Observation of sub-3nm particles and new particle formation at an urban location in India
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Environmental Sciences & Ecology↗
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Observation of sub-3nm particles and new particle formation at an urban location in India
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54 ENVIRONMENTAL SCIENCES↗
Investigating ultrafine aerosol turbulent fluxes during atmospheric new particle formation events
New particle formation (NPF) is an important source of atmospheric aerosols, yet quantitatively predicting its occurrence remains challenging, partly because ground-based measurements cannot capture NPF accurately if they occur in the upper atmosphere. While observations have confirmed the presence of new particles near the top of the planetary boundary layer (PBL), their origins and the direction of their vertical transport have remained ambiguous. Here, we propose and validate an analytical framework using airborne eddy-covariance (EC) and continuous wavelet transform (CWT) to directly quantify the vertical flux of newly formed particles and determine its dominant vertical transportation direction. Analyzing data from a dedicated airborne campaign over the Southern Great Plains, we observed a persistent and strong downward particle flux during NPF events, with a mean value of 133.8 cm?3 m s?¹ downward flux in the entrainment zone, whereas fluxes on non-NPF days were negligible. Our spectral analysis further confirms that these directional fluxes can be reliably captured using standard 1 Hz aerosol instrumentation. These findings suggest that new particle formation, driven by the entrainment of air from the overlying residual/stable layer during PBL growth, is a significant and potentially understudied source of boundary layer aerosols. The framework presented here provides a methodology to correctly attribute NPF events to specific altitudes, thereby improving the mechanistic understanding required for accurate atmospheric models.
Zhang, Ruoyu↗
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↗
Model independent constraints on charges of new particles
Any particle that is charged under SU(3) C and U(1) EM can mediate the gg →γγ process through loops. Near the threshold for the new particle pair production, gauge boson exchanges necessitate the resummation of ladder diagrams. We discuss the leading log order matching of the one-loop result with the nonrelativistic effective theory resummed result. We show how the diphoton invariant mass spectrum varies depending on decay width, color representation, and electric charge of the new particle. In conclusion, the exclusion limits on the product of SU(3) C and U(1) EM charges of the new scalar or fermion particle are obtained from current LHC data.
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
New Particle Formation and Growth in an Isoprene-Dominated Ozark Forest: From Sub-5 nm to CCN-Active Sizes
Particle Investigations at a Northern Ozarks Tower: NOx, Oxidant, Isoprene Research (PINOT-NOIR) were conducted in a Missouri forest dominated by isoprene emissions, from May to October 2012. This study presents results of new particle formation (NPF) and the growth of new particles to cloud condensation nuclei (CCN)-active sizes (~100 nm) observed from this field campaign. The measured sub-5 nm particles were up to ~20000 cm-3 during a typical NPF event. Nucleation rates J1 were relatively high (11.0±10.6 cm-3s-1), and one order of magnitude higher than formation rates of 5 nm particles (J5). Sub-5 nm particle events were observed on 64% of the measurement days, with a high preference in biogenic volatile organic compounds (BVOCs)- and SO2-poor northwesterly (90%) air masses than in BVOCs-rich southerly air masses (13%). About 80% of sub-5 nm particle events led to the further growth. While high temperatures and high aerosol loadings in the southerly air masses were not favorable for nucleation, high BVOCs in the southerly air masses facilitated the growth of new particles to CCN-active sizes. In overall, 0.4-9.4% of the sub-5 nm particles grew to CCN-active sizes within a NPF event. During a regional NPF event period that took place consecutively over several days, concentrations of CCN size particles increased by a factor of 5 in average. This enhanced production of CCN particles from new particles was commonly observed during all 13 regional NPF events observed during the campaign.
cloud condensation nuclei, isoprene, BVOC↗
Evidence for Diverse Biogeochemical Drivers of Boreal Forest New Particle Formation
New particle formation (NPF) is an important contributor to particle number in many locations, but the chemical drivers for this process are not well understood. Daytime NPF events occur regularly in the springtime Finnish boreal forest and strongly impact aerosol abundance. In April 2014 size-resolved chemical measurements of ambient nanoparticles were made using the Time-of-Flight Thermal Desorption Chemical ionization Mass Spectrometer and we report results from two NPF events. While growth overall was dominated by terpene oxidation products, newly formed 20–70 nm particles showed enhancement in apparent alkanoic acids. The events occurred on days with rapid transport of marine air, which correlated with low background aerosol loading and higher gas phase methanesulfonic acid levels. These results are broadly consistent with previous studies on Nordic NPF but indicate that further attention should be given to the sources and role of non-terpenoid organics and the possible contribution of transported marine compounds in this process.
