Frequent rainfall-induced new particle formation within the canopy in the Amazon rainforest

The formation of new atmospheric aerosol particles and their subsequent growth have been observed under different environmental conditions globally; such observations are few over northwest China. Here, we present an analysis of some case studies for new particle formation (NPF) events from two distinct suburban locations in northern China during May and June of two consecutive years, and provide more information to understand the characteristics of NPF events in North China. Particle number size distribution was measured at suburbs of Beijing (39.75° N, 116.96° E) during 1 June to 2 July 2013 and at suburbs of Xi’an (34.09° N, 108.55° E) during 1 to 25 May 2014. The average of total particle number concentration in the similar size range of 10–487 nm at the suburbs of Beijing (9.0 × 103 cm−3) was about two times higher than those observed at Xi’an (4.7 × 103 cm−3), and the mean particle mode diameter at Beijing was 1.4-fold higher than that at Xi’an. The estimated total condensation sink (CS) at Beijing (3.11 × 10−2 s−1) was also higher than at Xi’an (1.13 × 10−2 s−1). The frequency of NPF events at suburb of Beijing was 24%, lower than that in Xi’an (50%), and also lower than urban site of Beijing (35% in June) and another suburb of Beijing (over 50% in June). The NPF events with (Class I) or without (Class II) subsequent growth were both observed at the two suburb sites. The derived GR at the suburb of Beijing (range from 4.6 to 8.6 nm h−1) was a little higher than that at Xi’an (range from 3.3 to 6.7 nm h−1), which are generally comparable to typical values in mid-latitude reported in previous studies. The air masses coming from north or northwest China favor the occurrence of NPF event under low condensation sink and clear days. The number size distributions of freshly nucleated particles showed clear bimodal distributions on both sites. Additionally, Mode Dp of nucleated particles at the two sites was 17 ± 1 nm and 22 ± 4 nm, respectively during the periods with NPF events. The case study of NPF events at the two suburb sites shows that the surface area concentration and total scattering coefficient (SC) was significant decreased during the NPF events at both sites. High temperature, low condensation sink and low relative humidity furthered the occurrence of NPF events, and wind direction shifts were important for the subsequent growth of particles. NPF events in the suburbs of Beijing usually occurred when relative humidity (RH) < 55%, CS < 0.02 s−1, or 55% < RH < 68%, CS < 0.01 s−1. However, there is no clear range for Xi’an. Furthermore, we observed that some NPF events occurred at higher RH and very low CS in this study on both sites, which means that low CS may be more important than low RH for the particle formation on clear days.

Abstract. Aerosol nucleation occurs frequently in the atmosphere and is an important source of particle number. Observations suggest that nucleated particles are capable of growing to sufficiently large sizes that they act as cloud condensation nuclei (CCN), but some global models have reported that CCN concentrations are only modestly sensitive to large changes in nucleation rates. Here we present a novel approach for using long-term size distribution observations to evaluate a global aerosol model's ability to predict formation rates of CCN from nucleation and growth events. We derive from observations at five locations nucleation-relevant metrics such as nucleation rate of particles at diameter of 3 nm (J3), diameter growth rate (GR), particle survival probability (SP), condensation and coagulation sinks, and CCN formation rate (J100). These quantities are also derived for a global microphysical model, GEOS-Chem-TOMAS, and compared to the observations on a daily basis. Using GEOS-Chem-TOMAS, we simulate nucleation events predicted by ternary (with a 10−5 tuning factor) or activation nucleation over one year and find that the model slightly understates the observed annual-average CCN formation mostly due to bias in the nucleation rate predictions, but by no more than 50% in the ternary simulations. At the two locations expected to be most impacted by large-scale regional nucleation, Hyytiälä and San Pietro Capofiume, predicted annual-average CCN formation rates are within 34 and 2% of the observations, respectively. Model-predicted annual-average growth rates are within 25% across all sites but also show a slight tendency to underestimate the observations, at least in the ternary nucleation simulations. On days that the growing nucleation mode reaches 100 nm, median single-day survival probabilities to 100 nm for the model and measurements range from less than 1–6% across the five locations we considered; however, this does not include particles that may eventually grow to 100 nm after the first day. This detailed exploration of new particle formation and growth dynamics adds support to the use of global models as tools for assessing the contribution of microphysical processes such as nucleation to the total number and CCN budget.

