Non-linear optical properties of molecules in heterogeneous environments: a quadratic density functional/molecular mechanics response theory
2014 (English)In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 16, no 19, 8981-8989 p.Article in journal (Refereed) Published
We generalize a density functional theory/molecular mechanics approach for heterogeneous environments with an implementation of quadratic response theory. The updated methodology allows us to address a variety of non-linear optical, magnetic and mixed properties of molecular species in complex environments, such as combined metallic, solvent and confined organic environments. Illustrating calculations of para-nitroaniline on gold surfaces and in solution reveals a number of aspects that come into play when analyzing second harmonic generation of such systems - such as surface charge flow, coupled surface-solvent dynamics and induced geometric and electronic structure effects of the adsorbate. Some ramifications of the methodology for applied studies are discussed.
Place, publisher, year, edition, pages
Royal Society of Chemistry, 2014. Vol. 16, no 19, 8981-8989 p.
Enhanced Raman-Scattering, Para-Nitroaniline, 2nd-Harmonic Generation, Force-Fields, Hyperpolarizabilities, Polarizabilities, Nanoclusters, Model
Other Physics Topics Other Chemistry Topics
IdentifiersURN: urn:nbn:se:kth:diva-145620DOI: 10.1039/c4cp00992dISI: 000335015700033ScopusID: 2-s2.0-84898812949OAI: oai:DiVA.org:kth-145620DiVA: diva2:719109
FunderSwedish e‐Science Research Center
QC 201405232014-05-232014-05-232014-08-26Bibliographically approved