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All sourcesNASA NTRSDOE OSTI
NASA NTRS2024

Stratospheric Air Intrusions Promote Global-Scale New Particle Formation

New particle formation in the free troposphere is a major source of cloud condensation nuclei globally. The prevailing view is that in the free troposphere, new particles are formed predominantly in convective cloud outflows. We present another mechanism using global observations. We find that during stratospheric air intrusion events, the mixing of descending ozone-rich stratospheric air with more moist free tropospheric background results in elevated hydroxyl radical (OH) concentrations. Such mixing is most prevalent near the tropopause where the sulfur dioxide (SO 2 ) mixing ratios are high. The combination of elevated SO 2 and OH levels leads to enhanced sulfuric acid concentrations, promoting particle formation. Such new particle formation occurs frequently and over large geographic regions, representing an important particle source in the midlatitude free troposphere.

Jiaoshi Zhang↗
NASA NTRS2022

Observations of Particle Number Size Distributions and New Particle Formation in Six Indian Locations

Atmospheric new particle formation (NPF) is a crucial process driving aerosol number concentrations in the atmosphere; it can significantly impact the evolution of atmospheric aerosol and cloud processes. This study analyses at least 1 year of asynchronous particle number size distributions from six different locations in India. We also analyze the frequency of NPF and its contribution to cloud condensation nuclei (CCN) concentrations. We found that the NPF frequency has a considerable seasonal variability. At the measurement sites analyzed in this study, NPF frequently occurs in March–May (pre-monsoon, about 21 % of the days) and is the least common in October–November (post-monsoon, about 7 % of the days). Considering the NPF events in all locations, the particle formation rate (J_(SDS)) varied by more than 2 orders of magnitude (0.001–0.6 /cu.cm s) and the growth rate between the smallest detectable size and 25 nm (GR_(SDS-25 nm)) by about 3 orders of magnitude (0.2–17.2 nm/h). We found that JSDS was higher by nearly 1 order of magnitude during NPF events in urban areas than mountain sites. GRSDS did not show a systematic difference. Our results showed that NPF events could significantly modulate the shape of particle number size distributions and CCN concentrations in India. The contribution of a given NPF event to CCN concentrations was the highest in urban locations (4.3 × 10^(3) /cu.cm per event and 1.2 × 10^(3)/cu.cm per event for 50 and 100 nm, respectively) as compared to mountain background sites (2.7 × 10^(3)/cu.cm per event and 1.0 × 10^(3)/cu.cm per event, respectively). We emphasize that the physical and chemical pathways responsible for NPF and factors that control its contribution to CCN production require in situ field observations using recent advances in aerosol and its precursor gaseous measurement techniques.

particle number size distributions↗
NASA NTRS2021

New Particle Formation and Growth to Climate‐Relevant Aerosols at a Background Remote Site in the Western Himalaya

New particle formation (NPF) can influence the Earth's radiative budget when the newly formed particles grow to climate‐relevant sizes. Here, we present analysis of 21 months of continuous aerosol size distribution measurements at a background remote site in the western Himalaya and provide observational evidence that newly formed particles grow to cloud condensation nuclei (CCN)‐active sizes (i.e., >20–100 nm in diameter). Out of total 55 NPF events, 38 (66%) events occurred in the pre‐monsoon season (March–May). NPF events were classified into those with and without pollution influence as polluted and cleaner, respectively, using black carbon data. The analysis of air mass age, based on the ratio of number concentration of Aitken to accumulation mode aerosols, indicated that NPF occurred in the relatively cleaner air masses reaching to the site. The median formation rate of 10 nm particles and particle growth rates for cleaner events were three‐fold and two‐fold, respectively, higher than polluted events. We present the first estimates of the survival probability of newly formed particles to 50 and 100 nm size, which was not attempted in an Indian environment previously. The survival probability to 50 nm particles ranged from 44% to 98%, with a mean and standard deviation of 82 ± 18%. On average, ∼60% of the particles surviving to 50 nm survived to 100 nm, making the overall survival probability of 100 nm to 53 ± 31%. This indicates that the probability of nucleated particles growing to CCN‐active sizes under a large source of condensing vapor (transported from nearby lower‐altitude regions) and low pre‐existing particle concentrations (background mountain site) is high compared to the previous studies. These findings highlight the importance of the efficiency of nucleation events for producing CCN, which is a critical basis of aerosol indirect effects.

cloud condensation nuclei↗
NASA NTRS2019

A Large Source of Cloud Condensation Nuclei from New Particle Formation in the Tropics

