Title: Why hyperpolarizabilities fall short of the fundamental quantum limits
Authors: Tripathy, K ×
Moreno, JP
Kuzyk, MG
Coe, BJ
Clays, Koen
Kelley, AM #
Issue Date: Jan-2004
Publisher: Amer inst physics
Series Title: Journal of Chemical Physics vol:121 issue:16 pages:7932-7945
Abstract: Quantum sum rules impose limits on the hyperpolarizability, beta. A survey of the largest second-order molecular susceptibilities finds what appears to be a universal gap between the experimental results and the fundamental limits. In this work, we use theory, linear spectroscopy, Raman spectroscopy, and measured values of beta (using hyper-Rayleigh scattering and Stark Spectroscopy) to show that this gap is due to an unfavorable arrangement of excited state energies. The question of whether this result is a universal property of a quantum system or a matter of present paradigms for making molecules is discussed. (C) 2004 American Institute of Physics.
ISSN: 0021-9606
Publication status: published
KU Leuven publication type: IT
Appears in Collections:Molecular Imaging and Photonics
× corresponding author
# (joint) last author

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