54 ENVIRONMENTAL SCIENCES↗
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↗
Search for new particles in events with one lepton and missing transverse momentum in pp collisions at $ \sqrt{s} $ = 8 TeV with the ATLAS detector
This paper presents a search for new particles in events with one lepton (electron or muon) and missing transverse momentum using 20.3 fb -1 of proton-proton collision data at $ \sqrt{s} $ = 8 TeV recorded by the ATLAS experiment at the Large Hadron Collider. No significant excess beyond Standard Model expectations is observed. A W' with Sequential Standard Model couplings is excluded at the 95% confidence level for masses up to 3.24 TeV. Excited chiral bosons (W*) with equivalent coupling strengths are excluded for masses up to 3.21 TeV. In the framework of an effective field theory limits are also set on the dark matter-nucleon scattering cross-section as well as the mass scale M* of the unknown mediating interaction for dark matter pair production in association with a leptonically decaying W.[Figure not available: see fulltext.]
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
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 cm –3 s –1 ) and the growth rate between the smallest detectable size and 25nm (GR SDS-25nm ) by about 3 orders of magnitude (0.2–17.2nm h –1 ). We found that J SDS was higher by nearly 1 order of magnitude during NPF events in urban areas than mountain sites. GR SDS 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 cm –3 per event and 1.2 × 10 3 cm –3 per event for 50 and 100nm, respectively) as compared to mountain background sites (2.7 × 10 3 cm –3 per event and 1.0 × 10 3 cm –3 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.
54 ENVIRONMENTAL SCIENCES↗
Going Off Grid: A Comparative Study of the Lagrangian and Eulerian Perspectives of New Particle Formation Events
New particle formation and growth (NPF&G) is the process by which ultrafine particles are formed from gas-phase precursors. NPF&G is the dominant source of global aerosol number with important influences on climate. Most observations of NPF&G events are conducted at stationary sites; however, NPF&G observed from stationary sites is influenced by gradual or rapid changes in the air masses passing over the site, complicating NPF&G analysis. In this work, we use observations and a 3D aerosol model to compare aerosol size distributions at a stationary site (Southern Great Plains [SGP] observatory, Oklahoma, USA) and along Lagrangian trajectories crossing the site. The model simulates the NPF&G events reasonably well at SGP. Using the model to compare the Lagrangian and stationary perspectives, we can explain previously unanalyzable days with some evidence of NPF&G as either non-event or analyzable NPF&G days. We find most of the unanalyzable NPF&G days are due to isolated and inhomogeneous NPF&G occurring upwind of the stationary site, often in the outflow of urban regions. Finally, we compare formation rates of 3 nm particles, growth rates, and the survival probability of 3 nm particles growing to 25 nm between the stationary and Lagrangian perspectives. Because of the much larger number of analyzable days along the Lagrangian trajectories, this perspective potentially provides more robust statistics and better characterization of NPF&G event extremes. Our method for extracting chemical/physical properties along Lagrangian trajectories from 3D models can be applied to a wide range of science questions.
O’Donnell, Samuel E. [Colorado State Univ., Fort C↗
Vertical distribution of boundary layer new particle formation and implications for nanoparticle growth mechanisms (Final Report)
New particles can form high above ground in the atmosphere before such formation events are observed by ground-based instruments. Once formed, these particles can take up significant amounts of water vapor, which has implications on the mechanisms by which nanoparticles grow and, ultimately, impact cloud formation processes. These observations motivated the research performed in this project using a combination of modeling, laboratory experiments, and the analysis of field observations. We hypothesized is that ground-based measurements do not always accurately represent the location and timing of new particle formation events, nor do they adequately characterize the dominant physical and chemical processes that are responsible for the subsequent growth of newly formed particles. Essentially, we wanted to study the new particle formation process under conditions that we expect may be more relevant to the actual location in the atmosphere where such events take place, which are often characterized by higher relative humidities, lower temperatures, and a broader range of precursors and oxidants compared to those observed at ground level. This project had two main objectives, each of which directly addressed our hypothesis. Our first is to investigate the timing, distribution, meteorological conditions, and nanoparticle properties associated with boundary layer new particle formation through the analysis of ARM field campaigns such as HI-SCALE and long-term observations and observations performed in other locales such as in China and India where atmospheric conditions could play a crucial role in determining the mechanisms of new particle formation. This activity provided a comprehensive description, both in time and in space, of the gases and nanoparticle properties that are responsible for these events. We also performed modeling studies to explore the vertical profile and timing of new particle formation events from these campaigns. Our second objective was to perform laboratory and process-level modeling studies to investigate the role that conditions such as low ambient temperature, high relative humidity, and different oxidants such as nitrate radical play in determining unique chemical pathways for nanoparticle growth. In doing so, we revisited the representation of nanoparticle growth in global models and updated assumptions of formation and growth based on the findings of the field, laboratory, and process-level-model work. Our research provides crucial insights into the most important regions of the atmospheric boundary layer for future observational and modeling studies. It also identifies the most relevant environmental conditions, precursors, and oxidants that are responsible for nanoparticle growth, which will aid in the design of laboratory studies and process-level model experiments. The unique pathways that we discovered can be incorporated into regional and global models, thereby improving predictions and attribution of the role of new particle formation in, e.g., air pollution formation and cloud properties.
