8,476 research outputs found

    Demonstrating that the non orthogonal orbital optimized coupled cluster model converges to full configuration interaction

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    Coupled cluster (CC) methods are among the most accurate methods in quantum chemistry. However, the standard CC linear response formulation is not gauge invariant resulting in errors when modelling properties like optical rotation and electron circular dichroism. Including an explicit unitary orbital rotation in the CC Lagrangian makes the linear response function gauge invariant, but the resulting models are not equivalent to full configuration interaction (FCI) in the untruncated limit. In this contribution, such methods are briefly discussed and it is demonstrated that methods using a nonorthogonal orbital transformation, such as nonorthogonal orbital optimized CC (NOCC), can converge to FCI in the untruncated limit. This has been disputed in the literature.Comment: 18 page

    Advanced 30/20 GHz multiple-beam antennas for communications satellites

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    Design concepts under development utilize two separate spacecraft antenna systems, one uplink at 30 GHz and the other a downlink at 20 GHz, where each antenna provides multiple fixed and scanning beams. Two contractors completed configuration trade-off studies and breadboarding of critical technology components, and are fabricating and testing proof-of-concept (POC) models to demonstrate the technology feasibility. Technology developments required for the proposed systems are presented, along with each contractor's progress to date. The technology development areas discussed include: (1) offset Cassegrain and shaped reflector systems for narrow beams with low sidelobes and wideangle off-axis scan; (2) diplexed beam-forming networks for dual polarization, low sidelobes, and fixed and scan-beam operation; (3) fast switching networks for scanning beams; and (4) fabrication of precision feed components and large offset reflectors

    Crossing conditions in coupled cluster theory

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    We derive the crossing conditions at conical intersections between electronic states in coupled cluster theory, and show that if the coupled cluster Jacobian matrix is nondefective, two (three) independent conditions are correctly placed on the nuclear degrees of freedom for an inherently real (complex) Hamiltonian. Calculations using coupled cluster theory on an 21A/31A2 {^{1}}A' / 3 {^{1}}A' conical intersection in hypofluorous acid illustrate the nonphysical artifacts associated with defects at accidental same-symmetry intersections. In particular, the observed intersection seam is folded about a space of the correct dimensionality, indicating that minor modifications to the theory are required for it to provide a correct description of conical intersections in general. We find that an accidental symmetry allowed 11A"/21A"1 {^{1}}A" / 2 {^{1}}A" intersection in hydrogen sulfide is properly described, showing no artifacts as well as linearity of the energy gap to first order in the branching plane.Comment: 9 pages and 4 figure

    Extensive reduction of surface UV radiation since 1750 in world's populated regions

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    Human activity influences a wide range of components that affect the surface UV radiation levels, among them ozone at high latitudes. We calculate the effect of human-induced changes in the surface erythemally weighted ultra-violet radiation (UV-E) since 1750. We compare results from a radiative transfer model to surface UV-E radiation for year 2000 derived by satellite observations (from Total Ozone Mapping Spectroradiometer) and to ground based measurements at 14 sites. The model correlates well with the observations; the correlation coefficients are 0.97 and 0.98 for satellite and ground based measurements, respectively. In addition to the effect of changes in ozone, we also investigate the effect of changes in SO<sub>2</sub>, NO<sub>2</sub>, the direct and indirect effects of aerosols, albedo changes and aviation-induced contrails and cirrus. The results show an increase of surface UV-E in polar regions, most strongly in the Southern Hemisphere. Furthermore, our study also shows an extensive surface UV-E reduction over most land areas; a reduction up to 20% since 1750 is found in some industrialized regions. This reduction in UV-E over the industrial period is particularly large in highly populated regions

    Combined observational and modeling based study of the aerosol indirect effect

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    International audienceThe indirect effect of aerosols via liquid clouds is investigated by comparing aerosol and cloud characteristics from the Global Climate Model CAM-Oslo to those observed by the MODIS instrument onboard the TERRA and AQUA satellites http://modis.gsfc.nasa.gov). The comparison is carried out for 15 selected regions ranging from remote and clean to densely populated and polluted. For each region, the regression coefficient and correlation coefficient for the following parameters are calculated: Aerosol Optical Depth vs. Liquid Cloud Optical Thickness, Aerosol Optical Depth vs. Liquid Cloud Droplet Effective Radius and Aerosol Optical Depth vs. Cloud Liquid Water Path. Modeled and observed correlation coefficients and regression coefficients are then compared for a 3-year period starting in January 2001. Additionally, global maps for a number of aerosol and cloud parameters crucial for the understanding of the aerosol indirect effect are compared for the same period of time. Significant differences are found between MODIS and CAM-Oslo both in the regional and global comparison. However, both the model and the observations show a positive correlation between Aerosol Optical Depth and Cloud Optical Depth in practically all regions and for all seasons, in agreement with the current understanding of aerosol-cloud interactions. The correlation between Aerosol Optical Depth and Liquid Cloud Droplet Effective Radius is variable both in the model and the observations. However, the model reports the expected negative correlation more often than the MODIS data. Aerosol Optical Depth is overall positively correlated to Cloud Liquid Water Path both in the model and the observations, with a few regional exceptions

    Modelling of nitrate particles: importance of sea salt

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    International audienceA thermo dynamical model for treatment of gas/aerosol partitioning of semi volatile inorganic aerosols has been implemented in a global chemistry and aerosol transport model (Oslo CTM2). The sulphur cycle and sea salt particles have been implemented earlier in the Oslo CTM2 and the focus of this study is on whether nitrate particles are formed as fine mode ammonium nitrate or react on existing sea salt particles. The model results show that ammonium nitrate particles play a non-negligible role in the total aerosol composition in certain industrialized regions and therefore have a significant local radiative forcing. On a global scale the aerosol optical depth of ammonium nitrate is relatively small due to limited availability of ammonia and reaction with sea salt particles. Inclusion of sea salt in the calculations reduces the aerosol optical depth and burden of ammonium nitrate particles by 25% on a global scale but with large regional variations
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