Cloud condensation nuclei (CCN) can affect cloud properties and therefore the Earth’s radiative balance. New particle formation (NPF) from condensable vapours in the free troposphere has been suggested to contribute to CCN, especially in remote, pristine atmospheric regions, but direct evidence is sparse, and the magnitude of this contribution is uncertain. Here we use in-situ aircraft measurements of vertical profiles of aerosol size distributions to present a global-scale survey of NPF occurrence. We observed intense NPF occurring at high altitude in tropical convective regions over both the Pacific and Atlantic Oceans. Together with the results of chemical-transport models, our findings indicate that NPF persists at all longitudes as a global-scale band in the tropical upper troposphere, covering about 40% of the Earth’s surface. Furthermore, we find that this NPF in the tropical upper troposphere is a globally important source of CCN in the lower troposphere, where they can affect cloud properties. Our findings suggest that the production of CCN, as these new particles descend towards the surface, is currently not adequately captured in global models, because they tend to underestimate both the magnitude of tropical upper tropospheric NPF and the subsequent growth to CCN sizes. This has potential implications for cloud albedo and the global radiative balance.

Atmospheric chemistry↗
NASA NTRS2020

Saharan Dust Aerosols Change Deep Convective Cloud Prevalence, Possibly by Inhibiting Marine New Particle Formation

Deep convective clouds (DCCs) are important to global climate, atmospheric chemistry, and precipitation. Dust, a dominant aerosol type over the tropical North Atlantic, has potentially large microphysical impacts on DCCs over this region. However, dust effects are difficult to identify, being confounded by co-varying meteorology and other factors. Here, a method is developed to quantify DCC responses to dust and other aerosols at large spatial and temporal scales despite these uncertainties. Over 7 million tropical North Atlantic cloud, aerosol, and meteorological profiles from CloudSat satellite data and MERRA-2 reanalysis products are used to stratify cloud observations into meteorological regimes, objectively select a priori assumptions, and iteratively test uncertainty sensitivity. Dust is robustly associated with a 54% increase in DCC prevalence. However, marine aerosol proxy concentrations are five times more predictive of dust-associated increases in DCC prevalence than the dust itself, or any other aerosol or meteorological factor. Marine aerosols are also the most predictive factor for the even larger increases in DCC prevalence (61-87%) associated with enhanced dimethyl sulfide and combustion and sulfate aerosols. Dust-associated increases in DCC prevalence are smaller at high dust concentrations than at low concentrations. These observations suggest that not only is dust a comparatively ineffective CCN source, but it may also act as a condensation/coagulation sink for chemical precursors to CCN, reducing total CCN availability over large spatial scales by inhibiting new particle formation from marine emissions. These observations represent the first time this rocess, previously predicted by models, is supported and quantified by measurements.

Aerosol-cloud interactions↗
NASA NTRS1989

Observations of condensation nuclei in the Airborne Antarctic Ozone Experiment - Implications for new particle formation and polar stratospheric cloud formation

This paper discusses the results of the ER-2 Condensation Nucleus Counter operated in the Airborne Ozone Experiment in August, September, and October 1987, providing data on the mixing ratio of aerosol condensation nuclei (CN) with diameters between about 0.02 and 1 micron. It is shown that the vertical profile of the CN mixing ratio is closely related to that of N2O, and that, between the -71 and -53 deg latitude, the location of the minima in the CN mixing ratio profile was near the 160 ppbv N2O isopleth, indicating that the processes of mixing and subsidence, which determine the inclination of that isopleth, also strongly affect the spatial distribution of the sulfate aerosol. Evidence for new sulfate particle formation is presented and related to the amount of subsidence experienced by air parcels in the formation of the polar vortex. Concentrations of CN are compared with those of larger particles (with diameters between 0.81 micron and 9.75 microns) to study polar stratospheric cloud formation mechanisms.

Wilson, J. C.↗
NASA NTRS1991

Measurements of condensation nuclei above the jet stream - Evidence for cross jet transport by waves and new particle formation at high altitudes

Condensation nuclei were used as a tracer in midlatitude NASA Stratosphere-Troposphere Exchange Project (STEP) experiments in April and May 1984 in order to study transport in the stratosphere. The very large scale, mean CN distribution was distorted by waves which had the effect of transporting air with anticyclonic properties several degrees to the cyclonic side of the jet and created a strongly layered structure in the CN distribution. Unfiltered CN data revealed short-wavelength oscillations in the CN distribution at the interface between the transported anticyclonic air parcel and the adjacent cyclonic air mass. These oscillations were also seen in the ozone data and increase the potential for mixing along that interface. If the mixing does occur, a wave mechanism for cross-jet transport has been observed.

