An investigation was made of nonlinear optical properties of Langmuir-
Blodgett films of rhodamine B and rhodamine 6G on hydrophilic and hydr
ophobic substrates. Second-harmonic generation showed that more homoge
neous films were formed on hydrophilic substrates. Quantum-chemical ca
lculations of molecular hyperpolarisabilities, carried out subject to
absorption at the second-harmonic frequency, made it possible to deter
mine (on the basis of a proposed model) the orientation of molecules a
nd quadratic susceptibilities of films, which were in satisfactory agr
eement with the experimental results.