Journal article
Fundamental limits of all nonlinear-optical phenomena that are representable by a second-order nonlinear susceptibility
The Journal of chemical physics, Vol.125(15), pp.154108-154108-10
10/21/2006
Handle:
https://hdl.handle.net/2376/108169
PMID: 17059240
Abstract
Applying the three-level ansatz and the sum rules to the new dipole-free sum-over-states expression, we develop a rigorous method for calculating the fundamental limits of the dispersion of the real and imaginary parts of the second-order electronic nonlinear-optical susceptibilities. These results can be applied to all orders of nonlinearity, hence can be used to study any nonlinear-optical phenomena at any wavelength. The theory can be used to understand how strongly light interacts with matter and can be applied to optimizing a material's properties for applications. In particular, we find that the resonant first hyperpolarizability peaks when the energy difference between excited states is small. In contrast, the maximal off-resonance hyperpolarizability requires the excited states to be well separated. Therefore, one molecular design strategy does not fit all applications.
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Details
- Title
- Fundamental limits of all nonlinear-optical phenomena that are representable by a second-order nonlinear susceptibility
- Creators
- Mark G Kuzyk - Department of Physics and Astronomy, Washington State University, Pullman, Washington 99164-2814, USA. kuz@wsu.edu
- Publication Details
- The Journal of chemical physics, Vol.125(15), pp.154108-154108-10
- Academic Unit
- Physics and Astronomy, Department of
- Publisher
- United States
- Identifiers
- 99900547316901842
- Language
- English
- Resource Type
- Journal article