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Analytic ab initio calculations of coherent anti-Stokes Raman scattering (CARS)
KTH, School of Biotechnology (BIO), Theoretical Chemistry.ORCID iD: 0000-0002-1763-9383
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2009 (English)In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 11, no 13, 2293-2304 p.Article in journal (Refereed) Published
Abstract [en]

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.

Place, publisher, year, edition, pages
2009. Vol. 11, no 13, 2293-2304 p.
Keyword [en]
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
URN: urn:nbn:se:kth:diva-18259DOI: 10.1039/b812045eISI: 000264374700019ScopusID: 2-s2.0-63049097825OAI: diva2:336305
QC 20100525Available from: 2010-08-05 Created: 2010-08-05 Last updated: 2011-01-24Bibliographically approved

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