scholarly journals Final report: Studies of surface adsorbate electronic structure and femtochemistry at the fundamental length and time scales

2020 ◽  
Author(s):  
Hrvoje Petek ◽  
Keyword(s):  
Electronic Structure ◽  
Time Scales ◽  
Final Report ◽  
Fundamental Length

scholarly journals Uncertainty quantification for quantum chemical models of complex reaction networks

2016 ◽  
Vol 195 ◽  
pp. 497-520 ◽  
Author(s):  
Jonny Proppe ◽  
Tamara Husch ◽  
Gregor N. Simm ◽  
Markus Reiher
Keyword(s):  
Free Energy ◽  
Electronic Structure ◽  
State Space ◽  
Time Scales ◽  
Reaction Network ◽  
Reaction Networks ◽  
Multiple Time Scales ◽  
Complex Reaction ◽  
Discrete State ◽  
Continuous State

For the quantitative understanding of complex chemical reaction mechanisms, it is, in general, necessary to accurately determine the corresponding free energy surface and to solve the resulting continuous-time reaction rate equations for a continuous state space. For a general (complex) reaction network, it is computationally hard to fulfill these two requirements. However, it is possible to approximately address these challenges in a physically consistent way. On the one hand, it may be sufficient to consider approximate free energies if a reliable uncertainty measure can be provided. On the other hand, a highly resolved time evolution may not be necessary to still determine quantitative fluxes in a reaction network if one is interested in specific time scales. In this paper, we present discrete-time kinetic simulations in discrete state space taking free energy uncertainties into account. The method builds upon thermo-chemical data obtained from electronic structure calculations in a condensed-phase model. Our kinetic approach supports the analysis of general reaction networks spanning multiple time scales, which is here demonstrated for the example of the formose reaction. An important application of our approach is the detection of regions in a reaction network which require further investigation, given the uncertainties introduced by both approximate electronic structure methods and kinetic models. Such cases can then be studied in greater detail with more sophisticated first-principles calculations and kinetic simulations.

scholarly journals Postglacial Fire Frequency and its Relation to Long-Term Vegetational and Climatic Changes in Yellowstone Park

1994 ◽  
Vol 18 ◽  
pp. 160-165
Author(s):  
Cathy Whitlock
Keyword(s):  
Carbon Dioxide ◽  
Time Scales ◽  
Lake Sediment ◽  
Sediment Cores ◽  
Fire Frequency ◽  
Response Surfaces ◽  
Potential Range ◽  
Final Report ◽  
History Of

The paleoecologic record provides unique insights into the response of communities to environmental perturbations of different duration and intensity. Climate is a primary agent of environmental change and its long-term effect on the vegetation of the Yellowstone/Grand Teton region is revealed in a network of pollen records. Fire frequency is controlled by climate, and as climate changes so too does the importance of fire in shaping spatial patterns of vegetation. The prehistoric record of Yellowstone's Northern Range, for example, shows the response of vegetation to the absence of major fires in the last 150 years (Whitlock et al., 1991; Engstrom et al., 1991, 1994). In longer records spanning the last 14,000 years, periods of frequent fire are suggested by sediments containing high percentages of fire-adapted trees, including lodgepole pine and Douglas-fir, and high amounts of charcoal (Whitlock, 1993; Whitlock and Bartlein, 1993; Whitlock et al., 1995; Millspaugh and Whitlock, 1995). The primary research objective has been to study the vegetational history of the Yellowstone region and examine the sensitivity of vegetation to changes in climate and fire frequency on different time scales. This information is necessary to understand better the relative effects of climate, natural disturbance, and human perturbation in the present and future. Fossil pollen and plant macrofossils from dated-lake sediment cores provide information on past vegetation and climate. The frequency of charcoal particles and other fire indicators in dated lake-sediment cores offer evidence of past fires. Studies of future climate and vegetation in the Yellowstone region were based on climate simulations produced by general circulation models that incorporate a doubling of carbon dioxide and an equilibrium model to project potential range displacement of selected tree taxa. Relations between present distributions of tree taxa and climate were established by the use of response surfaces. The study has been divided into three parts: (1) an investigation of the vegetation history of Yellowstone National Park (YNP), (2) an analysis of charcoal accumulation in lakes following the 1988 fires and a reconstruction of fire history in central YNP on long time scales, and (3) a study of the potential ranges of tree taxa in the future with global increases in atmospheric carbon dioxide. A final report to the UW-NPS Research Center describes the methodology and findings in detail (Whitlock et al., 1994).

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