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  • Author or Editor: John H. Seinfeld x
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Miao-Ling Lu
and
John H. Seinfeld

Abstract

A total of 98 three-dimensional large-eddy simulations (LESs) of marine stratocumulus clouds covering both nighttime and daytime conditions were performed to explore the response of cloud optical depth (τ) to various aerosol number concentrations (Na = 50–2500 cm−3) and the covarying meteorological conditions (large-scale divergence rate and SST). The idealized First International Satellite Cloud Climatology Project (ISCCP) Regional Experiment (FIRE) and the Atlantic Stratocumulus Transition Experiment (ASTEX) Lagrangian 1 sounding profiles were used to represent the lightly and heavily drizzling cases, respectively. The first and second aerosol indirect effects are identified. Through statistical analysis, τ is found be to both positively correlated with Na and cloud liquid water path (LWP) with a higher correlation associated with LWP, which is predominantly regulated by large-scale subsidence and SST. Clouds with high LWP occur under low SST or weak large-scale subsidence. Introduction of a small amount of giant sea salt aerosol into the simulation lowers the number of cloud droplets activated, results in larger cloud droplets, and initiates precipitation for nondrizzling polluted clouds or precedes the precipitation process for drizzling clouds. However, giant sea salt aerosol is found to have a negligible effect on τ for lightly precipitating cases, while resulting in a relative reduction of τ of 3%–77% (increasing with Na , for Na = 1000–2500 cm−3) for heavily precipitating cases, suggesting that the impact of giant sea salt is only important for moist and potentially convective clouds. Finally, a regression analysis of the simulations shows that the second indirect effect is more evident in clear than polluted cases. The second indirect effect is found to enhance (reduce) the overall aerosol indirect effect for heavily (lightly) drizzling clouds; that is, τ is larger (smaller) for the same relative change in Na than considering the Twomey (first indirect) effect alone. The aerosol indirect effect (on τ) is lessened in the daytime afternoon conditions and is dominated by the Twomey effect; however, the effect in the early morning is close but slightly smaller than that in the nocturnal run. Diurnal variations of the aerosol indirect effect should be considered to accurately assess its magnitude.

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Robert G. Lamb
,
Wen H. Chen
, and
John H. Seinfeld

Abstract

Numerico-empirical expressions for the particle displacement probability density function from which the mean concentration of material in turbulent fluid may be obtained are derived from the numerical planetary boundary layer model of Deardorff. These expressions are then used to compute profiles of the mean, cross-wind-integrated concentration of an inert pollutant issuing from a continuous point source below a stable layer. Profiles are derived for each of two conditions of atmospheric stability: zi/L=0 and –4.5, where zi is the inversion base height and L the Monin-Obukhov length. The resulting concentration profiles [referred to as the numerico-empirical (NE) profiles] are then used in two separate experiments designed to assess the adequacy of conventional atmospheric diffusion formulations.

First, the validity of the atmospheric diffusion equation is assessed by determining for each of the two stabilities cited above the profile of vertical eddy diffusivity that produces the closest fit of the mean concentration predicted by the atmospheric diffusion equation with the NE profiles.

Second, comparisons are made between the NE profiles and the corresponding concentration distributions predicted by the Gaussian plume formula with Pasquill-Gifford dispersion parameters, and the Gaussian puff equation with McElroy-Pooler travel-time-dependent dispersion parameters.

