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| 2. |
- Aidas, Kestutis, et al.
(författare)
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The Dalton quantum chemistry program system
- 2014
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Ingår i: WIREs Computational Molecular Science. - : Wiley. - 1759-0876 .- 1759-0884. ; 4:3, s. 269-284
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Tidskriftsartikel (refereegranskat)abstract
- Dalton is a powerful general-purpose program system for the study of molecular electronic structure at the Hartree-Fock, Kohn-Sham, multiconfigurational self-consistent-field, MOller-Plesset, configuration-interaction, and coupled-cluster levels of theory. Apart from the total energy, a wide variety of molecular properties may be calculated using these electronic-structure models. Molecular gradients and Hessians are available for geometry optimizations, molecular dynamics, and vibrational studies, whereas magnetic resonance and optical activity can be studied in a gauge-origin-invariant manner. Frequency-dependent molecular properties can be calculated using linear, quadratic, and cubic response theory. A large number of singlet and triplet perturbation operators are available for the study of one-, two-, and three-photon processes. Environmental effects may be included using various dielectric-medium and quantum-mechanics/molecular-mechanics models. Large molecules may be studied using linear-scaling and massively parallel algorithms. Dalton is distributed at no cost from for a number of UNIX platforms.
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| 4. |
- Gozem, Samer, et al.
(författare)
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Dynamic Electron Correlation Effects on the Ground State Potential Energy Surface of a Retinal Chromophore Model
- 2012
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Ingår i: Journal of Chemical Theory and Computation. - : American Chemical Society (ACS). - 1549-9618 .- 1549-9626. ; 8:11, s. 4069-4080
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Tidskriftsartikel (refereegranskat)abstract
- The ground state potential energy surface of the retinal chromophore of visual pigments (e.g., bovine rhodopsin) features a low-lying conical intersection surrounded by regions with variable charge-transfer and diradical electronic structures. This implies that dynamic electron correlation may have a large effect on the shape of the force fields driving its reactivity. To investigate this effect, we focus on mapping the potential energy for three paths located along the ground state CASSCF potential energy surface of the penta-2,4-dieniminium cation taken as a minimal model of the retinal chromophore. The first path spans the bond length alternation coordinate and intercepts a conical intersection point. The other two are minimum energy paths along two distinct but kinetically competitive thermal isomerization coordinates. We show that the effect of introducing the missing dynamic electron correlation variationally (with MRCISD) and perturbatively (with the CASPT2, NEVPT2, and XMCQDPT2 methods) leads, invariably, to a stabilization of the regions with charge transfer character and to a significant reshaping of the reference CASSCF potential energy surface and suggesting a change in the dominating isomerization mechanism. The possible impact of such a correction on the photoisomerization of the retinal chromophore is discussed.
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| 5. |
- Gozem, Samer, et al.
(författare)
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Shape of Multireference, Equation-of-Motion Coupled-Cluster, and Density Functional Theory Potential Energy Surfaces at a Conical Intersection
- 2014
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Ingår i: Journal of Chemical Theory and Computation. - : American Chemical Society (ACS). - 1549-9618 .- 1549-9626. ; 10:8, s. 3074-3084
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Tidskriftsartikel (refereegranskat)abstract
- We report and characterize ground-state and excited-state potential energy profiles using a variety of electronic structure methods along a loop lying on the branching plane associated with a conical intersection (Cl) of a reduced retinal model, the penta-2,4-dieniminium cation (PSB3). Whereas the performance of the equation-of-motion coupled-duster, density functional theory, and multireference methods had been tested along the excited- and ground-state paths of PSB3 in our earlier work, the ability of these methods to correctly describe the potential energy surface shape along a CI branching plane has not yet been investigated. This is the focus of the present contribution. We find, in agreement with earlier studies by others, that standard time-dependent DFT (TDDFT) does not yield the correct two-dimensional (i.e., conical) crossing along the branching plane but rather a one-dimensional (i.e., linear) crossing along the same plane. The same type of behavior is found for SS-CASPT2(IPEA=0), SS-CASPT2(IPEA=0.25), spin-projected SF-TDDFT, EOM-SF-CCSD, and, finally, for the reference MRCISD+Q method. In contrast, we found that MRCISD, CASSCF, MS-CASPT2(IPEA=0), MS-CASPT2(IPEA=0.25), XMCQDPT2, QD-NEVPT2, non-spin-projected SF-TDDFT, and SI-SA-REKS yield the expected conical crossing. To assess the effect of the different crossing topologies (i.e., linear or conical) on the PSB3 photoisomerization efficiency, we discuss the results of 100 semiclassical trajectories computed by CASSCF and SS-CASPT2(IPEA=0.25) for a PSB3 derivative. We show that for the same initial conditions, the two methods yield similar dynamics leading to isomerization quantum yields that differ by only a few percent.
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| 6. |
- Laguardia, L., et al.
(författare)
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Formation of dust in low-pressure magnetized hydrocarbon plasmas
- 2011
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Ingår i: New Journal of Physics. - : IOP Publishing. - 1367-2630. ; 13, s. 063006-
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Tidskriftsartikel (refereegranskat)abstract
- The rapid formation of large molecules and the subsequent production of solid-state dust particles in a low-pressure discharge is unlikely, because of the low rates of the polymerization reactions and short lifetimes of the species. Here, we suggest that C dust particles can form in atypically low (10(-3) mbar)-pressure hydrocarbon plasmas if the dust charging time is much shorter than the gas residence time in the device; we present supporting experimental evidence for this. Such a condition can be obtained by the production of high-density plasmas. The results show that dust formation from the gaseous phase can occur in a much wider parameter range than is commonly assumed.
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| 7. |
- Ratynskaiy, Svetlana, et al.
(författare)
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Plasma fluctuation spectra as a diagnostic tool for submicron dust
- 2010
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Ingår i: Physics of Plasmas. - : AIP Publishing. - 1070-664X .- 1089-7674. ; 17:4, s. 043703-
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Tidskriftsartikel (refereegranskat)abstract
- It is shown that the measurements of density fluctuation spectra in dusty plasmas can constitute a basis for in situ diagnostic of invisible submicron dust. The self-consistent kinetic theory that includes the charging processes and the natural density fluctuations of the dust particles predicts modifications of the spectra due to the presence of dust. A laboratory experiment was carried out where submicron dust was produced in a gas phase and diagnosed by surface analysis of samples and by measurements of its influence on the plasma density fluctuation spectra. Quantitative comparison of the latter with the theory yields information on dust density, size, and distribution in agreement with the results of the surface analysis. The method can be applied to various plasma environments in laboratory and space.
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| 8. |
- Ratynskaya, Svetlana, et al.
(författare)
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Dust-surface collisions in adhesion regime for tokamak relevant materials
- 2013
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Ingår i: Journal of Nuclear Materials. - : Elsevier BV. - 0022-3115 .- 1873-4820. ; 438:Suppl., s. S796-S799
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Tidskriftsartikel (refereegranskat)abstract
- Empirical studies of dust-surface collisions for metal and carbon projectiles impacting on metal targets in the velocity range from a few m/s to those in excess of 1 km/s have been carried out with the use of a modified pellet injection system. The selected projectile/target shapes, sizes and materials are mimicking the scenario of dust colliding with plasma facing components (PFCs) of a metal machine. The low velocities (10's m/s) reported here, characteristic for dust motion in tokamak scrape-off layer plasmas, are in the range of sticking phenomenon; the critical velocity and size for bouncing off are essential and timely inputs for the dust dynamics codes and statistical models aiming to predict dust transport and redepo-sition on PFCs.
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