ALBERT

Description: Individual particles that on a mass basis consist dominantly of the components ammonium sulfate, oxygenated organic material, and water are a common class of submicron particles found in today's atmosphere. Here we use (1) the organic-to-sulfate (org:sulf) mass ratio of the overall particle and (2) the oxygen-to-carbon (O:C) elemental ratio of the organic component as input variables in parameterisations that predict the critical relative humidity of several different types of particle phase transitions. Specifically these variables were used to predict the critical relative humidity of liquid-liquid phase separation (SRH), efflorescence (ERH), and deliquescence (DRH). Experiments were conducted by optical microscopy for 11 different oxygenated organic-ammonium sulfate systems covering the range 0.1〈 org:sulf

Description: The hygroscopic phase transitions of ammonium sulfate mixed with isoprene-derived secondary organic material were investigated in aerosol experiments. The organic material was produced by isoprene photo-oxidation at 40% and 60% relative humidity. The low volatility fraction of the photo-oxidation products condensed onto ammonium sulfate particles. The particle-phase organic material had oxygen-to-carbon ratios of 0.67 to 0.74 (±0.2) for mass concentrations of 20 to 30 μg m−3. The deliquescence, efflorescence, and phase miscibility of the mixed particles were investigated using a dual arm tandem differential mobility analyzer. The isoprene photo-oxidation products induced deviations in behavior relative to pure ammonium sulfate. Compared to an efflorescence relative humidity (ERH) of 30 to 35% for pure ammonium sulfate, efflorescence was eliminated for aqueous particles having organic volume fractions ϵ of 0.6 and greater. Compared to a deliquescence relative humidity (DRH) of 80% for pure ammonium sulfate, the DRH steadily decreased with increasing ϵ, approaching a DRH of 40% for ϵ of 0.9. Parameterizations of the DRH(ϵ) and ERH(ϵ) curves were as follows: DRH(ϵ)= ∑i ci,d ϵi valid for 0 ≤ ϵ ≤0.86 and ERH(ϵ)= ∑ i ci,e ϵi valid for 0 ≤ ϵ ≤ 0.55 for the coefficients c0,d= 80.67, c0,e = 28.35, c1,d = −11.45, c1,e = −13.66, c2,d = 0, c2,e = 0, c3,d = 57.99, c3,e = -83.80, c4,d = −106.80, and c4,e = 0. The molecular description that is thermodynamically implied by these strongly sloped DRH(ϵ) and ERH(ϵ) curves is that the organic isoprene photo-oxidation products, the inorganic ammonium sulfate, and water form a miscible liquid phase even at low relative humidity. This phase miscibility is in contrast to the liquid-liquid separation that occurs for some other types of secondary organic material. These differences in liquid-liquid separation are consistent with a prediction recently presented in the literature that the bifurcation between liquid-liquid phase separation versus mixing depends on the oxygen-to-carbon ratio of the organic material. The conclusions are that the influence of secondary organic material on the hygroscopic properties of ammonium sulfate varies with organic composition and that the degree of oxygenation of the organic material, which is a measurable characteristic of complex organic materials, is an important variable influencing the hygroscopic properties of mixed organic-inorganic particles.

Description: Individual particles that on a mass basis consist dominantly of the components ammonium sulfate, organic material, and water are a common class of submicron particles found in today's atmosphere. Here we use (1) the organic-to-sulfate (org:sulf) mass ratio of the overall particle and (2) the oxygen-to-carbon (O:C) elemental ratio of the organic component as input variables in parameterisations that predict the critical relative humidity of several different types of particle phase transitions. These transitions include liquid-liquid phase separation (SRH), efflorescence (ERH), and deliquescence (DRH). Experiments were conducted by optical microscopy for 11 different oxygenated organic-ammonium sulfate systems covering the range 0.1 〈 org:sulf

