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Hyper-Rayleigh and hyper-Raman scatterings with intermediate and two-photon resonances
Weinan Leng1, Anne Myers Kelley
1School of Natural Sciences, University of California, P.O. Box 2039, Merced, California 95344, USA.
The Journal of Chemical Physics
|November 6, 2007
Summary
Hyper-Raman scattering, a weak process, can be enhanced via two-photon resonance. Surprisingly, adding a one-photon resonance intermediate state did not significantly boost hyperpolarizabilities in organic chromophores.
Area of Science:
- Nonlinear Optics
- Molecular Spectroscopy
- Quantum Chemistry
Background:
- Hyper-Raman scattering is typically a weak nonlinear optical process.
- Two-photon resonant excitation can significantly enhance hyper-Raman scattering.
- Intermediate state resonance is hypothesized to further enhance such processes.
Purpose of the Study:
- To develop the theory of triply resonant hyper-Raman scattering.
- To experimentally investigate the effect of intermediate state resonance on hyperpolarizabilities in organic chromophores.
- To analyze the contributions of different resonant pathways to hyperpolarizability.
Main Methods:
- Theoretical development of triply resonant hyper-Raman scattering.
- Experimental synthesis and characterization of a donor-acceptor substituted push-pull chromophore.
- Solvent tuning to control the energy of the one-photon allowed state.
- Measurement of resonance Raman, hyper-Rayleigh, and hyper-Raman scattering profiles.
Main Results:
- The theory for triply resonant hyper-Raman scattering in organic nonlinear chromophores was established.
- Experimental results for a push-pull chromophore showed that intermediate one-photon resonance did not significantly enhance hyperpolarizabilities.
- Analysis indicated that the triply resonant pathway was not dominant in the studied system.
Conclusions:
- Intermediate state resonance does not necessarily enhance hyper-Raman scattering as expected.
- The dominant contribution to hyperpolarizability in this system arises from non-triply resonant pathways.
- Further research is needed to understand the complex interplay of resonant effects in nonlinear spectroscopy.
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