A model investigation of vegetation-atmosphere interactions on a millennial timescale

A terrestrial biosphere model with dynamic vegetation capability, Integrated Biosphere Simulator (IBIS2), coupled to the NCAR Community Atmosphere Model (CAM2) is used to investigate the multiple climate-forest equilibrium states of the climate system. A 1000-year control simulation and another 1000-year land cover change simulation that consisted of global deforestation for 100 years followed by re-growth of forests for the subsequent 900 years were performed. After several centuries of interactive climate-vegetation dynamics, the land cover change simulation converged to essentially the same climate state as the control simulation. However, the climate system takes about a millennium to reach the control forest state. In the absence of deep ocean feedbacks in our model, the millennial time scale for converging to the original climate state is dictated by long time scales of the vegetation dynamics in the northern high latitudes. Our idealized modeling study suggests that the equilibrium state reached after complete global deforestation followed by re-growth of forests is unlikely to be distinguishable from the control climate. The real world, however, could have multiple climate-forest states since our modeling study is unlikely to have represented all the essential ecological processes (e. g. altered fire regimes, seed sources and seedling establishment dynamics) for the reestablishment of major biomes.

Quantifying the role of biosphere-atmosphere feedbacks in climate change: coupled model simulation for 6000 years B.P. and comparison with palaeodata for northern Eurasia and northern Africa

The LMD AGCM was iteratively coupled to the global BIOME1 model in order to explore the role of vegetation-climate interactions in response to mid-Holocene (6000 y BP) orbital forcing. The sea-surface temperature and sea-ice distribution used were present-day and CO2 concentration was pre-industrial. The land surface was initially prescribed with present-day vegetation. Initial climate “anomalies” (differences between AGCM results for 6000 y BP and control) were used to drive BIOME1; the simulated vegetation was provided to a further AGCM run, and so on. Results after five iterations were compared to the initial results in order to identify vegetation feedbacks. These were centred on regions showing strong initial responses. The orbitally induced high-latitude summer warming, and the intensification and extension of Northern Hemisphere tropical monsoons, were both amplified by vegetation feedbacks. Vegetation feedbacks were smaller than the initial orbital effects for most regions and seasons, but in West Africa the summer precipitation increase more than doubled in response to changes in vegetation. In the last iteration, global tundra area was reduced by 25% and the southern limit of the Sahara desert was shifted 2.5 °N north (to 18 °N) relative to today. These results were compared with 6000 y BP observational data recording forest-tundra boundary changes in northern Eurasia and savana-desert boundary changes in northern Africa. Although the inclusion of vegetation feedbacks improved the qualitative agreement between the model results and the data, the simulated changes were still insufficient, perhaps due to the lack of ocean-surface feedbacks.

Influence of historic land use change on the biosphere-atmosphere-exchange of C and N trace gases in the humid, subtropical region of Queensland

Increases in atmospheric concentrations of the greenhouse gases (GHGs) carbon dioxide (CO2), methane (CH4), and nitrous oxide (N2O) due to human activities have been linked to climate change. GHG emissions from land use change and agriculture have been identified as significant contributors to both Australia’s and the global GHG budget. This is expected to increase over the coming decades as rates of agriculture intensification and land use change accelerate to support population growth and food production. Limited data exists on CO2, CH4 and N2O trace gas fluxes from subtropical or tropical soils and land uses. To develop effective mitigation strategies a full global warming potential (GWP) accounting methodology is required that includes emissions of the three primary greenhouse gases. Mitigation strategies that focus on one gas only can inadvertently increase emissions of another. For this reason, detailed inventories of GHGs from soils and vegetation under individual land uses are urgently required for subtropical Australia. This study aimed to quantify GHG emissions over two consecutive years from three major land uses; a well-established, unfertilized subtropical grass-legume pasture, a 30 year (lychee) orchard and a remnant subtropical Gallery rainforest, all located near Mooloolah, Queensland. GHG fluxes were measured using a combination of high resolution automated sampling, coarser spatial manual sampling and laboratory incubations. Comparison between the land uses revealed that land use change can have a substantial impact on the GWP on a landscape long after the deforestation event. The conversion of rainforest to agricultural land resulted in as much as a 17 fold increase in GWP, from 251 kg CO2 eq. ha-1 yr-1 in the rainforest to 889 kg CO2 eq. ha-1 yr-1 in the pasture to 2538 kg CO2 eq. ha-1 yr-1 in the lychee plantation. This increase resulted from altered N cycling and a reduction in the aerobic capacity of the soil in the pasture and lychee systems, enhancing denitrification and nitrification events, and reducing atmospheric CH4 uptake in the soil. High infiltration, drainage and subsequent soil aeration under the rainforest limited N2O loss, as well as promoting CH4 uptake of 11.2 g CH4-C ha-1 day-1. This was among the highest reported for rainforest systems, indicating that aerated subtropical rainforests can act as substantial sink of CH4. Interannual climatic variation resulted in significantly higher N2O emission from the pasture during 2008 (5.7 g N2O-N ha day) compared to 2007 (3.9 g N2O-N ha day), despite receiving nearly 500 mm less rainfall. Nitrous oxide emissions from the pasture were highest during the summer months and were highly episodic, related more to the magnitude and distribution of rain events rather than soil moisture alone. Mean N2O emissions from the lychee plantation increased from an average of 4.0 g N2O-N ha-1 day-1, to 19.8 g N2O-N ha-1 day-1 following a split application of N fertilizer (560 kg N ha-1, equivalent to 1 kg N tree-1). The timing of the split application was found to be critical to N2O emissions, with over twice as much lost following an application in spring (emission factor (EF): 1.79%) compared to autumn (EF: 0.91%). This was attributed to the hot and moist climatic conditions and a reduction in plant N uptake during the spring creating conditions conducive to N2O loss. These findings demonstrate that land use change in subtropical Australia can be a significant source of GHGs. Moreover, the study shows that modifying the timing of fertilizer application can be an efficient way of reducing GHG emissions from subtropical horticulture.