Relatively high concentrations of preexisting particles, acting as a condensation sink (CS) of gaseous precursors, have been thought to suppress the occurrence of new particle formation (NPF) in urban environments, yet NPF still occurs frequently. Here, we aim to understand the factors promoting and inhibiting NPF events in urban Beijing by combining one-year-long measurements of particle number size distributions and PM2.5 chemical composition. Our results show that indeed the CS is an important factor controlling the occurrence of NPF events, with its chemical composition affecting the efficiency of the background particles in removing gaseous H2SO4 (effectiveness of the CS) driving NPF. During our observation period, the CS was found to be more effective for ammonium nitrate-rich (NH4NO3-rich) fine particles. On non-NPF event days, particles acting as CS contained a larger fraction of NH4NO3 compared to NPF event days under comparable CS levels. In particular, in the CS range from 0.02 to 0.03 s–1, the nitrate fraction was 17% on NPF event days and 26% on non-NPF event days. Overall, our results highlight the importance of considering the chemical composition of preexisting particles when estimating the CS and their role in inhibiting NPF events, especially in urban environments.

Observations of atmospheric sub‐3 nm particles are essential for understanding the initial stages of new particle formation (NPF) and the origin of aerosol particles. In this study, 3 years (2018–2020) of measurements of sub‐3 nm particles were conducted in the Yangtze River Delta (YRD) of eastern China. High concentrations of sub‐3 nm particles were observed, with number concentration in the range from 103 to 106 cm−3. During the daytime, the sub‐3 nm particle concentration was found to peak at around the noon, indicating strong photochemical nucleation processes. The formation rates of sub‐3 nm particles were high during the NPF event days, with an average value of 86 cm−3 s−1, and this rate was related to the sulfuric acid (SA) concentration. The particle growth rates below 3 nm were about 1–2 nm h−1, much lower than the growth rates of larger particles. At nighttime, sub‐3 nm particle concentrations remained relatively high (3 × 103 to 1.2 × 104 cm−3) and were related to the NOx concentration, suggesting traffic emission to be a significant source. The sub‐3 nm proxy was developed to estimate the contributions of NPF and traffic emission. During the daytime, 74.8% and 12.4% of the sub‐3 nm particles were estimated to originate from SA‐driven NPF and traffic emissions, respectively. However, other sources were estimated to contribute 61.8% of sub‐3 nm particles at nighttime, suggesting the formation mechanisms of sub‐3 nm particles are still unclear in this environment. Our study sheds more light on the characteristics and sources of sub‐3 nm particles in polluted environments.

Context. Clouds appear to be an unavoidable phenomenon in cool and dense environments. Hence, their inclusion is a necessary part of explaining observations of exoplanet atmospheres, most recently those of WASP 96b with the James Webb Space Telescope (JWST). Understanding the formation of cloud condensation nuclei in non-terrestrial environments is therefore crucial in developing accurate models to interpret current and future observations. Aims. The goal of the paper is to support observations with infrared spectra for (TiO2)N clusters to study cloud formation in exoplanet atmospheres. Methods. We derived vibrational frequencies from quantum-chemical calculations for 123 (TiO2)-clusters and their isomers and we evaluated their line-broadening mechanisms. Cluster spectra were calculated for several atmospheric levels for two example exoplanet atmospheres (WASP 121b-like and WASP 96b-like) to identify possible spectral fingerprints for cloud formation. Results. The rotational motion of clusters and the rotational transitions within them cause significant line broadening, so that individual vibrational lines are broadened beyond the spectral resolution of the medium-resolution mode of the JWST mid-infrared instrument (MIRI) at R = 3000. However, each individual cluster isomer exhibits a ‘fingerprint’ IR spectrum. In particular, larger (TiO2) clusters have distinctly different spectra from smaller clusters. The morning and evening terminator for the same planet can exhibit different total absorbances, due to the greater abundance of different cluster sizes. Conclusions. The largest (TiO2) clusters are not necessarily the most abundant (TiO2) clusters in the high-altitude regions of ultra-hot Jupiters and the different cluster isomers do contribute to the local absorbance. Planets with a considerable day-night asymmetry will be most suitable in the search for (TiO2) cluster isomers with the goal of improving cloud formation modelling.

