Charge Dependence of Temperature-Driven Phase Transitions of Molecular Nanoclusters: Molecular Dynamics Simulation

Phase transitions (liquid-solid, solid-solid) triggered by temperature changes are studied in free nanosized clusters of TeF_6 (SF_6) with different negative charges assigned to the fluorine atoms. Molecular dynamics simulations at constant energy show that the charge increase from q_F=0.1 e to q_F=0.25 e shifts the melting temperature towards higher values and some of the metastable solid states disappear. The increased repulsive interaction maintains the order in molecular systems at higher temperatures.Comment: 4 pages, 8 figures; presented at the conference on computational physics, Aachen (2001) accepted for publication in Comp.Phys.Com

Exploring the Atmosphere of Neoproterozoic Earth: The Effect of O2_{2} on Haze Formation and Composition

Previous studies of haze formation in the atmosphere of the Early Earth have focused on N$_{2}$/CO$_{2}$/CH$_{4}$ atmospheres. Here, we experimentally investigate the effect of O$_{2}$ on the formation and composition of aerosols to improve our understanding of haze formation on the Neoproterozoic Earth. We obtained in situ size, particle density, and composition measurements of aerosol particles produced from N$_{2}$/CO$_{2}$/CH$_{4}$/O$_{2}$ gas mixtures subjected to FUV radiation (115-400 nm) for a range of initial CO$_{2}$/CH$_{4}$/O$_{2}$ mixing ratios (O$_{2}$ ranging from 2 ppm to 0.2\%). At the lowest O$_{2}$ concentration (2 ppm), the addition increased particle production for all but one gas mixture. At higher oxygen concentrations (20 ppm and greater) particles are still produced, but the addition of O$_{2}$ decreases the production rate. Both the particle size and number density decrease with increasing O$_{2}$, indicating that O$_{2}$ affects particle nucleation and growth. The particle density increases with increasing O$_{2}$. The addition of CO$_{2}$ and O$_{2}$ not only increases the amount of oxygen in the aerosol, but it also increases the degree of nitrogen incorporation. In particular, the addition of O$_{2}$ results in the formation of nitrate bearing molecules. The fact that the presence of oxygen bearing molecules increases the efficiency of nitrogen fixation has implications for the role of haze as a source of molecules required for the origin and evolution of life. The composition changes also likely affect the absorption and scattering behavior of these particles but optical properties measurements are required to fully understand the implications for the effect on the planetary radiative energy balance and climate.Comment: 15 pages, 3 tables, 8 figures, accepted in Astrophysical Journa

Did melting glaciers cause volcanic eruptions in eastern California? Probing the mechanics of dike formation

Peer Reviewedhttp://deepblue.lib.umich.edu/bitstream/2027.42/94661/1/jgrb14086.pd

Coupling between downstream variations of channel width and local pool–riffle bed topography

A potential control of downstream channel width variations on the structure and planform of pool–riffle sequence local bed topography is a key to the dynamics of gravel bed rivers. How established pool–riffle sequences respond to time-varying changes in channel width at specific locations, however, is largely unexplored and challenging to address with field-based study. Here, we report results of a flume experiment aimed at building understanding of how statistically steady pool–riffle sequence profiles adjust to spatially prescribed channel width changes. We find that local bed slopes near steady-state conditions inversely correlate with local downstream width gradients when the upstream sediment supply approximates the estimated transport capacity. This result constrains conditions prior to and following the imposed local width changes. Furthermore, this relationship between local channel bed slope and downstream width gradient is consistent with expectations from scaling theory and a broad set of field-based, numerical, and experimental studies (n=88). However, upstream disruptions to coarse sediment supply through actions such as dam removal can result in a transient flipping of the expected inverse correlation between bed slope and width gradient, collectively highlighting that understanding local conditions is critical before typically implemented spatial averaging schemes can be reliably applied.Postprint (published version

Gully Formation at the Haughton Impact Structure (Arctic Canada) Through the Melting of Snow and Ground Ice, with Implications for Gully Formation on Mars

