Experimental verification of a self-consistent theory of the first-, second-, and third-order (non)linear optical response

Abstract

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 two-photon absorption cross-section of the dye AF455 that agrees with 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.

10 pages, 9 figures

References in corpus (4)

• Compact Sum-Over-States Expression without Dipolar Terms for Calculating Nonlinear Susceptibilities
• Fundamental Limits of the Dispersion of the Two-Photon Absorption Cross-Section
• A new dipole-free sum-over-states expression for the second hyperpolarizability
• Monte Carlo Studies of the Fundamental Limits of the Intrinsic Hyperpolarizability

Cited by in corpus (5)

• Physics of the fundamental limits of nonlinear optics: A theoretical perspective
• Applying universal scaling laws to identify the best molecular design paradigms for third-order nonlinear optics
• Applying universal scaling laws to identify the best molecular design paradigms for second-order nonlinear optics
• Using a proxy state to improve the accuracy of truncated hyperpolarizability calculations
• Three-state interactions determine the second-order nonlinear optical response