Shedding light on the increased carbon uptake by a boreal forest under diffuse solar radiation across multiple scales.

Solar radiation is scattered by cloud cover, aerosols and other particles in the atmosphere, all of which are affected by global changes. Furthermore, the diffuse fraction of solar radiation is increased by more frequent forest fires and likewise would be if climate interventions such as stratospheric aerosol injection were adopted. Forest ecosystem studies predict that an increase in diffuse radiation would result in higher productivity, but ecophysiological data are required to identify the processes responsible within the forest canopy. In our study, the response of a boreal forest to direct, diffuse and heterogeneous solar radiation conditions was examined during the daytime in the growing season to determine how carbon uptake is affected by radiation conditions at different scales. A 10-year data set of ecosystem, shoot and forest floor vegetation carbon and water-flux data was examined. Ecosystem-level carbon assimilation was higher under diffuse radiation conditions in comparison with direct radiation conditions at equivalent total photosynthetically active radiation (PAR). This was driven by both an increase in shoot and forest floor vegetation photosynthetic rate. Most notably, ecosystem-scale productivity was strongly related to the absolute amount of diffuse PAR, since it integrates both changes in total PAR and diffuse fraction. This finding provides a gateway to explore the processes by which absolute diffuse PAR enhances productivity, and the long-term persistence of this effect under scenarios of higher global diffuse radiation.

Drought effects on volatile organic compound emissions from Scots pine stems.

Tree stems have been identified as sources of volatile organic compounds (VOCs) that play important roles in tree defence and atmospheric chemistry. Yet, we lack understanding on the magnitude and environmental drivers of stem VOC emissions in various forest ecosystems. Due to the increasing importance of extreme drought, we studied drought effects on the VOC emissions from mature Scots pine (Pinus sylvestris L.) stems. We measured monoterpenes, acetone, acetaldehyde and methanol emissions with custom-made stem chambers, online PTR-MS and adsorbent sampling in a drought-prone forest over the hot-dry summer of 2018 and compared the emission rates and dynamics between trees in naturally dry conditions and under long-term irrigation (drought release). The pine stems were significant monoterpene sources. The stem monoterpene emissions potentially originated from resin, based on their similar monoterpene spectra. The emission dynamics of all VOCs followed temperature at a daily scale, but monoterpene and acetaldehyde emission rates decreased nonlinearly with drought over the summer. Despite the dry conditions, large peaks of monoterpene, acetaldehyde and acetone emissions occurred in late summer potentially due to abiotic or biotic stressors. Our results highlight the potential importance of stem emissions in the ecosystem VOC budget, encouraging further studies in diverse environments.

A modelling study of OH, NO3 and H2SO4 in 2007-2018 at SMEAR II, Finland: analysis of long-term trends.

Major atmospheric oxidants (OH, O3 and NO3) dominate the atmospheric oxidation capacity, while H2SO4 is considered as a main driver for new particle formation. Although numerous studies have investigated the long-term trend of ozone in Europe, the trends of OH, NO3 and H2SO4 at specific sites are to a large extent unknown. The one-dimensional model SOSAA has been applied in several studies at the SMEAR II station and has been validated by measurements in several projects. Here, we applied the SOSAA model for the years 2007-2018 to simulate the atmospheric chemical components, especially the atmospheric oxidants OH and NO3, as well as H2SO4 at SMEAR II. The simulations were evaluated with observations from several shorter and longer campaigns at SMEAR II. Our results show that daily OH increased by 2.39% per year and NO3 decreased by 3.41% per year, with different trends of these oxidants during day and night. On the contrary, daytime sulfuric acid concentrations decreased by 2.78% per year, which correlated with the observed decreasing concentration of newly formed particles in the size range of 3-25 nm with 1.4% per year at SMEAR II during the years 1997-2012. Additionally, we compared our simulated OH, NO3 and H2SO4 concentrations with proxies, which are commonly applied in case a limited number of parameters are measured and no detailed model simulations are available.

Propagating ice front induces gas bursts and ultrasonic acoustic emissions from freezing xylem.

