Systematic Perturbation Theory for Dynamical Coarse-Graining

We demonstrate how the dynamical coarse-graining approach can be systematically extended to higher orders in the coupling between system and reservoir. Up to second order in the coupling constant we explicitly show that dynamical coarse-graining unconditionally preserves positivity of the density matrix -- even for bath density matrices that are not in equilibrium and also for time-dependent system Hamiltonians. By construction, the approach correctly captures the short-time dynamics, i.e., it is suitable to analyze non-Markovian effects. We compare the dynamics with the exact solution for highly non-Markovian systems and find a remarkable quality of the coarse-graining approach. The extension to higher orders is straightforward but rather tedious. The approach is especially useful for bath correlation functions of simple structure and for small system dimensions.Comment: 17 pages, 5 figures, version accepted for publication in PR

Weak coupling approximations in non-Markovian Transport

We study the transport properties of the Fano-Anderson model with a Lorentzian-shaped density of states in one of the electronic reservoirs. We explicitly show that the energy dependence of the density of states can cause non-Markovian effects and that the non-Markovian master equation may fail if these effects are strong. We evaluate the stationary current, the zero frequency current noise and the occupation dynamics of the resonant level by means of a quantum master equation approach within different approximation schemes and compare the results to the exact solution obtained by scattering theory and Green's functions.Comment: 9 pages, 6 figures; due to suggestions of a referee we have added an appendix where our kernel is derived in detail; a few typos are correcte

Multifunctional Polyoxometalate Platforms for Supramolecular Light-Driven Hydrogen Evolution

Multifunctional supramolecular systems are a central research topic in light-driven solar energy conversion. Here, we report a polyoxometalate (POM)-based supramolecular dyad, where two platinum-complex hydrogen evolution catalysts are covalently anchored to an Anderson polyoxomolybdate anion. Supramolecular electrostatic coupling of the system to an iridium photosensitizer enables visible light-driven hydrogen evolution. Combined theory and experiment demonstrate the multifunctionality of the POM, which acts as photosensitizer/catalyst-binding-site[1] and facilitates light-induced charge-transfer and catalytic turnover. Chemical modification of the Pt-catalyst site leads to increased hydrogen evolution reactivity. Mechanistic studies shed light on the role of the individual components and provide a molecular understanding of the interactions which govern stability and reactivity. The system could serve as a blueprint for multifunctional polyoxometalates in energy conversion and storage

NOS2-deficient mice with hypoxic necrotizing lung lesions predict outcomes of tuberculosis chemotherapy in humans

10.1038/s41598-017-09177-2Scientific Reports71885

Influence of cloud processing on CCN activation behaviour in the Thuringian Forest, Germany during HCCT-2010

Within the framework of the "Hill Cap Cloud Thuringia 2010" (HCCT-2010) international cloud experiment, the influence of cloud processing on the activation properties of ambient aerosol particles was investigated. Particles were probed upwind and downwind of an orographic cap cloud on Mt Schmücke, which is part of a large mountain ridge in Thuringia, Germany. The activation properties of the particles were investigated by means of size-segregated cloud condensation nuclei (CCN) measurements at 3 to 4 different supersaturations. The observed CCN spectra together with the total particle spectra were used to calculate the hygroscopicity parameter κ for the upwind and downwind stations. The upwind and downwind critical diameters and κ values were then compared for defined cloud events (FCE) and non-cloud events (NCE). Cloud processing was found to increase the hygroscopicity of the aerosol particles significantly, with an average increase in κ of 50%. Mass spectrometry analysis and isotopic analysis of the particles suggest that the observed increase in the hygroscopicity of the cloud-processed particles is due to an enrichment of sulfate and possibly also nitrate in the particle phase

Advocating For Science: Amici Curiae Brief Of Wetland And Water Scientists In Support Of The Clean Water Rule

The Trump administration has proposed replacing the Clean Water Rule, a 2015 regulation that defined the statutory term waters of the United States to clarify the geographic jurisdiction of the Clean Water Act. Since its promulgation, the Clean Water Rule has been subjected to numerous judicial challenges. We submitted an amici curiae brief to the United States Court of Appeals for the Sixth Circuit, explaining why the Clean Water Rule, and its definition of waters of the United States, is scientifically sound. The definition of waters of the United States is a legal determination informed by science. The best available science supports the Clean Water Rule\u27s categorical treatment of tributaries because compelling scientific evidence demonstrates that tributaries significantly affect the chemical, physical, and biological integrity of traditional navigable waters (primary waters). Similarly, the best available science supports the Clean Water Rule\u27s categorical treatment of adjacent waters based on geographic proximity. Compelling scientific evidence demonstrates that waters within 100ft of an ordinary high water mark (OHWM) significantly affect the chemical, physical, and biological integrity of primary waters, as do waters within 100-year floodplains and waters within 1500ft of high tide lines of tidally influenced primary waters or OHWMs of the Great Lakes. This review article is adapted from that amici brief