

Unraveling luminescence mechanisms in zero-dimensional halide perovskites

DOE Office of Scientific and Technical Information (OSTI.GOV)

Han, Dan; Shi, Hongliang; Ming, Wenmei

Zero-dimensional (0D) halides perovskites, in which anionic metal-halide octahedra (MX 6 ) 4− are separated by organic or inorganic countercations, have recently shown promise as excellent luminescent materials.

Unraveling luminescence mechanisms in zero-dimensional halide perovskites

DOE PAGES

Han, Dan; Shi, Hongliang; Ming, Wenmei; ...

2018-05-18

Here, zero-dimensional (0D) halides perovskites, in which anionic metal-halide octahedra (MX 6) 4– are separated by organic or inorganic countercations, have recently shown promise as excellent luminescent materials.

Statistical properties of a cloud ensemble - A numerical study

NASA Technical Reports Server (NTRS)

Tao, Wei-Kuo; Simpson, Joanne; Soong, Su-Tzai

1987-01-01

The statistical properties of cloud ensembles under a specified large-scale environment, such as mass flux by cloud drafts and vertical velocity as well as the condensation and evaporation associated with these cloud drafts, are examined using a three-dimensional numerical cloud ensemble model described by Soong and Ogura (1980) and Tao and Soong (1986). The cloud drafts are classified as active and inactive, and separate contributions to cloud statistics in areas of different cloud activity are then evaluated. The model results compare well with results obtained from aircraft measurements of a well-organized ITCZ rainband that occurred on August 12, 1974, during the Global Atmospheric Research Program's Atlantic Tropical Experiment.

Myeloperoxidase-Halide-Hydrogen Peroxide Antibacterial System

PubMed Central

Klebanoff, Seymour J.

1968-01-01

An antibacterial effect of myeloperoxidase, a halide, such as iodide, bromide, or chloride ion, and H2O2 on Escherichia coli or Lactobacillus acidophilus is described. When L. acidophilus was employed, the addition of H2O2 was not required; however, the protective effect of catalase suggested that, in this instance, H2O2 was generated by the organisms. The antibacterial effect was largely prevented by preheating the myeloperoxidase at 80 C or greater for 10 min or by the addition of a number of inhibitors; it was most active at the most acid pH employed (5.0). Lactoperoxidase was considerably less effective than was myeloperoxidase when chloride was the halide employed. Myeloperoxidase, at high concentrations, exerted an antibacterial effect on L. acidophilus in the absence of added halide, which also was temperature- and catalase-sensitive. Peroxidase was extracted from intact guinea pig leukocytes by weak acid, and the extract with peroxidase activity had antibacterial properties which were similar, in many respects, to those of the purified preparation of myeloperoxidase. Under appropriate conditions, the antibacterial effect was increased by halides and by H2O2 and was decreased by catalase, as well as by cyanide, azide, Tapazole, and thiosulfate. This suggests that, under the conditions employed, the antibacterial properties of a weak acid extract of guinea pig leukocytes is due, in part, to its peroxidase content, particularly if a halide is present in the reaction mixture. A heat-stable antibacterial agent or agents also appear to be present in the extract. PMID:4970226

Eulerian and Lagrangian approaches to multidimensional condensation and collection

NASA Astrophysics Data System (ADS)

Li, Xiang-Yu; Brandenburg, A.; Haugen, N. E. L.; Svensson, G.

2017-06-01

Turbulence is argued to play a crucial role in cloud droplet growth. The combined problem of turbulence and cloud droplet growth is numerically challenging. Here an Eulerian scheme based on the Smoluchowski equation is compared with two Lagrangian superparticle (or superdroplet) schemes in the presence of condensation and collection. The growth processes are studied either separately or in combination using either two-dimensional turbulence, a steady flow or just gravitational acceleration without gas flow. Good agreement between the different schemes for the time evolution of the size spectra is observed in the presence of gravity or turbulence. The Lagrangian superparticle schemes are found to be superior over the Eulerian one in terms of computational performance. However, it is shown that the use of interpolation schemes such as the cloud-in-cell algorithm is detrimental in connection with superparticle or superdroplet approaches. Furthermore, the use of symmetric over asymmetric collection schemes is shown to reduce the amount of scatter in the results. For the Eulerian scheme, gravitational collection is rather sensitive to the mass bin resolution, but not so in the case with turbulence.