A discrete interaction model/quantum mechanical method for simulating nonlinear optical properties of molecules near metal surfaces

Autor:	John M. Rinaldi, Seth M. Morton, Lasse Jensen
Rok vydání:	2013
Předmět:	Surface (mathematics) Chemistry Biophysics Interaction model Time-dependent density functional theory Condensed Matter Physics Elementary charge Molecular physics Quantum mechanics Molecule Density functional theory Physical and Theoretical Chemistry Molecular Biology Local field Quantum
Zdroj:	Molecular Physics. 111:1322-1331
ISSN:	1362-3028 0026-8976
DOI:	10.1080/00268976.2013.793419
Popis:	In this work, we extend the discrete interaction model/quantum mechanics (DIM/QM) method to calculate the frequency-dependent hyperpolarisabilities of molecules near metal surfaces. The DIM/QM method is a polarisable quantum mechanics/molecular mechanics method, which represents the metal surface atomistically and thus allows for explicitly modelling the influence of the local environment on the optical properties of a molecule. The interactions between the metal surface and the molecules include both the image field and local field effects. The image field effects arise from the response induced in the metal surface due to the molecule’s electronic charge distributions whereas the local field effects arise from interactions between the metal surface and the external light. The frequency-dependent first-hyperpolarisability is obtained in an efficient way based on time-dependent density functional theory and the (2n+1) rule. The method was tested for calculating the first-hyperpolarisability responsible fo...
Databáze:	OpenAIRE
Externí odkaz:	https://explore.openaire.eu/search/publication?articleId=doi_________::2a1eeafc62d7bad28272a135295dfc44 https://doi.org/10.1080/00268976.2013.793419 Zobrazit plný text záznamu