Jaana Bäck

Direct Observations of Atmospheric Aerosol Nucleation

Aerosol Formation Most atmospheric aerosol particles result from a growth process that begins with atmospheric molecules and clusters, progressing to larger and larger sizes as they acquire other molecules, clusters, and particles. The initial steps of this process involve very small entities—with diameters of less than 2 nanometers—which have been difficult to observe. Kulmala et al. (p. 943; see the Perspective by Andreae) developed a sensitive observational protocol that allows these tiny seeds to be detected and counted, and they mapped out the process of aerosol formation in detail. Detailed aerosol measurements provide a consistent framework for the formation of particles from atmospheric gases. [Also see Perspective by Andreae] Atmospheric nucleation is the dominant source of aerosol particles in the global atmosphere and an important player in aerosol climatic effects. The key steps of this process occur in the sub–2-nanometer (nm) size range, in which direct size-segregated observations have not been possible until very recently. Here, we present detailed observations of atmospheric nanoparticles and clusters down to 1-nm mobility diameter. We identified three separate size regimes below 2-nm diameter that build up a physically, chemically, and dynamically consistent framework on atmospheric nucleation—more specifically, aerosol formation via neutral pathways. Our findings emphasize the important role of organic compounds in atmospheric aerosol formation, subsequent aerosol growth, radiative forcing and associated feedbacks between biogenic emissions, clouds, and climate.

PRI assessment of long-term changes in carotenoids/chlorophyll ratio and short-term changes in de-epoxidation state of the xanthophyll cycle.

The Photochemical Reflectance Index (PRI), an index based on leaf reflectance at 531 nm, has been found suitable for tracking variations in photosynthetic activity from leaf to ecosystem levels. This suitability has been attributed to PRI correlation with xanthophyll interconversion and photosynthetic radiation-use efficiency. However, other pigments and factors may be involved in such relationships. We studied the relationship between PRI and xanthophylls and other carotenoids in saplings of two widely distributed evergreen species (Scots pine and Holm oak) submitted to experimentally changing light conditions in a field experiment. PRI was strongly correlated with the de-epoxidation state of xanthophylls (DEPS, an expression of the relative concentration of the three xanthophyll cycle pigments), but also with carotenoids/chlorophyll ratio and β-carotene/chlorophyll ratio in both species. However, following momentary decreases in light due to clouds, PRI changed following the DEPS changes, while the carotenoids/chlorophyll ratio remained constant. The results show that PRI was able to reveal short-term changes in de-epoxidation state, i.e. the signal of xanthophyll interconversion, but it also tracked long-term changes in carotenoids/chlorophyll. Carotenoids other than xanthophylls, e.g. β-carotene, are also related to photoprotective processes, thus also making PRI effective as a measure of changes in photosynthetic light-use efficiency in response to stress on a long-term level.

Climate Feedbacks Linking the Increasing Atmospheric CO2 Concentration, BVOC Emissions, Aerosols and Clouds in Forest Ecosystems

Biogenic volatile organic compounds (BVOCs) play a central role in atmospheric chemistry via their high reactivity in the gas phase and via their participation in atmospheric new particle formation and secondary organic aerosol formation. The emissions of BVOC to the atmosphere depend on several climate-related variables, making these compounds part of complex, yet potentially very important, climate feedback mechanisms. Here we illustrated the role of BVOCs in enhancing gross primary production (GPP) and cloud droplet number concentrations. The first of these phenomena forms a positive feedback loop for the terrestrial carbon sink (GPP feedback), whereas the second one forms a negative feedback loop for the ambient temperature increase (temperature feedback).

