scholarly journals Modelling the contribution of biogenic VOCs to new particle formation in the Jülich plant atmosphere chamber

2014 ◽  
Vol 14 (20) ◽  
pp. 27973-28018 ◽  
Author(s):  
L. Liao ◽  
M. Dal Maso ◽  
D. Mogensen ◽  
P. Roldin ◽  
A. Rusanen ◽  
...  
Keyword(s):  
Organic Compounds ◽  
Particle Number ◽  
Particle Formation ◽  
Oxidation Products ◽  
New Particle Formation ◽  
Particle Volume ◽  
Aerosol Dynamics ◽  
Total Particle Number ◽  
Total Particle ◽  
Air Chemistry

Abstract. We used the MALTE-BOX model including near-explicit air chemistry and detailed aerosol dynamics to study the mechanisms of observed new particle formation events in the Jülich Plant Atmosphere Chamber. The modelled and measured H2SO4 (sulfuric acid) concentrations agreed within a factor of two. The modelled total monoterpene concentration was in line with PTR-MS observations, and we provided the distributions of individual isomers of terpenes, when no measurements were available. The aerosol dynamic results supported the hypothesis that H2SO4 is one of the critical compounds in the nucleation process. However, compared to kinetic H2SO4 nucleation, nucleation involving OH oxidation products of monoterpenes showed a better agreement with the measurements, with R2 up to 0.97 between modelled and measured total particle number concentrations. The nucleation coefficient for kinetic H2SO4 nucleation was 2.1 × 10−11 cm3 s−1, while the organic nucleation coefficient was 9.0 × 10−14 cm3 s−1. We classified the VOC oxidation products into two sub-groups including extremely low-volatility organic compounds (ELVOCs) and semi-volatile organic compounds (SVOCs). These ELVOCs and SVOCs contributed approximately equally to the particle volume production, whereas only ELVOCs made the smallest particles to grow in size. The model simulations revealed that the chamber walls constitute a major net sink of SVOCs on the first experiment day. However, the net wall SVOC uptake was gradually reduced because of SVOC desorption during the following days. Thus, in order to capture the observed temporal evolution of the particle number size distribution, the model needs to consider reversible gas-wall partitioning.

scholarly journals Seasonal cycle and modal structure of particle number size distribution at Dome C, Antarctica

2013 ◽  
Vol 13 (15) ◽  
pp. 7473-7487 ◽  
Author(s):  
E. Järvinen ◽  
A. Virkkula ◽  
T. Nieminen ◽  
P. P. Aalto ◽  
E. Asmi ◽  
...  
Keyword(s):  
Size Distribution ◽  
Seasonal Cycle ◽  
Particle Number ◽  
Formation Rate ◽  
Particle Growth ◽  
Particle Formation ◽  
Distribution Data ◽  
New Particle Formation ◽  
Total Particle Number ◽  
Total Particle

Abstract. We studied new particle formation and modal behavior of ultrafine aerosol particles on the high East Antarctic plateau at the Concordia station, Dome C (75°06' S, 123°23' E). Aerosol particle number size distributions were measured in the size range 10–600 nm from 14 December 2007 to 7 November 2009. We used an automatic algorithm for fitting up to three modes to the size distribution data. The total particle number concentration was low with the median of 109 cm−3. There was a clear seasonal cycle in the total particle number and the volume concentrations. The concentrations were at their highest during the austral summer with the median values of 260 cm−3 and 0.086 μm3 cm−3, and at their lowest during the austral winter with corresponding values of 15 cm−3 and 0.009 μm3 cm−3. New particle formation events were determined from the size distribution data. During the measurement period, natural new particle formation was observed on 60 days and for 15 of these days the particle growth rates from 10 to 25 nm in size could be determined. The median particle growth rate during all these events was 2.5 nm h−1 and the median formation rate of 10 nm particles was 0.023 cm−3 s−1. Most of the events were similar to those observed at other continental locations, yet also some variability in event types was observed. Exceptional features in Dome C were the winter events that occurred during dark periods, as well as the events for which the growth could be followed during several consecutive days. We called these latter events slowly growing events. This paper is the first one to analyze long-term size distribution data from Dome C, and also the first paper to show that new particle formation events occur in central Antarctica.

scholarly journals Seasonal cycle and modal structure of particle number size distribution at Dome C, Antarctica