54 ENVIRONMENTAL SCIENCES↗
New Particle Formation Study Final Campaign Report
The scientific foci of the New Particle Formation Study were the formation and evolution of atmospheric aerosols and the impacts of newly formed particles on cloud processes. Specifically, we planned to: (1) to identify the species and mechanisms responsible for the initial steps of new particle formation, i.e., the formation of thermodynamically stable clusters; (2) investigate the role of acid-base chemistry in new particle growth through measurements of ammonia and amines as well as organic and inorganic acids in both atmospheric nanoparticles and the gas phase; (3) investigate the contribution of other surface area or volume-controlled processes to nanoparticle formation and growth; (4) create a comprehensive dataset related to new particle formation and growth that can be used as input for our own thermodynamic models as well as the modeling efforts by our Department of Energy (DOE) Aerosol Life Cycle working group collaborators; (5) characterize the increase of the number and activity of cloud condensation nuclei (CCN) due to particle formation and growth; (6) determine the regional extent of new particle formation to address the role that atmospheric transport plays in determining the impacts, if any, of new particle formation on cloud number and properties.
Smith, JN↗
Characterizing New Particle Formation and Growth (Field Campaign Report)
New particle formation (NPF) and subsequent growth to sizes at which the aerosol particles can act as cloud condensation nuclei (CCN) is critical for understanding and modeling aerosol-climate interactions (Gordon et al. 2017, Dunne et al. 2016). While sulfuric acid is generally understood to play a central role in NPF and growth, measured sulfuric acid concentrations are insufficient to explain measured formation and growth rates in many locations even when stabilization by ammonia is considered (Kulmala et al. 2014, Riipinen et al. 2012). Extensive laboratory investigations have revealed that amines (Almeida et al. 2013), other reduced nitrogen compounds (Glasoe et al. 2015), and/or oxidized organic compounds (Kirkby et al. 2016) can enhance new particle formation rates and thus may explain, at least in part, the gap between our understanding of new particle formation and the measurements. Our knowledge, however, of the relative importance of these various pathways remains incomplete due to the limited number of ambient measurements, particularly in diverse ecosystems. Agricultural land use areas are particularly understudied despite accounting for ~41% of global land cover (Ellis et al. 2010). Improving our understanding of NPF requires measurements of NPF and the precursors to NPF and growth in a variety of ecosystems and ideally across seasons.
54 ENVIRONMENTAL SCIENCES↗
Investigating the contribution of grown new particles to cloud condensation nuclei with largely varying preexisting particles – Part 1: Observational data analysis
This study employed multiple techniques to investigate the contribution of grown new particles to the number concentration of cloud condensation nuclei (CCN) at various supersaturation (SS) levels at a rural mountain site in the North China Plain from 29 June to 14 July 2019. On 8 new particle formation (NPF) days, the total particle number concentrations (N cn ) were 8.4 ± 6.1×10 3 cm -3 , which was substantially higher compared to 4.7 ± 2.6×10 3 cm -3 on non-NPF days. However, the CCN concentration (Nccn) at 0.2 % SS and 0.4 % SS on the NPF days was significantly lower than those observed on non-NPF days (p<0.05). This was due to the lower cloud activation efficiency of preexisting particles resulting from organic vapor condensation and smaller number concentrations of preexisting particles on NPF days. A case-by-case examination showed that the grown new particles only yielded a detectable contribution to N ccn at 0.4 % SS and 1.0 % SS during the NPF event on 1 July 2019, accounting for 12 % ± 11 % and 23 % ± 12 % of N ccn , respectively. The increased N ccn during two other NPF events and at 0.2 % SS on 1 July 2019 were detectable but determined mainly by varying preexisting particles rather than grown new particles. In addition, the hygroscopicity parameter values, concentrations of inorganic and organic particulate components, and surface chemical composition of different sized particles were analyzed in terms of chemical drivers to grow new particles. The results showed that the grown new particles via organic vapor condensation generally had no detectable contribution to N ccn but incidentally did. However, this conclusion was drawn from a small size of observational data, leaving more observations, particularly long-term observations and the growth of preexisting particles to the CCN required size, needed for further investigation.
