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"Aalto, P."
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Semi-continuous gas and inorganic aerosol measurements at a Finnish urban site: comparisons with filters, nitrogen in aerosol and gas phases, and aerosol acidity
2012
Concentrations of 5 gases (HCl, HNO3, HONO, NH3, SO2) and 8 major inorganic ions in particles (Cl−, NO3−, SO42−, NH4+, Na+, K+, Mg2+, Ca2+) were measured with an online monitor MARGA 2S in two size ranges, Dp <2.5 μm and Dp < 10 μm, in Helsinki, Finland from November 2009 to May 2010. The results were compared with filter sampling, mass concentrations obtained from particle number size distributions, and a conventional SO2 monitor. The MARGA yielded lower concentrations than those analyzed from the filter samples for most ions. Linear regression yielded the following MARGA vs. filter slopes: 0.72 for Cl−, 0.90 for NO3−, 0.85 for SO42−, 0.91 for NH4+ , 0.49 for Na+, 3.0 for Mg2+, and 3.0 for Ca2+ and 0.90 for the MARGA vs. SO2 monitor. For K+ there were not enough data points to calculate a statistically significant linear regression. There were clear seasonal cycles in the concentrations of the nitrogen-containing gases: the median concentrations of HNO3, HONO, and NH3 were 0.09 ppb, 0.37 ppb, and 0.01 ppb in winter, respectively, and 0.15, 0.15, and 0.14 in spring, respectively. The gas-phase fraction of nitrogen decreased roughly with decreasing temperature, so that in the coldest period from January to February the median contribution was 28% but in April to May was 53%. There were also large fractionation variations that temperature alone cannot explain. HONO correlated well with NOx but a large fraction of the HONO-to-NOx ratios were larger than published ratios in a road traffic tunnel, suggesting that a large amount of HONO had other sources than vehicle exhaust. Aerosol acidity was estimated by calculating ion equivalent ratios. The sources of acidic aerosols were studied with trajectory statistics that showed that continental aerosol is mainly neutralized and marine aerosol acidic.
Journal Article
High Natural Aerosol Loading over Boreal Forests
by
Tunved, P
,
Ström, J
,
Lihavainen, H
in
Aerosols
,
Animal, plant and microbial ecology
,
Anthropogenic factors
2006
Aerosols play a key role in the radiation balance of the atmosphere. Here, we present evidence that the European boreal region is a substantial source of both aerosol mass and aerosol number. The investigation supplies a straightforward relation between emissions of monoterpenes and gas-to-particle formation over regions substantially lacking in anthropogenic aerosol sources. Our results show that the forest provides an aerosol population of 1000 to 2000 particles of climatically active sizes per cubic centimeter during the late spring to early fall period. This has important implications for radiation budget estimates and relevancy for the evaluation of feedback loops believed to determine our future climate.
Journal Article
Sesquiterpenes and oxygenated sesquiterpenes dominate the VOC (C 5 –C 20 ) emissions of downy birches
by
Praplan, Arnaud P.
,
Schallhart, Simon
,
Hakola, Hannele
in
Acetates
,
Acetic acid
,
Air pollution
2021
Biogenic volatile organic compounds (BVOCs) emitted by the forests are known to have strong impacts in the atmosphere. However, lots of missing reactivity is found, especially in the forest air. Therefore better characterization of sources and identification/quantification of unknown reactive compounds is needed. While isoprene and monoterpene (MT) emissions of boreal needle trees have been studied quite intensively, there is much less knowledge on the emissions of boreal deciduous trees and emissions of larger terpenes and oxygenated volatile organic compounds (OVOCs). Here we quantified the downy birch (Betula pubescens) leaf emissions of terpenes, oxygenated terpenes and green leaf volatiles (GLVs) at the SMEAR II boreal forest site using in situ gas chromatographs with mass spectrometers. Sesquiterpenes (SQTs) and oxygenated sesquiterpenes (OSQTs) were the main emitted compounds. Mean emission rates of SQTs and OSQTs were significantly higher in the early growing season (510 and 650 ng gdw-1 h−1, respectively) compared to in the main (40 and 130 ng gdw-1 h−1, respectively) and late (14 and 46 ng gdw-1 h−1, respectively) periods, indicating that early leaf growth is a strong source of these compounds. The emissions had a very clear diurnal variation with afternoon maxima being on average 4 to 8 times higher than seasonal means for SQTs and OSQTs, respectively. β-Caryophyllene and β-farnesene were the main SQTs emitted. The main emitted OSQTs were tentatively identified as 14-hydroxy-β-caryophyllene acetate (M=262 g mol−1) and 6-hydroxy-β-caryophyllene (M=220 g mol−1). Over the whole growing season, the total MT emissions were only 24 % and 17 % of the total SQT and OSQT emissions, respectively. A stressed tree growing in a pot was also studied, and high emissions of α-farnesene and an unidentified SQT were detected together with high emissions of GLVs. Due to the relatively low volatility and the high reactivity of SQTs and OSQTs, downy birch emissions are expected to have strong impacts on atmospheric chemistry, especially on secondary organic aerosol (SOA) production.
