Highly efficient third-order optical nonlinearities in donor-substituted cyanoethynylethene molecules.
We investigated the third-order nonlinear optical properties of several donor-substituted cyanoethynylethene molecules in the zero-frequency limit. We observed nonlinearities that are extraordinarily large relative to the small molecular mass of these molecules and that are within a factor of 50 from the fundamental limit. At a wavelength of 1.5 microm, the rotational average of the third-order molecular polarizability is 53 +/- 13 x 10(-48) m5 V(-2) (3.8 x 10(-33) esu) for the best molecule, which corresponds to 1.7 x 10(-48) m5 V(-2) per delocalized electron. The high nonlinear efficiency of these molecules is due to the compact two-dimensional conjugated system and the effective donor-acceptor substitution patterns.
May
Joshua C
JC
Department of Physics and Center for Optical Technologies, Lehigh University, Bethlehem, Pennsylvania 18015, USA.
Lim
Jin H
JH
Biaggio
Ivan
I
Moonen
Nicolle N P
NN
Michinobu
Tsuyoshi
T
Diederich
François
F