Exact limits in nonlinear optics
We determined the exact fundamental limits in nonlinear optics by modifying the statistical (Monte Carlo) computation of the first and second hyperpolarizabilities to ensure that the spectra and transition moments satisfied all of the sum rules. The figure shows the change in the distribution of the second hyperpolarizability with the X parameter of the molecule when the new theory is applied. This is a new design rule for all-optical molecular materials and devices.
“Exact fundamental limits of the first and second hyperpolarizabilities", Rick Lytel, Sean Mossman, Ethan Crowell, and Mark G. Kuzyk, Phys. Rev. Lett. 119, 073902 (2017).
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