Ice formation and propagation in the xylem of plants is a complex process. During freezing of xylem sap, gases dissolved in liquid sap are forced out of the ice lattice due to their low solubility in ice, and supersaturation of xylem sap as well as low water potential (Ñ°) are induced at the ice-liquid interface. Supersaturation of gases near the ice front may lead to bubble formation and potentially to cavitation and/or to burst of gases driven out from the branch. In this study, we investigated the origin and dynamics of freezing-related gas bursts and ultrasonic acoustic emissions (AEs), which are suggested to indicate cavitation. Picea abies (L.) H. Karst. and Salix caprea L. branch segments were exposed to frost cycles in a temperature test chamber, and CO2 efflux (indicating gas bursts) and AEs were recorded. On freezing, two-thirds of the observed gas bursts originated from the xylem and only one-third from the bark. Simultaneously with gas bursts, AEs were detected. Branch Ñ° affected both gas bursts and AEs, with high gas burst in saturated and dry samples but relevant AEs only in the latter. Repeated frost cycles led to decreasing gas burst volumes and AE activity. Experiments revealed that the expanding ice front in freezing xylem was responsible for observed gas bursts and AEs, and that branch Ñ° influenced both processes. Results also indicated that gas bursts and cavitation are independently induced by ice formation, though both may be relevant for bubble dynamics during freezing.

Do all chlorophyll fluorescence emission wavelengths capture the spring recovery of photosynthesis in boreal evergreen foliage?

Chlorophyll a fluorescence (ChlF) is closely related to photosynthesis and can be measured remotely using multiple spectral features as solar-induced fluorescence (SIF). In boreal regions, SIF shows particular promise as an indicator of photosynthesis, in part because of the limited variation of seasonal light absorption in these ecosystems. Seasonal spectral changes in ChlF could yield new information on processes such as sustained nonphotochemical quenching (NPQS ) but also disrupt the relationship between SIF and photosynthesis. We followed ChlF and functional and biochemical properties of Pinus sylvestris needles during the photosynthetic spring recovery period to answer the following: (a) How ChlF spectra change over seasonal timescales? (b) How pigments, NPQS , and total photosynthetically active radiation (PAR) absorption drive changes of ChlF spectra? (c) Do all ChlF wavelengths track photosynthetic seasonality? We found seasonal ChlF variation in the red and far-red wavelengths, which was strongly correlated with NPQS , carotenoid content, and photosynthesis (enhanced in the red), but not with PAR absorption. Furthermore, a rapid decrease in red/far-red ChlF ratio occurred in response to a cold spell, potentially relating to the structural reorganization of the photosystems. We conclude that all current SIF retrieval features can track seasonal photosynthetic dynamics in boreal evergreens, but the full SIF spectra provides additional insight.

Interannual and Seasonal Dynamics of Volatile Organic Compound Fluxes From the Boreal Forest Floor.

In the northern hemisphere, boreal forests are a major source of biogenic volatile organic compounds (BVOCs), which drive atmospheric processes and lead to cloud formation and changes in the Earth's radiation budget. Although forest vegetation is known to be a significant source of BVOCs, the role of soil and the forest floor, and especially interannual variations in fluxes, remains largely unknown due to a lack of long-term measurements. Our aim was to determine the interannual, seasonal and diurnal dynamics of boreal forest floor volatile organic compound (VOC) fluxes and to estimate how much they contribute to ecosystem VOC fluxes. We present here an 8-year data set of forest floor VOC fluxes, measured with three automated chambers connected to the quadrupole proton transfer reaction mass spectrometer (quadrupole PTR-MS). The exceptionally long data set shows that forest floor fluxes were dominated by monoterpenes and methanol, with relatively comparable emission rates between the years. Weekly mean monoterpene fluxes from the forest floor were highest in spring and in autumn (maximum 59 and 86 µg m-2 h-1, respectively), whereas the oxygenated VOC fluxes such as methanol had highest weekly mean fluxes in spring and summer (maximum 24 and 79 µg m-2 h-1, respectively). Although the chamber locations differed from each other in emission rates, the inter-annual dynamics were very similar and systematic. Accounting for this chamber location dependent variability, temperature and relative humidity, a mixed effects linear model was able to explain 79-88% of monoterpene, methanol, acetone, and acetaldehyde fluxes from the boreal forest floor. The boreal forest floor was a significant contributor in the forest stand fluxes, but its importance varies between seasons, being most important in autumn. The forest floor emitted 2-93% of monoterpene fluxes in spring and autumn and 1-72% of methanol fluxes in spring and early summer. The forest floor covered only a few percent of the forest stand fluxes in summer.

Influences of light and humidity on carbonyl sulfide-based estimates of photosynthesis.

