Transferable atomic multipole machine learning models for small organic molecules

Accurate representation of the molecular electrostatic potential, which is often expanded in distributed multipole moments, is crucial for an efficient evaluation of intermolecular interactions. Here we introduce a machine learning model for multipole coefficients of atom types H, C, O, N, S, F, and Cl in any molecular conformation. The model is trained on quantum chemical results for atoms in varying chemical environments drawn from thousands of organic molecules. Multipoles in systems with neutral, cationic, and anionic molecular charge states are treated with individual models. The models' predictive accuracy and applicability are illustrated by evaluating intermolecular interaction energies of nearly 1,000 dimers and the cohesive energy of the benzene crystal.Comment: 11 pages, 6 figure

Heat transfer characteristics of hypersonic waveriders with an emphasis on the leading edge effects

The heat transfer characteristics in surface radiative equilibrium and the aerodynamic performance of blunted hypersonic waveriders are studied along two constant dynamic pressure trajectories for four different Mach numbers. The inviscid leading edge drag was found to be a small (4 to 8 percent) but not negligible fraction of the inviscid drag of the vehicle. Although the viscous drag at the leading edge can be neglected, the presence of the leading edge will influence the transition pattern of the upper and the lower surfaces and therefore affect the viscous drag of the entire vehicle. For an application similar to the National Aerospace Plane (NASP), the present study demonstrates that the waverider remains a valuable concept at high Mach numbers if a state-of-the-art active cooling device is used along the leading edge. At low Mach number (less than 5), the study shows the surface radiative cooling might be sufficient. In all cases, radiative cooling is sufficient for the upper and lower surfaces of the vehicle if ceramic composites are used as thermal protection

Coarse-grained interaction potentials for polyaromatic hydrocarbons

Using Kohn-Sham density functional theory (KS-DFT), we have studied the interaction between various polyaromatic hydrocarbon molecules. The systems range from mono-cyclic benzene up to hexabenzocoronene (hbc). For several conventional exchange-correlation functionals potential energy curves of interaction of the $\pi$-$\pi$ stacking hbc dimer are reported. It is found that all pure local density or generalized gradient approximated functionals yield qualitatively incorrect predictions regarding structure and interaction. Inclusion of a non-local, atom-centered correction to the KS-Hamiltonian enables quantitative predictions. The computed potential energy surfaces of interaction yield parameters for a coarse-grained potential, which can be employed to study discotic liquid-crystalline mesophases of derived polyaromatic macromolecules

Identification of point defects in HVPE-grown GaN by steady-state and time-resolved photoluminescence

We have investigated point defects in GaN grown by HVPE by using steady-state and time-resolved photoluminescence (PL). Among the most common PL bands in this material are the red luminescence band with a maximum at 1.8 eV and a zero-phonon line (ZPL) at 2.36 eV (attributed to an unknown acceptor having an energy level 1.130 eV above the valence band), the blue luminescence band with a maximum at 2.9 eV (attributed to ZnGa), and the ultraviolet luminescence band with the main peak at 3.27 eV (related to an unknown shallow acceptor). In GaN with the highest quality, the dominant defect-related PL band at high excitation intensity is the green luminescence band with a maximum at about 2.4 eV. We attribute this band to transitions of electrons from the conduction band to the 0/+ level of the isolated CN defect. The yellow luminescence (YL) band, related to transitions via the −/0 level of the same defect, has a maximum at 2.1 eV. Another yellow luminescence band, which has similar shape but peaks at about 2.2 eV, is observed in less pure GaN samples and is attributed to the CNON complex. In semi-insulating GaN, the GL2 band with a maximum at 2.35 eV (attributed to VN) and the BL2 band with a maximum at 3.0 eV and the ZPL at 3.33 eV (attributed to a defect complex involving hydrogen) are observed. We also conclude that the gallium vacancy-related defects act as centers of nonradiative recombination

Localized Electron States Near a Metal-Semiconductor Nanocontact

The electronic structure of nanowires in contact with metallic electrodes of experimentally relevant sizes is calculated by incorporating the electrostatic polarization potential into the atomistic single particle Schr\"odinger equation. We show that the presence of an electrode produces localized electron/hole states near the electrode, a phenomenon only exhibited in nanostructures and overlooked in the past. This phenomenon will have profound implications on electron transport in such nanosystems. We calculate several electrode/nanowire geometries, with varying contact depths and nanowire radii. We demonstrate the change in the band gap of up to 0.5 eV in 3 nm diameter CdSe nanowires and calculate the magnitude of the applied electric field necessary to overcome the localization.Comment: 11 pages 4 figure

Scattering rates and lifetime of exact and boson excitons

Although excitons are not exact bosons, they are commonly treated as such provided that their composite nature is included in effective scatterings dressed by exchange. We here \emph{prove} that, \emph{whatever these scatterings are}, they cannot give both the scattering rates $T_{ij}^{-1}$ and the exciton lifetime $\tau_0$, correctly: A striking factor 1/2 exists between $\tau_0^{-1}$ and the sum of $T_{ij}^{-1}$'s, which originates from the composite nature of excitons, irretrievably lost when they are bosonized. This result, which appears as very disturbing at first, casts major doubts on bosonization for problems dealing with \emph{interacting} excitons

Identifying ENSO Phase Impacts on Area Yield Insurance Rates: An Application of Non-Parametric Analysis

The paper reports results of non-parametric analysis of peanut, corn, and cotton yield distributions by the ElNino Southern Oscillation (ENSO) phases in the Southeastern U.S. For validation purposes, the historical yield data is complemented by a set of simulated peanut yields generated using daily weather data. The hypothesis, justified by the observed South-Eastern climate differences and research on ENSO cycles and planting dates, is that different climate conditions during ENSO cycles translate into different yield distributions and, therefore, insurance premiums (loss to coverage ratios). Kernel density estimates of historical county yield data show consistent patterns in the actuarially fair rate schedules grouped by ENSO phases and geographical areas. In particular, corn and cotton yield insurance premiums appear to be the most dependent on the ENSO phases and are the highest, regardless of coverage, during ElNino and the lowest during LaNina. Peanut premiums are higher during Neutral years and lowest during LaNina. The results appear to be robust to the transformations used to make the yield series stationary. While these dependencies do not necessarily correspond to the precipitation and solar radiation characteristics of the corresponding ENSO cycles in the Southeastern US, drawing direct analogies with yield variability is premature as many less documented factors, like the spacing of sunny and rainy days, may be just as important. The comparisons of the empirical and simulated peanut yield distributions show that they are similar in many ways and that the dissimilarities can be explained by known factors. These findings should be more relevant for the area yield insurance as opposed to the APH arrangements as the yield data used in designing contracts for the former reflects the systemic risk more influenced by climate than by the farm-level, basis risk factors accommodated in the APH plans.Risk and Uncertainty, Q140, C220, G220,

Fermi-Edge Singularities in the Mesoscopic X-Ray Edge Problem

We study the x-ray edge problem for a chaotic quantum dot or nanoparticle displaying mesoscopic fluctuations. In the bulk, x-ray physics is known to produce deviations from the naively expected photoabsorption cross section in the form of a peaked or rounded edge. For a coherent system with chaotic dynamics, we find substantial changes and in particular that a photoabsorption cross section showing a rounded edge in the bulk will change to a slightly peaked edge on average as the system size is reduced to a mesoscopic (coherent) scale.Comment: 4 pages, 3 figures, final version as published in PR