2013 ◽  
Vol 13 (3) ◽  
pp. 5729-5768
Author(s):  
E. Järvinen ◽  
A. Virkkula ◽  
T. Nieminen ◽  
P. P. Aalto ◽  
E. Asmi ◽  
...  
Keyword(s):  
Size Distribution ◽  
Seasonal Cycle ◽  
Particle Number ◽  
Formation Rate ◽  
Particle Growth ◽  
Particle Formation ◽  
Distribution Data ◽  
New Particle Formation ◽  
Total Particle Number ◽  
Total Particle

Abstract. We studied new particle formation and modal behavior of ultrafine aerosol particles on the high Antarctic East-Plateau at the Concordia station, Dome C (75°06' S, 123°23' E). Aerosol particle number size distributions were measured in the size range 10–600 nm from 14 December 2007 to 7 November 2009. We used an automatic algorithm for fitting up to three modes to the size distribution data. The total particle number concentration was low with the median of 109 cm−3. There was a clear seasonal cycle in the total particle number and the volume concentrations. The concentrations were at their highest during the austral summer with the median values of 260 cm−3 and 0.086 μm3 cm−3, and at their lowest during the austral winter with corresponding values of 15 cm−3 and 0.009 μm3 cm−3. New particle formation events were determined from the size distribution data. During the measurement period, new particle formation was seen on 80 days and for 15 of these days the particle growth rates from 10 to 25 nm size could be determined. The median particle growth rate during all these events was 2.5 nm h−1 and the median formation rate of 10 nm particles was 0.023 cm−3 s−1. Most of the events were similar to those observed in other continental locations, yet also some variability in event types was observed. Exceptional features in Dome C were the winter events that occurred during dark periods, as well as the events for which the growth could be followed during several consecutive days. We called these latter events as slowly-growing events. This paper is the first one to analyze long-term size distribution data from Dome C, and also the first paper to show that new particle formation events occur in the central Antarctica.

scholarly journals Production, growth and properties of ultrafine atmospheric aerosol particles in an urban environment

2011 ◽  
Vol 11 (3) ◽  
pp. 1339-1353 ◽  
Author(s):  
I. Salma ◽  
T. Borsós ◽  
T. Weidinger ◽  
P. Aalto ◽  
T. Hussein ◽  
...  
Keyword(s):  
Standard Deviation ◽  
Atmospheric Aerosol ◽  
Particle Number ◽  
Aerosol Particles ◽  
Formation Rate ◽  
Particle Formation ◽  
Number Concentration ◽  
New Particle Formation ◽  
Total Particle Number ◽  
Total Particle

Abstract. Number concentrations of atmospheric aerosol particles were measured by a flow-switching type differential mobility particle sizer in an electrical mobility diameter range of 6–1000 nm in 30 channels near central Budapest with a time resolution of 10 min continuously from 3 November 2008 to 2 November 2009. Daily median number concentrations of particles varied from 3.8 × 103 to 29 ×103 cm−3 with a yearly median of 11.8 × 103 cm−3. Contribution of ultrafine particles to the total particle number ranged from 58 to 92% with a mean ratio and standard deviation of (79 ± 6)%. Typical diurnal variation of the particle number concentration was related to the major emission patterns in cities, new particle formation, sinks of particles and meteorology. Shapes of the monthly mean number size distributions were similar to each other. Overall mean for the number median mobility diameter of the Aitken and accumulation modes were 26 and 93 nm, respectively, which are substantially smaller than for rural or background environments. The Aitken and accumulation modes contributed similarly to the total particle number concentrations at the actual measurement location. New particle formation and growth unambiguously occurred on 83 days, which represent 27% of all relevant days. Hence, new particle formation and growth are not rare phenomena in Budapest. Their frequency showed an apparent seasonal variation with a minimum of 7.3% in winter and a maximum of 44% in spring. New particle formation events were linked to increased gas-phase H2SO4 concentrations. In the studied area, new particle formation is mainly affected by condensation sink and solar radiation. The formation process seems to be not sensitive to SO2, which was present in a yearly median concentration of 6.7 μg m−3. This suggests that the precursor gas was always available in excess. Formation rate of particles with a diameter of 6 nm varied between 1.65 and 12.5 cm−3 s−1 with a mean and standard deviation of (4.2 ± 2.5) cm−3 s−1. Seasonal dependency for the formation rate could not be identified. Growth curves of nucleated particles were usually superimposed on the characteristic diurnal pattern of road traffic direct emissions. The growth rate of the nucleation mode with a median diameter of 6 nm varied from 2.0 to 13.3 nm h−1 with a mean and standard deviation of (7.7 ± 2.4) nm h−1. There was an indicative tendency for larger growth rates in summer and for smaller values in winter. New particle formation events increased the total number concentration by a mean factor and standard deviation of 2.3 ± 1.1 relative to the concentration that occurred immediately before the event. Several indirect evidences suggest that the new particle formation events occurred at least over the whole city, and were of regional type. The results and conclusions presented are the first information of this kind for the region over one-year long time period.

