dorsal/arxiv
View SchemaThe Effects of Geometry on the Hyperpolarizability
| Authors | Mark G. Kuzyk, David S. Watkins |
|---|---|
| Categories | |
| ArXiv ID | physics/0601172 |
| URL | https://arxiv.org/abs/physics/0601172 |
| DOI | 10.1063/1.2205859 |
Abstract
Extensive studies in the past have focused on precise calculations of the nonlinear-optical susceptibility of thousands of molecules. In this work, we use the broader approach of considering how geometry and symmetry alone play a role. We investigate the nonlinear optical response of potential energy functions that are given by a superposition of force centers (representing the nuclear charges) that lie in various planar geometrical arrangements. We find that for certain specific geometries, such as an octupolar-like molecule with donors and acceptors of varying strengths at the branches, the hyperpolarizability is near the {\em fundamental limit}. In these cases, the molecule is observed to be well approximated by a three-level model - consistent with the three-level ansatz previously used to calculate the {\em fundamental limits}. However, when the hyperpolarizability is below the {\em apparent limit} (about a factor of thirty below the {\em fundamental limit}) the system is no longer representable by a three-level model; where both two-level and a many-state models are found to be appropriate, depending on the symmetry.
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"abstract": "Extensive studies in the past have focused on precise calculations of the\nnonlinear-optical susceptibility of thousands of molecules. In this work, we\nuse the broader approach of considering how geometry and symmetry alone play a\nrole. We investigate the nonlinear optical response of potential energy\nfunctions that are given by a superposition of force centers (representing the\nnuclear charges) that lie in various planar geometrical arrangements. We find\nthat for certain specific geometries, such as an octupolar-like molecule with\ndonors and acceptors of varying strengths at the branches, the\nhyperpolarizability is near the {\\em fundamental limit}. In these cases, the\nmolecule is observed to be well approximated by a three-level model -\nconsistent with the three-level ansatz previously used to calculate the {\\em\nfundamental limits}. However, when the hyperpolarizability is below the {\\em\napparent limit} (about a factor of thirty below the {\\em fundamental limit})\nthe system is no longer representable by a three-level model; where both\ntwo-level and a many-state models are found to be appropriate, depending on the\nsymmetry.",
"arxiv_id": "physics/0601172",
"authors": [
"Mark G. Kuzyk",
"David S. Watkins"
],
"categories": [
"physics.optics",
"physics.chem-ph"
],
"doi": "10.1063/1.2205859",
"title": "The Effects of Geometry on the Hyperpolarizability",
"url": "https://arxiv.org/abs/physics/0601172"
},
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