| 1. |
- Jonsson, D., et al.
(författare)
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Excited state polarizabilities in solution obtained by cubic response theory : Calculations on para-, ortho-, and meta-nitroaniline
- 1998
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Ingår i: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 109:15, s. 6351-6357
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Tidskriftsartikel (refereegranskat)abstract
- We show that response theory implemented with a self-consistent reaction field theory model is a viable approach to simulate excited state polarizabilities of molecules in solution. The excited state polarizabilities are in this approach given by the double residue of the ground state cubic response functions, accounting for both equilibrium and nonequilibrium contributions to the interaction with the outer medium. The effects of the inertial polarization of the solvent on the polarizabilities of the solutes are shown to strongly depend on the solvent configuration, whether the solvent is in equilibrium or in nonequilibrium with the charge distribution of the investigated compound. The inertial polarization vector in the nonequilibrium solvent configuration represents the equilibrated solvent configuration when solvating the ground state of the solute. This inertial polarization vector is not in equilibrium with any of the excited states and therefore one observes a rather different behavior between nonequilibrium and equilibrium solvent descriptions of the solute. Illustrative calculations are presented for para-, meta-, and ortho-nitroanilines in gas and solution phases. Results have been compared with experimental data where available. © 1998 American Institute of Physics.
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| 2. |
- Luo, Y., et al.
(författare)
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Dielectric and optical properties of pure liquids by means of ab initio reaction field theory
- 1998
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Ingår i: Physical Review E. Statistical, Nonlinear, and Soft Matter Physics. - : American Physical Society (APS). - 1063-651X .- 1095-3787. ; 57:4, s. 4778-4785
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Tidskriftsartikel (refereegranskat)abstract
- A general Onsager-type reaction field theory approach for simulating dielectric and optical properties is proposed, thereby giving a unified description for both macroscopic and microscopic properties of pure liquids. A demonstration is given for ab initio computations of the refractive index, the density fluctuation of the refractive index, and the local field factors of benzene and acetonitrile in the liquid phase, showing good agreement with available experimental data.
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| 3. |
- Norman, P., et al.
(författare)
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Hyperpolarizability depolarization ratios of nitroanilines
- 1997
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Ingår i: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 107:21, s. 9063-9066
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Tidskriftsartikel (refereegranskat)abstract
- The depolarization ratios for the first hyperpolarizabilities of para-, meta-, and ortho-nitroanilines have been calculated in gas and solution phases. The results resolve ambiguities in the interpretation of experimental results for these quantities, and pinpoint the actual problems in previous simulations. It is argued that extraction of individual components of β of low symmetry molecules from experimental depolarization measurements alone is difficult, and that the support from simulations to extract the proper information is indispensable in most cases.
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| 4. |
- Sylvester-Hvid, K. O., et al.
(författare)
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Cubic optical response of molecules in a nonequilibrium and equilibrium solvation model
- 1999
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Ingår i: Journal of Physical Chemistry A. - : American Chemical Society (ACS). - 1089-5639 .- 1520-5215. ; 103:42, s. 8375-8383
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Tidskriftsartikel (refereegranskat)abstract
- The cubic response equations governing nonequilibrium and equilibrium solvation in the continuum approach are derived and implemented. We consider solvent effects on the frequency dependent second hyperpolarizability. We illustrate the effects of optical and static dielectric constants through sample calculations on H2O and H2CO.
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| 5. |
- Sylvester-Hvid, K. O., et al.
(författare)
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Nonlinear optical response of molecules in a nonequilibrium solvation model
- 1998
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Ingår i: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 109:13, s. 5576-5584
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Tidskriftsartikel (refereegranskat)abstract
- The response equations governing nonequilibrium solvation in the continuum approach are derived and implemented for second order in response theory. Applications to a simple benchmark system consisting of a solvated water molecule are presented. We consider the role of nonequilibrium solvent configurations on the first hyperpolarizability. Effects of solvation parameters, such as optical and static dielectric constants, and frequency dispersion are discussed.
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| 6. |
- Sylvester-Hvid, K. O., et al.
(författare)
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Sign change of hyperpolarizabilities of solvated water, revised : Effects of equilibrium and nonequilibrium solvation
- 2004
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Ingår i: Journal of Physical Chemistry A. - : American Chemical Society (ACS). - 1089-5639 .- 1520-5215. ; 108:41, s. 8961-8965
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Tidskriftsartikel (refereegranskat)abstract
- The second harmonic and electro-optical responses for the water molecule in its liquid state are theoretically revised. The continuum, semicontinuum, and supermolecular solvation models are employed using quadratic response theory at the Hartree-Fock level, either in the equilibrium or nonequilibrium implementation. The experimentally observed sign change of the second harmonic response of water on liquefaction is reproduced using the supermolecular and semicontinuum model for both equilibrium and nonequilibrium solvation. The conclusions of a previous study, which rested upon linear response theory in an equilibrium implementation, are confirmed. Also, the assumption of Kleinman symmetry and dispersion is addressed.
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| 7. |
- 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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