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X-ray free-electron lasers have, over the past decade, opened up the possibility of understanding the ultrafast response of matter to intense X-ray pulses. In earlier research on atoms and small molecules, new aspects of this response were uncovered, such as rapid sequences of inner-shell photoionization and Auger ionization. Here, we studied a larger molecule, buckminsterfullerene (C-60), exposed to 640 eV X-rays, and examined the role of chemical effects, such as chemical bonds and charge transfer, on the fragmentation following multiple ionization of the molecule. To provide time resolution, we performed femtosecond-resolved X-ray pump/X-ray probe measurements, which were accompanied by advanced simulations. The simulations and experiment reveal that despite substantial ionization induced by the ultrashort (20 fs) X-ray pump pulse, the fragmentation of C-60 is considerably delayed. This work uncovers the persistence of the molecular structure of C-60, which hinders fragmentation over a timescale of hundreds of femtoseconds. Furthermore, we demonstrate that a substantial fraction of the ejected fragments are neutral carbon atoms. These findings provide insights into X-ray free-electron laser-induced radiation damage in large molecules, including biomolecules.
The global warming potential of nitrous oxide (N2O) and its long atmospheric lifetime mean its presence in the atmosphere is of major concern, and that methods are required to measure and reduce emissions. Large spatial and temporal variations means, however, that simple extrapolation of measured data is inappropriate, and that other methods of quantification are required. Although process-based models have been developed to simulate these emissions, they often require a large amount of input data that is not available at a regional scale, making regional and global emission estimates difficult to achieve. The spatial extent of organic soils means that quantification of emissions from these soil types is also required, but will not be achievable using a process-based model that has not been developed to simulate soil water contents above field capacity or organic soils. The ECOSSE model was developed to overcome these limitations, and with a requirement for only input data that is readily available at a regional scale, it can be used to quantify regional emissions and directly inform land-use change decisions. ECOSSE includes the major processes of nitrogen (N) turnover, with material being exchanged between pools of SOM at rates modified by temperature, soil moisture, soil pH and crop cover. Evaluation of its performance at site-scale is presented to demonstrate its ability to adequately simulate soil N contents and N2O emissions from cropland soils in Europe. Mitigation scenarios and sensitivity analyses are also presented to demonstrate how ECOSSE can be used to estimate the impact of future climate and land-use change on N2O emissions.
Metabolic signatures of healthy lifestyle patterns and colorectal cancer risk in a European cohort
(2020)
BACKGROUND & AIMS: Colorectal cancer risk can be lowered by adherence to the World Cancer Research Fund/American Institute for Cancer Research (WCRF/AICR) guidelines. We derived metabolic signatures of adherence to these guidelines and tested their associations with colorectal cancer risk in the European Prospective Investigation into Cancer and Nutrition cohort.
METHODS: Scores reflecting adherence to the WCRF/AICR recommendations (scale, 1-5) were calculated from participant data on weight maintenance, physical activity, diet, and alcohol among a discovery set of 5738 cancer-free European Prospective Investigation into Cancer and Nutrition participants with metabolomics data. Partial least-squares regression was used to derive fatty acid and endogenous metabolite signatures of the WCRF/AICR score in this group. In an independent set of 1608 colorectal cancer cases and matched controls, odds ratios (ORs) and 95% CIs were calculated for colorectal cancer risk per unit increase in WCRF/AICR score and per the corresponding change in metabolic signatures using multivariable conditional logistic regression.
RESULTS: Higher WCRF/AICR scores were characterized by metabolic signatures of increased odd-chain fatty acids, serine, glycine, and specific phosphatidylcholines. Signatures were inversely associated more strongly with colorectal cancer risk (fatty acids: OR, 0.51 per unit increase; 95% CI, 0.29-0.90; endogenous metabolites: OR, 0.62 per unit change; 95% CI, 0.50-0.78) than the WCRF/AICR score (OR, 0.93 per unit change; 95% CI, 0.86-1.00) overall. Signature associations were stronger in male compared with female participants.
CONCLUSIONS: Metabolite profiles reflecting adherence to WCRF/AICR guidelines and additional lifestyle or biological risk factors were associated with colorectal cancer. Measuring a specific panel of metabolites representative of a healthy or unhealthy lifestyle may identify strata of the population at higher risk of colorectal cancer.
