Search: id:"swepub:oai:DiVA.org:kth-18259" >
Analytic ab initio ...
Analytic ab initio calculations of coherent anti-Stokes Raman scattering (CARS)
-
Thorvaldsen, Andreas J. (author)
-
Ferrighi, Lara (author)
-
Ruud, Kenneth (author)
-
show more...
-
- Ågren, Hans (author)
- KTH,Teoretisk kemi
-
Coriani, Sonia (author)
-
Jorgensen, Poul (author)
-
show less...
-
(creator_code:org_t)
- Royal Society of Chemistry (RSC), 2009
- 2009
- English.
-
In: Physical Chemistry, Chemical Physics - PCCP. - : Royal Society of Chemistry (RSC). - 1463-9076 .- 1463-9084. ; 11:13, s. 2293-2304
- Related links:
-
https://urn.kb.se/re...
-
show more...
-
https://doi.org/10.1...
-
show less...
Abstract
Subject headings
Close
- We present a theory for the analytic calculation of frequency-dependent polarizability gradients, and apply the methodology to the calculation of coherent anti-Stokes Raman scattering (CARS). The formalism used is based on an open-ended theory for the calculation of frequency-dependent molecular response properties of arbitrary order, also including contributions from perturbation-dependent basis sets. An important feature of our approach is the close connection between the formalism-which is fully matrix-based in an atomic orbital basis-and the implementation, allowing for the rapid implementation of higher-order molecular properties. Care is taken to allow the formalism to be utilized with linearly-scaling Hartree-Fock and density-functional theory codes. By avoiding the evaluation of responses due to geometry distortions, only 9 response equations need to be solved for the calculation of the CARS intensities, independent of the size of the molecular system. The theory is illustrated by calculations on a set of polyaromatic hydrocarbons using a DFT/B3LYP force field and Hartree-Fock polarizability gradients. Good agreement with the experimental CARS spectra of these compounds is obtained.
Keyword
- density-functional theory
- frequency-dependent polarizabilities
- polycyclic aromatic-hydrocarbons
- dynamic dipole polarizabilities
- cluster response theory
- hartree-fock schemes
- perturbation-theory
- excitation-energies
- quasi-energy
- hyperpolarizabilities
Publication and Content Type
- ref (subject category)
- art (subject category)
Find in a library
To the university's database