37 research outputs found
Probabilistic concepts in intermediate-complexity climate models: A snapshot attractor picture
Abstract
A time series resulting from a single initial condition is shown to be insufficient for quantifying the internal variability in a climate model, and thus one is unable to make meaningful climate projections based on it. The authors argue that the natural distribution, obtained from an ensemble of trajectories differing solely in their initial conditions, of the snapshot attractor corresponding to a particular forcing scenario should be determined in order to quantify internal variability and to characterize any instantaneous state of the system in the future. Furthermore, as a simple measure of internal variability of any particular variable of the model, the authors suggest using its instantaneous ensemble standard deviation. These points are illustrated with the intermediate-complexity climate model Planet Simulator forced by a CO2 scenario, with a 40-member ensemble. In particular, the leveling off of the time dependence of any ensemble average is shown to provide a much clearer indication of reaching a steady state than any property of single time series. Shifts in ensemble averages are indicative of climate changes. The dynamical character of such changes is illustrated by hysteresis-like curves obtained by plotting the ensemble average surface temperature versus the CO2 concentration. The internal variability is found to be the most pronounced on small geographical scales. The traditionally used 30-yr temporal averages are shown to be considerably different from the corresponding ensemble averages. Finally, the North Atlantic Oscillation (NAO) index, related to the teleconnection paradigm, is also investigated. It is found that the NAO time series strongly differs in any individual realization from each other and from the ensemble average, and climatic trends can be extracted only from the latter.</jats:p
Identifizierung der Realstrukturen im System VOHPO<sub>4</sub> x 0.5 H<sub>2</sub>O - (VO)<sub>2</sub>P<sub>2</sub>O<sub>7</sub>
Vanadylpyrophosphate werden seit langer Zeit in der selektiven Partialoxidation von n-Butan zu Maleinsäureanhydrid (MSA) eingesetzt. Entscheidend für die katalytische Aktivität sowie Selektivität gegenüber MSA ist der Syntheseweg des Precursors VOHPO4 x 0.5 H2O sowie des durch Kalzinierung erhaltenen Vanadylpyrophosphates (VO)2P2O7 [1, 2]. Ziel dieser Untersuchungen ist es, einen Beitrag zum fundamentalen Verständnis der Struktur – Wirkungsbeziehung dieser Katalysatoren in der Partialoxidation zu liefern. Hierzu wurde eingehend die Realstruktur, d.h. Defektarten wie Atompositionen und Besetzungszahlen sowie Kristallitmorphologien und Mikrospannungen in der Verbindung (VO)2P2O7 untersucht
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On the importance of the convergence to climate attractors
Ensemble approaches are becoming widely used in climate research. In contrast to weather forecast, however, in the climatic context one is interested in long-time properties, those arising on the scale of several decades. The well-known strong internal variability of the climate system implies the existence of a related dynamical attractor with chaotic properties. Under the condition of climate change this should be a snapshot attractor, naturally arising in an ensemble-based framework. Although ensemble averages can be evaluated at any instant of time, results obtained during the process of convergence of the ensemble towards the attractor are not relevant from the point of view of climate. In simulations, therefore, attention should be paid to whether the convergence to the attractor has taken place. We point out that this convergence is of exponential character, therefore, in a finite amount of time after initialization relevant results can be obtained. The role of the time scale separation due to the presence of the deep ocean is discussed from the point of view of ensemble simulations
Sub-surface Oxygen and Surface Oxide Formation at Ag(111): A Density-functional Theory Investigation
To help provide insight into the remarkable catalytic behavior of the
oxygen/silver system for heterogeneous oxidation reactions, purely sub-surface
oxygen, and structures involving both on-surface and sub-surface oxygen, as
well as oxide-like structures at the Ag(111) surface have been studied for a
wide range of coverages and adsorption sites using density-functional theory.