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Miao-Ling Lu
,
Jian Wang
,
Richard C. Flagan
,
John H. Seinfeld
,
Andrew Freedman
,
Robert A. McClatchey
, and
Haflidi H. Jonsson

Abstract

Regions of enhanced humidity in the vicinity of cumulus clouds, so-called cloud halos, reflect features of cloud evolution, exert radiative effects, and may serve as a locus for new particle formation. Reported here are the results of an aircraft sampling campaign carried out near Oahu, Hawaii, from 31 July through 10 August 2001, aimed at characterizing the properties of trade wind cumulus cloud halos. An Aerodyne Research, Inc., fast spectroscopic water vapor sensor, flown for the first time in this campaign, allowed characterization of humidity properties at 10-m spatial resolution. Statistical properties of 60 traverses through cloud halos over the campaign were in general agreement with measurements reported by Perry and Hobbs. One particularly long-lived cloud is analyzed in detail, through both airborne measurement and numerical simulation, to track evolution of the cloud halos over the cloud's lifetime. Results of both observation and the simulation show that cloud halos tend to be broad at lower levels and narrow at upper levels, and broader on the downshear side than on the upshear side, broadening with time particularly in the downshear direction. The high correlation of clear-air turbulence distribution with the halo distribution temporally and spatially suggests that the halo forms, in part, due to turbulent mixing at the cloud boundary. Radiative calculations carried out on the simulated cloud and halo field indicate that the halo radiative effect is largest near cloud top during mature and dissipation stages. The halo-enhanced atmospheric shortwave absorption, averaged over this period, is about 1.3% of total solar absorption in the column.

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Lynn M. Russell
,
Kevin J. Noone
,
Ronald J. Ferek
,
Robert A. Pockalny
,
Richard C. Flagan
, and
John H. Seinfeld

Abstract

Polycyclic aromatic hydrocarbons (PAHs) have been sampled in marine stratiform clouds to identify the contribution of anthropogenic combustion emissions in activation of aerosol to cloud droplets. The Monterey Area Ship Track experiment provided an opportunity to acquire data on the role of organic compounds in ambient clouds and in ship tracks identified in satellite images. Identification of PAHs in cloud droplet residual samples indicates that several PAHs are present in cloud condensation nuclei in anthropogenically influenced air and do result in activated droplets in cloud. These results establish the presence of combustion products, such as PAHs, in submicrometer aerosols in anthropogenically influenced marine air, with enhanced concentrations in air polluted by ship effluent. The presence of PAHs in droplet residuals in anthropogenically influenced air masses indicates that some fraction of those combustion products is present in the cloud condensation nuclei that activate in cloud. Although a sufficient mass of droplet residuals was not collected to establish a similar role for organics from measurements in satellite-identified ship tracks, the available evidence from the fraction of organics present in the interstitial aerosol is consistent with part of the organic fraction partitioning to the droplet population. In addition, the probability that a compound will be found in cloud droplets rather than in the unactivated aerosol and the compound’s water solubility are compared. The PAHs studied are only weakly soluble in water, but most of the sparse data collected support more soluble compounds having a higher probability of activation.

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Tarah M. Sharon
,
Bruce A. Albrecht
,
Haflidi H. Jonsson
,
Patrick Minnis
,
Mandana M. Khaiyer
,
Timothy M. van Reken
,
John Seinfeld
, and
Rick Flagan

Abstract

A cloud rift is characterized as a large-scale, persistent area of broken, low-reflectivity stratocumulus clouds usually surrounded by a solid deck of stratocumulus. A rift observed off the coast of California was investigated using an instrumented aircraft to compare the aerosol, cloud microphysical, and thermodynamic properties in the rift with those of the surrounding solid stratocumulus deck. The microphysical characteristics in the solid stratocumulus deck differ substantially from those of a broken, cellular rift where cloud droplet concentrations are a factor of 2 lower than those in the solid cloud. Furthermore, cloud condensation nuclei (CCN) concentrations were found to be about 3 times greater in the solid-cloud area compared with those in the rift. Although drizzle was observed near cloud top in parts of the solid stratocumulus cloud, the largest drizzle rates were associated with the broken clouds within the rift area and with extremely large effective droplet sizes retrieved from satellite data. Minimal thermodynamic differences between the rift and solid cloud deck were observed. In addition to marked differences in particle concentrations, evidence of a mesoscale circulation near the solid cloud–rift boundary is presented. This mesoscale circulation may provide a mechanism for maintaining a rift, but further study is required to understand the initiation of a rift and the conditions that may cause it to fill. A review of results from previous studies indicates similar microphysical characteristics in rift features sampled serendipitously. These observations indicate that cloud rifts are depleted of aerosols through the cleansing associated with drizzle and are a manifestation of natural processes occurring in marine stratocumulus.