The formation of gullies on Mars has been the topic of active debate and scientific study since their first discovery by Malin and Edgett in 2000. Several mechanisms have been proposed to account for gully formation on Mars, from dry mass movement processes, release of water or brine from subsurface aquifers, and the melting of near-surface ground ice or snowpacks. In their global documentation of martian gullies, report that gullies are confined to ~2783S and ~2872N latitudes and span all longitudes. Gullies on Mars have been documented on impact crater walls and central uplifts, isolated massifs, and on canyon walls, with crater walls being the most common situation. In order to better understand gully formation on Mars, we have been conducting field studies in the Canadian High Arctic over the past several summers, most recently in summer 2018 and 2019 under the auspices of the Canadian Space Agency-funded Icy Mars Analogue Program. It is notable that the majority of previous studies in the Arctic and Antarctica, including our recent work on Devon Island, have focused on gullies formed on slopes generated by regular endogenic geological processes and in regular bedrock. How-ever, as noted above, meteorite impact craters are the most dominant setting for gullies on Mars. Impact craters provide an environment with diverse lithologies including impact-generated and impact-modified rocks and slope angle, and thus greatly variable hill slope processes could occur within a localized area. Here, we investigate the formation of gullies within the Haughton impact structure and compare them to gullies formed in unimpacted target rock in the nearby Thomas Lee Inle

A New Volcanic Stratospheric Sulfate Aerosol Forcing Emulator (EVA_H): Comparison With Interactive Stratospheric Aerosol Models

Idealized models or emulators of volcanic aerosol forcing have been widely used to reconstruct the spatiotemporal evolution of past volcanic forcing. However, existing models, including the most recently developed Easy Volcanic Aerosol (EVA; Toohey et al., doi: 10.5194/gmd‐2016‐83), (i) do not account for the height of injection of volcanic SO urn:x-wiley:jgrd:media:jgrd55987:jgrd55987-math-0001; (ii) prescribe a vertical structure for the forcing; and (iii) are often calibrated against a single eruption. We present a new idealized model, EVA_H, that addresses these limitations. Compared to EVA, EVA_H makes predictions of the global mean stratospheric aerosol optical depth that are (i) similar for the 1979–1998 period characterized by the large and high‐altitude tropical SO urn:x-wiley:jgrd:media:jgrd55987:jgrd55987-math-0002 injections of El Chichón (1982) and Mount Pinatubo (1991); (ii) significantly improved for the 1998–2015 period characterized by smaller eruptions with a large variety of injection latitudes and heights. Compared to EVA, the sensitivity of volcanic forcing to injection latitude and height in EVA_H is much more consistent with results from climate models that include interactive aerosol chemistry and microphysics, even though EVA_H remains less sensitive to eruption latitude than the latter models. We apply EVA_H to investigate potential biases and uncertainties in EVA‐based volcanic forcing data sets from phase 6 of the Coupled Model Intercomparison Project (CMIP6). EVA and EVA_H forcing reconstructions do not significantly differ for tropical high‐altitude volcanic injections. However, for high‐latitude or low‐altitude injections, our reconstructed forcing is significantly lower. This suggests that volcanic forcing in CMIP6 last millenium experiments may be overestimated for such eruptions

A new volcanic stratospheric sulfate aerosol forcing emulator (EVA_H): Comparison with interactive stratospheric aerosol models.

Idealized models or emulators of volcanic aerosol forcing have been widely used to reconstruct the spatio‐temporal evolution of past volcanic forcing. However, existing models, including the most recently developed Easy Volcanic Aerosol (EVA, Toohey et al. (2016): i) do not account for the height of injection of volcanic SO2; ii) prescribe a vertical structure for the forcing; and iii) are \NEW{often} calibrated against a single eruption. We present a new idealized model, EVA_H, that addresses these limitations. Compared to EVA, EVA_H makes predictions of the global mean stratospheric aerosol optical depth that are: i) similar for the 1979‐1998 period characterized by the large and high‐altitude tropical SO2 injections of El Chichón (1982) and Mt. Pinatubo (1991); ii) significantly improved for the 1998‐2015 period characterized by smaller eruptions with a large variety of injection latitudes and heights. Compared to EVA, the sensitivity of volcanic forcing to injection latitude and height in EVA_H is much more consistent with results from climate models that include interactive aerosol chemistry and microphysics, even though EVA_H remain less sensitive to eruption latitude than the latter models. We apply EVA_H to investigate potential biases and uncertainties in EVA‐based volcanic forcing datasets from phase 6 of the Coupled Model Intercomparison Project (CMIP6). EVA and EVA_H forcing reconstructions do not significantly differ for tropical high‐altitude volcanic injections. However, for high‐latitude or low altitude injections, our reconstructed forcing is significantly lower. This suggests that volcanic forcing in CMIP6 last millenium experiments may be overestimated for such eruptions.Includes NERC