Journal Article
Long-term sub-micrometer aerosol chemical composition in the boreal forest: inter- and intra-annual variability
by
Keskinen, Helmi
,
Ehn, Mikael
,
Petäjä, Tuukka
in
Aerosol concentrations
,
Aerosol particles
,
Aerosols
2020
The Station for Measuring Ecosystem–Atmosphere Relations (SMEAR) II is well known among atmospheric scientists due to the immense amount of observational data it provides of the Earth–atmosphere interface. Moreover, SMEAR II plays an important role for the large European research infrastructure, enabling the large scientific community to tackle climate- and air-pollution-related questions, utilizing the high-quality long-term data sets recorded at the site. So far, this well-documented site was missing the description of the seasonal variation in aerosol chemical composition, which helps understanding the complex biogeochemical and physical processes governing the forest ecosystem. Here, we report the sub-micrometer aerosol chemical composition and its variability, employing data measured between 2012 and 2018 using an Aerosol Chemical Speciation Monitor (ACSM). We observed a bimodal seasonal trend in the sub-micrometer aerosol concentration culminating in February (2.7, 1.6, and 5.1 µg m−3 for the median, 25th, and 75th percentiles, respectively) and July (4.2, 2.2, and 5.7 µg m−3 for the median, 25th, and 75th percentiles, respectively). The wintertime maximum was linked to an enhanced presence of inorganic aerosol species (ca. 50 %), whereas the summertime maximum (ca. 80 % organics) was linked to biogenic secondary organic aerosol (SOA) formation. During the exceptionally hot months of July of 2014 and 2018, the organic aerosol concentrations were up to 70 % higher than the 7-year July mean. The projected increase in heat wave frequency over Finland will most likely influence the loading and chemical composition of aerosol particles in the future. Our findings suggest strong influence of meteorological conditions such as radiation, ambient temperature, and wind speed and direction on aerosol chemical composition. To our understanding, this is the longest time series reported describing the aerosol chemical composition measured online in the boreal region, but the continuous monitoring will also be maintained in the future.
Journal Article
Global analysis of continental boundary layer new particle formation based on long-term measurements
by
10092390 - Beukes, Johan Paul
,
Laakso, Lauri
,
Petäjä, Tuukka
in
Aerosols
,
Anthropogenic factors
,
Atmosphere
2018
Atmospheric new particle formation (NPF) is an important phenomenon in terms of global particle number concentrations. Here we investigated the frequency of NPF, formation rates of 10 nm particles, and growth rates in the size range of 10–25 nm using at least 1 year of aerosol number size-distribution observations at 36 different locations around the world. The majority of these measurement sites are in the Northern Hemisphere. We found that the NPF frequency has a strong seasonal variability. At the measurement sites analyzed in this study, NPF occurs most frequently in March–May (on about 30% of the days) and least frequently in December–February (about 10% of the days). The median formation rate of 10 nm particles varies by about 3 orders of magnitude (0.01–10 cm3 s1) and the growth rate by about an order of magnitude (1–10 nm h1). The smallest values of both formation and growth rates were observed at polar sites and the largest ones in urban environments or anthropogenically influenced rural sites. The correlation between the NPF event frequency and the particle formation and growth rate was at best moderate among the different measurement sites, as well as among the sites belonging to a certain environmental regime. For a better understanding of atmospheric NPF and its regional importance, we would need more observational data from different urban areas in practically all parts of the world, from additional remote and rural locations in North America, Asia, and most of the Southern Hemisphere (especially Australia), from polar areas, and from at least a few locations over the oceans
Journal Article
Opposing roles of microRNA Argonautes during Caenorhabditis elegans aging
by
Pasquinelli, Amy E.
,
Chipman, Laura B.
