Nonlinear properties of one-dimensional organic molecular aggregates in
nanometer films
Roman V. Markov1 (

), A. I. Plekhanov
1,
Z. M. Ivanova
2, V. V. Shelkovnikov
2
1Institute of Automation and Electrometry SB RAS, Novosibirsk,
Russia.
2Novosibirsk Institute of Organic Chemistry, Novosibirsk, Russia.
Low-dimensional molecular J-aggregates are extensively studied during past
decades. The interest is caused by the unique nonlinear optical properties of
these systems. The J-aggregates possess extremely high value of nonlinear
susceptibility of third order with picosecond relaxation time. That makes this
materials perspective for photonics and optical communication. The unique
properties of the J-aggregates are explained by the delocalization of an
excitation in an aggregate. However, the nature of the extremely high
nonlinear susceptibility and its relation with excitation delocalization were
not experimentally tested yet.
Molecular aggregates of pseudoisocyanine with various width of a distinctive
absorption line were obtained in thin (15nm) films on glass substrates (30x30
mm). These films possess a giant optical nonlinearity of third order and high
photochemical stability at the room conditions. Exciton delocalization length
was derived from absorption line width that is attributed to a mixing of
lowest exciton band states. Nonlinear optical susceptibility of third order
within resonance absorption band was measured by Z-scan and Pump-Probe
techniques. Experimental results reveal a scaling dependence of the nonlinear
optical susceptibility versus the exciton delocalization length, with a power
factor about 2.3. This result coincides with the theoretical prediction for
the phenomenon of size enhancement.
High optical quality of the obtained film surfaces makes them perspective for
applications as two-dimensional optical switches.