54 ENVIRONMENTAL SCIENCES↗
Chemistry of new particle growth in mixed urban and biogenic emissions – insights from CARES
Regional new particle formation and growth events (NPEs) were observed on most days over the Sacramento and western Sierra foothills area of California in June 2010 during the Carbonaceous Aerosols and Radiative Effect Study (CARES). Simultaneous particle measurements at both the T0 (Sacramento, urban site) and the T1 (Cool, rural site located ~40 km northeast of Sacramento) sites of CARES indicate that the NPEs usually occurred in the morning with the appearance of an ultrafine mode at ~15 nm (in mobility diameter, D m , measured by a mobility particle size spectrometer operating in the range10-858 nm) followed by the growth of this modal diameter to ~50 nm in the afternoon. These events were generally associated with southwesterly winds bringing urban plumes from Sacramento to the T1 site. The growth rate was on average higher at T0 (7.1±2.7 nm h -1 ) than at T1 (6.2±2.5 nm h -1 ), likely due to stronger anthropogenic influences at T0. Using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), we investigated the evolution of the size-resolved chemical composition of new particles at T1. Our results indicate that the growth of new particles was driven primarily by the condensation of oxygenated organic species and, to a lesser extent, ammonium sulfate. New particles appear to be fully neutralized during growth, consistent with high NH 3 concentration in the region. Nitrogen-containing organic ions (i.e., CHN + , CH 4 N+,C2H3N + , and C 2 H N + ) that are indicative of the presence of alkyl-amine species in submicrometer particles enhanced significantly during the NPE days, suggesting that amines might have played a role in these events. Our results also indicate that the bulk composition of the ultrafine mode organics during NPEs was very similar to that of anthropogenically influenced secondary organic aerosol (SOA) observed in transported urban plumes. In addition, the concentrations of species representative of urban emissions (e.g., black carbon,CO, NO x , and toluene) were significantly higher whereas thephoto-oxidation products of biogenic VOCs (volatile organic compounds) and the biogenically influenced SOA also increased moderately during the NPE days compared to the non-event days. These results indicate that the frequently occurring NPEs over the Sacramento and Sierra Nevada regions were mainly driven by urban plumes from Sacramento and the San Francisco Bay Area, and that the interaction of regional biogenic emissions with the urban plumes has enhanced the new particle growth. This finding has important implications for quantifying the climate impacts of NPEs on global scale.
Setyan, Ari↗
High concentration of ultrafine particles in the Amazon free troposphere produced by organic new particle formation
The large concentrations of ultrafine particles consistently observed at high altitudes over the tropics represent one of the world’s largest aerosol reservoirs, which may be providing a globally important source of cloud condensation nuclei. However, the sources and chemical processes contributing to the formation of these particles remain unclear. Here we investigate new particle formation (NPF) mechanisms in the Amazon free troposphere by integrating insights from laboratory measurements, chemical transport modeling, and field measurements. To account for organic NPF, we develop a comprehensive model representation of the temperature-dependent formation chemistry and thermodynamics of extremely low volatility organic compounds as well as their roles in NPF processes. We find that pure-organic NPF driven by natural biogenic emissions dominates in the uppermost troposphere above 13 km and accounts for 65 to 83% of the column total NPF rate under relatively pristine conditions, while ternary NPF involving organics and sulfuric acid dominates between 8 and 13 km. The large organic NPF rates at high altitudes mainly result from decreased volatility of organics and increased NPF efficiency at low temperatures, somewhat counterbalanced by a reduced chemical formation rate of extremely low volatility organic compounds. These findings imply a key role of naturally occurring organic NPF in high-altitude preindustrial environments and will help better quantify anthropogenic aerosol forcing from preindustrial times to the present day.
54 ENVIRONMENTAL SCIENCES↗
Formation Process of Particles and Cloud Condensation Nuclei Over the Amazon Rainforest: The Role of Local and Remote New-Particle Formation
Understanding the formation processes of particles and cloud condensation nuclei (CCN) in pristine environments is a major challenge in accurately assessing anthropogenic radiative forcing. Here, using a state-of-the-art model that systematically simulates the chemical processes controlling new-particle formation (NPF) and multi-scale chemical transport, we find that NPF contributes ~90% of the particle number and ~80% of the CCN at 0.5% supersaturation (CCN0.5%) in the pristine Amazon boundary layer during the wet season. The corresponding contributions are only ~30% and ~20% during the dry season because of prevalent biomass burning. In both seasons, about half of the NPF-induced particles and ~85% of the NPF-induced CCN0.5% in the boundary layer originate from the long-range transport of new particles formed hundreds to thousands of kilometers away. Moreover, about 50–65% of the NPF-induced particles and 35–50% of the NPF induced CCN0.5% originate from the downward transport of new particles formed in the free troposphere.
54 ENVIRONMENTAL SCIENCES↗