To better assess ecosystem C budgets of croplands and understand their potential response to climate and management changes, detailed information on the mechanisms and environmental controls driving the individual C flux components are needed. This accounts in particular for the ecosystem respiration (R-eco) and its components, the autotrophic (R-a) and heterotrophic respiration (R-h) which vary tremendously in time and space. This study presents a method to separate R-eco into R-a [as the sum of R-a (shoot) and R-a (root)] and R-h in order to detect temporal and small-scale spatial dynamics within their relative contribution to overall R-eco. Thus, predominant environmental drivers and underlying mechanisms can be revealed. R-eco was derived during nighttime by automatic chamber CO2 flux measurements on plant covered plots. R-h was derived from CO2 efflux measurements, which were performed in parallel to R-eco measurements on a fallow plot using CO2 sampling tubes in 10 cm soil depth. R-a (root) was calculated as the difference between sampling tube CO2 efflux measurements on a plant covered plot and R-h. R-a (shoot) was calculated as R-eco - R-a (root) - R-h. Measurements were carried out for winter wheat (Triticum aestivum L.) during the crop season 2015 at an experimental plot located in the hummocky ground moraine landscape of NE Germany. R-eco varied seasonally from < 1 to 9.5 g C m(-2) d(-1), and was higher in adult (a) and reproductive (r) than juvenile (j) stands (gC m(-2) d(-1): j = 1.2, a = 4.6, r = 5.3). Observed R-a and R-h were in general smaller compared to the independently measured R-eco, contributing in average 58% and 42% to R-eco. However, both varied strongly regarding their environmental drivers and particular contribution throughout the study period, following the seasonal development of soil temperature and moisture (R-h) as well as crop development (R-a). Thus, our results consistently revealed temporal dynamics regarding the relative contribution of R-a (root) and R-a (shoot) to R-a, as well as of R-a and R-h to R-eco. Based on the observed results, implications for partitioning of R-eco in croplands are given.
Carbon (C) stored in soils represents the largest C pool of terrestrial ecosystems and consequently plays a crucial role in the global C cycle. So far, it is widely unclear to what extent different land uses and land use change influence soil C storage. The hummocky ground moraine landscape of northeastern Germany is characterized by distinct small-scale soil heterogeneity on the one hand, and intensive energy crop cultivation on the other. Both factors are assumed to significantly influence gaseous C exchange; as such, they likely drive soil organic carbon (SOC) stock dynamics in terrestrial agricultural ecosystems. To date, it is not clear to what extent N fertilization forms, which are associated with energy crop cultivation (e.g., application of biogas fermentation residues) and soil type relative to soil erosion state, influence soil C dynamics, nor is it clear whether one of these factors is more important than the other. To investigate the influence of soil erosion state and N fertilization form on soil C dynamics, we present dynamic and seasonal net ecosystem carbon balances (NECB) as a proxy for changes in soil organic carbon stocks. Measurements were conducted for maize (Zea mays L.) at five sites in the "CarboZALF-D" experimental field during the 2011 growing season. Measurement sites represent different soil erosion states (non-eroded Albic Luvisols, extremely eroded Calcaric Regosols and depositional Endogleyic Colluvic Regosols) and N fertilization forms (100% mineral fertilizer, 50% mineral and 50% organic fertilizer, and 100% organic fertilizer). Fertilization treatments were established on the Albic Luvisol. Net ecosystem CO2 exchange (NEE) and ecosystem respiration (R-eco) were measured every four weeks using a dynamic flow-through non-steady-state closed manual chamber system. Gap filling was performed based on empirical temperature and PAR dependency functions and was used to derive daily NEE values. In parallel, daily above-ground biomass production (NPFshoot) was estimated using a logistic growth equation, fitted on periodic biomass samples. Finally, C dynamics were calculated as the balance of daily NEE and NPPshoot based on the initial C input due to organic fertilization. Resulting NECB varied from pronounced soil C losses at the Endogleyic Colluvic Regosol (592 g C m(-2)) to soil C gains at the Calcaric Regosol (-124 g C m(-2)). Minor to modest C losses were observed for the Albic Luvisol. Compared to N fertilization forms, soil erosion states generally had a stronger impact on derived NECB. However, interannual variations in plant phonology and interactions between soil erosion states and fertilization forms might result in different NECB values over multiple years. Hence, long-term measurements of different fertilization treatments on characteristic soil landscape elements are needed.