Description: The hygroscopic phase transitions of ammonium sulfate mixed with isoprene-derived secondary organic material were investigated in aerosol experiments. The organic material was produced by isoprene photo-oxidation at 40% relative humidity. The low volatility fraction of the photo-oxidation products condensed onto ammonium sulfate particles. The particle-phase organic material had oxygen-to-carbon ratios of 0.67 to 0.74 for mass concentrations of 20 to 30 μg m−3. The deliquescence, efflorescence, and phase miscibility of the mixed particles were investigated using a dual arm tandem differential mobility analyzer. The isoprene photo-oxidation products induced deviations in behavior relative to pure ammonium sulfate. Compared to an efflorescence relative humidity (ERH) of 30 to 35% for pure ammonium sulfate, efflorescence was eliminated for mixed aqueous particles having organic volume fractions ε of approximately 0.6 and greater. Compared to a deliquescence relative humidity (DRH) of 80% for pure ammonium sulfate, the DRH steadily decreased for increasing ε, approaching a DRH of 40% for ε of 0.9. Parameterizations of the DRH(ε) and ERH(ε) curves were as follows: DRH(ε)= Σ i ci,d xi valid for 0 ≤ ε ≤ 0.86 and ERH(ε)= Σ i ci,e xi valid for 0 ≤ ε ≤ 0.55 for the coefficients c0,d= 80.67, c0,e = 28.35, c1,d= −11.45, c1,e = −13.66, c2,d = 0, c2,e = 0, c3,d = 57.99, c3,e = −83.80, c4,d = −106.80, and c4,d = 0. The molecular description that is thermodynamically implied by these strongly sloped DRH(ε) and ERH(ε) curves is that the organic isoprene photo-oxidation products, the inorganic ammonium sulfate, and water form a miscible liquid phase even at low relative humidity. This phase miscibility is in contrast to the liquid-liquid separation that occurs for some other types of secondary organic material. These differences in liquid-liquid separation are consistent with a prediction recently presented in the literature that the bifurcation between liquid-liquid phase separation versus mixing depends on the oxygen-to-carbon ratio of the organic material. The conclusions are that the influence of secondary organic material on the hygroscopic properties of ammonium sulfate varies with organic composition and that the degree of oxygenation of the organic material, which is a measurable characteristic of complex organic materials, is an important variable influencing the hygroscopic properties of mixed organic-inorganic particles.

Description: Developed coastal areas often exhibit a strong systemic coupling between shoreline dynamics and economic dynamics. "Beach nourishment", a common erosion-control practice, involves mechanically depositing sediment from outside the local littoral system onto an actively eroding shoreline to alter shoreline morphology. Natural sediment-transport processes quickly rework the newly engineered beach, causing further changes to the shoreline that in turn affect subsequent beach-nourishment decisions. To the limited extent that this landscape/economic coupling has been considered, evidence suggests that towns tend to employ spatially myopic economic strategies under which individual towns make isolated decisions that do not account for their neighbors. What happens when an optimization strategy that explicitly ignores spatial interactions is incorporated into a physical model that is spatially dynamic? The long-term attractor that develops for the coupled system (the state and behavior to which the system evolves over time) is unclear. We link an economic model, in which town-manager agents choose economically optimal beach-nourishment intervals according to past observations of their immediate shoreline, to a simplified coastal-dynamics model that includes alongshore sediment transport and background erosion (e.g. from sea-level rise). Simulations suggest that feedbacks between these human and natural coastal processes can generate emergent behaviors. When alongshore sediment transport and spatially myopic nourishment decisions are coupled, increases in the rate of sea-level rise can destabilize economically optimal nourishment practices into a regime characterized by the emergence of chaotic shoreline evolution.

Description: The feedback between climate and the terrestrial carbon cycle will be a key determinant of the dynamics of the Earth System over the coming decades and centuries. However Earth System Model projections of the terrestrial carbon-balance vary widely over these timescales. This is largely due to differences in their carbon cycle models. A major goal in biogeosciences is therefore to improve understanding of the terrestrial carbon cycle to enable better constrained projections. Essential to achieving this goal will be assessing the empirical support for alternative models of component processes, identifying key uncertainties and inconsistencies, and ultimately identifying the models that are most consistent with empirical evidence. To begin meeting these requirements we data-constrained all parameters of all component processes within a global terrestrial carbon model. Our goals were to assess the climate dependencies obtained for different component processes when all parameters have been inferred from empirical data, assess whether these were consistent with current knowledge and understanding, assess the importance of different data sets and the model structure for inferring those dependencies, assess the predictive accuracy of the model, and to identify a methodology by which alternative component models could be compared within the same framework in future. Although formulated as differential equations describing carbon fluxes through plant and soil pools, the model was fitted assuming the carbon pools were in states of dynamic equilibrium (input rates equal output rates). Thus, the parameterised model is of the equilibrium terrestrial carbon cycle. All but 2 of the 12 component processes to the model were inferred to have strong climate dependencies although it was not possible to data-constrain all parameters indicating some potentially redundant details. Similar climate dependencies were obtained for most processes whether inferred individually from their corresponding data sets or using the full terrestrial carbon model and all available data sets, indicating a strong overall consistency in the information provided by different data sets under the assumed model formulation. A notable exception was plant mortality, in which qualitatively different climate dependencies were inferred depending on the model formulation and data sets used, highlighting this component as the major structural uncertainty in the model. All but two component processes predicted empirical data better than a null model in which no climate dependency was assumed. Equilibrium plant carbon was predicted especially well (explaining around 70% of the variation in the withheld evaluation data). We discuss the advantages of our approach in relation to advancing our understanding of the carbon cycle and enabling Earth System Models make better constrained projections.