Comparing three short questionnaires to detect psychosocial dysfunction among primary school children: a randomized method

BACKGROUND: Good questionnaires are essential to support the early identification of children with psychosocial dysfunction in community based settings. Our aim was to assess which of three short questionnaires was most suitable for this identification among school-aged children METHODS: A community-based sample of 2,066 parents of children aged 7-12 years (85% of those eligible) filled out the Child Behavior Checklist (CBCL) and - randomly determined - one of three questionnaires to be compared: the Strengths and Difficulties Questionnaire with Impact Supplement (SDQ), the Pediatric Symptom Checklist (PSC) and the PSYBOBA, a Dutch-origin questionnaire. Preventive Child Healthcare professionals assessed children's psychosocial functioning during routine health examinations. We assessed the scale structure (by means of Structural Equation Modelling), validity (correlation coefficients, sensitivity and specificity) and usability (ratings by parents and professionals) of each questionnaire and the degree to which they could improve the identification based only on clinical assessment (logistic regression). RESULTS: For the three questionnaires, Cronbach's alphas varied between 0.80 and 0.89. Sensitivities for a clinical CBCL at a cut off point with specificity = 0.90 varied between 0.78 and 0.86 for the three questionnaires. Areas under the Receiver Operating Curve, using the CBCL as criterion, varied between 0.93 and 0.96. No differences were statistically significant. All three questionnaires added information to the clinical assessment. Odds ratios (95% confidence intervals) for added information were PSC: 29.3 (14.4-59.8), SDQ: 55.0 (23.1-131.2) and PSYBOBA: 68.5 (28.3-165.6). Parents preferred the SDQ and PSYBOBA. Preventive Child Health Care professionals preferred the SDQ. CONCLUSIONS: This randomized comparison of three questionnaires shows that each of the three questionnaires can improve the detection of psychosocial dysfunction among children substantially

Impact of global warming on the rise of volcanic plumes and implications for future volcanic aerosol forcing

©2016. American Geophysical Union. All Rights Reserved. Volcanic eruptions have a significant impact on climate when they inject sulfur gases into the stratosphere. The dynamics of eruption plumes is also affected by climate itself, as atmospheric stratification impacts plumes' height. We use an integral plume model to assess changes in volcanic plume maximum rise heights as a consequence of global warming, with atmospheric conditions from an ensemble of global climate models, using three representative concentration pathways (RCP) scenarios. Predicted changes in atmospheric temperature profiles decrease the heights of tropospheric and lowermost stratospheric volcanic plumes and increase the tropopause height, for the RCP4.5 and RCP8.5 scenarios in the coming three centuries. Consequently, the critical mass eruption rate required to cross the tropopause increases by up to a factor of 3 for tropical regions and up to 2 for high-latitude regions. A number of recent lower stratospheric plumes, mostly in the tropics (e.g., Merapi, 2010), would be expected to not cross the tropopause starting from the late 21st century, under RCP4.5 and RCP8.5 scenarios. This effect could result in a ≃5–25% decrease in the average SO2 flux into the stratosphere carried by small plumes, the frequency of which is larger than the rate of decay of volcanic stratospheric aerosol, and a ≃2–12% decrease of the total flux. Our results suggest the existence of a positive feedback between climate and volcanic aerosol forcing. Such feedback may have minor implications for global warming rate but can prove to be important to understand the long-term evolution of volcanic atmospheric inputs

On the Temperature Dependence of the Lifetime of Thermally Isolated Metastable Clusters

The temperature dependence of the lifetime of the thermally isolated metastable N8 cubane up to its decay into N2 molecules has been calculated by the molecular dynamics method. It has been demonstrated that this dependence significantly deviates from the Arrhenius law. The applicability of the finite heat bath theory to the description of thermally isolated atomic clusters has been proved using statistical analysis of the results obtained.Comment: 14 pages, 4 figure