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Timothy W. Juliano
,
Matthew M. Coggon
,
Gregory Thompson
,
David A. Rahn
,
John H. Seinfeld
,
Armin Sorooshian
, and
Zachary J. Lebo

Abstract

Modeling marine low clouds and fog in coastal environments remains an outstanding challenge due to the inherently complex ocean–land–atmosphere system. This is especially important in the context of global circulation models due to the profound radiative impact of these clouds. This study utilizes aircraft and satellite measurements, in addition to numerical simulations using the Weather Research and Forecasting (WRF) Model, to examine three well-observed coastally trapped disturbance (CTD) events from June 2006, July 2011, and July 2015. Cloud water-soluble ionic and elemental composition analyses conducted for two of the CTD cases indicate that anthropogenic aerosol sources may impact CTD cloud decks due to synoptic-scale patterns associated with CTD initiation. In general, the dynamics and thermodynamics of the CTD systems are well represented and are relatively insensitive to the choice of physics parameterizations; however, a set of WRF simulations suggests that the treatment of model physics strongly influences CTD cloud field evolution. Specifically, cloud liquid water path (LWP) is highly sensitive to the choice of the planetary boundary layer (PBL) scheme; in many instances, the PBL scheme affects cloud extent and LWP values as much as or more than the microphysics scheme. Results suggest that differences in the treatment of entrainment and vertical mixing in the Yonsei University (nonlocal) and Mellor–Yamada–Janjić (local) PBL schemes may play a significant role. The impact of using different driving models—namely, the North American Mesoscale Forecast System (NAM) 12-km analysis and the NCEP North American Regional Reanalysis (NARR) 32-km products—is also investigated.

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Cynthia H. Twohy
,
Paul J. DeMott
,
Kerri A. Pratt
,
R. Subramanian
,
Gregory L. Kok
,
Shane M. Murphy
,
Traci Lersch
,
Andrew J. Heymsfield
,
Zhien Wang
,
Kim A. Prather
, and
John H. Seinfeld

Abstract

Ice concentrations in orographic wave clouds at temperatures between −24° and −29°C were shown to be related to aerosol characteristics in nearby clear air during five research flights over the Rocky Mountains. When clouds with influence from colder temperatures were excluded from the dataset, mean ice nuclei and cloud ice number concentrations were very low, on the order of 1–5 L−1. In this environment, ice number concentrations were found to be significantly correlated with the number concentration of larger particles, those larger than both 0.1- and 0.5-μm diameter. A variety of complementary techniques was used to measure aerosol size distributions and chemical composition. Strong correlations were also observed between ice concentrations and the number concentrations of soot and biomass-burning aerosols. Ice nuclei concentrations directly measured in biomass-burning plumes were the highest detected during the project. Taken together, this evidence indicates a potential role for biomass-burning aerosols in ice formation, particularly in regions with relatively low concentrations of other ice nucleating aerosols.

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Kerri A. Pratt
,
Andrew J. Heymsfield
,
Cynthia H. Twohy
,
Shane M. Murphy
,
Paul J. DeMott
,
James G. Hudson
,
R. Subramanian
,
Zhien Wang
,
John H. Seinfeld
, and
Kimberly A. Prather

