Experimental verification of a self-consistent theory of the first-, second-, and third-order (non)linear optical response
- Department of Chemistry, University of Leuven, Celestijnenlaan 200D, B-3001 Leuven (Belgium)
We show that a combination of linear absorption spectroscopy, hyper-Rayleigh scattering, and a theoretical analysis using sum rules to reduce the size of the parameter space leads to a prediction of the imaginary part of the second hyperpolarizability of the dye AF-455 that agrees with the experimental data gathered through two-photon absorption spectroscopy. Our procedure, which demands self-consistency between several measurement techniques and does not use adjustable parameters, provides a means for determining transition moments between the dominant excited states based strictly on experimental characterization. This is made possible by our new approach that uses sum rules and molecular symmetry to rigorously reduce the number of required physical quantities.
- OSTI ID:
- 22072202
- Journal Information:
- Physical Review. A, Vol. 84, Issue 3; Other Information: (c) 2011 American Institute of Physics; Country of input: International Atomic Energy Agency (IAEA); ISSN 1050-2947
- Country of Publication:
- United States
- Language:
- English
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