Ambient new particle formation parameter indicates potential rise in future events

Atmospheric new particle formation is a general phenomenon observed over coniferous forests. So far nucleation is described as a function of gaseous sulfuric acid concentration only, which is unable to explain the observed seasonality of nucleation events at different measurement sites. Here we introduce a new nucleation parameter including ozone and water vapor concentrations as well as UV-B radiation as a proxy for OH radical formation. Applying this new parameter to field studies conducted at Finnish and German measurement sites it is found capable to predict the occurrence of nucleation events and their seasonal and annual variation indicating a significant role of organics. Extrapolation to possible future conditions of ozone, water vapor and organic concentrations leads to a significant potential increase in nucleation event number

A new parametrization for ambient particle formation over coniferous forests and its potential implications for the future

Atmospheric new particle formation is a general phenomenon observed over coniferous forests. So far nucleation is either parameterised as a function of gaseous sulphuric acid concentration only, which is unable to explain the observed seasonality of nucleation events at different measurement sites, or as a function of sulphuric acid and organic molecules. Here we introduce different nucleation parameters based on the interaction of sulphuric acid and terpene oxidation products and elucidate the individual importance. They include basic trace gas and meteorological measurements such as ozone and water vapour concentrations, temperature (for terpene emission) and UV B radiation as a proxy for OH radical formation. We apply these new parameters to field studies conducted at conducted at Finnish and German measurement sites and compare these to nucleation observations on a daily and annual scale. General agreement was found, although the specific compounds responsible for the nucleation process remain speculative. This can be interpreted as follows: During cooler seasons the emission of biogenic terpenes and the OH availability limits the new particle formation while towards warmer seasons the ratio of ozone and water vapour concentration seems to dominate the general behaviour. Therefore, organics seem to support ambient nucleation besides sulphuric acid or an OH-related compound. Using these nucleation parameters to extrapolate the current conditions to prognosed future concentrations of ozone, water vapour and organic concentrations leads to a significant potential increase in the nucleation event number

Aerosol dynamics simulations of the anatomical variability of e-cigarette particle and vapor deposition in a stochastic lung

Electronic cigarette (EC) aerosols are typically composed of a mixture of nicotine, glycerine (VG), propylene glycol (PG), water, acidic stabilizers and a variety of flavors. Inhalation of e-cigarette aerosols is characterized by a continuous modification of particle diameters, concentrations, composition and phase changes, and smoker-specific inhalation conditions, i.e. puffing, mouthhold and bolus inhalation. The dynamic changes of inhaled e-cigarette droplets in the lungs due to coagulation, conductive heat and diffusive heat/convective vapor transport and particle phase chemistry are described by the Aerosol Dynamics in Containment (ADiC) model. For the simulation of the variability of inhaled particle and vapor deposition, the ADiC model is coupled with the IDEAL Monte Carlo code, which is based on a stochastic, asymmetric airway model of the human lung. We refer to the coupled model as "IDEAL/ADIC_v1.0". In this study, two different ecigarettes were compared, one without any acid ("no acid") and the other one with an acidic regulator (benzoic acid) to establish an initial pH level of about 7 ("lower pH"). Corresponding deposition patterns among human airways comprise total and compound-specific number and mass deposition fractions, distinguishing between inhalation and exhalation phases and condensed and vapor phases. Note that the inhaled EC aerosol is significantly modified in the oral cavity prior to inhalation into the lungs. Computed deposition fractions demonstrate that total particle mass is preferentially deposited in the alveolar region of the lung during inhalation. While nicotine deposits prevalently in the condensed phase for the "lower pH" case, vapor phase deposition is dominating the "no acid" case. The significant statistical fluctuations of the particle and vapor deposition patterns illustrate the inherent anatomical variability of the human lung structure.Peer reviewe

Understanding the formation of biogenic secondary organic aerosol formation from alpha-pinene in smog chamber studies: role of organic peroxy radicals

Non peer reviewe

A DNS study of aerosol and small-scale cloud turbulence interaction

The purpose of this study is to investigate the interaction between small-scale turbulence and aerosol and cloud microphysical properties using direct numerical simulations (DNS). We consider the domain located at the height of about 2000 m from the sea level, experiencing transient high supersaturation due to atmospheric fluctuations of temperature and humidity. To study the effect of total number of particles (Ntot) on air temperature, activation and supersaturation, we vary Ntot. To investigate the effect of aerosol dynamics on small-scale turbulence and vertical air motion, we vary the intensity of turbulent fluctuations and the buoyant force. We find that even a small number of aerosol particles (55.5 cm−3), and therefore a small droplet number concentration, strongly affects the air temperature due to release of latent heat. The system comes to an equilibrium faster and the relative number of activated particles appears to be smaller for larger Ntot. We conclude that aerosol particles strongly affect the air motion. In a case of updraught coursed by buoyant force, the presence of aerosol particles results in acceleration of air motion in vertical direction and increase of turbulent fluctuations

Estimating Blue Carbon Stocks in Native and Non-Native Seagrass Beds of Jobos Bay, PR