Enhanced Volatile Organic Compounds emissions and organic aerosol mass increase the oligomer content of atmospheric aerosols

Secondary organic aerosol (SOA) accounts for a dominant fraction of the submicron atmospheric particle mass, but knowledge of the formation, composition and climate effects of SOA is incomplete and limits our understanding of overall aerosol effects in the atmosphere. Organic oligomers were discovered as dominant components in SOA over a decade ago in laboratory experiments and have since been proposed to play a dominant role in many aerosol processes. However, it remains unclear whether oligomers are relevant under ambient atmospheric conditions because they are often not clearly observed in field samples. Here we resolve this long-standing discrepancy by showing that elevated SOA mass is one of the key drivers of oligomer formation in the ambient atmosphere and laboratory experiments. We show for the first time that a specific organic compound class in aerosols, oligomers, is strongly correlated with cloud condensation nuclei (CCN) activities of SOA particles. These findings might have important implications for future climate scenarios where increased temperatures cause higher biogenic volatile organic compound (VOC) emissions, which in turn lead to higher SOA mass formation and significant changes in SOA composition. Such processes would need to be considered in climate models for a realistic representation of future aerosol-climate-biosphere feedbacks.

Field and controlled environment measurements show strong seasonal acclimation in photosynthesis and respiration potential in boreal Scots pine

Understanding the seasonality of photosynthesis in boreal evergreen trees and its control by the environment requires separation of the instantaneous and slow responses, as well as the dynamics of light reactions, carbon reactions, and respiration. We determined the seasonality of photosynthetic light response and respiration parameters of Scots pine (Pinus sylvestris L.) in the field in southern Finland and in controlled laboratory conditions. CO2 exchange and chlorophyll fluorescence were measured in the field using a continuously operated automated chamber setup and fluorescence monitoring systems. We also carried out monthly measurements of photosynthetic light, CO2 and temperature responses in standard conditions with a portable IRGA and fluorometer instrument. The field and response measurements indicated strong seasonal variability in the state of the photosynthetic machinery with a deep downregulation during winter. Despite the downregulation, the photosynthetic machinery retained a significant capacity during winter, which was not visible in the field measurements. Light-saturated photosynthesis (Psat) and the initial slope of the photosynthetic light response (α) obtained in standard conditions were up to 20% of their respective summertime values. Respiration also showed seasonal acclimation with peak values of respiration in standard temperature in spring and decline in autumn. Spring recovery of all photosynthetic parameters could be predicted with temperature history. On the other hand, the operating quantum yield of photosystem II and the initial slope of photosynthetic light response stayed almost at the summertime level until late autumn while at the same time Psat decreased following the prevailing temperature. Comparison of photosynthetic parameters with the environmental drivers suggests that light and minimum temperature are also decisive factors in the seasonal acclimation of photosynthesis in boreal evergreen trees.

Dynamics of the energy flow through photosystem II under changing light conditions: a model approach

Several biochemical models of photosynthesis exist that consider the effects of the dynamic adjustment of enzymatic and stomatal processes on carbon assimilation under fluctuating light. However, the rate of electron transport through the light reactions is commonly modelled by means of an empirical equation, parameterised with data obtained at the steady state. A steady-state approach cannot capture the dynamic nature of the adjustment of the light reactions under fluctuating light. Here we present a dynamic model approach for photosystem II that considers the adjustments in the regulative non-photochemical processes. The model is initially derived to account for changes occurring at the seconds-to-minutes time-scale under field conditions, and is parameterised and tested with chlorophyll fluorescence data. Results derived from this model show good agreement with experimentally obtained photochemical and non-photochemical quantum yields, providing evidence for the effect that the dark reactions exert in the adjustment of the energy flows at the light reactions. Finally, we compare the traditional steady-state approach with our dynamic approach and find that the steady-state approach produces an underestimation of the modelled electron transport rate (ETR) under rapidly fluctuating light (1 s or less), whereas it produces overestimations under slower fluctuations of light (5 s or more).

Pinus sylvestris as a missing source of nitrous oxide and methane in boreal forest

Boreal forests comprise 73% of the world’s coniferous forests. Based on forest floor measurements, they have been considered a significant natural sink of methane (CH4) and a natural source of nitrous oxide (N2O), both of which are important greenhouse gases. However, the role of trees, especially conifers, in ecosystem N2O and CH4 exchange is only poorly understood. We show for the first time that mature Scots pine (Pinus sylvestris L.) trees consistently emit N2O and CH4 from both stems and shoots. The shoot fluxes of N2O and CH4 exceeded the stem flux rates by 16 and 41 times, respectively. Moreover, higher stem N2O and CH4 fluxes were observed from wet than from dry areas of the forest. The N2O release from boreal pine forests may thus be underestimated and the uptake of CH4 may be overestimated when ecosystem flux calculations are based solely on forest floor measurements. The contribution of pine trees to the N2O and CH4 exchange of the boreal pine forest seems to increase considerably under high soil water content, thus highlighting the urgent need to include tree-emissions in greenhouse gas emission inventories.