On the afternoon of 3 July 2004 in Hyytiälä (Juupajoki, Finland), convective cells produced a strong downburst causing forest damage. The SMEAR II field station, situated near the damage site, enabled a unique micrometeorological analysis of a microburst with differences above and inside the canopy. At the time of the event, a squall line associated with a cold front was crossing Hyytiälä with a reflectivity maximum in the middle of the squall line. A bow echo, rear-inflow notch, and probable mesovortex were observed in radar data. The bow echo moved west-north-west, and its apex travelled just north of Hyytiälä. The turbulence data were analysed at two locations above the forest canopy and at one location at sub-canopy. At 1412 EET (Eastern European Time, UTC+2), the horizontal and vertical wind speed increased and the wind veered, reflecting the arrival of a gust front. At the same time, the carbon dioxide concentration increased due to turbulent mixing, the temperature decreased due to cold air flow from aloft and aerosol particle concentration decreased due to rain scavenging. An increase in the number concentration of ultra-fine particles (< 10 nm) was detected, supporting the new particle formation either from cloud outflow or due to rain. Five minutes after the gust front (1417 EET), strong horizontal and downward vertical wind speed gusts occurred with maxima of 22 and 15 m s−1, respectively, reflecting the microburst. The turbulence spectra before, during and after the event were consistent with traditional turbulence spectral theory.

New particle formation is one of the major sources of atmospheric aerosol particles. Beside daytime nucleation, nocturnal new particle formation was also found in different regions around the world. Compared with daytime nucleation events, the understanding of nocturnal ones is still sparse. The variety of aerosol particle physico-chemical properties, including particle number size distribution, volatility and hygroscopicity were measured in the North China Plain during July–August 2013. During the observation period, rapid increase in ultrafine particle number concentration was attributed to new particle formation. The nocturnal new particle formation rate was 45 cm–3s–1, which is 1.25 times higher than an observed daytime value. Condensation sink was found to be 0.055 s–1.