Total OH reactivity measurements at the biosphere-atmosphere interface

The biosphere emits copiously volatile organic compounds (VOCs) into the atmosphere, which are removed again depending on the oxidative capacity of the atmosphere and physical processes such as mixing, transport and deposition. Biogenic VOCs react with the primary oxidant of the atmosphere, the hydroxyl radical (OH), and potentially lead to the formation tropospheric ozone and aerosol, which impact regional climate and air quality. The rate of OH decay in the atmosphere, the total OH reactivity is a function of the atmospheric, reactive compound's concentration and reaction velocity with OH. One way to measure the total OH reactivity, the total OH sink, is with the Comparative Reactivity Method - CRM. Basically, the reaction of OH with a reagent (here pyrrole) in clean air and in the presence of atmospheric, reactive molecules is compared. This thesis presents measurements of the total OH reactivity at the biosphere-atmosphere interface to analyze various influences and driving forces. For measurements in natural environment the instrument was automated and a direct, undisturbed sampling method developed. Additionally, an alternative detection system was tested and compared to the originally used detector (Proton Transfer Reaction-Mass Spectrometer, PTR-MS). The GC-PID (Gas Chromatographic Photo-Ionization Detector) was found as a smaller, less expensive, and robust alternative for total OH reactivity measurements. The HUMPPA-COPEC 2010 measurement campaign in the Finish forest was impacted by normal boreal forest emissions as well as prolonged heat and biomass burning emissions. The measurement of total OH reactivity was compared with a comprehensive set of monitored individual species ambient concentration levels. A significant discrepancy between those individually measured OH sinks and the total OH reactivity was observed, which was characterized in detail by the comparison of within and above the forest canopy detected OH reactivity. Direct impact of biogenic emissions on total OH reactivity was examined on Kleiner Feldberg, Germany, 2011. Trans-seasonal measurements of an enclosed Norway spruce branch were conducted via PTR-MS, for individual compound's emission rates, and CRM, for total OH reactivity emission fluxes. Especially during summertime, the individually monitored OH sink terms could not account for the measured total OH reactivity. A controlled oxidation experiment in a low NOx environment was conducted in the EUPHORE reaction chamber (CHEERS, Spain 2011). The concentration levels of the reactant isoprene and its major products were monitored and compared to total OH reactivity measurements as well as to the results of two models. The individually measured compounds could account for the total OH reactivity during this experiment as well as the traditional model-degradation scheme for isoprene (MCM 3.2). Due to previous observations of high OH levels in the isoprene-rich environment of the tropics, a novel isoprene mechanism was recently suggested. In this mechanism (MIME v4) additional OH is generated during isoprene oxidation, which could not be verified in the conditions of the CHEERS experiment.

Ice-atmosphere interactions and sea ice predictability at multiple resolutions in the Community Earth System Model

Thesis (Master's)--University of Washington, 2016-06

Hierarchical structures in Northern Hemispheric extratropical winter ocean-atmosphere interactions

Acknowledgements MW and RVD have been supported by the German Federal Ministry for Education and Research via the BMBF Young Investigators Group CoSy-CC2 (grant 18 Marc Wiedermann et al. no. 01LN1306A). JFD thanks the Stordalen Foundation and BMBF (project GLUES) for financial support. JK acknowledges the IRTG 1740 funded by DFG and FAPESP. Coupled climate network analysis has been performed using the Python package pyunicorn (Donges et al, 2015a) that is available at https://github.com/pik-copan/pyunicorn.