Wilson, J. C.↗
NASA NTRS2003

New Particle Formation in Anthropogenic Plumes Advecting from Asia Observed During TRACE-P

The characteristics and sources of what are believed to be newly formed 3 to 4 nm particles in anthropogenic plumes advecting from Asian are reported. Airborne measurements were made from March to April 2001 as part of the NASA TRACE-P experiment at latitudes ranging from North of the Philippines to Northern Japan (20 to 45 deg. N). In the more polluted plumes, high concentrations of 3 to 4 nm diameter particles (less than 100/qu cm) were observed both within and along the upper outer edges of plumes that were identified by enhanced carbon monoxide and fine particulate sulfate concentrations. The results from two research flights are investigated in detail. Three to four-nm particle concentrations are generally correlated with gas phase sulfuric acid and found in regions of low surface areas relative to the immediate surroundings or where there are steep transitions to lower surface areas. Sulfuric acid and surface area concentrations in the most polluted plume reached 6 x l0(exp 7) and 750 micro sq m/qu cm, respectively, in regions of particle formation. In contrast to these anthropogenic plumes, few 3 to 4 nm particles were observed in the clean background and few were detected within a volcanic plume where the studies highest H2SO4 concentrations (less than lO(exp 8)/qu cm) were recorded. Enhanced SO2 concentrations in the range of approximately 2 to 7 ppb, in conjunction with other unidentified, possibly coemitted species, appear to be the driving factor for nucleation. (0345, 4801); 0322 Atmospheric Composition and Structure: Constituent sources and sinks; 0345 Atmospheric Composition and Structure: Pollution-urban and regional (0305); 4801 Oceanography: Biological and Chemical: Aerosols (0305).

Weber, R. J.↗
NASA NTRS1996

Comparisons Between the Formation of Polar Stratospheric Clouds and Cirrus Clouds

Analyses of lidar data taken during the 1989 AASE I program show that polar stratospheric clouds most often contain frozen particles, but sometimes contain spherical, presumably liquid, particles. In this paper the mechanisms that lead to the freezing of particles, and to the formation of liquid particles will be discussed based largely upon analyses of existing data. For example, trajectory studies help shed light on the conditions that lead to particle freezing. During April of 1996 an experiment using the NASA DC-8 and ER-2 aircraft will be conducted over the central U.S. Some of the goals of the project are to better understand the mechanisms of cirrus cloud formation, and to investigate the properties of freezing nuclei in the upper troposphere. Results from this field program will be presented as they apply to the topic of ice crystal nucleation. Comparisons will be drawn between the mechanisms that lead to new particle formation in the polar stratosphere, and the mechanisms that lead to new particles formation in the upper troposphere.

Toon, Owen B.↗
NASA NTRS1990

Aerosol nucleation in the winter Arctic and Antarctic stratospheres

The formation rate of sulfuric-acid-water aerosol particles is calculated as a function of altitude for the conditions of the winter Arctic and Antarctic stratospheres. The theoretical results indicate that sulfate particle formation can occur in the polar winter stratosphere. Conditions for new particle formation are increasingly favorable as the altitude increases between 20 and 30 km because of the decrease in surface area of preexisting particles and increasing sulfuric-acid vapor supply. The theoretical predictions are consistent with observations of a high-altitude CN layer over Antarctica in the spring. Available vapor-pressure data indicate that ternary particles composed of sulfuric acid, nitric acid, and water are not thermodynamically stable under winter stratospheric conditions.

Hamill, Patrick↗
NASA NTRS2021

Investigation of several proxies to estimate sulfuric acid concentration in volcanic plume conditions

Sulfuric acid (H2SO4) is commonly accepted as a key precursor for atmospheric new particle formation (NPF). However, direct measurements of [H2SO4] remain challenging, thus preventing the determination of this important quantity, and, consequently, a complete understanding of its contribution to the NPF process. Several proxies have been developed to bridge the gaps, but their ability to predict [H2SO4] in very specific conditions such as those encountered in volcanic plumes (including in particular high sulphur dioxide mixing ratios) has not been evaluated so far. In this context, the main objective of the present study was to develop new proxies for daytime [H2SO4] in volcanic plume conditions and compare their performance to that of the proxies available in the literature. In specific, the data collected at Maïdo during the OCTAVE 2018 campaign, in the volcanic eruption plume of the Piton de la Fournaise, were first used to derive seven proxies based on the knowledge of sulphur dioxide (SO2) mixing ratio, global radiation, condensation sink (CS) and relative humidity (RH). In three of the seven proxies (F1–F3), all variables were given equal weight in the prediction of [H2SO4], while adjusted powers were allowed for the different variables in the other four proxies (A1–A4). Proxies A1–A4 were overall found to perform better compared to F1–F3, with, in specific, improved predictive ability for [H2SO4] > 2 × 108 per cu.cm. The CS was observed to play an important role in regulating [H2SO4], while, in contrast, the inclusion of RH did not improve the predictions. A last expression accounting for an additional sink term related to cluster formation, S1, was also tested and showed a very good predictive ability over the whole range of measured [H2SO4]. The newly developed proxies were in a second step further evaluated using airborne measurements performed in the passive degassing plume of Etna during the STRAP 2016 campaign. Increased correlations between observed and predicted [H2SO4] were obtained when the dependence of predicted [H2SO4] over CS was the lowest, and when the dependence over [SO2] was concurrently the highest. The best predictions were finally retrieved by the simple formulation of F2 (in which [SO2] and radiation alone were assumed to explain the variations of [H2SO4] with equal contributions), with a pre factor adapted to the STRAP data. All in all, our results illustrate the fairly good capacity of the proxy available in the literature to describe [H2SO4] in volcanic plume conditions, but highlight at the same time the benefit of the newly developed proxies for the prediction of the highest concentrations ([H2SO4] > 2–3 × 108 per cu.cm). Also, the contrasting behaviours of the new proxies in the two investigated datasets indicate that in volcanic plumes like in other environments, the relevance of a proxy can be affected by changes in environmental conditions, and that location specific coefficients do logically improve the predictions.

