Technical University of Berlin

About: Technical University of Berlin is a education organization based out in Berlin, Germany. It is known for research contribution in the topics: Laser & Catalysis. The organization has 27292 authors who have published 59342 publications receiving 1414623 citations. The organization is also known as: Technische Universität Berlin & TU Berlin.

Machine learning of accurate energy-conserving molecular force fields

Abstract: Using conservation of energy-a fundamental property of closed classical and quantum mechanical systems-we develop an efficient gradient-domain machine learning (GDML) approach to construct accurate molecular force fields using a restricted number of samples from ab initio molecular dynamics (AIMD) trajectories. The GDML implementation is able to reproduce global potential energy surfaces of intermediate-sized molecules with an accuracy of 0.3 kcal mol-1 for energies and 1 kcal mol-1 A-1 for atomic forces using only 1000 conformational geometries for training. We demonstrate this accuracy for AIMD trajectories of molecules, including benzene, toluene, naphthalene, ethanol, uracil, and aspirin. The challenge of constructing conservative force fields is accomplished in our work by learning in a Hilbert space of vector-valued functions that obey the law of energy conservation. The GDML approach enables quantitative molecular dynamics simulations for molecules at a fraction of cost of explicit AIMD calculations, thereby allowing the construction of efficient force fields with the accuracy and transferability of high-level ab initio methods.

Where water is oxidized to dioxygen: structure of the photosynthetic Mn4Ca cluster.

Abstract: The oxidation of water to dioxygen is catalyzed within photosystem II (PSII) by a Mn4Ca cluster, the structure of which remains elusive. Polarized extended x-ray absorption fine structure (EXAFS) measurements on PSII single crystals constrain the Mn4Ca cluster geometry to a set of three similar high-resolution structures. Combining polarized EXAFS and x-ray diffraction data, the cluster was placed within PSII, taking into account the overall trend of the electron density of the metal site and the putative ligands. The structure of the cluster from the present study is unlike either the 3.0 or 3.5 angstrom–resolution x-ray structures or other previously proposed models.

Electrocatalytic Oxygen Evolution Reaction in Acidic Environments – Reaction Mechanisms and Catalysts

Abstract: The low efficiency of the electrocatalytic oxidation of water to O2 (oxygen evolution reaction-OER) is considered as one of the major roadblocks for the storage of electricity from renewable sources in form of molecular fuels like H2 or hydrocarbons Especially in acidic environments, compatible with the powerful proton exchange membrane (PEM), an earth-abundant OER catalyst that combines high activity and high stability is still unknown Current PEM-compatible OER catalysts still rely mostly on Ir and/or Ru as active components, which are both very scarce elements of the platinum group Hence, the Ir and/or Ru amount in OER catalysts has to be strictly minimized Unfortunately, the OER mechanism, which is the most powerful tool for OER catalyst optimization, still remains unclear In this review, we first summarize the current state of our understanding of the OER mechanism on PEM-compatible heterogeneous electrocatalysts, before we compare and contrast that to the OER mechanism on homogenous catalysts Thereafter, an overview over monometallic OER catalysts is provided to obtain insights into structure-function relations followed by a review of current material optimization concepts and support materials Moreover, missing links required to complete the mechanistic picture as well as the most promising material optimization concepts are pointed out

The singlet and triplet states of phenyl cation. A hybrid approach for locating minimum energy crossing points between non-interacting potential energy surfaces

Abstract: The phenyl cation is known to have two low-energy minima, corresponding to 1 A 1 and 3 B 1 states, the first of which is more stable by ca. 25 kcal/mol. The minimum energy crossing point between these two surfaces, located at various levels including a hybrid method first described here, lies just above the minimum of the triplet, 0.12 kcal/mol at the CCSD(T)/cc-pVDZ//B3LYP/SV level, and there is significant spin-orbit coupling between the surfaces at this point. On the basis of these results, the lifetime of the triplet is expected to be very short.

Experiments on drag-reducing surfaces and their optimization with an adjustable geometry

Abstract: Previous research has established that surfaces with tiny ribs (riblets) aligned in the streamwise direction can reduce the turbulent wall-shear stress below that of a smooth surface. Typical skin-friction reductions have been found to be about 5%. The results of the present investigation, however, demonstrate a considerable improvement over this value. This improvement is achieved by a systematic experimental optimization which has been guided by theoretical concepts.A key feature of our experiments is the utilization of an oil channel. Previous experiments in wind tunnels had to contend with very small riblet dimensions which typically had a lateral rib spacing of about 0.5 mm or less. By contrast, in our oil channel, the ribs can have a lateral spacing of between about 2 and 10 mm. This increased size of the surface structures enables test surfaces to be manufactured with conventional mechanical methods, and it also enables us to build test surfaces with adjustable geometry. In addition, the Berlin oil channel has a novel shear stress balance with an unprecedented accuracy of ±0.3%. This latter feature is a prerequisite for a systematic experimental optimization.In the present investigation, surfaces with longitudinal ribs and additional slits are studied. The experiments cover a fairly large range of parameters so that the drag reduction potential of a surface with ribs and/or slits is worked out conclusively. A large parameter range is made possible because of the adjustability of the surfaces as well as the automatic operation of the oil channel. In particular, the following tests were run:(i) Shear stress measurements with conventional riblet configurations, i.e. with triangular and semi-circular grooves, have been carried out. These measurements were necessary in order to establish the connection between our oil channel data and previous data from wind tunnels. As was previously established, we found a drag reduction of about 5%.(ii) An adjustable surface with longitudinal blade ribs and with slits was built and tested. Both groove depth and slit width could be varied separately and continuously during the experiment. It turned out, that slits in the surface did not contribute to the drag reduction. Nevertheless, these investigations show how perforated surfaces (e.g. for boundary-layer control) can be designed for minimal parasitic drag. On the other hand, with closed slits, an optimal groove depth for the rib surface could be determined, i.e. half of the lateral rib spacing. For this configuration, we found an 8.7% skin-friction reduction. By carefully eliminating deleterious effects (caused by little gaps, etc.), the skin-friction reduction could be improved to a record value of 9.9%.(iii) A quantitative comparison between theory and experiment was carried out. The theory is based on the assumption that riblets impede the fluctuating turbulent crossflow near the wall. In this way, momentum transfer and shear stress are reduced. The simplified theoretical model proposed by Luchini (1992) is supported by the present experiments.(iv) For technological applications of riblets, e.g. on long-range commercial aircraft, the above thin-blade ribs are not practical. Therefore, we have devised a surface that combines a significantly improved performance (8.2 %) with a geometry which exhibits better durability and enables previously developed manufacturing methods for plastic riblet film production to be used. Our riblet geometry exhibits trapezoidal grooves with wedge-like ribs. The flat floor of the trapezoidal grooves permits an undistorted visibility through the transparent riblet film which is essential for crack inspection on aircraft.