Hierarchical structures in Northern Hemispheric extratropical winter ocean-atmosphere interactions

Acknowledgements MW and RVD have been supported by the German Federal Ministry for Education and Research via the BMBF Young Investigators Group CoSy-CC2 (grant 18 Marc Wiedermann et al. no. 01LN1306A). JFD thanks the Stordalen Foundation and BMBF (project GLUES) for financial support. JK acknowledges the IRTG 1740 funded by DFG and FAPESP. Coupled climate network analysis has been performed using the Python package pyunicorn (Donges et al, 2015a) that is available at https://github.com/pik-copan/pyunicorn.

Bridging the Scale Gap from Leaf to Canopy in Biosphere-Atmosphere Gas and Particle Exchanges

Terrestrial ecosystems, occupying more than 25% of the Earth's surface, can serve as

`biological valves' in regulating the anthropogenic emissions of atmospheric aerosol

particles and greenhouse gases (GHGs) as responses to their surrounding environments.

While the signicance of quantifying the exchange rates of GHGs and atmospheric

aerosol particles between the terrestrial biosphere and the atmosphere is

hardly questioned in many scientic elds, the progress in improving model predictability,

data interpretation or the combination of the two remains impeded by

the lack of precise framework elucidating their dynamic transport processes over a

wide range of spatiotemporal scales. The diculty in developing prognostic modeling

tools to quantify the source or sink strength of these atmospheric substances

can be further magnied by the fact that the climate system is also sensitive to the

feedback from terrestrial ecosystems forming the so-called `feedback cycle'. Hence,

the emergent need is to reduce uncertainties when assessing this complex and dynamic

feedback cycle that is necessary to support the decisions of mitigation and

adaptation policies associated with human activities (e.g., anthropogenic emission

controls and land use managements) under current and future climate regimes.

With the goal to improve the predictions for the biosphere-atmosphere exchange

of biologically active gases and atmospheric aerosol particles, the main focus of this

dissertation is on revising and up-scaling the biotic and abiotic transport processes

from leaf to canopy scales. The validity of previous modeling studies in determining

iv

the exchange rate of gases and particles is evaluated with detailed descriptions of their

limitations. Mechanistic-based modeling approaches along with empirical studies

across dierent scales are employed to rene the mathematical descriptions of surface

conductance responsible for gas and particle exchanges as commonly adopted by all

operational models. Specically, how variation in horizontal leaf area density within

the vegetated medium, leaf size and leaf microroughness impact the aerodynamic attributes

and thereby the ultrane particle collection eciency at the leaf/branch scale

is explored using wind tunnel experiments with interpretations by a porous media

model and a scaling analysis. A multi-layered and size-resolved second-order closure

model combined with particle

uxes and concentration measurements within and

above a forest is used to explore the particle transport processes within the canopy

sub-layer and the partitioning of particle deposition onto canopy medium and forest

oor. For gases, a modeling framework accounting for the leaf-level boundary layer

eects on the stomatal pathway for gas exchange is proposed and combined with sap

ux measurements in a wind tunnel to assess how leaf-level transpiration varies with

increasing wind speed. How exogenous environmental conditions and endogenous

soil-root-stem-leaf hydraulic and eco-physiological properties impact the above- and

below-ground water dynamics in the soil-plant system and shape plant responses

to droughts is assessed by a porous media model that accommodates the transient

water

ow within the plant vascular system and is coupled with the aforementioned

leaf-level gas exchange model and soil-root interaction model. It should be noted

that tackling all aspects of potential issues causing uncertainties in forecasting the

feedback cycle between terrestrial ecosystem and the climate is unrealistic in a single

dissertation but further research questions and opportunities based on the foundation

derived from this dissertation are also brie

y discussed.

Novel Approaches to the Sampling of Atmospheric Aerosols and Determination of Chemical Composition