new particle formation↗
NASA NTRS1982

Temperature dependence of the formation of sulfate aerosols in the stratosphere

Classical nucleation theory is used in calculations of the temperature dependence of the characteristics and nucleation rates of sulfate aerosols in the binary H2SO4-H2O vapor mixture, in order to assess the influence of temperature on the formation of sulfate aerosols in the stratosphere, and to explore the possibility of new particle formation through homogeneous nucleation processes at regions where temperature is as low as -75 C, rather than the often-assumed -50 or -55 C. Calculation results indicate that the number of particles formed at a lower temperature is larger by several orders of magnitude than at higher temperatures, when water and sulfuric acid vapor concentrations are kept constant, and that large quantities of ultrafine particles which cannot be detected by conventional methods may exist at low-temperature stratospheric regions.

Yue, G. K.↗
NASA NTRS2002

Solid Hydrogen Experiments for Atomic Propellants: Particle Formation Energy and Imaging Analyses

This paper presents particle formation energy balances and detailed analyses of the images from experiments that were conducted on the formation of solid hydrogen particles in liquid helium during the Phase II testing in 2001. Solid particles of hydrogen were frozen in liquid helium and observed with a video camera. The solid hydrogen particle sizes and the total mass of hydrogen particles were estimated. The particle formation efficiency is also estimated. Particle sizes from the Phase I testing in 1999 and the Phase II testing in 2001 were similar. Though the 2001 testing created similar particles sizes, many new particle formation phenomena were observed. These experiment image analyses are one of the first steps toward visually characterizing these particles and it allows designers to understand what issues must be addressed in atomic propellant feed system designs for future aerospace vehicles.

Palaszewski, Bryan↗
NASA NTRS2005

Solid Hydrogen Experiments for Atomic Propellants: Particle Formation, Imaging, Observations, and Analyses

This report presents particle formation observations and detailed analyses of the images from experiments that were conducted on the formation of solid hydrogen particles in liquid helium. Hydrogen was frozen into particles in liquid helium, and observed with a video camera. The solid hydrogen particle sizes and the total mass of hydrogen particles were estimated. These newly analyzed data are from the test series held on February 28, 2001. Particle sizes from previous testing in 1999 and the testing in 2001 were similar. Though the 2001 testing created similar particles sizes, many new particle formation phenomena were observed: microparticles and delayed particle formation. These experiment image analyses are some of the first steps toward visually characterizing these particles, and they allow designers to understand what issues must be addressed in atomic propellant feed system designs for future aerospace vehicles.

Palaszewski, Bryan↗
NASA NTRS1981

The formation and growth of sulfate aerosols in the stratosphere

The critical compositions, critical radii, and nucleation rates of sulfuric acid droplets formed through homogeneous heteromolecular nucleation process in the stratosphere under a variety of ambient conditions are calculated. Results are plotted as a function of H2SO4 concentration and H2O concentration so that characteristics of sulfate aerosols can be quickly estimated whenever environmental conditions are known. The effect of the uncertainty in the saturated vapor pressure of H2SO4 on the estimated properties of sulfate aerosols is elucidated. Plottings are presented that illustrate the relative importance of new particle formation by homogeneous nucleation vs growth by heteromolecular condensation on pre-existing nuclei in the stratosphere. The effects of ambient conditions, such as the concentrations of H2SO4 and H2O, the average stratospheric particle radius, and the number concentration of pre-existing nuclei on the relative importance of these two competing processes are discussed.

Yue, G. K.↗