Optimization of eigenstates and spectra for quasi-linear nonlinear optical systems

Abstract

Quasi-one-dimensional quantum structures with spectra scaling faster than the square of the eigenmode number (superscaling) can generate intrinsic, off-resonant optical nonlinearities near the fundamental physical limits, independent of the details of the potential energy along the structure. The scaling of spectra is determined by the topology of the structure, while the magnitudes of the transition moments are set by the geometry of the structure. This paper presents a comprehensive study of the geometrical optimization of superscaling quasi-one-dimensional structures and provides heuristics for designing molecules to maximize intrinsic response. A main result is that designers of conjugated structures should attach short side groups at least a third of the way along the bridge, not near its end as is conventionally done. A second result is that once a side group is properly placed, additional side groups do not further enhance the response.

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Cited by in corpus (6)

• Green's function approach for quantum graphs: an overview
• Phase disruption as a new design paradigm for optimizing the nonlinear-optical response
• Physics of the fundamental limits of nonlinear optics: A theoretical perspective
• Polynomial potentials determined from the energy spectrum and transition dipole moments that give the largest hyperpolarizabilities
• General solution to nonlinear optical quantum graphs using Dalgarno-Lewis summation techniques
• Maximizing the hyperpolarizability of 1D potentials with multiple electrons