scholarly journals Vertical marine snow distribution in the stratified, hypersaline, and anoxic Orca Basin (Gulf of Mexico)

Elem Sci Anth ◽  
2019 ◽  
Vol 7 ◽  
Author(s):  
Arne Diercks ◽  
Kai Ziervogel ◽  
Ryan Sibert ◽  
Samantha B. Joye ◽  
Vernon Asper ◽  
...  
Keyword(s):  
Organic Carbon ◽  
Gulf Of Mexico ◽  
Particle Number ◽  
Sea Surface ◽  
Marine Snow ◽  
Particle Volume ◽  
Total Particle Number ◽  
Total Particle ◽  
Snow Distribution ◽  
Orca Basin

We present a complete description of the depth distribution of marine snow in Orca Basin (Gulf of Mexico), from sea surface through the pycnocline to within 10 m of the seafloor. Orca Basin is an intriguing location for studying marine snow because of its unique geological and hydrographic setting: the deepest ~200 m of the basin are filled with anoxic hypersaline brine. A typical deep ocean profile of marine snow distribution was observed from the sea surface to the pycnocline, namely a surface maximum in total particle number and midwater minimum. However, instead of a nepheloid (particle-rich) layer positioned near the seabed, the nepheloid layer in the Orca Basin was positioned atop the brine. Within the brine, the total particle volume increased by a factor of 2–3 while the total particle number decreased, indicating accumulation and aggregation of material in the brine. From these observations we infer increased residence time and retention of material within the brine, which agrees well with laboratory results showing a 2.2–3.5-fold reduction in settling speed of laboratory-generated marine snow below the seawater-brine interface. Similarly, dissolved organic carbon concentration in the brine correlated positively with measured colored dissolved organic matter (r2 = 0.92, n = 15), with both variables following total particle volume inversely through the pycnocline. These data indicate the release of dissolved organic carbon concomitant with loss in total particle volume and increase in particle numbers at the brine-seawater interface, highlighting the importance of the Orca Basin as a carbon sink.

scholarly journals New insights into nocturnal nucleation

2012 ◽  
Vol 12 (9) ◽  
pp. 4297-4312 ◽  
Author(s):  
I. K. Ortega ◽  
T. Suni ◽  
M. Boy ◽  
T. Grönholm ◽  
H. E. Manninen ◽  
...  
Keyword(s):  
Quantum Chemical ◽  
Aerosol Particles ◽  
Particle Formation ◽  
Nucleation And Growth ◽  
Oxidation Products ◽  
New Particle Formation ◽  
Aerosol Dynamics ◽  
Different Types ◽  
Consistent Manner ◽  
Dynamics Models

Abstract. Formation of new aerosol particles by nucleation and growth is a significant source of aerosols in the atmosphere. New particle formation events usually take place during daytime, but in some locations they have been observed also at night. In the present study we have combined chamber experiments, quantum chemical calculations and aerosol dynamics models to study nocturnal new particle formation. All our approaches demonstrate, in a consistent manner, that the oxidation products of monoterpenes play an important role in nocturnal nucleation events. By varying the conditions in our chamber experiments, we were able to reproduce the very different types of nocturnal events observed earlier in the atmosphere. The exact strength, duration and shape of the events appears to be sensitive to the type and concentration of reacting monoterpenes, as well as the extent to which the monoterpenes are exposed to ozone and potentially other atmospheric oxidants.

scholarly journals Secondary organic aerosol production from pinanediol, a semi-volatile surrogate for first-generation oxidation products of monoterpenes

2018 ◽  
Vol 18 (9) ◽  
pp. 6171-6186 ◽  
Author(s):  
Penglin Ye ◽  
Yunliang Zhao ◽  
Wayne K. Chuang ◽  
Allen L. Robinson ◽  
Neil M. Donahue
Keyword(s):  
Organic Compounds ◽  
First Generation ◽  
Secondary Organic Aerosol ◽  
Organic Aerosol ◽  
Particle Formation ◽  
Oxidation Products ◽  
Basis Set ◽  
New Particle Formation ◽  
Aerosol Mass ◽  
Volatile Precursor

