Inorganic Chemistry
Inorganic Chemistry
5 years ago

Organoimido-Polyoxometalate Nonlinear Optical Chromophores: A Structural, Spectroscopic, and Computational Study

Organoimido-Polyoxometalate Nonlinear Optical Chromophores: A Structural, Spectroscopic, and Computational Study
Koen Clays, Hani El Moll, Joseph A. Wright, Karen Faulds, Bruce S. Brunschwig, John Fielden, Ahmed Al-Yasari, Hayleigh Kearns, Nick Van Steerteghem
Donor-functionalized organoimido-polyoxometalates are efficient quadratic nonlinear optical (NLO) materials. With short (phenyl) π-bridges, hyper-Rayleigh scattering (HRS) β0 values break empirical performance limits for planar organic chromophores, but extended π-conjugation loses this advantage. Stark-derived dipole moment changes (versus nitro analogues) and density functional theory (DFT) calculations suggest this results from charge transfer to the POM with short π-bridges, but to the POM and imido ring in extended systems. Donor-free systems are NLO inactive, as their electronic transitions lack sufficient dipolar charge transfer character.

Publisher URL: http://dx.doi.org/10.1021/acs.inorgchem.7b00708

DOI: 10.1021/acs.inorgchem.7b00708

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