Seagrasses are keystone species that support coastal biodiversity, but not all species of seagrasses provide the same ecosystem services. Although seagrasses occupy a small area of marine habitat, they provide many ecosystem services. They stabilize sediments, remove nutrients, provide habitat and food for diverse marine life, and promote carbon storage in sediments. Jobos Bay is the second largest estuary in Puerto Rico and contains salt marshes, mangroves, and seagrass beds. The native seagrass, Thalassia testudinum, is the most abundant seagrass in the bay; however, a seagrass species from the Indian Ocean, Halophila stipulacea, began invading in recent years. The impacts of H. stipulacea have not been well-studied, and it is not yet known if the invasive species is displacing the native species or growing only in areas that were previously non-vegetated. This study investigates the effect of the invasive species on carbon storage in Jobos Bay. If the native species contributes more detritus to the sediments but is being outcompeted by the invasive species, it will mean less organic matter is stored in the sediments as the invasion progresses. Between March 7-20, nine cores were extracted from four different habitat types: 1) a T. testudinum bed, 2) a H. stipulacea bed, 3) an unvegetated area, and 4) an area where an algal accumulation extirpated an H. stipulacea population. The cores were sliced in 1 cm increments. Slices were dried and combusted at 500 C to determine bulk density and organic carbon content. Patterns in the amount of carbon storage across the depths and habitat types will be compared. Estimates of carbon storage will help natural resource managers understand potential impacts of the invasive species on ecosystem services

Aerosol mass yields of selected biogenic volatile organic compounds– a theoretical study with nearly explicit gas-phase chemistry

In this study we modeled secondary organic aerosol (SOA) mass loadings from the oxidation (by O-3, OH and NO3) of five representative biogenic volatile organic compounds (BVOCs): isoprene, endocyclic bond-containing monoterpenes (alpha-pinene and limonene), exocyclic double-bond compound (beta-pinene) and a sesquiterpene (beta-caryophyllene). The simulations were designed to replicate an idealized smog chamber and oxidative flow reactors (OFRs). The Master Chemical Mechanism (MCM) together with the peroxy radical autoxidation mechanism (PRAM) were used to simulate the gas-phase chemistry. The aim of this study was to compare the potency of MCM and MCM + PRAM in predicting SOA formation. SOA yields were in good agreement with experimental values for chamber simulations when MCM + PRAM was applied, while a stand-alone MCM underpredicted the SOA yields. Compared to experimental yields, the OFR simulations using MCM + PRAM yields were in good agreement for BVOCs oxidized by both O-3 and OH. On the other hand, a stand-alone MCM underpredicted the SOA mass yields. SOA yields increased with decreasing temperatures and NO concentrations and vice versa. This highlights the limitations posed when using fixed SOA yields in a majority of global and regional models. Few compounds that play a crucial role (> 95% of mass load) in contributing to SOA mass increase (using MCM + PRAM) are identified. The results further emphasized that incorporating PRAM in conjunction with MCM does improve SOA mass yield estimation.Peer reviewe

SOSAA — a new model to simulate the concentrations of organic vapours, sulphuric acid and aerosols inside the ABL — Part 2: Aerosol dynamics and one case study at a boreal forest site

Natural and anthropogenic aerosols may have a great impact on climate as they directly interact with solar radiation and indirectly affect the Earth’s radiation balance and precipitation by modifying clouds. In order to quantify the direct and indirect effects, it is essential to understand the complex processes that connect aerosol particles to cloud droplets. Modern measurement techniques are able to detect particle sizes down to 1 nm in diameter, from ground to the stratosphere. However, the data are not sufficient in order to fully understand the processes. Here we demonstrate how the newly developed one-dimensional column model SOSAA was used to investigate the complex processes of aerosols at a boreal forest site for a six-month period during the spring and summer of 2010. Two nucleation mechanisms (kinetic and organic) were tested in this study, and both mechanisms produced a good prediction of the particle number concentrations in spring. However, overestimation of the particle number concentration in summer by the organic mechanism suggests that the OH oxidation products from monoterpenes may not be the essential compounds in atmospheric nucleation. In general, SOSAA was correct in predicting new particle formation events for 35% of the time and partly correct for 45% of the time.Peer reviewe

Synthesis and Physical Properties of Iridium-Based Sulfide Ca1−xIr4S6(S2) [x = 0.23–0.33]

We present the synthesis and characterization of the iridium-based sulfide Ca1−xIr4S6(S2). Quality and phase analysis were conducted by means of energy-dispersive X-ray spectroscopy (EDXS) and powder X-ray diffraction (XRD) techniques. Structure analysis reveals a monoclinic symmetry with the space group C 1 2/m 1 (No. 12), with the lattice constants a = 15.030 (3) Å, b = 3.5747 (5) Å and c = 10.4572 (18) Å. Both X-ray diffraction and EDXS suggest an off-stoichiometry of calcium, leading to the empirical composition Ca1−xIr4.0S6(S2) [x = 0.23–0.33]. Transport measurements show metallic behavior of the compound in the whole range of measured temperatures. Magnetic measurements down to 1.8 K show no long range order, and Curie–Weiss analysis yields θCW = −31.4 K, suggesting that the compound undergoes a magnetic state with short range magnetic correlations. We supplement our study with calculations of the band structure in the framework of the density functional theory