In this study, the observation site Himalayan Cloud Observatory is located at the high-altitude location (30.34 N, 78.40 E, 1706 m above mean sea level) and established at Swami Ram Tirth Campus, Badshahithaul, Tehri Garhwal, Uttarakhand in the western Himalaya. We have identified and characterized the new particle formation events for 12-months period (January to December, 2021) of continuous monitoring of the aerosol size distribution using NanoScan Scanning Mobility Particle Sizer. Another year-long observation was carried out at the Himalayan Atmospheric and Space Physics Research Laboratory (HASPRL), Department of Physics, Hemvati Nandan Bahuguna Garhwal University (A Central University), Srinagar Garhwal, Uttarakhand, in the Alaknanda Valley (30°13'37.3"N, 78°48'14.2"E, 640 m AMSL), from January 1, 2023, to December 31, 2023.We have observed 51 new particle formation events out of 278 days of observations having 14% frequency of new particle formation occurrence. New particle formation events were most frequent in March-April-May (pre-monsoon) and least frequent in June-July-August-September (monsoon). This trend is linked to high temperatures, strong solar radiation, and low relative humidity in pre-monsoon, which enhance the formation of low-volatility organic compounds, while in monsoon, wet scavenging reduces aerosol precursor gases. The seasonal mean of growth rate (GR11.5-27.4 nm), formation rate (J11.5), coagulation sink (CoagS11.5-27.4) and condensation sink (CSTOT, 11.5-154 nm) during the study period were 1.27±0.23 nm h-1, 0.12±0.08 cm-3 s-1, 2.92±1.65×10-5 s-1 and 9.91±3.13×10-3 s-1 respectively. Seasonal distributions show particles within 11.5–100 nm predominantly originate from secondary emissions, while particles 100–154 nm result from both direct and nucleated process, highlighting the seasonal sources of particles at Himalayan Cloud Observatory. A significant reduction (by 25%) found in incoming solar radiation on non-event days limits the oxidation of precursor gases, thereby inhibiting particle formation. Polar bivariate analysis reveals that winter airmasses, transported via mountain winds from the southwest and northeast, introduce mixed particle sizes. In contrast, the localized concentration of particles with elevated GR11.5-27.4 nm and J11.5 during pre-monsoon highlights the role of aerosol precursors, condensable vapors, and favorable meteorological conditions, emphasizing new particle formation as the dominant particle source. Comparison with prior cloud condensation nuclei study at Himalayan Cloud Observatory reveals that new particle formation significantly supplements cloud condensation nuclei production beyond primary emissions, especially in pre-monsoon. The satellite-based observation of sulfur dioxide and formaldehyde complement and support the condensable vapours during event days at Himalayan Cloud Observatory. At HASPRL, smaller-sized aerosol particles showed an increase in the morning, likely due to emissions from anthropogenic sources originating from the southwest. In the evening, larger-sized aerosol particles were observed to increase, possibly resulting from various human activities such as vehicular emissions, transportation of sand and stone, and other anthropogenic emissions from the southeast. At HCO, particle transport is likely influenced by movement from valley and forested regions, with air masses traveling from the southeast to the southwest.In summary, this research offers fresh perspectives on the characterization of new particle formation events in the Himalayan region of Uttarakhand. These insights are crucial for comprehending secondary aerosol formation processes worldwide, particularly at the process level.

Particulate organic nitrates at Mount Tai in winter and spring: Variation characteristics and effects of mountain-valley breezes and elevated emission sources

New Particle Formation (NPF) is regularly observed to occur in heavily polluted Chinese megacities. However, in these NPF events, the survival probability of small clusters into larger aerosol particles is higher than theoretically predicted. One explanation for this could be that the loss rate of clusters due to scavenging by pre-existing particles, which is described by condensation sink, is lower than expected. In this study, we describe the loss of clusters due to condensation sink by using heterogeneous nucleation theory, and investigate if ineffectiveness of heterogeneous nucleation can result in a significantly lowered effective condensation sink. We find that in principle it is possible that due to properties of the system there is no heterogeneous nucleation, and this can significantly influence the magnitude of effective condensation sink and thus increase the survival probability of clusters.

Incorporation of new particle formation and early growth treatments into WRF/Chem: Model improvement, evaluation, and impacts of anthropogenic aerosols over East Asia

Understanding new particle formation and their subsequent growth in the troposphere has a critical impact on our ability to predict atmospheric composition and global climate change. High pre-existing particle loadings have been thought to suppress the formation of new atmospheric aerosol particles due to high condensation and coagulation sinks. Here, based on field measurements at a mountain site in South China, we report, for the first time, in situ observational evidence on new particle formation and growth in remote ambient atmosphere during heavy dust episodes mixed with anthropogenic pollution. Both the formation and growth rates of particles in the diameter range 15–50 nm were enhanced during the dust episodes, indicating the influence of photo-induced, dust surface-mediated reactions and resulting condensable vapor production. This study provides unique in situ observations of heterogeneous photochemical processes inducing new particle formation and growth in the real atmosphere, and suggests an unexpected impact of mineral dust on climate and atmospheric chemistry.

Heavy rain in Semarang on 1 January 2020 caused flooding. The existence of heavy rain cannot be separated from the dynamics of weather parameters which are closely related to the convection process and cloud formation. In this paper research has been conducted using Weather Research and Forecasting (WRF), to analyze the growth patterns of convective clouds as an effort to mitigate the initial events of extreme rainfall disasters. Several weather parameters that support cloud growth are very significant, namely the parameter values ​​that support the convection process to form convective clouds (Cumulonimbus). The results of the model show that there has been extreme rainfall which can be used as initial mitigation of hydrometeorological disasters.

