Pushing the hyperpolarizability to the limit

Abstract

We use numerical optimization to find a one-dimensional potential energy function that yields the largest hyperpolarizability, which we find is within 30% of the fundamental limit. Our results reveal insights into the character of the potential energy functions and wavefunctions that lead to the largest hyperpolarizability. We suggest that donor-acceptor molecules with a conjugated bridge with many sites of reduced conjugation to impart conjugation modulation may be the best paradigm for making materials with huge hyperpolarizabilities that approach the fundamental limit.

4 pages, 3 figures

References in corpus (2)

• Compact Sum-Over-States Expression without Dipolar Terms for Calculating Nonlinear Susceptibilities
• Truncated Sum Rules and their use in Calculating Fundamental Limits of Nonlinear Susceptibilities

Cited by in corpus (23)

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• The influence of geometry and topology of quantum graphs on their nonlinear-optical properties
• The critical role of the energy spectrum in determining the nonlinear-optical response of a quantum system
• Monte Carlo Studies of the Intrinsic Second Hyperpolarizability
• Geometry-Controlled Nonlinear Optical Response of Quantum Graphs
• The paradox of the many-state catastrophe of fundamental limits and the three-state conjecture
• Physics of the fundamental limits of nonlinear optics: A theoretical perspective
• Dressed quantum graphs with optical nonlinearities approaching the fundamental limit
• The effect of extreme confinement on the nonlinear-optical response of quantum wires
• A quantum mechanical model of the upper bounds of the cascading contribution to the second hyperpolarizability
• A bird's-eye view of nonlinear-optical processes: unification through scale invariance
• Lowest-order relativistic corrections to the fundamental limits of nonlinear-optical coefficients
• Optimization of eigenstates and spectra for quasi-linear nonlinear optical systems
• Optimum topology of quasi-one dimensional nonlinear optical quantum systems
• Hybrid quantum systems for enhanced nonlinear optical susceptibilities
• Maximizing the hyperpolarizability of one-dimensional systems
• Scaling and universality in nonlinear optical quantum graphs containing star motifs
• A Heuristic Approach for Treating Pathologies of Truncated Sum Rules in Limit Theory of Nonlinear Susceptibilities
• Polynomial potentials determined from the energy spectrum and transition dipole moments that give the largest hyperpolarizabilities
• Three-state interactions determine the second-order nonlinear optical response