,
Aalto, Antti P.
in
Aging
,
Aging (Biology)
,
ALG-2 protein
2018
Argonaute (AGO) proteins partner with microRNAs (miRNAs) to target specific genes for post-transcriptional regulation. During larval development in Caenorhabditis elegans, Argonaute-Like Gene 1 (ALG-1) is the primary mediator of the miRNA pathway, while the related ALG-2 protein is largely dispensable. Here we show that in adult C. elegans these AGOs are differentially expressed and, surprisingly, work in opposition to each other; alg-1 promotes longevity, whereas alg-2 restricts lifespan. Transcriptional profiling of adult animals revealed that distinct miRNAs and largely non-overlapping sets of protein-coding genes are misregulated in alg-1 and alg-2 mutants. Interestingly, many of the differentially expressed genes are downstream targets of the Insulin/ IGF-1 Signaling (IIS) pathway, which controls lifespan by regulating the activity of the DAF-16/ FOXO transcription factor. Consistent with this observation, we show that daf-16 is required for the extended lifespan of alg-2 mutants. Furthermore, the long lifespan of daf-2 insulin receptor mutants, which depends on daf-16, is strongly reduced in animals lacking alg-1 activity. This work establishes an important role for AGO-mediated gene regulation in aging C. elegans and illustrates that the activity of homologous genes can switch from complementary to antagonistic, depending on the life stage.
Journal Article
Measurement of the nucleation of atmospheric aerosol particles
by
Lehtinen, Kari E J
,
Petäjä, Tuukka
,
Dal Maso, Miikka
in
639/638/11
,
704/172/169/824
,
Aerosols
2012
The formation of new atmospheric aerosol particles and their subsequent growth have been observed frequently at various locations all over the world. The atmospheric nucleation rate (or formation rate) and growth rate (GR) are key parameters to characterize the phenomenon. Recent progress in measurement techniques enables us to measure atmospheric nucleation at the size (mobility diameter) of 1.5 (±0.4) nm. The detection limit has decreased from 3 to 1 nm within the past 10 years. In this protocol, we describe the procedures for identifying new-particle-formation (NPF) events, and for determining the nucleation, formation and growth rates during such events under atmospheric conditions. We describe the present instrumentation, best practices and other tools used to investigate atmospheric nucleation and NPF at a certain mobility diameter (1.5, 2.0 or 3.0 nm). The key instruments comprise devices capable of measuring the number concentration of the formed nanoparticles and their size, such as a suite of modern condensation particle counters (CPCs) and air ion spectrometers, and devices for characterizing the pre-existing particle number concentration distribution, such as a differential mobility particle sizer (DMPS). We also discuss the reliability of the methods used and requirements for proper measurements and data analysis. The time scale for realizing this procedure is 1 year.
Journal Article
New foliage growth is a significant, unaccounted source for volatiles in boreal evergreen forests
by
Schiestl-Aalto, P.
,
Bäck, J.
,
Kolari, P.
in
Buds
,
Emission measurements
,
Emissions (Pollution)
2014
Estimates of volatile organic compound (VOC) emissions from forests are based on the assumption that foliage has a steady emission potential over its lifetime, and that emissions are mainly modified by short-term variations in light and temperature. However, in many field studies this has been challenged, and high emissions and atmospheric concentrations have been measured during periods of low biological activity, such as in springtime. We conducted measurements during three years, using an online gas-exchange monitoring system to observe volatile organic emissions from a mature (1 year-old) and a growing Scots pine shoot. The emission rates of organic vapors from vegetative buds of Scots pine during the dehardening and rapid shoot growth stages were one to two orders of magnitude higher than those from mature foliage; this difference decreased and finally disappeared when the new shoot was maturing in late summer. On average, the springtime monoterpene emission rate of the bud was about 500 times higher than that of the mature needles; during the most intensive needle elongation period, the monoterpene emission rate of the growing needles was 3.5 higher than that of the mature needles, and in September the monoterpene emission rate of the same years' needles was even lower (50%) than that of the previous years' needles. For other measured compounds (methanol, acetone and methylbutenol) the values were of the same order of magnitude, except before bud break in spring, when the emission rates of buds for those compounds were on average about 20–30 times higher than that of mature needles. During spring and early summer the buds and growing shoots are a strong source of several VOCs, and if they are not accounted for in emission modeling a significant proportion of the emissions – from a few percent to even half of the annual cumulative emissions – will remain concealed. The diurnal emission pattern of growing shoots differed from the diurnal cycle in temperature as well as from the diurnal emission pattern of mature shoots, which may be related to processes involved in shoot or needle elongation. Our findings imply that global estimations of monoterpene emission rates from forests are in need of revision, and that the physiological state of the plants should be taken into account when emissions of the reactive gases such as monoterpenes are estimated.