Abstract. Understanding the particle number size distributions in diversified atmospheric environments is important in order to design mitigation strategies related to submicron particles and their effects on regional air quality, haze and human health. In this study, we conducted 15 different field measurement campaigns between 2007 and 2011 at 13 individual sites in China, including five urban sites, four regional sites, three coastal/background sites and one ship cruise measurement along eastern coastline of China. Size resolved particles were measured in the 15–600 nm size range. The median particle number concentrations (PNCs) were found to vary in the range of 1.1−2.2 × 104 cm−3 at urban sites, 0.8−1.5 × 104 cm−3 at regional sites, 0.4−0.6 × 104 cm−3 at coastal/background sites, and 0.5 × 104 cm−3 during cruise measurement. Peak diameters at each of these sites varied greatly from 24 to 115 nm. Particles in the 15–25 nm (nucleation mode), 25–100 nm (Aitken mode) and 100–600 nm (accumulation mode) range showed different characteristics at each sites, indicating the features of primary emissions and secondary formation in these diversified atmospheric environments. Diurnal variations show a build-up of accumulation mode particles belt at regional sites, suggesting the contribution of regional secondary aerosol pollution. Frequencies of new particle formation (NPF) events were much higher at urban and regional sites than at coastal sites and during cruise measurement. The average growth rates (GRs) of nucleation mode particles were 8.0–10.9 nm h−1 at urban sites, 7.4–13.6 nm h−1 at regional sites and 2.8–7.5 nm h−1 at coastal sites and during cruise measurement. The high gaseous precursors and strong oxidation at urban and regional sites not only favored the formation of particles, but also accelerated the growth rate of the nucleation mode particles. No significant difference in condensation sink (CS) during NPF days were observed among different site types, suggesting that the NPF events in background areas were more influenced by the pollutant transport. In addition, average contributions of NPF events to potential cloud condensation nuclei (CCN) at 0.2% super-saturation in the afternoon of all sampling days were calculated as 11% and 6% at urban sites and regional sites, respectively. On the other hand, NPF events at coastal sites and during cruise measurement had little impact on potential production of CCN. This study provides a large data set of particle size distribution in diversified atmosphere of China, improving our general understanding of emission, secondary formation, new particle formation and corresponding CCN activity of submicron aerosols in Chinese environments.

Formation of Ultrafine particles (UFPs) in the urban atmosphere is expected to be less favored than in the rural atmosphere due to the high existing particle surface area acting as a sink for newly-formed particles Despite the large condensation sink (CS) values, previous comparative studies between rural and urban site reported higher frequency of new particle formation (NPF) events over urban sites in comparison to background sites as well as higher particle formation and growth rates attributed to the higher concentration of condensable species. The present study aims to better understand the environmental factors favoring, or disfavoring, atmospheric NPF over Lille, a large city North of France and to analyze their impact on particle number concentration using a long-term dataset (4 years : 1st July 2017 to 31st December 2020). The results highlight a strong seasonal variation of the NPF occurrences with a maximum observed during spring (27 events) and summer (53 events). It was found that high temperature (T > 295 K), low RH (RH < 45 %) and high solar radiation are ideal to observe NPF events over Lille. Relatively high values of condensation sink (CS ~ 2.10-2 s-1) are reported during event days suggesting that high CS does not inhibit the occurrence of NPFt over our site. Moreover, the particle Growth Rate (GR15.7-30 nm) was positively correlated with the temperature most probably linked to the higher emissions of precursors. Finally, the nucleation strength factor (NSF) was calculated to highlight the impact of those NPF events on particle number concentrations. NSF15.7-100 reaches a maximum of 4 in summer, indicating an enormous contribution of NPF events to particle number concentration at this time of the year.