Two-photon absorption in linear bis-dioxaborine compounds-the impact of correlation-induced oscillator-strength redistribution.
Quantum-chemical calculations of the two-photon absorption (TPA) cross-sections are used to determine the characteristics of the electronic excited states responsible for the observed peaks in the TPA spectra of two bis-dioxaborine-substituted biphenyl derivatives. We find two distinct TPA-active states with very different TPA cross-sections: the difference is explained on the basis of electron correlation. These effects, on the one hand, lead to TPA cross-sections of up to 500 x 10(-50) cm4 s photon(-1) for the state favored by correlation; on the other hand, they limit the overall cross-sections achievable in this class of materials.
Zojer
Egbert
E
Department of Chemistry, University of Arizona, Tucson 85721-0041, USA. egbert.zojer@chemistry.gatech.edu
Wenseleers
Wim
W
Halik
Marcus
M
Grasso
Cara
C
Barlow
Stephen
S
Perry
Joseph W
JW
Marder
Seth R
SR
Brédas
Jean-Luc
JL