Journal Article
Aerosol optical properties at SORPES in Nanjing, east China
2018
Aerosol optical properties (AOPs) and supporting parameters – particle number size distributions, PM2.5 mass concentrations, and the concentrations of trace gases (NOx and NOy) – were measured at SORPES, a regional background station in Nanjing, China from June 2013 to May 2015. The aerosol was highly scattering: the average scattering coefficient was σsp=403 ± 314 Mm−1, the absorption coefficient σap=26 ± 19 Mm−1, and the single-scattering albedo SSA = 0.93 ± 0.03 for green light. The SSA in Nanjing appears to be slightly higher than published values from several other sites in China and elsewhere. The average Ångström exponent of absorption (AAE) for the wavelength range 370–950 nm was 1.04 and the AAE range was 0.7–1.4. These AAE values can be explained with different amounts of non-absorbing coating on pure black carbon (BC) cores and different core sizes rather than contribution by brown carbon. The AOPs had typical seasonal cycles with high σsp and σap in winter and low ones in summer: the averages were σsp=544 ± 422 and σap=36 ± 24 Mm−1 in winter and σsp=342 ± 281 and σap=20 ± 13 Mm−1 in summer. The intensive AOPs had no clear seasonal cycles, the variations in them were rather related to the evolution of pollution episodes. The diurnal cycles of the intensive AOPs were clear and in agreement with the cycle of the particle number size distribution. The diurnal cycle of SSA was similar to that of the air photochemical age, suggesting that the darkest aerosol originated from fresh traffic emissions. A Lagrangian retroplume analysis showed that the potential source areas of high σsp and σap are mainly in eastern China. Synoptic weather phenomena dominated the cycle of AOPs on a temporal scale of 3–7 days. During pollution episodes, modeled boundary layer height decreased, whereas PM2.5 concentrations and σsp and σap typically increased gradually and remained high during several days but decreased faster, sometimes by even more than an order of magnitude within some hours. During the growth phase of the pollution episodes the intensive AOPs evolved clearly. The mass scattering efficiency MSE of PM2.5 grew during the extended pollution episodes from ∼ 4 to ∼ 6 m2 g−1 and the mass fraction of BCe decreased from ∼ 10 to ∼ 3 % during the growth phase of the episodes. Particle growth resulted in the backscatter fraction decreasing from more than 0.16 to less than 0.10, SSA growing from less than 0.9 to more than 0.95, and radiative forcing efficiency (RFE) changing from less than −26 W m−2 to more than −24 W m−2, which means that the magnitude of RFE decreased. The RFE probability distribution at SORPES was clearly narrower than at a clean background site which is in agreement with a published RFE climatology.
Journal Article
Aerosol size distribution and new particle formation in the western Yangtze River Delta of China: 2 years of measurements at the SORPES station
2015
Aerosol particles play important roles in regional air quality and global climate change. In this study, we analyzed 2 years (2011–2013) of measurements of submicron particles (6–800 nm) at a suburban site in the western Yangtze River Delta (YRD) of eastern China. The number concentrations (NCs) of particles in the nucleation, Aitken and accumulation modes were 5300 ± 5500, 8000 ± 4400, 5800 ± 3200 cm−3, respectively. The NCs of total particles are comparable to those at urban/suburban sites in other Chinese megacities, such as Beijing, but about 10 times higher than in the remote western China. Long-range and regional transport largely influenced number concentrations and size distributions of submicron particles. The highest and lowest accumulation-mode particle number concentrations were observed in air masses from the YRD and coastal regions, respectively. Continental air masses from inland brought the highest concentrations of nucleation-mode particles. New particle formation (NPF) events, apparent in 44 % of the effective measurement days, occurred frequently in all the seasons except winter. The frequency of NPF in spring, summer and autumn is much higher than other measurement sites in China. Sulfuric acid was found to be the main driver of NPF events. The particle formation rate was the highest in spring (3.6 ± 2.4 cm−3 s−1), whereas the particle growth rate had the highest values in summer (12.8 ± 4.4 nm h−1). The formation rate was typically high in relatively clean air masses, whereas the growth rate tended to be high in the polluted YRD air masses. The frequency of NPF events and the particle growth rates showed a strong year-to-year difference. In the summer of 2013, associated with a multi-week heat wave and strong photochemical processes, NPF events occurred with larger frequency and higher growth rates compared with the same period in 2012. The difference in the location and strength of the subtropical high pressure system, which influences the air mass transport pathways and solar radiation, seems to be the cause for year-to-year differences. This study reports, up to now, the longest continuous measurement records of submicron particles in eastern China and helps to achieve a comprehensive understanding of the main factors controlling the seasonal and year-to-year variation of the aerosol size distribution and NPF in this region.
Journal Article