BAECC: A Field Campaign to Elucidate the Impact of Biogenic Aerosols on Clouds and Climate

AbstractDuring Biogenic Aerosols—Effects on Clouds and Climate (BAECC), the U.S. Department of Energy’s Atmospheric Radiation Measurement (ARM) Program deployed the Second ARM Mobile Facility (AMF2) to Hyytiala, Finland, for an 8-month intensive measurement campaign from February to September 2014. The primary research goal is to understand the role of biogenic aerosols in cloud formation. Hyytiala is host to the Station for Measuring Ecosystem–Atmosphere Relations II (SMEAR II), one of the world’s most comprehensive surface in situ observation sites in a boreal forest environment. The station has been measuring atmospheric aerosols, biogenic emissions, and an extensive suite of parameters relevant to atmosphere–biosphere interactions continuously since 1996. Combining vertical profiles from AMF2 with surface-based in situ SMEAR II observations allows the processes at the surface to be directly related to processes occurring throughout the entire tropospheric column. Together with the inclusion of extensi...

Effects of elevated [CO2] and O3 on stomatal and surface wax characteristics in leaves of pubescent birch grown under field conditions

Abstract. The responses of pubescent birch (Betula pubescens Ehrh.) leaves to elevated levels of carbon dioxide and ozone were investigated. The micropropagated birch clones used in this research were divided into coastal (Kempele 64°N °25E) and inland (Ylikiiminki 65° N 26°E) clones according to the provenance of the parent tree. The seedlings were exposed to elevated levels of CO2 and CO2+O3 in open-top chambers over four growing seasons (1993–1996). The leaves used in this investigation were gathered in 1995 and 1996. Leaf characteristics seemed to be dependent on leaf age and weather conditions. Stomatal density was greater in plants grown in open-top chambers relative to unchambered controls. The CO2 and CO2+O3 treatments did not affect the stomatal density of the birches. However, the mean stomatal size of the coastal clone increased significantly (13%) in the CO2 treatment compared with the filtered and ambient controls in 1995. In 1996, the mean stomatal sizes of the inland clones were also significantly higher in the CO2 (10%), CO2+O3 (11%) and non-filtered (12%) treatments compared with the filtered control. The distribution of wax deposits on the abaxial leaf surface increased in the inland clone under elevated levels of CO2. The growth environment affected the development of the epicuticular waxes: non-filtered air, CO2 and CO2+O3 treatments seemed to stimulate the formation of wax deposits compared with the charcoal filtered control in which wax formation was the weakest. The combined effects of elevated CO2 and O3 levels on the stomatal size and epicuticular wax deposits were similar in comparison to the effects of elevated CO2 levels alone.

Precipitation and net ecosystem exchange are the most important drivers of DOC flux in upland boreal catchments

According to recent studies, dissolved organic carbon (DOC) concentrations in rivers throughout the boreal zone are increasing. However, the mechanistic explanation of this phenomenon is not yet well known. We studied how the short and long-term changes in precipitation, soil temperature, soil water content, and net ecosystem exchange (NEE) are reflected to DOC concentrations and runoff DOC fluxes in two small forested upland catchments in Southern Finland. We used continuous eddy covariance measurements above the forest and runoff flow measurements from the catchment areas conducted over a 15 year long time period to study the correlation between NEE, gross photosynthetic production, total ecosystem respiration, litter production, and runoff DOC. In addition, we looked for the most important environmental variables in explaining the interannual changes in runoff DOC by using multiple linear regression. Finally, we studied the temporal connection between runoff DOC concentrations, precipitation, soil water content, and NEE by using wavelet coherence analysis technique. Our results indicate that the DOC concentrations have increased over the last 15 years. The DOC flux was to a large extent determined by the amount of precipitation, but the previous years NEE and litter production had also a small but significant effect on runoff DOC fluxes.