Abstract

During the Ice in Clouds Experiment–Layer Clouds (ICE-L), aged biomass-burning particles were identified within two orographic wave cloud regions over Wyoming using single-particle mass spectrometry and electron microscopy. Using a suite of instrumentation, particle chemistry was characterized in tandem with cloud microphysics. The aged biomass-burning particles comprised ∼30%–40% by number of the 0.1–1.0-μm clear-air particles and were composed of potassium, organic carbon, elemental carbon, and sulfate. Aerosol mass spectrometry measurements suggested these cloud-processed particles were predominantly sulfate by mass. The first cloud region sampled was characterized by primarily homogeneously nucleated ice particles formed at temperatures near −40°C. The second cloud period was characterized by high cloud droplet concentrations (∼150–300 cm−3) and lower heterogeneously nucleated ice concentrations (7–18 L−1) at cloud temperatures of −24° to −25°C. As expected for the observed particle chemistry and dynamics of the observed wave clouds, few significant differences were observed between the clear-air particles and cloud residues. However, suggestive of a possible heterogeneous nucleation mechanism within the first cloud region, ice residues showed enrichments in the number fractions of soot and mass fractions of black carbon, measured by a single-particle mass spectrometer and a single-particle soot photometer, respectively. In addition, enrichment of biomass-burning particles internally mixed with oxalic acid in both the homogeneously nucleated ice and cloud droplets compared to clear air suggests either preferential activation as cloud condensation nuclei or aqueous phase cloud processing.

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Ewan Crosbie
,
Zhen Wang
,
Armin Sorooshian
,
Patrick Y. Chuang
,
Jill S. Craven
,
Matthew M. Coggon
,
Michael Brunke
,
Xubin Zeng
,
Haflidi Jonsson
,
Roy K. Woods
,
Richard C. Flagan
, and
John H. Seinfeld

Abstract

Data from three research flights, conducted over water near the California coast, are used to investigate the boundary between stratocumulus cloud decks and clearings of different sizes. Large clearings exhibit a diurnal cycle with growth during the day and contraction overnight and a multiday life cycle that can include oscillations between growth and decay, whereas a small coastal clearing was observed to be locally confined with a subdiurnal lifetime. Subcloud aerosol characteristics are similar on both sides of the clear–cloudy boundary in the three cases, while meteorological properties exhibit subtle, yet important, gradients, implying that dynamics, and not microphysics, is the primary driver for the clearing characteristics. Transects, made at multiple levels across the cloud boundary during one flight, highlight the importance of microscale (~1 km) structure in thermodynamic properties near the cloud edge, suggesting that dynamic forcing at length scales comparable to the convective eddy scale may be influential to the larger-scale characteristics of the clearing. These results have implications for modeling and observational studies of marine boundary layer clouds, especially in relation to aerosol–cloud interactions and scales of variability responsible for the evolution of stratocumulus clearings.

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Kevin J. Noone
,
Elisabeth Öström
,
Ronald J. Ferek
,
Tim Garrett
,
Peter V. Hobbs
,
Doug W. Johnson
,
Jonathan P. Taylor
,
Lynn M. Russell
,
Richard C. Flagan
,
John H. Seinfeld
,
Colin D. O’Dowd
,
Michael H. Smith
,
Philip A. Durkee
,
Kurt Nielsen
,
James G. Hudson
,
Robert A. Pockalny
,
Lieve De Bock
,
René E. Van Grieken
,
Richard F. Gasparovic
, and
Ian Brooks

Abstract

The effects of anthropogenic particulate emissions from ships on the radiative, microphysical, and chemical properties of moderately polluted marine stratiform clouds are examined. A case study of two ships in the same air mass is presented where one of the vessels caused a discernible ship track while the other did not. In situ measurements of cloud droplet size distributions, liquid water content, and cloud radiative properties, as well as aerosol size distributions (outside cloud, interstitial, and cloud droplet residual particles) and aerosol chemistry, are presented. These are related to measurements of cloud radiative properties. The differences between the aerosol in the two ship plumes are discussed;these indicate that combustion-derived particles in the size range of about 0.03–0.3-μm radius were those that caused the microphysical changes in the clouds that were responsible for the ship track.

The authors examine the processes behind ship track formation in a moderately polluted marine boundary layer as an example of the effects that anthropogenic particulate pollution can have in the albedo of marine stratiform clouds.

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