Description: A number of nonlinear models have recently been proposed for simulating soil carbon decomposition. Their predictions of soil carbon responses to fresh litter input and warming differ significantly from conventional linear models. Using both stability analysis and numerical simulations, we showed that two of those nonlinear models (a two-pool model and a three-pool model) exhibit damped oscillatory responses to small perturbations. Stability analysis showed the frequency of oscillation is proportional to √ (ϵ −1−1)Ks/Vs in the two-pool model, and to √ (ϵ −1−1)Kl/Vl in the three-pool model, where ϵ is microbial growth efficiency, Ks and Kl are the half saturation constants of soil and litter carbon, respectively, and Vs and Vl are the maximal rates of carbon decomposition per unit of microbial biomass for soil and litter carbon, respectively. For both models, the oscillation has a period between 5 and 15 yr depending on other parameter values, and has smaller amplitude at soil temperatures between 0 °C to 15 °C. In addition, the equilibrium pool sizes of litter or soil carbon are insensitive to carbon inputs in the nonlinear model, but are proportional to carbon input in the conventional linear model. Under warming, the microbial biomass and litter carbon pools simulated by the nonlinear models can increase or decrease, depending whether ϵ varies with temperature. In contrast, the conventional linear models always simulate a decrease in both microbial and litter carbon pools with warming. Based on the evidence available, we concluded that the oscillatory behavior and insensitivity of soil carbon to carbon input in the nonlinear models are unrealistic. We recommend that a better model for capturing the soil carbon dynamics over decadal to centennial timescales would combine the sensitivity of the conventional models to carbon influx with the flexible response to warming of the nonlinear model.

Description: In this study, the diurnal atmospheric grass pollen concentration profile within the Danish city of Aarhus was shown to change in a systematic manner as the season progressed. Although diurnal grass pollen profiles can differ greatly from day-to-day, it is common practice to establish the time of day when peak concentrations are most likely to occur using seasonally-averaged diurnal profiles. Atmospheric pollen loads are highly dependent upon emissions, and different species of grass are known to flower and emit pollen at different times of the day and during different periods of the pollen season. Pollen concentrations are also influenced by meteorological factors – directly through those parameters that govern pollen dispersion and transport, and indirectly through the weather-driven flowering process. We found that three different profiles dominated the grass pollen season in Aarhus – a twin peak profile in the early season, a single evening profile in the mid-season, and a single midday peak in the late season. Whilst this variation could not be explained by meteorological factors, no inconsistencies were found with the theory that the variation was driven by a succession of different grass species with different diurnal flowering patterns dominating atmospheric pollen loads as the season progressed. The potential for exposure was found to be significantly greater during the late season period than during either the early or mid season periods.

Description: Precipitation and temperature drive many aspects of terrestrial ecosystem function. Climate change scenarios predict increasing precipitation variability and temperature, and long term experiments are required to evaluate the ecosystem consequences of interannual climate variation, increased growing season (intra-annual) rainfall variability, and warming. We present results from an experiment applying increased growing season rainfall variability and year round warming in native perennial grassland. During ten years of study, total growing season rainfall varied 2-fold, and we found ~50–200 % interannual variability in plant growth and aboveground net primary productivity, leaf carbon assimilation (ACO2), and soil CO2 efflux (JCO2) despite only ∼40 % variation in mean volumetric soil water content (0–15 cm, Θ15). Interannual variation in soil moisture was thus amplified in most measures of ecosystem response. Differences between years in Θ15 explained the greatest portion (14–52 %) of the variation in these processes. Experimentally increased intra-annual rainfall variability doubled the amplitude of intra-annual soil moisture variation and reduced Θ15 by 15 %, causing most ecosystem processes to decrease 8–40 % in some or all years with increased rainfall variability compared to ambient rainfall timing, suggesting reduced ecosystem rainfall use efficiency. Warming treatments increased 5 cm soil temperature, particularly during spring, fall, and winter. Warming advanced canopy green up in spring, increased winter JCO2, and reduced summer JCO2 and forb ANPP, suggesting that the effects of warming differed in cooler versus warmer parts of the year. We conclude that (1) major ecosystem processes in this grassland may be substantially altered by predicted changes in interannual climate variability, intra-annual rainfall variability, and temperature, (2) interannual climate variation was a larger source of variation in ecosystem function than intra-annual rainfall variability and warming, and (3) effects of increased growing season rainfall variability and warming were small, but ecologically important. The relative effects of these climate drivers are likely to vary for different ecosystem processes and in wetter or drier ecosystems.