Abstract

The search for new materials with ever-larger nonlinear-optical susceptibility is fueled by the promise of new applications. While much progress has been made, no new paradigms have been discovered that lead to significantly larger nonlinear susceptibilities when size has been taken into account. The next breakthrough requires a step back to consider the fundamental requirements for increasing the strength of light–matter interactions. In essence, the problem at hand is to understand how to get the most out of a system of fixed size (defined as the spread in the electronic wave function) that contains a given number of electrons. The intrinsic nonlinearity takes into account size so that the origin of what makes a large nonlinear response can be identified. Only then can a recipe be articulated for making the system larger in a way that scales optimally so that ultralarge nonlinear susceptibilities can become a reality.

© 2016 Optical Society of America

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