Non-linear optical properties of molecules in heterogeneous environments: a quadratic density functional/molecular mechanics response theory.
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.
Division of Theoretical Chemistry & Biology, School of Biotechnology, KTH Royal Institute of Technology, S-106 91 Stockholm, Sweden. rinkevic@kth.se.
Zilvinas
Z
Rinkevicius
Xin
X
Li
Jaime A R
JA
Sandberg
Hans
H
Ågren
D017711:Nonlinear Dynamics; D055620:Optical Phenomena; D011789:Quantum Theory