Abstract. We have investigated the production of secondary organic aerosol (SOA) from pinanediol (PD), a precursor chosen as a semi-volatile surrogate for first-generation oxidation products of monoterpenes. Observations at the CLOUD facility at CERN have shown that oxidation of organic compounds such as PD can be an important contributor to new-particle formation. Here we focus on SOA mass yields and chemical composition from PD photo-oxidation in the CMU smog chamber. To determine the SOA mass yields from this semi-volatile precursor, we had to address partitioning of both the PD and its oxidation products to the chamber walls. After correcting for these losses, we found OA loading dependent SOA mass yields from PD oxidation that ranged between 0.1 and 0.9 for SOA concentrations between 0.02 and 20 µg m−3, these mass yields are 2–3 times larger than typical of much more volatile monoterpenes. The average carbon oxidation state measured with an aerosol mass spectrometer was around −0.7. We modeled the chamber data using a dynamical two-dimensional volatility basis set and found that a significant fraction of the SOA comprises low-volatility organic compounds that could drive new-particle formation and growth, which is consistent with the CLOUD observations.

scholarly journals New insights into nocturnal nucleation

2011 ◽  
Vol 11 (11) ◽  
pp. 31323-31362 ◽  
Author(s):  
I. K. Ortega ◽  
T. Suni ◽  
M. Boy ◽  
T. Grönholm ◽  
H. E. Manninen ◽  
...  
Keyword(s):  
Quantum Chemical ◽  
Aerosol Particles ◽  
Particle Formation ◽  
Nucleation And Growth ◽  
Oxidation Products ◽  
New Particle Formation ◽  
Aerosol Dynamics ◽  
Different Types ◽  
Consistent Manner ◽  
Dynamics Models

Abstract. Formation of new aerosol particles by nucleation and growth is a significant source of aerosols in the atmosphere. New particle formation events usually take place during daytime, but in some locations they have been observed also at night. In the present study we have combined chamber experiments, quantum chemical calculations and aerosol dynamics models to study nocturnal new particle formation. All our approaches demonstrate, in a consistent manner, that the oxidation products of monoterpenes play an important role in nocturnal nucleation events. By varying the conditions in our chamber experiments, we were able to reproduce the very different types of nocturnal events observed earlier in the atmosphere. The exact strength, duration and shape of the events appears to be sensitive to the type and concentration of reacting monoterpenes, as well as the extent to which the monoterpenes are exposed to ozone and potentially other atmospheric oxidants.

scholarly journals The contribution of boundary layer nucleation events to total particle concentrations on regional and global scales

2006 ◽  
Vol 6 (12) ◽  
pp. 5631-5648 ◽  
Author(s):  
D. V. Spracklen ◽  
K. S. Carslaw ◽  
M. Kulmala ◽  
V.-M. Kerminen ◽  
G. W. Mann ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Sulfuric Acid ◽  
Particle Number ◽  
Formation Rate ◽  
Particle Surface ◽  
Particle Formation ◽  
New Particle Formation ◽  
Particle Surface Area ◽  
Primary Particles ◽  
Total Particle

Abstract. The contribution of boundary layer (BL) nucleation events to total particle concentrations on the global scale has been studied by including a new particle formation mechanism in a global aerosol microphysics model. The mechanism is based on an analysis of extensive observations of particle formation in the BL at a continental surface site. It assumes that molecular clusters form at a rate proportional to the gaseous sulfuric acid concentration to the power of 1. The formation rate of 3 nm diameter observable particles is controlled by the cluster formation rate and the existing particle surface area, which acts to scavenge condensable gases and clusters during growth. Modelled sulfuric acid vapour concentrations, particle formation rates, growth rates, coagulation loss rates, peak particle concentrations, and the daily timing of events in the global model agree well with observations made during a 22-day period of March 2003 at the SMEAR II station in Hyytiälä, Finland. The nucleation bursts produce total particle concentrations (>3 nm diameter) often exceeding 104 cm−3, which are sustained for a period of several hours around local midday. The predicted global distribution of particle formation events broadly agrees with what is expected from available observations. Over relatively clean remote continental locations formation events can sustain mean total particle concentrations up to a factor of 8 greater than those resulting from anthropogenic sources of primary organic and black carbon particles. However, in polluted continental regions anthropogenic primary particles dominate particle number and formation events lead to smaller enhancements of up to a factor of 2. Our results therefore suggest that particle concentrations in remote continental regions are dominated by nucleated particles while concentrations in polluted continental regions are dominated by primary particles. The effect of BL particle formation over tropical regions and the Amazon is negligible. These first global particle formation simulations reveal some interesting sensitivities. We show, for example, that significant reductions in primary particle emissions may lead to an increase in total particle concentration because of the coupling between particle surface area and the rate of new particle formation. This result suggests that changes in emissions may have a complicated effect on global and regional aerosol properties. Overall, our results show that new particle formation is a significant component of the aerosol particle number budget.

