Fitzsimmonsrandall9689

Electronic resonances commonly decay via internal conversion to vibrationally hot anions and subsequent statistical electron emission. We observed vibrational structure in such an emission from the nitrobenzene anion, in both the 2D electron energy loss and 2D photoelectron spectroscopy of the neutral and anion, respectively. The emission peaks could be correlated with calculated nonadiabatic coupling elements for vibrational modes to the electronic continuum from a nonvalence dipole-bound state. This autodetachment mechanism via a dipole-bound state is likely to be a common feature in both electron and photoelectron spectroscopies.Understanding the nonequilibrium dynamics of photoexcited polarons at the atomic scale is of great importance for improving the performance of photocatalytic and solar-energy materials. Using a pulsed-laser-combined scanning tunneling microscopy and spectroscopy, here we succeeded in resolving the relaxation dynamics of single polarons bound to oxygen vacancies on the surface of a prototypical photocatalyst, rutile TiO_2(110). The visible-light excitation of the defect-derived polarons depletes the polaron states and leads to delocalized free electrons in the conduction band, which is further corroborated by ab initio calculations. We found that the trapping time of polarons becomes considerably shorter when the polaron is bound to two surface oxygen vacancies than that to one. In contrast, the lifetime of photogenerated free electrons is insensitive to the atomic-scale distribution of the defects but correlated with the averaged defect density within a nanometer-sized area. Those results shed new light on the photocatalytically active sites at the metal-oxide surface.In small volumes, sample dimensions are known to strongly influence mechanical behavior especially strength and crystal plasticity. Caspase inhibitor This correlation fades away at the so-called "mesoscale," loosely defined at several micrometers in both experiments and simulations. However, this picture depends on the "entanglement" of the initial defect configuration. In this Letter, we study the effect of dislocation topology through the use of a novel observable for dislocation ensembles (the Λ invariant) that depends only on mutual dislocation linking It is built on the natural vortex character of dislocations, and it has a continuum-discrete correspondence that may assist multiscale modeling descriptions. We investigate arbitrarily complex initial dislocation microstructures in sub-micron-sized pillars using three-dimensional discrete dislocation dynamics simulations for finite volumes. We demonstrate how to engineer nanoscale dislocation ensembles that are independent from sample dimensions, either by biased-random dislocation loop deposition or by sequential mechanical loads of compression and torsion.The nontrivial geometry encoded in the quantum mechanical wave function has important consequences for both noninteracting and interacting systems. Yet, our understanding of the relationship between geometrical effects in noninteracting systems and their interacting counterparts is far from complete. Here, we demonstrate how the single-particle Berry curvature associated with the normal phase in two dimensions modifies the fluxoid quantization of a Bardeen-Cooper-Schrieffer superconductor. A discussion of the experimental scenarios where this anomalous quantization is expected is provided. Our work demonstrates the importance of variational Ansätze in making a clear connection between the Berry phases of single-particle and many-body wave functions.We apply a multiscale modeling approach to study lattice reconstruction in marginally twisted bilayers of transition metal dichalcogenides (TMD). For this, we develop density functional theory parametrized interpolation formulae for interlayer adhesion energies of MoSe_2, WSe_2, MoS_2, and WS_2, combine those with elasticity theory, and analyze the bilayer lattice relaxation into mesoscale domain structures. Paying particular attention to the inversion asymmetry of TMD monolayers, we show that 3R and 2H stacking domains, separated by a network of dislocations develop for twist angles θ^∘ less then θ_P^∘∼2.5° and θ^∘ less then θ_AP^∘∼1° for, respectively, bilayers with parallel (P) and antiparallel (AP) orientation of the monolayer unit cells and suggest how the domain structures would manifest itself in local probe scanning of marginally twisted P and AP bilayers.Network flows often exhibit a hierarchical treelike structure that can be attributed to the minimization of dissipation. The common feature of such systems is a single source and multiple sinks (or vice versa). In contrast, here we study networks with only a single source and sink. These systems can arise from secondary purposes of the networks, such as blood sugar regulation through insulin production. Minimization of dissipation in these systems leads to vascular shunting, a single vessel connecting the inlet and outlet. We show instead how optimizing the transport time yields network topologies that match those observed in the insulin-producing pancreatic islets. These are patterns of periphery-to-center and center-to-periphery flows. The obtained flow networks are broadly independent of how the flow velocity depends on the flow flux, but continuous and discontinuous phase transitions appear at extreme flux dependencies. Lastly, we show how constraints on flows can lead to buckling of the branches of the network, a feature that is also observed in pancreatic islets.The compaction behavior of deformable grain assemblies beyond jamming remains bewildering, and existing models that seek to find the relationship between the confining pressure P and solid fraction ϕ end up settling for empirical strategies or fitting parameters. Using a coupled discrete-finite element method, we analyze assemblies of highly deformable frictional grains under compression. We show that the solid fraction evolves nonlinearly from the jamming point and asymptotically tends to unity. Based on the micromechanical definition of the granular stress tensor, we develop a theoretical model, free from ad hoc parameters, correctly mapping the evolution of ϕ with P. Our approach unveils the fundamental features of the compaction process arising from the joint evolution of grain connectivity and the behavior of single representative grains. This theoretical framework also allows us to deduce a bulk modulus equation showing an excellent agreement with our numerical data.