The Earth s climate is a highly dynamic and complex system in which atmospheric aerosols have been increasingly recognized to play a key role. Aerosol particles affect the climate through a multitude of processes, directly by absorbing and reflecting radiation and indirectly by changing the properties of clouds. Because of the complexity, quantification of the effects of aerosols continues to be a highly uncertain science. Better understanding of the effects of aerosols requires more information on aerosol chemistry. Before the determination of aerosol chemical composition by the various available analytical techniques, aerosol particles must be reliably sampled and prepared. Indeed, sampling is one of the most challenging steps in aerosol studies, since all available sampling techniques harbor drawbacks. In this study, novel methodologies were developed for sampling and determination of the chemical composition of atmospheric aerosols. In the particle-into-liquid sampler (PILS), aerosol particles grow in saturated water vapor with further impaction and dissolution in liquid water. Once in water, the aerosol sample can then be transported and analyzed by various off-line or on-line techniques. In this study, PILS was modified and the sampling procedure was optimized to obtain less altered aerosol samples with good time resolution. A combination of denuders with different coatings was tested to adsorb gas phase compounds before PILS. Mixtures of water with alcohols were introduced to increase the solubility of aerosols. Minimum sampling time required was determined by collecting samples off-line every hour and proceeding with liquid-liquid extraction (LLE) and analysis by gas chromatography-mass spectrometry (GC-MS). The laboriousness of LLE followed by GC-MS analysis next prompted an evaluation of solid-phase extraction (SPE) for the extraction of aldehydes and acids in aerosol samples. These two compound groups are thought to be key for aerosol growth. Octadecylsilica, hydrophilic-lipophilic balance (HLB), and mixed phase anion exchange (MAX) were tested as extraction materials. MAX proved to be efficient for acids, but no tested material offered sufficient adsorption for aldehydes. Thus, PILS samples were extracted only with MAX to guarantee good results for organic acids determined by liquid chromatography-mass spectrometry (HPLC-MS). On-line coupling of SPE with HPLC-MS is relatively easy, and here on-line coupling of PILS with HPLC-MS through the SPE trap produced some interesting data on relevant acids in atmospheric aerosol samples. A completely different approach to aerosol sampling, namely, differential mobility analyzer (DMA)-assisted filter sampling, was employed in this study to provide information about the size dependent chemical composition of aerosols and understanding of the processes driving aerosol growth from nano-size clusters to climatically relevant particles (>40 nm). The DMA was set to sample particles with diameters of 50, 40, and 30 nm and aerosols were collected on teflon or quartz fiber filters. To clarify the gas-phase contribution, zero gas-phase samples were collected by switching off the DMA every other 15 minutes. Gas-phase compounds were adsorbed equally well on both types of filter, and were found to contribute significantly to the total compound mass. Gas-phase adsorption is especially significant during the collection of nanometer-size aerosols and needs always to be taken into account. Other aims of this study were to determine the oxidation products of β-caryophyllene (the major sesquiterpene in boreal forest) in aerosol particles. Since reference compounds are needed for verification of the accuracy of analytical measurements, three oxidation products of β-caryophyllene were synthesized: β-caryophyllene aldehyde, β-nocaryophyllene aldehyde, and β-caryophyllinic acid. All three were identified for the first time in ambient aerosol samples, at relatively high concentrations, and their contribution to the aerosol mass (and probably growth) was concluded to be significant. Methodological and instrumental developments presented in this work enable fuller understanding of the processes behind biogenic aerosol formation and provide new tools for more precise determination of biosphere-atmosphere interactions.

Within-plant isoprene oxidation confirmed by direct emissions of oxidation products methyl vinyl ketone and methacrolein

Isoprene is emitted from many terrestrial plants at high rates, accounting for an estimated 1/3 of annual global volatile organic compound emissions from all anthropogenic and biogenic sources combined. Through rapid photooxidation reactions in the atmosphere, isoprene is converted to a variety of oxidized hydrocarbons, providing higher order reactants for the production of organic nitrates and tropospheric ozone, reducing the availability of oxidants for the breakdown of radiatively active trace gases such as methane, and potentially producing hygroscopic particles that act as effective cloud condensation nuclei. However, the functional basis for plant production of isoprene remains elusive. It has been hypothesized that in the cell isoprene mitigates oxidative damage during the stress-induced accumulation of reactive oxygen species (ROS), but the products of isoprene-ROS reactions in plants have not been detected. Using pyruvate-2-13C leaf and branch feeding and individual branch and whole mesocosm flux studies, we present evidence that isoprene (i) is oxidized to methyl vinyl ketone and methacrolein (iox) in leaves and that iox/i emission ratios increase with temperature, possibly due to an increase in ROS production under high temperature and light stress. In a primary rainforest in Amazonia, we inferred significant in plant isoprene oxidation (despite the strong masking effect of simultaneous atmospheric oxidation), from its influence on the vertical distribution of iox uptake fluxes, which were shifted to low isoprene emitting regions of the canopy. These observations suggest that carbon investment in isoprene production is larger than that inferred from emissions alone and that models of tropospheric chemistry and biotachemistryclimate interactions should incorporate isoprene oxidation within both the biosphere and the atmosphere with potential implications for better understanding both the oxidizing power of the troposphere and forest response to climate change.