scholarly journals Production of extremely low volatile organic compounds from biogenic emissions: Measured yields and atmospheric implications

2015 ◽  
Vol 112 (23) ◽  
pp. 7123-7128 ◽  
Author(s):  
Tuija Jokinen ◽  
Torsten Berndt ◽  
Risto Makkonen ◽  
Veli-Matti Kerminen ◽  
Heikki Junninen ◽  
...  
Keyword(s):  
Double Bond ◽  
Organic Compounds ◽  
Cloud Condensation Nuclei ◽  
Particle Formation ◽  
Oxidation Products ◽  
Major Influence ◽  
Oh Radical ◽  
New Particle Formation ◽  
Modeling Framework ◽  
Laboratory Findings

Oxidation products of monoterpenes and isoprene have a major influence on the global secondary organic aerosol (SOA) burden and the production of atmospheric nanoparticles and cloud condensation nuclei (CCN). Here, we investigate the formation of extremely low volatility organic compounds (ELVOC) from O3 and OH radical oxidation of several monoterpenes and isoprene in a series of laboratory experiments. We show that ELVOC from all precursors are formed within the first minute after the initial attack of an oxidant. We demonstrate that under atmospherically relevant concentrations, species with an endocyclic double bond efficiently produce ELVOC from ozonolysis, whereas the yields from OH radical-initiated reactions are smaller. If the double bond is exocyclic or the compound itself is acyclic, ozonolysis produces less ELVOC and the role of the OH radical-initiated ELVOC formation is increased. Isoprene oxidation produces marginal quantities of ELVOC regardless of the oxidant. Implementing our laboratory findings into a global modeling framework shows that biogenic SOA formation in general, and ELVOC in particular, play crucial roles in atmospheric CCN production. Monoterpene oxidation products enhance atmospheric new particle formation and growth in most continental regions, thereby increasing CCN concentrations, especially at high values of cloud supersaturation. Isoprene-derived SOA tends to suppress atmospheric new particle formation, yet it assists the growth of sub-CCN-size primary particles to CCN. Taking into account compound specific monoterpene emissions has a moderate effect on the modeled global CCN budget.

scholarly journals Modelling the contribution of biogenic volatile organic compounds to new particle formation in the Jülich plant atmosphere chamber

2015 ◽  
Vol 15 (18) ◽  
pp. 10777-10798 ◽  
Author(s):  
P. Roldin ◽  
L. Liao ◽  
D. Mogensen ◽  
M. Dal Maso ◽  
A. Rusanen ◽  
...  
Keyword(s):  
Gas Phase ◽  
Organic Compounds ◽  
Particle Surface ◽  
Particle Formation ◽  
Heterogeneous Reactions ◽  
Chemical Mechanism ◽  
Particle Phase ◽  
New Particle Formation ◽  
Aerosol Dynamics ◽  
Phase Chemistry

Abstract. We used the Aerosol Dynamics gas- and particle-phase chemistry model for laboratory CHAMber studies (ADCHAM) to simulate the contribution of BVOC plant emissions to the observed new particle formation during photooxidation experiments performed in the Jülich Plant-Atmosphere Chamber and to evaluate how well smog chamber experiments can mimic the atmospheric conditions during new particle formation events. ADCHAM couples the detailed gas-phase chemistry from Master Chemical Mechanism with a novel aerosol dynamics and particle phase chemistry module. Our model simulations reveal that the observed particle growth may have either been controlled by the formation rate of semi- and low-volatility organic compounds in the gas phase or by acid catalysed heterogeneous reactions between semi-volatility organic compounds in the particle surface layer (e.g. peroxyhemiacetal dimer formation). The contribution of extremely low-volatility organic gas-phase compounds to the particle formation and growth was suppressed because of their rapid and irreversible wall losses, which decreased their contribution to the nano-CN formation and growth compared to the atmospheric situation. The best agreement between the modelled and measured total particle number concentration (R2 > 0.95) was achieved if the nano-CN was formed by kinetic nucleation involving both sulphuric acid and organic compounds formed from OH oxidation of BVOCs.

Sign in / Sign up

Export Citation Format

Share Document