Adsorption on the surface in fcc sites is energetically favorable for low
coverages, while for higher coverage a thin surface-oxide structure is
energetically favorable. This structure has been proposed to correspond to the
experimentally observed (4x4) phase. With increasing O concentrations, thicker
oxide-like structures resembling compressed Ag2O(111) surfaces are
energetically favored. Due to the relatively low thermal stability of these
structures, and the very low sticking probability of O2 at Ag(111), their
formation and observation may require the use of atomic oxygen (or ozone, O3)
and low temperatures. We also investigate diffusion of O into the sub-surface
region at low coverage (0.11 ML), and the effect of surface Ag vacancies in the
adsorption of atomic oxygen and ozone-like species. The present studies,
together with our earlier investigations of on-surface and
surface-substitutional adsorption, provide a comprehensive picture of the
behavior and chemical nature of the interaction of oxygen and Ag(111), as well
as of the initial stages of oxide formation.Comment: 17 pages including 14 figures, Related publications can be found at
http://www.fhi-berlin.mpg.de/th/paper.htm
Insights into the function of silver as an oxidation catalyst by ab initio, atomistic thermodynamics
To help understand the high activity of silver as an oxidation catalyst,
e.g., for the oxidation of ethylene to epoxide and the dehydrogenation of
methanol to formaldehyde, the interaction and stability of oxygen species at
the Ag(111) surface has been studied for a wide range of coverages. Through
calculation of the free energy, as obtained from density-functional theory and
taking into account the temperature and pressure via the oxygen chemical
potential, we obtain the phase diagram of O/Ag(111). Our results reveal that a
thin surface-oxide structure is most stable for the temperature and pressure
range of ethylene epoxidation and we propose it (and possibly other similar
structures) contains the species actuating the catalysis. For higher
temperatures, low coverages of chemisorbed oxygen are most stable, which could
also play a role in oxidation reactions. For temperatures greater than about
775 K there are no stable oxygen species, except for the possibility of O atoms
adsorbed at under-coordinated surface sites Our calculations rule out thicker
oxide-like structures, as well as bulk dissolved oxygen and molecular
ozone-like species, as playing a role in the oxidation reactions.Comment: 15 pages including 9 figures, Related publications can be found at
http://www.fhi-berlin.mpg.de/th/paper.htm
Investigating ENSO and its teleconnections under climate change in an ensemble view - A new perspective
© 2020 Museum National d'Histoire Naturelle. All rights reserved.The changes in the El Niño-Southern Oscillation (ENSO) phenomenon and its precipitation-related teleconnections over the globe under climate change are investigated in the Community Earth System Model Large Ensemble from 1950 to 2100. For the investigation, a recently developed ensemble-based method, the snapshot empirical orthogonal function (SEOF) analysis, is used. The instantaneous ENSO pattern is defined as the leading mode of the SEOF analysis carried out at a given time instant over the ensemble. The corresponding principal components (PC1s) characterize the ENSO phases. By considering sea surface temperature (SST) regression maps, we find that the largest changes in the typical amplitude of SST fluctuations occur in the June-July-August-September (JJAS) season, in the Niño3-Niño3.4 (5_ N-5_ S, 170-90_W; NOAA Climate Prediction Center) region, and the western part of the Pacific Ocean; however, the increase is also considerable along the Equator in December-January-February (DJF). The Niño3 amplitude also shows an increase of about 20% and 10% in JJAS and DJF, respectively. The strength of the precipitation-related teleconnections of the ENSO is found to be nonstationary, as well. For example, the anticorrelation with precipitation in Australia in JJAS and the positive correlation in central and northern Africa in DJF are predicted to be more pronounced by the end of the 21th century. Half-year-lagged correlations, aiming to predict precipitation conditions from ENSO phases, are also studied. The Australian and Indonesian precipitation and that of the eastern part of Africa in both JJAS and DJF seem to be well predictable based on the ENSO phase, while the southern Indian precipitation relates to the half-year previous ENSO phase only in DJF. The strength of these connections increases, especially from the African region to the Arabian Peninsula11Nsciescopu
Global warming: a result of increasing total solar 2 irradiance?
We address the question of whether an increasing total solar irradiance (TSI) trend, with out anthropogenic contributions, were sufficient to explain global warming
Global warming: a result of increasing total solar 2 irradiance?
We address the question of whether an increasing total solar irradiance (TSI) trend, with out anthropogenic contributions, were sufficient to explain global warming