Understanding climate controls on gross primary productivity (GPP) is crucial for accurate projections of the future land carbon cycle. Major uncertainties exist due to the challenge in separating GPP and respiration from observations of the carbon dioxide (CO2) flux. Carbonyl sulfide (COS) has a dominant vegetative sink, and plant COS uptake is used to infer GPP through the leaf relative uptake (LRU) ratio of COS to CO2 fluxes. However, little is known about variations of LRU under changing environmental conditions and in different phenological stages. We present COS and CO2 fluxes and LRU of Scots pine branches measured in a boreal forest in Finland during the spring recovery and summer. We find that the diurnal dynamics of COS uptake is mainly controlled by stomatal conductance, but the leaf internal conductance could significantly limit the COS uptake during the daytime and early in the season. LRU varies with light due to the differential light responses of COS and CO2 uptake, and with vapor pressure deficit (VPD) in the peak growing season, indicating a humidity-induced stomatal control. Our COS-based GPP estimates show that it is essential to incorporate the variability of LRU with environmental variables for accurate estimation of GPP on ecosystem, regional, and global scales.

Newtonian boreal forest ecology: The Scots pine ecosystem as an example.

Isaac Newton's approach to developing theories in his book Principia Mathematica proceeds in four steps. First, he defines various concepts, second, he formulates axioms utilising the concepts, third, he mathematically analyses the behaviour of the system defined by the concepts and axioms obtaining predictions and fourth, he tests the predictions with measurements. In this study, we formulated our theory of boreal forest ecosystems, called NewtonForest, following the four steps introduced by Newton. The forest ecosystem is a complicated entity and hence we needed altogether 27 concepts to describe the material and energy flows in the metabolism of trees, ground vegetation and microbes in the soil, and to describe the regularities in tree structure. Thirtyfour axioms described the most important features in the behaviour of the forest ecosystem. We utilised numerical simulations in the analysis of the behaviour of the system resulting in clear predictions that could be tested with field data. We collected retrospective time series of diameters and heights for test material from 6 stands in southern Finland and five stands in Estonia. The numerical simulations succeeded to predict the measured diameters and heights, providing clear corroboration with our theory.

Solar eclipse demonstrating the importance of photochemistry in new particle formation.

Solar eclipses provide unique possibilities to investigate atmospheric processes, such as new particle formation (NPF), important to the global aerosol load and radiative balance. The temporary absence of solar radiation gives particular insight into different oxidation and clustering processes leading to NPF. This is crucial because our mechanistic understanding on how NPF is related to photochemistry is still rather limited. During a partial solar eclipse over Finland in 2015, we found that this phenomenon had prominent effects on atmospheric on-going NPF. During the eclipse, the sources of aerosol precursor gases, such as sulphuric acid and nitrogen- containing highly oxidised organic compounds, decreased considerably, which was followed by a reduced formation of small clusters and nanoparticles and thus termination of NPF. After the eclipse, aerosol precursor molecule concentrations recovered and re-initiated NPF. Our results provide direct evidence on the key role of the photochemical production of sulphuric acid and highly oxidized organic compounds in maintaining atmospheric NPF. Our results also explain the rare occurrence of this phenomenon under dark conditions, as well as its seemingly weak connection with atmospheric ions.

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.

Molecular composition of boreal forest aerosol from Hyytiälä, Finland, using ultrahigh resolution mass spectrometry.

Organic compounds are important constituents of fine particulate matter (PM) in the troposphere. In this study, we applied direct infusion nanoelectrospray (nanoESI) ultrahigh resolution mass spectrometry (UHR-MS) and liquid chromatography LC/ESI-UHR-MS for the analysis of the organic fraction of PM1 aerosol samples collected over a two week period at a boreal forest site (Hyytiälä), southern Finland. Elemental formulas (460-730 in total) were identified with nanoESI-UHR-MS in the negative ionization mode and attributed to organic compounds with a molecular weight below 400. Kendrick Mass Defect and Van Krevelen approaches were used to identify compound classes and mass distributions of the detected species. The molecular composition of the aerosols strongly varied between samples with different air mass histories. An increased number of nitrogen, sulfur, and highly oxygenated organic compounds was observed during the days associated with continental air masses. However, the samples with Atlantic air mass history were marked by a presence of homologous series of unsaturated and saturated C12-C20 fatty acids suggesting their marine origin. To our knowledge, we show for the first time that the highly detailed chemical composition obtained from UHR-MS analyses can be clearly linked to meteorological parameters and trace gases concentrations that are relevant to atmospheric oxidation processes. The additional LC/ESI-UHR-MS analysis revealed 29 species, which were mainly attributed to oxidation products of biogenic volatile compounds BVOCs (i.e., α,ß-pinene, Δ3-carene, limonene, and isoprene) supporting the results from the direct infusion analysis.

Direct observations of atmospheric aerosol nucleation.

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.