Anharmonic Decay of Vibrational States in Amorphous Silicon

Anharmonic decay rates are calculated for a realistic atomic model of amorphous silicon. The results show that the vibrational states decay on picosecond timescales and follow the two-mode density of states, similar to crystalline silicon, but somewhat faster. Surprisingly little change occurs for localized states. These results disagree with a recent experiment.Comment: 10 pages, 4 Postscript figure

Numerical study of anharmonic vibrational decay in amorphous and paracrystalline silicon

The anharmonic decay rates of atomic vibrations in amorphous silicon (a-Si) and paracrystalline silicon (p-Si), containing small crystalline grains embedded in a disordered matrix, are calculated using realistic structural models. The models are 1000-atom four-coordinated networks relaxed to a local minimum of the Stillinger-Weber interatomic potential. The vibrational decay rates are calculated numerically by perturbation theory, taking into account cubic anharmonicity as the perturbation. The vibrational lifetimes for a-Si are found to be on picosecond time scales, in agreement with the previous perturbative and classical molecular dynamics calculations on a 216-atom model. The calculated decay rates for p-Si are similar to those of a-Si. No modes in p-Si reside entirely on the crystalline cluster, decoupled from the amorphous matrix. The localized modes with the largest (up to 59%) weight on the cluster decay primarily to two diffusons. The numerical results are discussed in relation to a recent suggestion by van der Voort et al. [Phys. Rev. B {\bf 62}, 8072 (2000)] that long vibrational relaxation inferred experimentally may be due to possible crystalline nanostructures in some types of a-Si.Comment: 9 two-column pages, 13 figure

Science with a lunar low-frequency array: from the dark ages of the Universe to nearby exoplanets

Low-frequency radio astronomy is limited by severe ionospheric distortions below 50 MHz and complete reflection of radio waves below 10-30 MHz. Shielding of man-made interference from long-range radio broadcasts, strong natural radio emission from the Earth's aurora, and the need for setting up a large distributed antenna array make the lunar far side a supreme location for a low-frequency radio array. A number of new scientific drivers for such an array, such as the study of the dark ages and epoch of reionization, exoplanets, and ultra-high energy cosmic rays, have emerged and need to be studied in greater detail. Here we review the scientific potential and requirements of these and other new scientific drivers and discuss the constraints for various lunar surface arrays. In particular we describe observability constraints imposed by the interstellar and interplanetary medium, calculate the achievable resolution, sensitivity, and confusion limit of a dipole array using general scaling laws, and apply them to various scientific questions. Whichever science is deemed most important, pathfinder arrays are needed to test the feasibility of these experiments in the not too distant future. Lunar low-frequency arrays are thus a timely option to consider, offering the potential for significant new insights into a wide range of today's crucial scientific topics. This would open up one of the last unexplored frequency domains in the electromagnetic spectrum.Comment: 36 pages, many figures, accepted for publication by New Astronomy Review

Electrocatalytic CO2 Reduction on CuOx Nanocubes: Tracking the Evolution of Chemical State, Geometric Structure, and Catalytic Selectivity using Operando Spectroscopy

The direct electrochemical conversion of carbon dioxide (CO2) into multi‐carbon (C2+) products still faces fundamental and technological challenges. While facet‐controlled and oxide‐derived Cu materials have been touted as promising catalysts, their stability has remained problematic and poorly understood. Herein we uncover changes in the chemical and morphological state of supported and unsupported Cu2O nanocubes during operation in low‐current H‐Cells and in high‐current gas diffusion electrodes (GDEs) using neutral pH buffer conditions. While unsupported nanocubes achieved a sustained C2+ Faradaic efficiency of around 60 % for 40 h, the dispersion on a carbon support sharply shifted the selectivity pattern towards C1 products. Operando XAS and time‐resolved electron microscopy revealed the degradation of the cubic shape and, in the presence of a carbon support, the formation of small Cu‐seeds during the surprisingly slow reduction of bulk Cu2O. The initially (100)‐rich facet structure has presumably no controlling role on the catalytic selectivity, whereas the oxide‐derived generation of under‐coordinated lattice defects, can support the high C2+ product yields.TU Berlin, Open-Access-Mittel – 2020DFG, 390540038, EXC 2008: Unifying Systems in Catalysis "UniSysCat"BMBF, 033RC004E, CO2Plus - Verbundvorhaben: eEthylen - Nutzung elektrischer Energie aus erneuerbaren Quellen zur elektrochemischen Herstellung von Ethylen aus CO2, Teilvorhaben 5: Charakterisierung und Testung für Synthese-Struktur-WirkungsbeziehungenBMBF, 03SF0523C, Verbundvorhaben CO2EKAT: Elektrokatalysatorsystem für stoffliche Energiespeicherung durch gekoppelte Wasserelektrolyse und CO2-UmwandlungEC/H2020/725915/EU/In situ and Operando Nanocatalysis: Size, Shape and Chemical State Effects/OPERANDOCA

Combined fit to the spectrum and composition data measured by the Pierre Auger Observatory including magnetic horizon effects

The measurements by the Pierre Auger Observatory of the energy spectrum and mass composition of cosmic rays can be interpreted assuming the presence of two extragalactic source populations, one dominating the flux at energies above a few EeV and the other below. To fit the data ignoring magnetic field effects, the high-energy population needs to accelerate a mixture of nuclei with very hard spectra, at odds with the approximate E$^{-2}$ shape expected from diffusive shock acceleration. The presence of turbulent extragalactic magnetic fields in the region between the closest sources and the Earth can significantly modify the observed CR spectrum with respect to that emitted by the sources, reducing the flux of low-rigidity particles that reach the Earth. We here take into account this magnetic horizon effect in the combined fit of the spectrum and shower depth distributions, exploring the possibility that a spectrum for the high-energy population sources with a shape closer to E$^{-2}$ be able to explain the observations